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D

DIM
COURSES
APPLIED
THERMOLUMINESCENCE
DOSIMETRY
Edited by
M Oberhofer and A Scharmann
Published for the Commission of the European Communities
by Adam Hilger
As the use of nuclear energy
increases, so too does the need for
methods of radiation detection and
dose assessment for a variety of
purposes, the most important being
personnel dosimetry and
environmental monitoring.
Thermoluminescence dosimetry
(TLD) is an important technique in
these areas and has also found
application in a wide range of
different fields in medicine and
biology, and industry and
archaeology.
The present volume, intended to
become the new standard reference
on TLD and its applications, arose out
of two courses held at the Joint
Research Centre, Ispra, in 1977 and
1979. The edited texts of twenty
lectures given by sixteen leading
experts in TLD are presented. The
book is divided into two parts, part I
dealing with fundamentals and part II
with applications.
Part I contains chapters on the
historical development of TLD; theory;
instrumentation; materials and their
properties; measurement; and
comparison of TLD to other solid state
methods in dosimetry. Part II covers
areas of application of TLD including
personnel dosimetry; environmental
monitoring; neutron dosimetry; glow-
curve analysis; medicine; biology
and related fields; high-level photon
dosimetry in industry; reactor
engineering; archaeology; and
dose standardisation and
intercomparison. An appendix is also
included which explains the system
of units adopted recently in radiation
and dosimetry.
Applied Thermoluminescence Dosimetry
Ispra Courses
Applied Thermoluminescence
Dosimetry
Lectures of a course held at the Joint Research Centre,
Ispra, Italy, 12-16 November 1979
EDITED BY M OBERHOFER
AND A SCHARMANN
Published for the Commission of the European Communities by
Adam Hilger Ltd, Bristol
EUftOP. Blblfoth.
ECSC, EEC, EAEC, Brussels and Luxembourg 1981
Published for the Commission of the European Communities,
Directorate-General Information Market and Innovation,
Luxembourg.
EUR 6990 EN
LEGAL NOTICE
Neither the Commission of the European Communities nor any
person acting on behalf of the Commission is responsible for the use
which might be made of the following information.
British Library Cataloguing in Publication Data
Applied thermoluminescence dosimetry.
1. Thermoluminescence - Congresses
I. Oberhofer, M II. Scharmann, A
III. Commission of the European Communities
5 35'.35 QC479
ISBN 0-85274-544-3
All rights reserved. No part of this publication may be reproduced,
stored in a retrieval system or transmitted in any form or by any
means, electronic, mechanical, photocopying, recording or otherwise,
without prior permission of the copyright holder.
Published by Adam Hilger Ltd, Techno House,
Redcliffe Way, Bristol, BS1 6NX.
The Adam Hilger book-publishing imprint is owned by
The Institute of Physics.
Printed in Great Britain by J W Arrowsmith Ltd, Bristol.
Lectures of a course held at the Joint Research Centre of the
Commission of the European Communities, Ispra (Varese), Italy, in
the framework of Ispra Courses.
Contents
List of contributors ix
Preface xi
Part I: Fundamentals
1 History 3
A SCHARMANN
2 Theory
M BOHM AND A SCHARMANN 11
11
11
16
18
21
24
26
30
32
36
39
39
40
48
52
53
64
2.1
2.2
2.3
2.4
2.5
2.6
2.7
2.8
2.9
2.10
Introduction
Excitation by radiation
Thermal excitation and recombination
Phenomenological analysis
Kinetic models
Determination of trap parameters
Additional parameters
Computer simulation
Comparison with experiment
Conclusions
3 Instrumentation
H W JULIUS
3.1
3.2
3.3
3.4
3.5
3.6
Introduction
The heating system
The light detecting system
Special items
TLD readers and systems
Address list
vi Contents
4 Accessory instrumentation 67
M OBERHOFER
67
67
69
70
71
74
74
75
75
76
77
79
80
83
83
83
86
88
89
91
93
94
95
5.10 Tribothermoluminescence (or triboluminescence) 95
6 Preparation and properties of principal TL products 97
G PORTAL
97
97
106
109
111
115
118
123
123
4.1
4.2
4.3
4.4
4.5
4.6
4.7
4.8
4.9
4.10
4.11
4.12
4.13
Introduction
Heating planchets
Gas flushing
Reference light sources
Powder dispensers
Mechanical tweezers
Vacuum tweezers
Sieves
Ultrasonic cleaners
Annealing furnaces
Annealing stands
Irradiators
Literature
5 General characteristics of TL materials
G BUSUOLI
5.1
5.2
5.3
5.4
5.5
5.6
5.7
5.8
5.9
Introduction
Linearity
Response to photons
Response to beta rays
Response to neutrons
Fading
Annealing procedures
Stability and reproducibility
Dose rate dependence
6.1
6.2
6.3
6.4
6.5
6.6
6.7
Introduction
Lithium fluoride
Lithium borate
Beryllium oxide
Calcium fluoride
Calcium sulphate
Aluminium oxide
7 Operational aspects
D F REGULLA
7.1 Introduction
Contents vii
7.2 Parameters affecting precision 124
7.3 Conclusion 140
8 Precision and accuracy of TLD measurements 143
G BUSUOLI
8.1 Introduction 143
8.2 Definitions 143
8.3 Assessment of random and systematic uncertainties 143
8.4 Sources of errors in TLD 145
8.5 Precision of TL measurements 146
8.6 Accuracy of TL measurements 149
8.7 Accuracy in low-dose measurements 150
9 Reference to other solid-state methods 151
E PITT AND A SCHARMANN
9.1 Introduction 151
9.2 Radiophotoluminescence (RPL) 153
9.3 Colouring 155
9.4 Photographic processes 156
9.5 Stimulated exoelectron emission 157
9.6 Track detection 159
9.7 Change of resistance in silicon diodes 161
9.8 Scintillation dosemeter 163
9.9 Conclusions 163
Part II: Applications
10 Application of TLD to personnel dosimetry 167
E PIESCH
10.1 Introduction 167
10.2 Performance specifications 168
10.3 Detector materials and specific requirements 170
10.4 Personnel dosemeter systems 177
10.5 Special applications 182
10.6 Future trends 192
11 Application of TLD systems for environmental monitoring 197
E PIESCH
11.1 Introduction 197
11.2 Performance specifications 198
11.3 Properties of commercial TLD systems 198
viii Contents
11.4 Calibration technique for dosemeter batch and reader 214
11.5 Reproducibility and overall uncertainty of measurement 219
11.6 Interpretation of field exposures 220
11.7 Practical application 224
12 Applications of TL materials in neutron dosimetry 229
J A DOUGLAS
12.1 Introduction 229
12.2 Neutrons and dosimetry 229
12.3 Thermal neutron detectors 232
12.4 Intermediate and fast neutron dosemeters 241
12.5 Possible future developments 253
13 Glow-curve analysis 259
A C LUCAS
13.1 Introduction 259
13.2 Recording of glow curves 259
13.3 Measurement of neutron dose equivalent 261
13.4 Beta-ray measurement 265
13.5 Fading correction 266
13.6 Determination of time from exposure 268
13.7 Verification of data 269
14 Application of TLD in medicine 271
A F McKINLAY
14.1 Radiotherapy measurements 271
14.2 Diagnostic radiology measurements 271
14.3 Factors in the choice of dosemeters for clinical use 273
14.4 Radiotherapy absorbed dose measurements 279
14.5 Examples of the use of TL dosemeters in radiotherapy 283
14.6 Diagnostic radiology absorbed dose measurements 284
15 Application of TLD in biology and related fields 289
M OBERHOFER
15.1 Introduction 289
15.2 Animal experiments 289
15.3 Bone dosimetry 290
15.4 Photon radiation quality measurements 291
15.5 Toxicity determinations 292
15.6 General biology and biochemistry 293
15.7 Ecology 293
15.8 Animal habit studies 295
Contents ix
16 High-level photon dosimetry with TLD materials 297
M OBERHOFER
16.1 Introduction 297
16.2 Lithium fluoride 298
16.3 Lithium borate 306
16.4 Calcium fluoride 308
16.5 Other TLD phosphors 308
16.6 Final remarks 310
17 Application of TLD in reactor engineering 315
JRAL AKEY
17.1 Introduction 315
17.2 A survey of the application of TL in reactor environments 316
17.3 Application to neutron dosimetry 327
17.4 Environmental monitoring 331
17.5 Miscellaneous applications 333
Appendix 17.1 Calculation of gamma photon absorbed dose 333
Appendix 17.2 Cavity ionisation theory 337
Appendix 17.3 The intrinsic TL response per absorbed neutron 340
18 Application of TLD for dating: a review 347
G A WAGNER
18.1 Introduction 347
18.2 Dating method 347
18.3 Dating applications 352
18.4 Conclusion 355
19 TL dating: techniques and problems 361
M J AITKEN
19.1 Introduction 361
19.2 Application 365
19.3 Recent research and outstanding problems 369
20 Application of TL dosemeters in dose standardisation and intercomparison 383
G SCARPA
20.1 Introduction 383
20.2 Dissemination of standards 383
20.3 Direct intercomparison methods 384
20.4 Characteristics of TL dosemeters used for mailed intercomparisons 386
20.5 Practical examples of mailed intercomparisons 386
20.6 Conclusions 390
x Contents
Appendix The new radiological (si) units and their conversion to the units
previously used 39 j
Index
3 9 3
List of contributors
Dr M J Aitken
Research Laboratory for Archaeology and the History of Art,
Oxford University, 6 Keble Road, Oxford 0X1 3QJ, UK
Dr M Bohm
Justus-Liebig-Universitat Giessen,
I Physikalisches Institut,
Heinrich-Buff-Ring 16, D-6300 Giessen, FRG
Dr G Busuoli
Comitato Nazionale per l'Energia Nucleare,
Laboratorio Fisica Sanitaria,
Via Mazzini, 2,1-40138, Bologna, Italy
Dr J A Douglas
Environmental and Medical Sciences Division,
AERE, Harwell, Oxfordshire 0X11 ORA, UK
Dr H W Julius
Radiologische Dienst TNO,
Utrechtsweg 310, N-6812 AR, Arnhem, The Netherlands
Professor J R A Lakey
Department of Nuclear Science and Technology,
Royal Naval College, Greenwich,
London SE10 9NN, UK
Dr A Lucas
Crystal and Electronic Products Department, The Harshaw Chemical Company
6801 Cochran Road, Solon, Ohio 44139, USA
Dr A F McKinlay
National Radiological Protection Board,
Chilton, Didcot, Oxfordshire 0X11 ORQ, UK
xii List of contributors
Dr M Oberhofer
Commission of the European Communities, Joint Research Centre,
Ispra Establishment, Applied Dosimetry Research,
1-21020 Ispra (Varese), Italy
Dipl. Phys. E Piesch
Kernforschungszentrum Karlsruhe GmbH, Hauptabteilung Sicherheit,
Postfach 3640, D-7500 Karlsruhe 1, FRG
Dr E Pitt
Justus-Liebig-Universitat Giessen,
I Physikalisches Institut,
Heinrich-Buff-Ring 16, D-6300 Giessen, FRG
Dr G Portal
Commissariat a l'Energie Atomique,
Institut de Protection et de Surete Nucleaire,
Departement de Protection,
BP No. 6, 92260, Fontenay-aux-Roses, France
Dr D F Regulla
Gesellschaft fur Strahlen- und Umweltforschung mbH Miinchen,
Institut fur Strahlenschutz,
Ingolstadter Landstrasse 1, D-8042 Neuherberg, FRG
Professor G Scarpa
Comitato Nazionale per l'Energia Nucleare,
Centro di Studi Nucleari della Casaccia,
Laboratorio di Dosimetria e Biofisica,
SJ?. Anguillarese km 1 + 300,1-00100 Rome, Italy
Professor Dr A Scharmann
Justus-Liebig-Universitat Giessen,
I Physikalisches Institut,
Heinrich-Buff-Ring 16, D-6300 Giessen, FRG
Dr G A Wagner
Max-Planck-Institut fiir Kernphysik,
Abt. Kosmochemie,
Saupfercheckweg 1, D-6900 Heidelberg 1, FRG
Preface
With the ever increasing use of nuclear energy, particularly for power production, there is
more and more need for radiation detection and dose assessment for a variety of pur-
poses. Two of these are environmental dose control and personnel dose determination.
These types of measurements are essential for ensuring the radiological safety of the
population as a whole and of individual radiation workers. Additionally they may have
great importance with respect to the legal aspects of nuclear energy.
Many radiation detectors and measuring devices have been developed over the last few
decades and some are being used routinely for environmental and personnel dose control.
One of them is based on the fact that some materials emit light when heated after
exposure to radiation. This technique is known as thermoluminescence dosimetry (TLD).
Because of its simplicity and suitability for automation much research and development
work has been put into this type of dosimetry, which has also turned out to be useful in
fields other than radiation protection.
The results of this research and development have been published in different scientific
journals, in various conference proceedings (like the proceedings of the International
Luminescence Meetings at Palo Alto, Gatlinburg, Riso, Krakow and Sao Paulo in 1965,
1968, 1971, 1974 and 1977, respectively), in some books on radiation protection and
solid-state dosimetry and in the only bibliography on the subject by J R Cameron,
N Suntharalingam and G N Kenney, which was published in 1968 by the University
of Wisconsin under the title Thermoluminescent Dosimetry.
According to the authors of this latter publication the book was 'designed to be a
comprehensive introduction to the technique giving much useful information as to
instrumentation, phosphor characteristics and applications'.
For many years this was considered as the standard reference book on the subject and
hence made use of by nearly all students and newcomers to the field. However, for some
years now there has been an increasingly felt need for an up-dated version of the book,
which sadly has not been produced.
Thus the idea was born at the Joint Research Centre (JRC) of the Commission of the
European Communities, Ispra Establishment, to collect all available material in the field
of TLD by organising a course.
Such a course was held within the framework of the Education and Training Program
of the JRC, 14-18 November 1977 in collaboration with the I Physikalisches Institut of
the Justus-Liebig-Universitat, Giessen. From the outset this Institute has contributed to
the understanding of the phenomenon of TL and to the development of TLD and is still
today actively engaged in many aspects of TLD research. Thirteen outstanding experts in
xiv Preface
the field of TLD agreed to present the latest state of the art. The course was such a success
that it was decided to repeat the course with the aim of perfecting the material with
regard to its content and presentation so that it would be suitable for later publication.
Only minor refinements in the course program needed to be made, including the addition
of lectures on subjects which had been missing in the first course, in order to have a com-
plete treatment of the field. The second course was held at the JRC, Ispra, 12-16 Novem-
ber 1979 and the contents now seemed to be worth presenting to a much larger audience
than the one which attended the course.
This book contains all the lectures given at the courses in sequence of their original
presentation with some changes in order to avoid too much overlap and repetition, which
understandably could not be eliminated completely. This was also not desirable in order
not to lose the independent character of each chapter. A number of cross-references have
been inserted into the texts to give maximum information on certain aspects of TLD.
The book starts with the historical development of TLD in chapter 1. In this first
chapter the reader's attention is drawn to the fact that TL is a widespread phenomenon
which has been known for a very long time. Of 3000 minerals, for example, three-quarters
exhibit this effect. The use of TL as a means for measuring radiation exposures or doses
actually started from the observation that many minerals exhibit natural TL and also from
the known uv sensitivity of manganese-activated calcium sulphate. In the late 1940s
much effort was put into the development of suitable TL dosemeters, mostly for military
purposes, and by 1950 many of the TL phosphors presently in use had already been dis-
covered and/or rediscovered for dosimetric applications. During the 1960s a second
generation of materials became available and a wide variety of commercial TLD systems
were developed to more and more sophisticated levels, taking advantage of rapid progress
in computer technology.
In chapter 2 an attempt is made to treat the phenomenon of TL theoretically on the
basis of general physics and with the help of the energy band model of solids. It is shown
that TL intensities can be simulated without any assumptions, but that other properties
of the material of interest need to be studied as well in order to obtain an overall picture
of the electronic processes occurring in the solid.
TLD instrumentation is the subject of chapter 3. The rather simple experimental
devices used for measuring the TL from various phosphors at the very beginning of TL
work have been developed into very sophisticated computerised TL readers which allow
hundreds or even thousands of TL dosemeters to be read fully automatically and also
include data processing. The most important common components of such a TL reader
system are described and examples of commercial instruments are given without going into
details of the electronics. The chapter ends with an address list of TLD instrumentation
manufacturers.
Besides some basic instrumentation, TLD work requires a number of accessories, like
powder dispensers, annealing stands, furnaces, etc, which are the subject of chapter 4.
This completes the instrumental aspects of TLD.
Chapter 5 is dedicated to the general requirements to be fulfilled by TLD materials
when intended to be used as dosemeters, in particular when worn in personal dosemeters.
Among other requirements, those discussed are the sensitivity of the phosphor, its energy
dependence, fading characteristics and the reproducibility obtainable.
There then follows, in chapter 6, a detailed description of each single phosphor of
current interest, starting in each case with a short historical review of its actual role in the
Preface xv
field of TLD. In this chapter the reader is informed about the preparation of the phosphor
and its thermal treatment afterwards, specific models are used to explain the physical
properties like glow curve and emission characteristics, and the actual dosimetric proper-
ties are discussed.
The aim of chapter 7 is to make the user of the materials described in chapter 6
familiar with the possibilities and limits of TL dosimetry. Experimental results obtained
with currently used techniques are reported and analysed to show the sources and magni-
tudes of errors. The author of this chapter shows that, besides the dependence of TL on
the energy and direction of the incident radiation, operational features such as the read-
out device, reading geometry, annealing cycle and dosemeter handling technique may be
major factors influencing the results. At the same time suggestions are made how to
minimise these effects in order to achieve maximum reliability in TL dosimetry.
While the main object of chapter 7 is to make the student familiar with sources of
error in TLD measurements, chapter 8 was written to clarify the difference between
accuracy and precision, to give examples and to show how error analyses are dealt with
mathematically.
Before concluding the first part of the book, reference is made in chapter 9 to other
solid-state methods such as radiophotoluminescence, coloration effects, the photographic
effect, exoelectron emission, track detection, neutron-induced defects and scintillation
which are used with success in the field of dosimetry. It turns out that, compared to all
the other solid-state methods, TLD is the best developed system.
Summarising, one can say that most of the fundamentals of TL which are needed for a
reasonable understanding of this phenomenon, its suitability and its advantages for dosi-
metric applications are discussed in the first part of the book.
The second part of the book has been compiled with the idea of showing where TL
already has been and is being applied successfully. Personnel dosimetry is such a field of
application. The near-tissue equivalence for the detection of photons, the low fading and
the high accuracy of a number of TL materials, coupled with the possibility of evaluating
a large number of dosemeters using automatic reader systems, proved to be very advant-
ageous. In chapter 10 the particular requirements for this field of application are discussed
and a comprehensive survey of TLD systems and dosemeter designs for routine personnel
dose control are given. Future trends of the development in this special field of applica-
tion are indicated.
Environmental monitoring is another application of TLD where interest is growing
rapidly. This subject is treated in chapter 11. TL dosemeters with low fading charac-
teristics, low zero reading and high accuracy are very well suited and mostly much cheaper
than other systems for monitoring the natural radiation background level and short-term
or long-term influences of nuclear installations. Proper individual calibration of the dose-
meters is of prime importance if high accuracy is to be achieved. Thus this chapter con-
tains a short section on calibration techniques.
Much work has also been put into the assessment of neutron doses using TL phosphors.
A review of this work is given in chapter 12.
Some knowledge of the complex processes involved when neutrons interact with
matter is required for a good understanding of the neutron response of TL materials. The
chapter therefore starts with a categorisation of the neutron reactions involved, a dis-
cussion of the appropriate parameters necessary to monitor the effects of neutrons and
some definitions of terms used throughout the chapter. The response of common TL
xvi Preface
materials to thermal neutrons and the factors affecting the measurement are dealt with in
more detail than in earlier chapters.
Methods of separating the- neutron component in a mixed radiation field and of pro-
ducing a high thermal neutron response by mixing a phosphor with non-luminous
6
Li salt
are discussed. Furthermore, techniques for increasing the intermediate and fast neutron
response of phosphors by the use of proton radiators, fission foils and moderators are
surveyed. The practical applications and limitations of these techniques in dosimetry are
assessed and the feasibility of using the neutron activation of a constituent of a phosphor
for dosimetry in therapy work or activity accidents is examined.
Finally, possible future developments in fast neutron dosimetry are considered.
In all cases treated in the last three chapters valuable additional information on the
type of radiation or the time since exposure, for instance, may be obtained from the glow
curves. The importance of this topic is underlined by the insertion into the course of a
lecture on glow-curve analysis, which is reproduced in chapter 13. It is shown there that
various analytical methods exist for complementing internal TL data with glow-curve
shape analysis. The chapter enumerates five such methods.
Many advantages of TLD over other dosimetric methods have favoured its application
in the medical field, where TL dosemeters are often preferred to ionisation dosemeters,
for example, mainly due to their small size and thus ease of placing them singly or in large
numbers within body cavities. The extent to which TL dosemeters are used today in
medicine is shown in chapter 14.
Biology is another field in which TLD has been applied successfully from the beginning.
Although this type of application was not included in the course the subject is treated
briefly, together with related ones, in this book in chapter 15 for the sake of completeness.
The possibility of assessing very high doses of 10
6
R or more with TL phosphors sug-
gests their application for certain dosimetric problems in technological fields (material
testing, electrical component testing, radiation sterilisation, etc), in the chemical indus-
tries (radiation chemistry, cracking of hydrocarbons, polymerisation, vulcanisation of
rubber, etc) and in food processing, for example. In chapter 16 an attempt has been made
to collect TL data relevant to high dose assessment. Some other TL-related phosphor
features, which in some cases may be useful for high dose measurements, have been
included in the text of chapter 16.
There have been a surprisingly large number of applications of TLD in the field of
reactor engineering. The published articles are widely dispersed in the literature and so are
not readily available. This is why this topic is summarised in chapter 17. Many practical
examples are described, such as reactor shield testing, fast reactor core measurements,
reactor gamma-heat measurements, problems associated with reactor neutrons, accumu-
lated activity transfer studies, etc. For a better understanding of certain peculiarities
associated with TLD in reactor engineering three appendices are added. These deal with
the calculation of gamma photon absorbed dose, an introduction to the cavity ionisation
theory and a short description of the intrinsic TL response per absorbed neutron and its
calculation.
In recent years a number of new 'atomic' tools, like radiocarbon dating, neutron
activation analysis and neutron radiography, have enabled archeologists to reveal new data
about ancient civilisations. A 'dating' method has been developed in parallel with these,
which takes advantage of the fact that many materials exist which show TL when exposed
Preface xvii
to radiation. Materials such as rocks, ceramics, slags, bones and meteorites, for instance,
can acquire significant levels of TL from 'natural' radiation. By measuring this TL the
radiation dose can be determined and from that the age of the object can be obtained.
This is the theme of the next two chapters which contain the contents of two unco-
ordinated lectures. Chapter 18, which was presented in the 1979 course, gives a summary
of the subject for the interested reader, while chapter 19, which was in the 1977 course,
gives the more specialised reader full details of the various techniques and their associated
problems. Although there is some overlap and repetition, the editors do not consider this
a drawback bearing in mind the much higher information content of both works taken
together.
The book concludes with a chapter on the applications of TL dosemeters in dose
standardisation and intercomparison. This is a field where TL detectors are increasingly
used as a consequence of the ease with which TL measurements can be performed and
also because their small size is an advantage, especially for postal intercomparisons.
Most authors refer to literature up to mid-1978, though in some instances literature
references up to the 6th International Conference on Solid State Dosimetry in Toulouse,
France, from 1-4 April 1980, have been inserted into the texts during the reviewing
period.
While writing their texts all of the authors were aware of the recent introduction of
the Systeme International d'Unites (si) and of the adoption, by the 10th General Confer-
ence of Weights and Measures, of special names for some units of this system used in the
field of ionising radiation and dosimetry. In spite of this, throughout the book the 'old'
units have been retained, such as the roentgen (R), the rad, the rem and the Curie (Ci).
This is because those units are still widely used and will continue to be used for a while,
together with the new units. They are also retained because many of the graphs selected
by the authors were drawn some time ago using the old units and could not be redrawn
economically and in a reasonable time using the new units. To convert from old to new
units, coulomb per kilogram (Ckg
-1
), gray (Gy), sievert (Sv) and becquerel (Bq), the
reader is referred to the Appendix.
The editors wish to thank all the authors who contributed to the courses and thus to
the realisation of this book. Without their ready acceptance of the invitation to lecture at
the courses and to prepare lecture notes this book could not have been published.
Furthermore, the editors would like to express their gratitude to Mr B Henry, Manager,
Education and Training Program of the JRC, Ispra, who fully supported the course series
and the publication of these proceedings, and to the Ispra Courses Secretarial staff for
their assistance in the organisation of the courses.
We are also grateful to Adam Hilger Ltd, and in particular to its Managing Editor, Mr
K J Hall, for having accepted the material of the courses for publication and for having
prepared an edition, which hopefully will be widely distributed throughout the world.
Ispra Martin Oberhofer
May, 1980 Arthur Scharmann
Part I: Fundamentals
Applied Thermoluminescence Dosimetry. Eds M Oberhofer and A Scharmann
1981 ECSC, EEC, EAEC, Brussels and Luxembourg
1
History
ASCHARMANN
Even prehistoric cavemen probably observed an effect which was surely known to the
medieval alchemists. Certain minerals, such as fluorite, exhibit a transient glow when they
are heated in darkness [1]. This phenomenon, today called thermoluminescence, is the
basis of one of the most important methods of modern integrating dosimetry.
One of the founders of modern chemistry, Sir Robert Boyle, described this effect. On
28 October 1663, he reported to the Royal Society in London the observation of a
strange 'glimmering light' when he warmed a diamond in the dark of his bedroom. He
said: i also brought it to some kind of glimmering light by taking it into bed with me,
and holding it a good while upon a warm part of my naked body'. Boyle also did some
other experiments on the shining of diamonds. He rubbed a diamond on several bodies
and held it near to the flame of a candle or a piece of hot iron.
In 1705 Oldenberg [2] described the phenomenon of thermoluminescence in the
mineral, fluorite. Besides this, other properties of such phosphors were also studied. In
1830 Pearsall [3] gave a description of the effects of electricity upon minerals which
phosphoresce upon heating.
Henri Becquerel [4] described in his work on measurements of infrared spectra in
1883 the effect of thermoluminescence, too: 'En chauffant dans l'obscurite une substance
phosphorescente a longue persistance, prealablement exposee a la lumiere, on voit la
phosphorescence s'aviver, puis s'eteindre ensuite rapidement'. This means: If you heat in
darkness a phosphorescent sample which was previously exposed to light, you can first
see the phosphorescence becoming brighter and then being extinguished rapidly. In this
work he remarked that the influence of red and infrared radiation was the same as that
of a rise in temperature. In 1842, his father E Becquerel [5] had already discovered
a new property of this radiation. The phosphorescence might be destroyed by red or
infrared light. An explanation of these results was given by the later measurements that
he carried out in the following way. Because of the influence of red and infrared radiation
the stored light is released very quickly as luminescence and therefore the usually slow
phosphorescence decay is no longer visible.
The fact that the spectrum consists of a part which leads to a rise in temperature was
found as early as 1800 by William Herschel [6] when he performed the following
experiment. He projected sunlight onto a thermometer bulb and noticed that there was a
different increase of temperature in the different regions of the spectrum. The blue
radiation showed only a small heating effect but, when moving towards the red, the effect
became more pronounced. Even in a region beyond the visible he was able to observe
maxima and minima of the heating effect.
4 A Scharmann
When it was known that there is an invisible region in the spectrum of the Sun beyond
the red, the other end of the spectrum was also examined and UV radiation was discovered
by its property of reducing silver salts (Ritter, Inglefield and Wollaston).
Since the time of BecquereFs first publication in 1883 on the phenomenon of lumi-
nescence, several research workers, mostly physicists, have devoted their whole scientific
careers to the investigation of 'fluorescence' and 'phosphorescence' [7]. The difference
between the two types of behaviour lies in the decay characteristic of light emission.
'Fluorescence' has only a short lifetime, whereas 'phosphorescence' consists of a slowly
decaying afterglow.
Much work was done in the field of cathodoluminescence (luminescence excited by
bombardment with cathode rays), in the field of electroluminescence (luminescence
excited by the application of electric fields), in the field of chemiluminescence and
biological processes, in the field of triboluminescence, where luminescence is stimulated
by mechanical stresses, and finally in the field of photoluminescence, stimulated by the
absorption of light.
The features common to all these forms of luminescence are:
(i) the existence of some process whereby an atom, molecule, or centre is excited to
higher energy states, and
(ii) the radiative transition to the ground state via the emission of a photon of appro-
priate energy after a certain time delay.
As early as 1895 the physical process for the thermal release of stored radiation-
induced luminescence (thermoluminescence) was used for the detection of ionising
radiation by Wiedemann and Schmidt [8] in Erlangen. They irradiated a great number of
minerals and inorganic compounds with cathode rays and found, among other things, that
natural fluorite and manganese-activated calcium fluorite in particular show a very
intense luminescence when they are heated in darkness, and there is no decay of the
stored luminescence even after storage for a few weeks. Both substances are still used as
thermoluminescent phosphors in solid-state dosimetry.
In the same year Rontgen [9] announced the discovery of x-rays and even in his first
preliminary communication [10] he reported on the sensitivity of photographic plates to
this new radiation. They enable the fixation of some phenomena and therefore a decep-
tion might be better detected and 'you can take exposures with a plate covered by the
paper envelope in a bright room'. Concerning the quantitative measurements he said: 'In
order to get some relation between transmission and thickness of the absorbing lay:r, I
took a number of exposures with photographic plates covered to some extent with tinfoil
of a gradually increasing number of leafs'.
As was shown, the first measurements were done on the effect of x-rays on photo-
graphic emulsions. But the influence of this radiation on thermoluminescence was
reported, too. In 1925 Wick [11], from Vassar College, gave a description of the effects of
x-rays in producing and modifying thermoluminescence. He observed in many substances
considerable changes in TL when irradiated with x-rays. Some materials which usually
showed no natural TL became thermoluminescent when excited by x-rays. He also found
out that the TL after x-irradiation normally started at lower temperatures and showed
higher intensities than the natural thermoluminescence of the same materials.
History 5
Today, one knows that the stability of the metastable states responsible for TL is
greater for higher values of the energy necessary for the system to release charge carriers
from these states. When a relatively low thermal energy is sufficient to release the charge
carriers, i.e. when the observed maximum temperature is near to the excitation tempera-
ture, then the charge carriers responsible for this maximum may be thermally liberated
due to longer storage at the exciting temperature. Consequently, in the following glow
curve this maximum cannot be observed. However, when the thermoluminescence experi-
ment is performed directly after excitation this maximum can also be measured. This
effect was observed by Wick but without any explanation. In 1928 he reported, together
with his coworker Slattery [12], further measurements of TL in synthetic materials previ-
ously excited by x-rays.
Thermoluminescence measurements in the modern sense were carried out for the first
time in the Przibram Institute in Vienna by Urbach and Frisch [13]. Urbach [14]
described in 1930 the luminescence of alkali halides. As well as the description of the
measurement he also reported the first results of a theory. The theory for the calculation
of model glow curves which is now used to estimate the trapping parameters was given in
1945 by Randall and Wilkins [15] and in 1948 by Garlick and Gibson [16]. These
theories will be discussed in more detail in chapter 2.
The thermoluminescence method was hardly used for dosimetric purposes up to this
time. In this field the film dosemeter reigned supreme. In the beginning the photographic
dose measurement was used less in radiological protection than in other problems of
medical dosimetry [10]. The reason for this is that little importance was attached to
radiological protection, and the sensitivity of the available photomaterials was too small
to detect the small doses then in use. Behnken [17], indeed, tried in 1922 to intensify the
radiation effect on the film by means of fluorescent foils. He found, however, that there
was a long-term error due to the contribution of light to the total density of the photo-
graphic emulsion.
In 1926 Quimby [18] studied scattered and secondary radiation in radiation labora-
tories by photographic methods, and in 1928, with increasing attention being given to the
safety of the people engaged in radiation research, this method was proposed for personal
dosimetry by Barclay and Cox [19]. In 1929 Eggert and Luft [20, 21] constructed a
badge with several metal filters to be carried on the body of radiation workers and which
was calibrated by known radiation doses. They called it a 'film dosemeter'. Bouwers and
Van Der Tuuk [22] extended the arrangement of Eggert and Luft using different filter
metals. In this way the photographic film was established in personal radiological
protection.
With the rapidly increasing use of radiation sources and reactors in civilian as well as
in military fields after World War II, far-sighted experts quickly realised that the proper-
ties of photographic emulsions as a large-scale long-term dosemeter were rather limited [1].
The main reasons are the inherent problems of a strong energy dependence (film dose-
meters are about 20-50 times more sensitive to 40 keV x-rays than to gamma radiation
and the metal filters only partially compensate for this energy dependence), of pro-
nounced fading at higher temperatures and humidities, high sensitivity to disturbing
agents such as light, pressure and certain chemicals, limited lifetime, dose range and sensi-
tivity, poor reproducibility, and the need for rather complex darkroom processing
procedures including development, fixing and washing, involving many potential sources
of error.
6 A Scharmann
In the USA especially, in the late 1940s, an intensive search therefore began for better
alternatives, more suitable for the dose control of larger military units. Radiophoto-
luminescence (RPL) dosemeters based on silver-activated phosphate glasses were developed
(Weyl et al [23], Schulman et al [24]). The glasses later became the first mass-produced
solid-state dosimetry system. More than a million units were used in the US Navy (Schul-
man et al [25]). In the early 1950s most of the TL phosphors mainly used at present were
discovered or rediscovered and seriously proposed for dosimetric purposes, e.g. LiF by
Daniels [26], CaS0
4
by Kossel et al [27] and CaF
2
by Ginther and Kirk [28].
The idea of dose measurements by means of TL phosphors started in two ways [7]:
(i) Since the beginning of this century, the natural TL of various materials has been
studied, mostly in Europe. In 75% of about 3000 investigated minerals TL was found.
(ii) Since the beginning of this century it has also been known that CaS0
4
:Mn could
be used for the quantitative measurement of ultraviolet radiation. Originally the green
luminescence of CaS0
4
:Mn obtained by heating the material after uv exposure was
evaluated visually. Later use was made of a photomultiplier for evaluation of the phos-
phor. Soon it was found that this method could also be used for measuring x-rays. A
practical application of this method was reported in 1951 by Purcell et al [29]. On
18 November 1948 and 17 February 1949 CaS0
4
and MnS0
4
phosphors were carried to
a height of 90 and 79 miles, respectively, by means of a V2 rocket. They were then
exposed to the Sun for about three minutes. Some of the phosphors were naked, while
others were covered with filters of CaF
2
, LiF and beryllium. Upon their return the differ-
ent phosphor strips were heated and the thermoluminescence was measured by a photo-
multiplier. In every case a glow curve was observed and the intensities registered with the
Be, CaF
2
and LiF filters were about 1/10, 1/3 and 1/2 of the naked phosphor, respectively.
The occurrence of thermoluminescence, even in the shielded phosphors, was evidence for
a high-energy region in the Sun's spectrum. At the height where the exposures were done
there was even a component in the x-ray region, proved by the thermoluminescence of
the Be-covered phosphor.
Basic work on CaS0
4
:Mn was also done by Kossel et al [27]. They described in 1954
the development of simultaneous dosimetry of radiation fields in living objects. The
motivation for these investigations came from Bickenbach who was the head of the
hospital in Tubingen at this time. He pointed out the urgent interest in measuring the
dose distribution of radiation sources (radium and hollow anode tubes) which were
introduced into small cavities of the body or even in the tissue.
It was obvious to the authors that they should use for this purpose the classical
method of the light sum which was founded quantitatively by Ltnard and Hausser [30]
in 1912. In this method phosphorescent substances in a low-energy state may store a light
sum which is at most proportional to the exciting radiation. This light sum is measured by
means of a photoelectric detector when the material is later heated. The method was
useful because of the small size of such storage phosphors, which enabled convenient
injection into the cavities of the body and because of the omission of leads necessary for
measurements using ionisation or photocurrent methods and experiments with a counter.
Another advantage of this method is the great number of phosphors which could be
deposited around the radiation source. This allows simultaneous dosimetry at different
places during a single radiation period. The classical phosphor, fluorite, turned out to be
too insensitive to the small doses which are of interest in this special case, but CaS0
4
:Mn,
History 7
which was suggested by Brauer, proved to be very suitabe. With this phosphor simul-
taneous dosimetry could be developed. The reproducibility of the data on intensity
relations was about 5%. The method was tested for up to 20 simultaneous working
observation points.
As mentioned above, the idea of dose measurements by means of TL phosphors started
in two ways. One was the early known uv sensitivity of CaS0
4
:Mn and the other was the
natural thermoluminescence observed in many minerals. Natural TL is excited in the
course of geological deposition of stone formations by background radiation, in particular
by naturally occurring radionuclides which are present everywhere in small quantities.
Some of the minerals were more sensitive to radiation than others, i.e. under the same
conditions they showed a higher TL intensity. The phosphor most investigated was the
very sensitive CaF
2
. So, materials were discovered which were suitable for dosimetric
purposes.
Since there is a close connection between TL and natural radiation, the TL measure-
ments were used to investigate the thermal and radiation history of minerals. A sum-
marising report on the application of thermoluminescence methods, in particular for the
study of the radiation history of natural minerals for the purposes of geology, mineralogy
and geological chronology but also for investigations of ceramic materials, glasses, cata-
lysts, etc, was given for example by Daniels et al in their publication of 1953 Thermo-
luminescence as a research tool [31].
The research work done by Houtermans et al [32] should also be mentioned here.
They described in 1957 an apparatus for the quantitative measurement of glow curves
with a heating rate of about 40-80 K s
_1
. This enormous heating rate strongly increased
the TL intensity. The resolution power of the apparatus relative to the separation of the
maxima, however, was nearly the same as at low heating rates. By comparing the natural
glow curves with those after artificial irradiation the natural dose of 'Wolsendorfer'
fluorite could be estimated. If the contents of uranium, thorium and potassium are
known, the dose rate in a mineral of sufficient size could be calculated from the ionisa-
tion energy of the a, 0 and y radiation of these elements. From the known stored radiation
dose and dose rate the period of irradiation could be estimated. But there are still further
results which could be obtained from the glow curves.
By means of annealing experiments information on the thermal history of meteorites
could be obtained. So one can say that the temperature at which the natural glow curve
of the material starts to increase is surely not exceeded for more than a few seconds in its
thermal history during its exposure to natural radiation and in particular during its fall
through the atmosphere.
In some cases it turns out that the glow curve is lower near the surface than in the
interior of the meteorite and that the crust itself, which was heated up to 500 C or more,
showed no TL signal. This dependence of the natural glow curves on the depth of the
material below the present crust is detectable only in the outermost layers. Deeper than
15 mm no differences between the glow curves could be observed, which proves that
during the passage through the atmosphere the heat wave advanced only up to a depth of
15 mm.
In the 1950s more and more thermoluminescent materials were examined for their
usefulness as dosimetric phosphors. Single crystals activated with metal ions were mostly
examined, beginning with manganese-activated calcium sulphate which was occasionally
8 A Scharmann
used as mentioned above between 1895 and 1954 for radiation and uv dosimetry, e.g.
in rockets. Manganese-activated calcium fluoride was also often suggested [1].
In the late 1940s studies on lithium fluoride, a material of low atomic number and
therefore low energy dependence for x-rays, began at the University of Wisconsin under
the guidance of Daniels. This work was interrupted between 1956 and 1960 because of
the less desirable dosimetric properties of a newer material. Later works of Cameron and
his coworkers in collaboration with the Harshaw Company led to the development of a
material which was mainly activated with magnesium and titanium and which is now
widely distributed under the name ' TLD 100'. Despite some unfavourable properties such
as non-linearity at higher doses and a complex behaviour when heated, it is still the most
popular TLD phosphor, and for many people knowing the field only slightly it is
synonymous with the term 'solid-state dosemeter'.
Further popular TLD phosphors have been developed. Since 1957 special interest has
been shown in natural fluorite, manganese-activated lithium borate, and, recently, beryl-
lium oxide as an alternative to lithium fluoride for energy-independent photon measure-
ments, as well as in dysprosium-activated calcium fluorite and calcium sulphate and
terbium-activated magnesium orthosilicate. Thermoluminescent glasses developed in
various countries, as well as infrared-stimulated detectors, have not been successful so far
in large quantities.
A second generation of materials including greatly improved RPL glasses and TL phos-
phors and a wide variety of commercial systems became available during the 1960s. The
new techniques of exoelectron dosimetry and track etching were also explored during this
period. In about 1965 an explosion of publications began which apparently has not yet
reached its peak (figure 1.1). Our available knowledge on solid-state dosemeters now
doubles every few years which makes it increasingly difficult for individual scientists,
particularly in small institutions or developing countries, to keep their knowledge up to
date. Today, scientists in about 25-30 countries are engaged in problems of solid-state
dosimetry.
Figure 1.1. Approximate number of publications per year
on thermoluminescence (TL) in LiF and in other materials,
on radiophotoluminescence (RPL), track etching and
exoelectron emission. (Based on data by Attix, Fleischer
and Becker.)
History 9
References
1 Becker K and Scharmann A 1975 Einfuhrung in die Festkorperdosimetrie (Miinchen: Verlag Karl
Thiemig)
2 Oldenberg H 1705 Phil. Trans. Abrdg. 3 345
3 Pearsall T J 1830/ . R. Inst. 1 267
4 Becquerel H 1883 Ann. Chim. Phys. 5
e
serie XXX 5
5 Becquerel E 1842 Bibl. Univ. Geneve-Arch. Set Phys. Nat.
6 HeischelW 1800Phil. Trans.
7 Oberhofer M 1973 Thermoluminescence Dosimetry, Pusat Reactor Atom Bandung PRAB: 335/
HP.40/73
8 Wiedemann E and Schmidt G C 1895 Ann. Phys. Chem. 54 604
9 Rntgen W C 1895 Verhandl. Phys.-Medizin. Akad. Wurzburg
10 Becker K 1962 Filmdosimetrie (Berlin: Springer-Verlag)
11 Wick F G 1925 Phys. Rev. 25 588
12 Wick F G and Slattery M K 1928 7. Opt. Soc. Am. 16 398
13 Scharmann A, Bohm M, Born G, Grasser R and May A 1971 Einfuhrung in die Lumineszenz
(Miinchen: Verlag Karl Thiemig)
14 Urbach F 1930 Wien. Ber. Ila 139 363
15 Randall J T and Wilkins M H F 1945 Proc. R. Soc. A 184 336, 390
16 Garlick G F J and Gibson A F 1948 Proc. Phys. Soc. 60 574
17 Behnken H 1922 Fortschr. Rontgenstr. 29 330
18 Quimby E H 1926 Radiology 7 211
19 Barclay A E and Cox S 1928 Fortschr. Rontgenstr. 38 311
20 Eggert J and Luft F 1929 Rontgenpraxis 1 188
21 Eggert J and Luft F 1929 Rontgenbltter 1 655
22 Bouwers A and Van Der Tuuk J H 1930 Br. J. Radiol. 3 503
23 Weyl W A, Schulman J H, Ginther R J and Evans L W 19497. Electrochem. Soc. 95 70
24 Schulman J H, Ginther R J, Klick C C, Alger R S and Levy R A 1951 7. Appl. Phys. 22 1479
25 Schulman J H, Shurcliff W, Ginther R J and Attix F H 1953 Nucleonics 11 (10) 52
26 Daniels F 1950 Report on 4th Symp. on Chemical Physics and Radiation Dosimetry part I (Edge-
wood, Md: Army Chemical Center) p 148
27 Kossel W, Mayer U and Wolf H 1954 Naturw. 41 209
28 Ginther R J and Kirk R D 1957 7. Electrochem. Soc. 104 365
29 Tousey R, Watanabe K and Purcell J D 1951 Phys. Rev. 83 792
30 Lenard P and Hausser W 1912 Sitzgsber. Heidelberger Akad. Wiss. Math.-Naturw. Kl. 12 Abh.
31 Daniels F, Boyd C A and Saunders D F 1953 Science 117 343
32 Houtermans F G, Jager E, Schon M and Staufer H 1957 Ann. Phys., Lpz. 20 283
Applied Thermoluminescence Dosimetry. Eds M Oberhofer and A Scharmann
1981 ECSC, EEC, EAEC, Brussels and Luxembourg
2
Theory
M BOHM AND A SCHARMANN
2.1. Introduction
Thermoluminescence involves two steps. In the first step, the solid is exposed to the
exciting radiation, such as particle or electromagnetic radiation, at a fixed temperature.
In the second step the excitation is interrupted and the sample is heated. One finds that
during the temperature increase the sample emits light. The intensity of luminescence as a
function of temperature, which possibly exhibits several maxima, is called the thermally
stimulated luminescence or thermoluminescence (TL) glow curve. In some cases glow
curves of thermally stimulated conductivity (TSC) and thermally stimulated exoelectron
emission (TSEE) can be observed which are usually correlated to thermoluminescence.
The theory of thermally stimulated phenomena is treated in a two-fold manner. First
the excitation, the thermal stimulation, the luminescence, the electrical conductivity and
the exoelectron emission are considered on the basis of general physics. Secondly, the
phenomena are phenomenologically analysed without considering the various processes,
such as thermal activation or recombination, from a physical point of view and without
considering the atomistic structure of centres. Finally, an experimental example is
theoretically analysed in this way.
2.2. Excitation by radiation
In the following the interaction of radiation with matter and defect creation are studied
more closely. The radiation possibly causes numerous changes in both the indigenous
lattice ion and in the impurities present. The end-products of these changes may be
classified in terms of three categories of defects: (i) electronic defects, which involve
changes in valence states; (ii) ionic defects, which consist of displaced lattice ions; and
(iii) gross imperfections, such as dislocation loops and voids. In the latter case large
macroscopic defects rarely occur and are mostly due to particle irradiation.
As for the electronic defects the valence state of both the impurities and lattice defects
can be changed. The simplest radiation products arise from the impurities which are
present in all samples. Thus the valence states are changed by trapping electrons and holes
created elsewhere in the lattice by radiation. It means that the impurities act as traps for
electrons and holes. The capture cross sections of impurities for electrons and holes vary
with the type of impurity and the nature of the host lattice. The experimental proof of
the change of valence state due to radiation can be obtained by studying the change in
optical, dielectric and magnetic properties. For instance, different optical absorption
bands or spin resonance spectra characteristic of the defect are observed.
12 M Bohm and A Scharmann
As mentioned above, imperfections in crystals can also change their nature by trapping
electrons or holes. More interesting perhaps is the fact that free charges can be trapped
even in perfect crystals. In alkali halides the so-called 'self-trapped holes' are obtained. Their
structure can be investigated by the methods of EPR [1,2] and optical absorption [3-5]
in a performed manner. The configuration of these centres is represented by figure 2.1.
They consist of two nearest-neighbour < 110> halide ions that have captured a hole or have
given up an electron respectively. The halide ions have moved together to form a halide
molecular ion. It should be emphasised that these centres are not lattice defects in the
usual sense of involving a vacancy or interstitial. The two halide ions are, however,
displaced from their normal lattice sites so that they have a smaller spacing than the
normal negatively charged halide ions. Also, it is noted that in order for a self-trapped
hole to be produced, the accompanying electron must be trapped at some other defect,
such as an impurity.
Figure 2.1. Model of the V^ centre in alkali halides.
As for the ionic defects the most important role is played by the vacancies, which are
probably the best-known radiation damage products. In simple elemental crystals (e.g.
metals), all vacancies are equivalent. In compounds and more complicated crystal struc-
tures, there are a number of possible vacancy configurations, depending upon which
elemental species is missing and which of a number of non-equivalent lattice sites are
vacant.
In principle, the energy to form a vacancy can be estimated by imagining that an
atom is removed from the interior of the crystal and then placed upon the surface. In the
first step some energy is required to break a number of bonds; in the second step the
re-establishing of a smaller number of bonds is responsible for energy becoming available.
Because of relaxation of the lattice around the vacancy, it is very difficult to calculate
accurately the formation energy directly from theory. However, a rough value of the
order of 1 eV may be estimated.
In the case of a binary ionic compound, such as NaCl, the vacancies tends to occur in
pairs in order to preserve equal numbers of alkali and halide ions. It is also true that
Theory 13
defects of one kind would leave the crystal charged or would produce high electric fields.
Consequently, positive and negative ion vacancies must occur in pairs in order to guaran-
tee charge neutrality. A pair of such vacancies is known as a 'Schottky defect'.
In polar compounds most of the observations of radiation defects have been made on
negative-ion vacancies. In singly charged compounds, the anion vacancy which contains
an electron is referred to as the F centre [6] (figure 2.2). The centre has the same charge
as the anion originally present there and is consequently uncharged with respect to the
perfect lattice. The electron density of the unpaired electron is not only localised to the
vacancy but extends to neighbouring nuclei. The interaction with these nuclei can be
detected as hyperfine structure (HFS) in the ESR or ENDOR measurements respectively.
Figure 2.2. Model of the F centre in alkali halides.
When another electron is captured by the F centre an F' centre is formed. It has a single
negative charge with respect to the lattice. No ESR absorption or dispersion from an
F' centre can be observed because it is a two-electron centre with a diamagnetic ground
state. In alkali halides containing impurities one nearest-neighbour cation of the F centre
can be replaced by an alkali ion of smaller size. A static perturbation is then applied to
the F centre and the original local symmetry is reduced. The reduction in symmetry
causes a splitting of the three-fold degenerate excited state into two states and therefore a
splitting of the main F absorption band into two components. These centres are called
F
A
centres [7].
There are also a number of defects which involve a positive-ion vacancy. For instance
the analogue to an F centre consists of a hole located on the site of a cation vacancy [8].
This centre is called a Vjr centre. However, the symmetry of the Vp centre differs greatly
from that of the F centre. The F centre has cubic symmetry in the ground state, and its
wavefunction is substantially s-wave in character. In the case of the V
F
centre, the hole is
in a p-like state. The degeneracy is removed due to a reduction in symmetry (Jahn-Teller
effect).
In many cases, it is possible to produce groups of vacancies, so-called vacancy aggre-
gates. For instance, aggregates of F centres which consist of two (M centre), three (R
centre) or four (N centre) F centres [9,10].
14 M Bohm and A Scharmann
Other ionic defects are formed by interstitials. A lattice atom or ion is displaced from
its normal site and remains in a position that is not a normal lattice site. The double
defect consisting of the vacancy and interstitial is called a 'Frenkel defect'. Obviously, the
energy to form a Frenkel defect is the sum of the energy to form the interstitial and the
energy to form the vacancy. Such defects might be generated in the interior of the crystal
by thermal vibrations. There are many possible types of interstitial centre. In compounds,
there may be cation and anion interstitial ions or atoms. Moreover, interstitial ions can sit
either at the centre of an interstitial site or may be drawn towards one of the lattice ions
to form a centre of differing configuration such as a molecular ion. An example is shown
in figure 2.3. It consists of an interstitial halide atom that has bonded itself to a lattice
halide ion and shares that ion's lattice site. This molecular ion defect, called an H
centre [2,11], is to be contrasted to the (halide)2-hole centre (V
k
centre) in the perfect
lattice, where the two anions have two lattice sites.
Figure 2.3. Model of the H centre in alkali halides.
In the following subsection, the mechanisms by which defects can be created in solids
by radiation will be considered. One can distinguish three generic classes of radiation
damage processes:
(i) electronic processes;
(ii) elastic collisions; and
(iii) radiolysis.
The electronic class includes all processes in which an electronic state is changed or a
charge is moved about by the absorption of radiant energy, but in which no ionic or
atomic defects are formed. The absorption occurs somewhat differently for various types
of radiation.
A heavy, energetic particle passing through matter is usually stripped of some or all of
its electrons and thus represents a rapidly moving point charge which interacts with the
crystal electrons. Similar considerations are valid for fast electrons. However, bombarding
Theory \ 5
electrons are not distinguishable from the crystal electrons. Moreover, since bombarding
electrons, in contrast to heavy particles, are as light as the crystal electrons, they can lose
an appreciable fraction of their energy in a single collision. The penetration depth of a
particle in a crystal, which is very important in radiation damage, depends on the energy
loss. Since the energy absorbed from a heavy particle is very much greater than that
absorbed from electrons, electrons will penetrate deep into crystals while heavy particles
are stopped near the surface.
Fast neutrons, since they are not charged, do not excite the crystal electronically as do
charged particles. However, when a fast neutron displaces a crystal ion, the ion gives up
some of its kinetic energy to the electronic structure of the crystal.
In some materials, thermal neutrons can be quite effective in producing electronic
excitation indirectly. This comes about when a thermal neutron is captured by a nucleus
and the excited new isotope decays.
Photons with energies in the range obtainable with x-ray or isotope sources can transfer
their energy to the electronic system of a crystal by a number of processes. In the photo-
electric effect, the full photon energy is transformed into ionisation and kinetic energy
of one of the crystal electrons. Energy transfer increases in efficiency as the photon
energy decreases until the energy becomes too small to excite K-shell electrons. If the
photon transfers only a portion of its energy to an electron of the crystal the process is
called the 'Compton effect'. This mechanism of energy transfer becomes important for
photon energies between about 0.1 and 1 MeV. At energies above 1.02 MeV the produc-
tion of electron-positron pairs ('pair production') becomes important.
In order to create defects through elastic collisions, it is necessary for the incident
particle to impart sufficient energy to a lattice atom or ion to displace it through its
neighbours into an interstitial site. Thus the effectiveness of an incident particle in creat-
ing damage depends on the maximum amount of kinetic energy it can transfer to a lattice
ion. This depends, in turn, on the energy and the mass of the incident particle and the
mass of the lattice ion. In general, five types of radiation may produce displaced atoms or
ions by elastic collision. These are:
(i) 7-rays,
(ii) energetic electrons,
(iii) thermal neutrons,
(iv) fast neutrons, and
(v) energetic atoms and ions.
It is clear that the heavier particles will be much more effective in displacing lattice
ions than the lighter ones. In fact, they are so effective that they produce so-called
'cascades'.
Finally, defects are created by radiolysis. This means that in certain ionic materials,
defect creation is highly efficient and is most probably due to the conversion of electronic
excitation energy into a form capable of manufacturing lattice defects rather than into
elastic collisions. Such photochemical processes are most probably involved in the photo-
graphic process and photosynthesis.
When energy is absorbed in a crystal by electronic processes as described in the first
part, it appears in the form of electrons in a normally empty conduction band and holes
in the normally occupied valence bands, or in the form of excitons (electron-hole pairs
16 M Bohm and A Scharmann
bound to each other) at lattice ions, impurity ions, or defects in the crystal. The excita-
tion is only the first step and must be followed by processes that lead to observable
electronic states. This usually involves separation of the electrons and holes, and trapping
of the separated charges at impurities, defects or in the perfect lattice. The capture cross
sections are determined by potential variations near the centres which can be attractive,
neutral or repulsive.
Normally, the crystal as a whole remains neutral, and free electrons and holes are
always created in pairs. For every electron trapping centre formed, there must also be a
corresponding hole centre formed.
2.3. Thermal excitation and recombination
Supposing the solid previously excited is heated, a thermal relaxation then occurs which
is the dominant mechanism in nearly all temperature-dependent processes in solids. It
means that the processes are started and accelerated if energy is supplied in the form of
thermal energy [12]. These thermally stimulated processes can be compared with chemi-
cal reactions. The increase in the rate of such reactions with temperature can usually be
expressed by an Arrhenius equation. This equation leads one to the concept of an activa-
tion energy: an energy barrier which must be overcome in order to reach equilibrium.
In this special case electrons and holes may escape from metastable states during
heating. These levels are known as traps. The probability of thermal excitation of a
carrier, the so-called escape probability a, is assumed to be given by a Boltzmann factor:
ct = a
0
exp(-E/kT) (2.1)
(a
0
= constant, E= thermal activation energy required to liberate a trapped electron,
k = Boltzmann's constant, T = absolute temperature).
Although this expression is well supported by experiment, a detailed theoretical treat-
ment is still lacking. In a semiclassical approach a trapping model with levels equidistant
in energy from each other and a successive absorption of phonons is assumed. Another
model is based on thermodynamic concepts as they are assumed to be valid in chemical
reactions. Finally, this relation can be deduced from a simple model using the law of
detailed balancing.
For this purpose one may consider traps with only one state. There are also H traps
(per unit volume) and many electrons, of which n are in the conduction band and (H n)
in the traps. Denoting by a the cross section for the capture of an electron in a trap
(= actual area multiplied by the probability of capture) and letting a be the probability
per unit time that it escapes, from the law of detailed balancing a relation between a and
a may be deduced. For a steady state one can write
n
2
va=(H-n)a (2.2)
(number of transitions into the traps = number of transitions into the conduction band),
where v is the mean velocity of the electrons.
The concentration n of the free carriers is calculated using the methods of statistical
mechanics. Thus the assumption is made that the crystal is in thermodynamic equilibrium
at a fixed temperature T. With the volume V of the crystal as a second state variable the
equilibrium value of n will then be given by the condition that the free energy F becomes
Theory V^ TWTE^ VV
1 7
a minimum:
(W73ii)
r
=0. | *
w
^
? / /
,
0
J (2.3)
Then one obtains
n
2
n-nmkTf
1
F ^ - ( ) ^-
E/kT) (2
'
4>
where E is the energy required to remove an electron from the trap into the conduction
band. Substituting n in equation (2.2) gives
a = a
0
exp(-E/kT) with a
0
=ovN
c
. (2.5)
N
c
is an effective density of states for electrons in the conduction band. Substituting v
from (\/2)mv
2
= (3/2)kT and assuming the effective cross section of the order of
10"
ls
cm
2
one obtains a
0
10
11
s
1
. This preexponential factor is of the order of the
frequency of the lattice vibrations and is called the 'frequency factor'. From this model
its temperature dependence is proportional to T
2
(v~T
112
, N
C
~T
3
'
2
). In most cases it
is neglected. The thermal activation energy, the socalled trap depth, is much smaller than
the optical ionisation energy because the thermal activation, which involves a multi
phonon process, occurs with the removal of ionic polarisation due to trapped carriers,
whereas in the case of optical activation the polarisation does not have enough time to
disappear according the FranckCondon principle.
The thermal release of carriers from traps possibly gives rise to a thermally stimulated
conductivity (TSC) when the sample is placed in an external electric field. Moreover,
electrons liberated from traps into the conduction band also have a chance of leaving the
solid if they are close to the surface and if their energy is sufficient to overcome the
barrier created by the electron affinity. This phenomenon is called thermally stimulated
exoelectron emission (TSEE) and according to this model it is expected to be associated
with TL and TSC.
When electrons (or holes) have been thermally excited into the conduction band (or
valence band) they will be captured by traps again or recombine with opposite carriers.
The retrapping is influenced by the thermal velocity v in the energy band and the effec
tive cross section a. It can be expressed by the transition coefficient :
P = ov. (2.6)
If recombination occurs with the emission of light, a TL glow curve can be observed.
Radiationless transitions are also possible. In this process the energy is transferred to
another electron (Auger recombination) or to the lattice in multiphonon processes. As
is known from absorption the energy and momentum must be conserved in each recombi
nation process. Let k be the wavenumber of the carrier in the initial state and k' in the
final state. Then
hk-hk' = h/\ (2.7)
or, since the momentum of the photon (h/X, X = wavelength) is small compared with the
smallest momentum of the carrier (h/a,a = lattice constant), the selection rule for optical
18 M Bohm and A Scharmann
transitions is given by
hk-hk' = 0. (2.8)
This states that direct recombination occurs only between carriers with the same wave-
number. In the energy band model the carriers may only make vertical transitions. The
change in momentum and energy due to electron-phonon interactions occurs in a time
that is much smaller than the carriers' mean lifetime. (In other words, the phonon energy
is large compared with the linewidth.) Thus a direct band-band recombination is very
unlikely.
A larger probability of radiative transitions is obtained in the presence of imperfec-
tions such as vacancies, interstitials or impurities. When the optical transition involves an
imperfection the selection rule (2.8) is satisfied even for different wavenumbers in the
conservation of momentum. In connection with luminescence these imperfections are
called activators.
2.4. Phenomenological analysis
The thermally stimulated processes may be phenomenologically analysed. The physical
processes such as interaction with the exciting radiation, thermal activation, charge and
energy transport or recombination are not considered at all. This means that one does not
investigate the kinds of transition involved and the contribution of phonons during
thermal stimulation. One is also not interested in the structure of centres, such as traps
and activators.
Several properties of solids may be explained by the energy band model. It involves
energy states which are allowed or forbidden to be occupied by electrons. These energy
levels are so closely spaced as to constitute a quasicontinuum or energy band. All the
bands which represent the closed electron shells of the individual atoms are always fully
occupied with electrons. The next higher-lying band contains the valence electrons and is
called the valence band. In the case of the insulators in question this valence band is
completely filled by the valence electrons. An energy gap without any allowed states lies
between the highest state in the valence band and the lowest state of the next highest
band called the conduction band. The width of the band gap is greater than 1 eV so that
transitions of electrons across this gap cannot occur at normal temperatures. The conduc-
tion band, normally empty, is responsible for electrical conductivity if an electron reaches
this band from the valence band. For such transitions to be possible more energy from
exciting radiation is necessary.
One can understand the origin of these bands from two limiting cases. In bringing free
atoms together to form a crystal, the discrete levels of these atoms split up into groups of
levels which then form an energy band, or by the influence of the lattice potential the
continuous energy spectrum of a free-electron gas is broken at certain characteristic
energies since electrons with these energies and corresponding momenta on their passage
through the crystal suffer Bragg reflections from the lattice. Both types of description
starting from tightly bound or completely free electrons meet in the band model of
solids.
The simplified energy level scheme is commonly used to describe the non-stationary
processes (figure 2.4). Wherever the perfect periodicity of the crystalline structure is dis-
turbed, it is possible for carriers to take on energies which are forbidden in the perfect
Theory
19
Y
a
>E
Ev
Figure 2.4. Energy level diagram for the phenomenological analysis of TL and TSC with
one type of trap level and recombination level.
crystal. The presence of a defect can introduce one or more additional energy levels in
the forbidden gap between the conduction and valence bands; unlike the bands them-
selves, which extend throughout the crystal, the additional level is localised at the crystal
defect. The activators and traps give rise to some discrete levels above the valence band
and below the conduction band, respectively. In the ground state the recombination
levels are occupied by electrons and the trapping levels are empty. After excitation by
energetic radiation electrons or holes can be captured in traps or recombination centres,
respectively. For the sake of simplicity the following consideration deals only with
electrons. If sufficient thermal energy is supplied the trapped electrons may again be
raised to the conduction band. The electrical conductivity can now be measured. From
the bottom of the conduction band the electron may be retrapped by the traps or they
may recombine with empty activators in a radiative manner. The latter process gives rise
to thermoluminescence. The possible transitions are represented by arrows. The simplest
model involves only a single trap level and a single type recombination level. The symbols
used are h, the density of trapped charge carriers, H, the density of trap levels, n, the
density of free charge carriers, and /, the density of recombination levels.
The transition probabilities are replaced by transition coefficients: a, the escape
coefficient for trapped carriers, (3, the retrapping coefficient, and y, the recombination
coefficient.
It is not probable that such a model accurately represents an actual situation occurring
in solids since essential simplifications have been introduced. For instance:
(i) The free carriers are electrons and there is no thermal quenching. This implies that
transitions of electrons from the valence band to the recombination centres are
neglected.
(ii) No interaction exists between centres which excludes donor-acceptor recombina-
tion and trap distributions.
20 M Bohm and A Scharmann
(iii) Only one kind of centre is involved in the recombination process; thus no killer
centres are present,
(iv) Recombination of trapped electrons via excited states of defect centres does not
occur.
The phenomenological analysis now deals with the kinetic balance. Some transition rates
are necessary.
(i) The rate at which trapped carriers are thermally released (the rate of liberation) is
proportional to the number of occupied traps h:
rate of liberation = ah.
(ii) The retrapping rate, which means the number of trapping transitions per unit time
and volume, is proportional to the density of free carriers n in the conduction band
and the density of empty traps (// - h):
rate of retrapping = &n{H h).
(iii) The recombination rate, which means the number of recombination transitions per
unit time and volume, is proportional to the density of free carriers n in the conduc-
tion band and the density of empty recombination centres/:
rate of recombination = ynf.
In this simple model the kinetic processes involving the change in the density of
trapped and free charge carriers during thermal stimulation are described by the following
system of differential equations.
The rate of change of the density of trapped electrons is given by
dh/dt = -ah+pn(H-h). (2.9)
The rate of change of the density of free electrons is given by
dn/dt = ah-Pn(H-h)-ynf. (2.10)
Since the solid is electrically neutral, the density of carriers in the conduction band must
be equal to the density of empty recombination centres. The condition of charge
neutrality then yields
/ =n+A (2-11)
The thermoluminescence intensity / is given by the number of radiative transitions per
unit time and volume and is therefore proportional to the recombination rate:
I~ynf. (2.12)
The electrical conductivity a is determined by the free charge carriers in the conduction
band when the mobility ju is assumed to be constant:
a = nen (2.13)
(e = electron charge).
The purpose of phenomenological analysis is to obtain explicit functions of the carrier
density and, by that, explicit functions of the current and luminescence intensities. The
Theory 21
experimental glow curves are then fitted to the calculated ones by variation of some
trapping parameters. This procedure possibly gives some physical quantities such as the
thermal activation energy E and the frequency factor a
0
. However, all attempts to find
explicit functions have been unsuccessful. Therefore one introduces some approximations
or simplifying models.
2.5. Kinetic models
It is assumed that the lifetime of free carriers in the conduction band is short when com-
pared with the lifetime of trapped carriers [13], which probably holds in high-resistivity
solids [50]. As a result one obtains a small quasistationary electron concentration in the
conduction band. This means that the density of free charge carriers is always much
smaller than the density of trapped charge carriers:
n<h (2.14)
and that the time rate of change of the free carrier density is much less than the time rate
of change of the trapped carrier density:
dn/dt<dh/dt. (2.15)
Also a constant heating rate q is used:
T=T
0
+ qt or q = dT,'dt (2.16)
(T
0
~ initial temperature).
With these assumptions an analytical solution is obtained only in two special cases. In
the first case the retrapping transitions are neglected (fi = 0) [14]. In the other case the
transition coefficients for retrapping and recombination are equal (fi/y = 1) [15].
Substituting equation (2.16) into (2.9) and (2.10) one obtains the following differen-
tial equations for the first case (fi = 0):
qdhldT=-ah (2.17)
q dnldT=ah-ynf (2.18)
with a = a
0
exp(E/kT); the temperature dependence of a
0
is neglected. From equation
(2.17) this case corresponds to 'first-order' or 'monomolecular' kinetics.
With the approximation (2.15) and by adding equations (2.17) and (2.18) one obtains:
qdh/dT=-ynf. (2.19)
Since the luminescence intensity is given by equation (2.12) from equations (2.19) and
(2.17)
/ = constant x ah. (2.20)
The density of trapped carriers h is a function of temperature and can be calculated
from equation (2.17). The integration yields
h(T) = h
0
exp[-f(T)] (2.21a)
22 M Bohm and A Scharmann
with
f(T) = exp(-E/kT)dT'
VJT
(h
0
= initial density of trapped carriers).
With equation (2.20) the luminescence intensity is explicitly given by
I(T) = constant x a
0
h
0
exp(-E/kT) exp [-f(T)].
(2.21b)
( 2.22)
After integration by parts the function f(T) can be represented by an exponential
integral function which is approximately substituted by a series. Since the initial tempera-
ture T
0
is far below the peak temperature the limit of integration can be replaced by zero:
I
' exp(-*/*r)- - jl e*p(-

/*r, i <- i
r
J ^ ( 2.23)
With four terms of the semiconvergent series a glow curve of thermoluminescence is
calculated from equation (2.22) represented in figure 2.5. The first exponential function
is responsible for the initial increase, the second for the decay of the glow curve. A non-
symmetrical shape with a steep high-temperature tail is obtained.
The error made in approximating the integral by four terms of the series can be
estimated to be less than 1% [50] and is unimportant in the following calculations. This
approximation is avoided by using a hyperbolic heating rate [19-21]:
1 1
= St (5= constant)
T
0
T
as can be experimentally realised. Now the integral is integrable in a closed form.
( 2.24)
< 10
60 70
TEMPERATURE I K)
Figure 2.5. Glow curves of TL (a) and TSC (b)
calculated from equations (2.22) and (2.27)
with - =0. 13eV, o = 2 X 10' s"\ hJH = 1 and
q = 1 Ks
1
.
Theory 23
In this model, however, there are some problems in calculating the conductivity glow
curve. From equation (2.13) the electrical conductivity is proportional to the density of
free carriers n. Using the approximation (2.14) in the condition of neutrality (2.11) one
has
f*>h (2.25)
and from equation (2.19) one obtains
q dh/dT=-ynh. (2.26)
Combining this with equation (2.17) the density of free carriers is found to be
n(T) = (a
0
/7) exp(-E/kT). (2.27)
The result is physically absurd because there is an exponential increase in the density of
conduction electrons and no maximum occurs (figure 2.5). At sufficiently high tempera-
tures the condition n >h becomes valid. This is in contradiction to the initial assumption
(2.14). To obtain reasonable solutions for the conductivity, too, the model must be
varied, which will be discussed later.
In the second case one expects liberated electrons to be recaptured by traps with some
definite probability since traps are lattice-positive. With the special assumption j3 = y from
equations (2.9), (2.10) and (2.16) one obtains the differential equations
qdh/dT=-ah+yn(H-h) (2.28)
qdn/dT=ah-yn(H-h)-ynf (2.29)
and by adding these equations and using the approximations (2.14) and (2.15)
qdhldT=-ynh. (2.30)
Comparison with equation (2.28) yields
n=ah/yH. (2.31)
With that one may substitute n in equation (2.30) and one obtains
q dh/dT=-ah
2
/H. (2.32)
This equation describes 'second-order' or 'bimolecular' kinetics.
The integration of equation (2.32) yields
ho
h (T) = (2.33)
l + (h
0
IH)f{T)
where f(T) is given by equation (2.21b). From equation (2.20), which is valid in this case
also, the luminescence intensity / can be expressed by an explicit function of temperature:
a
0
h\ exp(-E/kT)
I(T) = constant x . (2.34)
H [l + (h
0
IH)f(T)]
2
Combining equation (2.32) with equation (2.31), the conductivity a (see equation (2.13))
24 M Bohm and A Scharmann
is given by
a(T) = en
a
0
h
0
exp(-E/kT)
yH [\ + (h
0
/H)f(T)]'
(2.35)
The curves of TL and TSC calculated from this model are shown in figure 2.6. The integral
of function f(T) is again approximated by four terms of the series (2.23). Above the
maximum temperature the TL intensity drops more slowly than in firstorder kinetics, i.e.
the glow peak is more extended and more symmetrical. The conductivity glow curve is
shifted to higher temperatures and shows a very slow decrease after reaching the maximum.
/
/ /
J J
b
a /v^
V
TEMPERATURE(K)
Figure 2.6. Glow curves of TL (a) and TSC (ft)
calculated from equations (2.34) and (2.35)
with =0 . 1 9 e V, o
0
= 7 Xl O
l !
s '
1
, hJH=l,
q = 1 Ks"' and (3/7= 1.
2.6. Determination of trap parameters
The kinetic processes and the transitions of carriers are essentially influenced by the two
quantities E and a
0
. The thermal activation energy E is of particular interest because of
its importance to the lifetime of the excited state of the solid. According to the above
mentioned models one may derive many methods for the determination of activation
energy and frequency factor. Sometimes additional approximations are used, for instance,
the integral in equation (2.21b) is approximated only by the first term of the series
expansion (2.23).
The methods can be divided into several groups according to the experimental pro
cedure which must be used in order to obtain the parameter. In the first approximation
it is possible to calculate a formula which provides a linear dependence of the trap depth
E and the maximum temperature T
m
[14, 16]:
E~75kT
m
(2.36)
The derivation uses a frequency factor a
0
=2. 9xl 0
9
s '. The rough formula is quite
useful for a quick first estimation of the trap depth. However, the numerical factor in
Theory 25
equation (2.36) is dependent upon the value of a
0
, and hence the values of E thus obtained
only have the right order of magnitude. The frequency factor, in fact, may be different
for each trap in the same substance.
The position of the maximum is obtained by differentiating equation (2.22) with
respect to temperature and equating to zero. Then the relation between E, a
0
and T
m
is
given by
E/kT^ = (a
0
lq)exp(-E/kT). (2.37)
From this equation the peak position is influenced both by the thermal activation energy
and the frequency factor (figure 2.7). A decrease of a
0
or an increase of E, respectively,
gives rise to a shift of the maximum to higher temperatures. If either of the parameters
E and a
0
are known equation (2.37) can serve as a transcendental equation which can be
solved numerically for the unknown parameter.
400 500 600
MAXIMUM TEMPERATURE IK)
Figure 2.7. Thermal activation energy E as a function of maximum temperature 7 ^ of TL
glow peak with the frequency factor a
0
as parameter (calculated from equation (2.37) using
a heating rate of 1 K s~')-
By taking the logarithm one obtains from equation (2.37)
\n(T^/q)=E/kT
m
+ \n(a
0
k/E). (2.38)
Thus the plot of the left-hand side against 1/T
m
is linear, having a slope E/k. E and a
0
can
be determined from the slope and intercept [17, 18]. From equation (2.38) we can
eliminate the frequency factor for two different heating rates q
l
and q
2
[22, 23]:
T
2
E = k
J ml T,
1 -<m2
7mi T,
m2
" ( - % )
\Q2TlJ
(2.39)
The glow curve must be measured with two different heating rates q^ and q
2
which yield
the different maximum temperatures T
ml
and 7
m2
[16, 24].
26 M Bohm and A Scharmann
Other methods use different temperatures besides the maximum temperature. If one
lets T\ be the temperature corresponding to half-intensity, we can write [25]
E=\.5\kT
m
~
L
. (2.40)
Similar relations are obtained if the temperatures are considered where the intensity is
decreased to 1/2 [26, 27], to 2/3 and 4/5 of the maximal height [28]. The inflection
temperature [29] and the half-width [30] may also be utilised.
Frequently, the so-called 'initial rise method' is used to determine E. This technique is
based on the fact that the function f(T) in equation (2.22) is nearly temperature-
independent when the traps begin to empty as the temperature is raised.
Then, in the initial part of the glow curve the intensity is given by / ~exp(E/kT) or
lnI=-E/kT+ constant (2.41)
for either type of kinetics. Thus, the plots of In/ against 1/7 are linear, having slopes
equal to E/k. This provides a quick analysis of the initial ascending part of the glow
peak which yields the value of E without any knowledge of a
0
[31-33]. However, the
peaks will become wider and shallower with increasing retrapping. The temperature limit-
ing the validity of equation (2.41) is therefore decreasing [34]. Then the slope will be
equal to E/k at very low intensities where exact measurements are impossible.
From numerical methods of analysis some initial approximate values of E and a
0
are
chosen and they are suitably varied to determine the values giving the best fit to the
experimental data [35-37]. Finally the area under the glow curve can be used for para-
meter determination [38-40].
The methods may be improved by considering the temperature dependence of the
frequency factor a
0
[16, 24]. However, its influence on the shape of the glow curve and
on the determination of activation energy is only small. It amounts to about 10% from a
temperature dependence proportional to T
1
'
2
[41] and T~" {a = 1 or 2) [27], respectively.
A survey of methods from the literature is given in references [42-44].
2.7. Additional parameters
The above-mentioned models are often extended to obtain, on the one hand, a simpler
mathematical treatment and, on the other, better agreement with the experimental
results, mainly with respect to the conductivity glow curve. In this subsection two such
models are considered in detail. Both cases show first-order conditions.
In the first case a constant lifetime of free electrons in the conduction band is assumed.
This corresponds to the assumption that the density of recombination centres remains
approximately constant during the thermal stimulation. So one obtains the new condition
of neutrality (see equation (2.11)) [21, 41, 45-47]
n + h =/o 0* constant) (2.42)
and the balance equations
qdh/dT=-ah (2.43)
q dn/dT = ah - ynf
0
. (2.44)
Theory 27
By adding the differential equations and considering the approximation (2.15) one
obtains
n=ahhf
0
. (2.45)
The density of captured carriers h as a function of temperature is calculated by integrat-
ing equation (2.43) (see equation (2.21))
h(T) = h
0
exp[-f(T)]. (2.46)
Combining equations (2.46) and (2.45) the free carrier density is given by
n = ^y exp(-E/kT) exp [-f(T)]. (2.47)
T/o
Since from equations (2.12), (2.42) and (2.13) both the luminescence and the conducti-
vity are proportional to the density of free carriers we obtain the same temperature
dependence of both intensities as is represented by equations (2.47) or (2.22). Therefore
the glow curves exhibit the same shape as shown in figure 2.5. In this case the maximum
of the two phenomena peaks exactly at the same temperature. This means there is no
shift of the TSC glow curve to higher temperatures.
This model is used to explain the experimental results observed in x-rayed LiF crystals
[48]. X-irradiation creates H centres and V^ centres in addition to other paramagnetic
centres. The concentration of V^ centres is larger than that of H centres by one order of
magnitude. Concerning the behaviour under thermal treatment the H centres disappear
rapidly if the temperature approaches 105 K. This thermal decay is connected with a
relatively small drop in the number of V^ centres [49]. Glow peaks are observed in TL
and TSC measurements at about 107 K which show first-order conditions and nearly no
temperature shift. This might suggest that the H centre decays by emitting an electron,
and thus transforms into an F
2
molecule. The electron in turn annihilates a V
k
centre.
From the above-mentioned model the observed conductivity is possibly due to this charge
transfer and the thermoluminescence to the electron-hole recombination. Thereby the
density of recombination centres remains approximately constant and the neutrality
condition (2.42) is valid.
In the second model it is assumed that as well as the mentioned traps H there are
additional traps M which are thermally disconnected and act merely as a reservoir for
trapped charge carriers [50-52]. Now one obtains the neutrality condition
f=n+h+M (2.48)
and the rate equations (2.9) and (2.10) change to
qdh/AT=-ah+Pn(H-h) (2.49)
q dnjdT=ah - $n(H- h) - yn(n + h +M). (2.50)
By adding the differential equations and considering the approximations (2.14) and
(2.15) one obtains
qdhldT=-yn(h+M). (2.51)
28 M Bohm and A Scharmann
Substituting q dh/dT from equation (2.19) one obtains the density of free carriers n:
ah
Combining equations (2.51) and (2.52) the following equation results:
(2.52)
dh ah(M + h)
-q = (2.53)
dT h(l-P/y) + (ply)H + M
The integration of this equation yields
l& PH\ (M + h \ i PH\ (h\
- + In - ( 1 - In - =/ ( 7) (2.54)
\y yMI \M + h
0
) \ yM< \h
0
J
wi t h/ (f) defined by equation (2.21b).
As it is a first-order process, retrapping is neglected and p/y < 1 is valid. In addition
the assumptions H/M> 1 and $H/yM< 1 are made as a way of simulating a changing life-
time of the charge carriers [50]. Then we obtain
-\n(h/h
0
)=f(T) (2.55)
A=A
0
e xp[ - / ( r ) ] . (2.56)
This equation yields a calculation of TL because from equations (2.12) and (2.51) the
intensity is proportional to dh/dT:
I(T) = constant x a
0
h
0
exp(-E/kT) exp [-f(T)]. (2.57)
It is exactly the same relation as is obtained from a theoretical treatment of a first-order
process without additional parameter M (see equation (2.22)).
In contrast the calculated shape of TSC shows another result. Formerly one finds that
the density of charge carriers increases with constant increasing temperature according to
an exponential law without reaching a maximum, whereas now from the above-mentioned
relations one has
-q dh/dT
n= (2.58)
y(M + h)
and
7"
1
^"
1
ao/*oexp(-' /fc7' )exp[-/(7' )]
t N
" (T) = (2.59)
1 + (z
0
H/M) exp [ - / ( D]
where z
0
= H/h
0
is the fraction of initially filled traps. In the calculation of I(T) and
n(T) from equations (2.57) and (2.59) the function f(T) is approximated by four terms
of the semiconvergent series (2.23).
A TL glow curve and a family of TSC glow curves obtained in this way are shown in
figure 2.8. The temperature function in the denominator of equation (2.59) gives rise to
a shift of the TSC maxima to higher temperatures as compared with the TL maximum
usually obtained by measurement. The shift increases with increasing z
0
H/M.
Theory 29
130 160
TEMPERATURE(K)
Figure 2.8. Calculated glow curves of TL (I) and TSC (II, III, IV) from equations (2.57)
and (2.59) with E = 0.28 eV, a
0
= 10
10
s"', q = 0.05 K s
M
, and the parameter z
0
H/M = 1 (II),
10(111), 10
3
(IV).
For comparison with experiment the glow curves of x-rayed LiF crystals are chosen.
With a heating rate of 0.05 K s"
1
the crystal shows a TL maximum at 138 K and a TSC
maximum near 141 K (figure 2.9(a)). With the values of the trap depth E and the
frequency factor a
0
revealed from another measurement [32] and with the parameter
z
0
H/M=3 the calculated glow curves (figure 2.9(b)) defined by equations (2.57) and
(2.59) show good agreement with the experimental results. Because of the influence of the
parameter z
0
H/M on the magnitude of the temperature shift it is in principle possible to
verify the model by the dependence upon the initial occupancy z
0
. However, it may be
very difficult to measure the low currents.
If one applies the model with additional traps M to second-order processes, there are
three cases that must be distinguished [50]. In the first case (H/M< l,f3H/yM<: 1) where
a constant lifetime of charge carriers is simulated, the calculated glow curves show once
again a shape similar to those in first-order kinetics and consequently there is no shift of
TL and TSC maxima. In the second case (H/M < 1, (3H/yM> 1) there exist relatively large
half-widths. Even larger half-widths result theoretically from the third case (H/M> 1,
(3H/yM< 1) where the lifetime changes during heating. Moreover, there are large shifts of
TL and TSC maxima and with increasing H/M ratio the TSC shape decreases slower after
reaching the maximum [50, 53].
As well as the above cases many other models are known. For instance, additional
occupied traps and direct recombination of trapped electrons with free holes are con-
sidered by a changed neutrality condition and an effective non-radiative transition [54].
Another model involves the transition between trap and activator in a non-radiative way.
Analytical expressions for both TL and TSC intensities are obtained and the shifts of
maxima can be explained [47, 55]. Now the frequency factor and the activation energy
30
M Bohm and A Scharmann
( 0 )
n
\\
rs
'n~u
120 UO
TEMPERATURE (Kl
120 HO
TEMPERATURE ( Kl
Figure
rate: 0.
eV, a
2.9. (a) Glow peaks of TL and TSC obtained from an xrayed L iF crystal (heating
05 Ks"
1
). (b) Calculated glow curves from equations (2.57) and (2.59) with = 0.27
= 5 X I O ' V , ? = 0. 05Ks"' and z
0
H/M= 3.
for nonradiative transitions and charge transfer between an excited state and a spatially
separated recombination centre are considered, too. The shape of the glow curve calcu
lated with this model again shows firstorder characteristics.
2.8. Computer simulation
In this subsection the correlated phenomena of TL and TSC will be described in simple
models but without recourse to any simplifying approximations (2.14) and (2.15) and the
results calculated in this way will be compared with approximate solutions. The dif
ferential equations are solved rigorously on an electronic analog computer [57]. When
the equations are amplitude and temperaturescaled the densities of free and captured
carriers can be generated. However, one obtains no analytical solution but a simulation
of TL and TSC intensities against temperature.
A typical solution in the case "=0.13 eV, ct
0
= 2 x 10
9
s~
!
, /2
0
/#
=
1 and q = 1 K s"
1
is
shown in figure 2.10. In the TL glow curve the maximum temperature differs to some
extent from that curve showing the change in the trapped carrier density (dh/dT) and is
often mistaken for the TL glow curve [18, 25, 5860]. A maximum can clearly be
observed in the TSC glow curve. Moreover the exact calculation gives rise to a shift of
the TSC maximum of about 23 K to a higher temperature when compared with the TL
maximum. The break in the simulation at about 66 K is caused by the maximal limiting
voltage of the analog computer. The TL glow curve calculated approximately with the
abovementioned parameters (figure 2.5) shows the same shape. However, the maxima
are shifted to a somewhat higher temperature.
Theory 31
j
1
J
[ t
n
'
\
50 60
TEMPERATURE (K)
Figure 2.10. Computer simulation of TL (a),
TSC (b) and the change in density of trapped
carriers (c) with first-order conditions and
= 0.12eV, a
o
= 2xl 0' s-' , hJH=l, q = lKs''
and 7//=0.5 cnvV'.
a
A
f
1
50 60
TEMPERATURE [Kl
Figure 2.11. Computer simulation of TL (a)
and TSC (b) with first-order conditions and
additional thermally disconnected traps (A/);
^ O. De V, a
o
=2xl0' s-
1
, h
0
/H=l, q = lKs~
l
and H/M = 0.2.
Two special cases with first-order conditions described in 2.7 are also calculated
without making approximations. In the first case, the density of recombination centres
/ and therefore the lifetime of free charge carriers are to be assumed as approximately
constant during the glow experiment. This corresponds directly to the case where addi-
tional thermally disconnected traps M exist and their density is assumed large in com-
parison with the above-mentioned traps H [50]. This yields the neutrality condition
f-n +h +M and the assumption H/M<. 1 is made. Figure 2.11 shows the glow curves
simulated by analog computer calculations, again without the approximations (2.14) and
(2.15). Only if the density of the additional traps is increased by a factor of five do the
two glow curves have the same shape and no shift of maximum temperatures exists, as is
found in the approximate calculation.
In the other case the assumptions H/M> 1 and fiH/yM< 1 are made. With these a
changing lifetime of carriers is simulated (see 2. 7). The exact solution of the differential
equations yields the same result as is obtained in approximate calculations. The TSC curve
shows a shift in the maximum temperature and a longer exponential increase at the begin-
ning of the heating because of the increase in the lifetime.
Considering transitions to the traps one obtains the condition |3 = 0. From the special
case with second-order conditions ()3 = 7) calculated approximately in 2.5 the glow
curves of TL and TSC are exactly simulated. As a result the shape of the TSC glow curve is
parallel with that of TL in contrast to the approximate calculation. It also shows a shift to
higher temperatures winch is of the same magnitude as in the case of first-order kinetics
32 M Bohm and A Scharmann
[57]. Increasing retrapping leads to a shift of the TL maximum to higher temperatures
and a reduction of intensity as is known from approximate solutions [57, 34].
In a special case the maxima of TL and TSC show no shift although retrapping
occurs [57]. As a condition the density of thermally disconnected traps must be assumed
as being large when compared with the traps H involved in the TL process (H/M> 1).
This corresponds to a similar case in first-order kinetics. The other condition (!H/yM<: 1
must also be fulfilled.
As the computer simulation has shown, the anomaly in the TSC shape such as the
failure of a peak in first-order kinetics (figure 2.5) or the slow decrease in second-order
kinetics lies purely in the approximations (2.14) and (2.15), and is not contained in the
original rate equations. The shift of the TSC maximum to higher temperatures compared
with the TL maximum is also obtained by the exact simulation. It amounts to a few
degrees. This value has the same magnitude as is found, for example, in alkali halides
[47,48,61,62]. Furthermore it is seen that the shift gives neither information on the
trap depth nor on the kinetic process. It depends above all on the absolute value of the
recombination coefficient and the density of traps and has the same value in first- and
second-order kinetics. Only if no shift is measured, i.e. when TL and TSC peaks exactly
coincide, are two special cases possible, as the computer simulation has confirmed.
AH methods used to determine trapping parameters such as trap depths and frequency
factors are derived from approximate solutions of the rate equations with the assump-
tions relating to the density and charge of free carriers. Therefore they are only approxi-
mately valid. The same kinetic model after exact simulation shows smaller maximum
temperatures and half-widths [64]. Consequently the trap depths calculated so far with the
usual methods are too small. For instance when, in the case of the method of different
heating rates, a computer simulation is performed and the approximate formula (2.39)
is applied a trap depth reduced to about 50% is determined. Parameters obtained from
the initial rise method, which only uses the exponential increase at the beginning of the
glow curve, are relatively independent of the kinetic reaction mechanism [34, 63].
2.9. Comparison with experiment
Considering the kinetic processes involving the change of charge carrier densities during
thermal stimulation helps to explain the phenomena of TL and TSC. The experimental
results can sometimes be analysed in simple kinetic models which allow the determina-
tion of some trapping parameters of the solids. Moreover, the analysis should yield
information on thermal relaxation processes and on the structure of defects. The useful-
ness of such an approach, however, is questionable. In different kinetic models a reason-
able fit to experimental results can also be obtained by suitable variation of the para-
meters. This means that, unless the model which is applicable to the solid and the specific
problem in question is known beforehand, any particular process can be analysed in a
large variety of ways.
Therefore the atomic processes and structures must be studied first in greater detail.
As well as TL and TSC other techniques must be performed to obtain information on
optical, dielectric and magnetic properties. Only if the mechanism of charge and energy
transfer and the defects are well understood can one try to construct a specific kinetic
model. The following theoretical treatment consisting of an analysis of TL and TSC data
Theory 33
is performed not to obtain further information but only to confirm the existing atomic
picture.
In the following example the electron paramagnetic resonance (EPR) technique is used
in addition to TL and TSC [67]. The thermally stimulated processes of a specific glow
peak in an x-rayed BaWC>4 crystal are analysed in the above-mentioned way. After
x-irradiation at 80 K the EPR spectrum exhibits several lines due to the (WC^)
3
.
-
com-
plex [65, 66]. From the small positiveg shift which is characteristic of orbitals which are
more than half full a defect electron is assumed located in a completely occupied oxygen
orbital. An isotropic hyperfine line originates by the interaction of the hole and
183
W
nuclei (natural abundance 14.3%). From the intensity of the lines a simultaneous interac-
tion with two equivalent
183
W nuclei must be assumed. This leads to the model of a 'self-
trapped hole' spread over two neighbouring WO4 tetrahedra. Thus the centre is related to
the V
k
centre in the alkali halides.
Another line accompanied by two satellites of relative intensity 7.14% can be detected
in the high-field region. The relative intensity corresponds exactly to that calculated for
the interaction with the tungsten isotope
183
W. Thus this centre is associated with a W
5+
in
a WO|~ complex.
The thermal stability of the centres is studied using the fractional heating technique.
The x-irradiated crystal is heated up to a fixed temperature and the density of centres
is then determined at 80 K again. The results are shown in figure 2.12. The hole centres
disappear completely in the temperature region between 90 and 105 K. A corresponding
decrease of the electron centre W
s+
is observed but the concentration only decreases to
one-half of the initial value. Further heating gives rise to a complete decrease of the W
s+
centres.
In the same temperature region the TL glow curve shows one maximum which can be
correlated with the decrease of centres. As well as the TL a glow curve of TSC is also
90 100
TEMPERATURE ( K)
110
Figure 2.12. Relative concentrations of hole centres (a) and W
s+
centres (6) in x-rayed
BaW0
4
crystals measured after annealing at the temperatures given on the abscissa.
34 M Bohm and A Scharmann
obtained after xirradiation (figure 2.13). The shape of TSC peak is nearly identical with
that of TL . The peak temperature of TSC shifts to a higher temperature only by about
0.6 K. The small halfwidth is another important feature of these peaks.
102 103 104 105 106 107
TEMPERATURE(K)
Figure 2.13. Thermoluminescence (TL ) and thermally stimulated conductivity (TSC) of
BaWO, crystals measured simultaneously after xirradiation at 90 K.
It can be assumed that the migration of hole centres is due to warming the crystal
above 80 K. This means that a thermally activated hole is recaptured at an adjacent site
into an occupied t! orbital. This hopping process is to be considered as the diffusion of
small polarons. The mechanism of recombination in TL can then be described by a transi
tion of an electron from a W
5+
complex to an adjacent hole centre. The assumption is
based upon the fact that the thermal decay of hole centres can be correlated with that of
W
5+
centres.
The motion of polarons can be explained in a model involving thermally liberated
electrons from traps. Thus, during thermal stimulation the kinetic processes are calculated
in rate equations based on the simplest kinetic model with only a single trap and recombi
nation level. As mentioned in 2.4 in the case of neglected retrapping the rate equations
are
q dh/dT=-ah (2.60)
q dn/dT=ah - ynf (2.61)
with a = a
0
exp(E/kT) and a = transition probability of a polaron, E = thermal activa
tion energy, h = density of hole centres, n = density of hopping hole centres,/= density
of electron centres W
s+
, and 7 = capture cross section for capturing a hole by a W
5+
ion
(recombination).
The exact computer simulation of TL calculated from equations (2.60) and (2.61)
yields a glow curve which exhibits an asymmetric shape and a very small halfwidth just
Theory 35
like the experimental one (see 2.8). However, in the case of TSC the agreement between
theory and experiment must be considered unsatisfactory. In the computer simulation
the TSC peak is shifted by about 2-3 K to higher temperatures with respect to the TL
peak whereas the measurement yields a shift of only AT = 0.6 K. Hence the kinetic model
is to be extended by precisely considering all experimental data.
As a result from the EPR measurements and fractional heating technique the initial
value of the density of recombination centres W
5+
is diminished only by 2/3 to 1/2 during
the thermal stimulation (figure 2.12). This result is considered in the kinetic model by the
assumption that the density of recombination centres is to be approximately constant
during the glow peak. This is the model described in 2.7 (see equation (2.42)). The
calculation results in identical glow curves for TL and TSC. This means that no shift of the
TSC peak is to be expected from this model.
As already mentioned this case is also discussed in a more common model with addi-
tional thermally disconnected traps M. In this the density of additional traps is to be
assumed as being large when compared with the density of traps involved in the TL
process (H/MKl). The computer simulation also shows identical curves of TL and
TSC [57]. The five-fold density of additional traps is sufficient to obtain equal shapes and
maximum temperatures.
In the cases considered so far retrapping is neglected. By assuming such retrapping
(j3/7>0) it is very difficult to obtain analytical expressions for TL and TSC. However, the
computer simulation succeeds in representing the intensities of TL and TSC without the
approximations commonly used. From the special case j3/y> l,H/M< 1 and fiH/yM< 1
the simulation shows equal behaviour of both thermally stimulated phenomena [57].
Hence, the glow peak in x-irradiated BaW0
4
at about 105 K may be approximately
described in both models due to EPR, TL and TSC measurements. From hopping processes
a retrapping may be assumed, as is proposed in the second model. However, this cannot
be decided from kinetic considerations.
In a more precise analysis of this glow peak the small but finite shift of the TSC peak
must be considered. This can be done in a qualitative manner [68,69]. Starting from
both possible cases (5/y = 0 and 0/ 7>O, respectively, equations (2.12) and (2.13) are
commonly valid. Combining these equations and eliminating the density of free carriers
n leads directly to the relation.
en
a = /. (2.62)
constant x jf
Let T^ be the temperature where the conductivity exhibits a maximum. Then one
obtains the condition at this temperature:
3a
37
= 0. (2.63)
Now, if one takes the temperature derivative of equation (2.62) and evaluates it at the
TSC peak 7^, where equation (2.63) is valid, one has
3/ / 3/
= at T=1%. (2.64)
3 7 / 3 7
36 M Bohm and A Scharmann
The quantities JJL and y are assumed to be temperature-independent. Using the facts that
the derivative of the density of recombination centres with respect to temperature is
always negative due to the decrease (9/ / 37' <0 at all temperatures) and the quantity
/ / / i s always positive one notes from equation (2.64) that
3/ / 3r <0 at T=T^. (2.65)
This expression indicates that the TL showing a negative slope is decreasing at the TSC
peak. It means that the TSC peak is at higher temperatures than the TL peak. Thus, the
smaller the slope of TL (dl/dT) is at T= T^, the smaller is the shift of the TSC peak. The
small slope of the TL curve involves a slow decrease of recombination centres (df/dT).
Consequently, in the case of constant density of recombination centres (df/dT = 0) the
slope of the TL curve vanishes and no shift of the TSC peak occurs. Therefore the shift of
the two glow curves depends on the rate of decrease of recombination centres.
In BaW0
4
crystals the density of recombination centres W
5+
is not exactly constant
during heating and thus identical glow curves of TL and TSC cannot be expected. How-
ever, a complete decrease that gives rise to a shift of 2-3 K from computer calculations
is not observed but the density of recombination centres decreases partially (figure 2.12).
Hence, the TSC peak should be partially shifted to higher temperatures. The small
measured shift of only 0.6 K leads to the idea of partially decreasing recombination
centres. The good agreement between the experimental results and kinetic considerations
confirms the assumption that W
s+
ions act as recombination centres for thermally activated
holes.
2.10. Conclusions
In the literature many attempts have been made to calculate the related phenomena of
TL and TSC from a kinetic model primarily in order to study defect properties and to
have a tool for determining trapping parameters such as activation energies and frequency
factors. Because of the changes in densities of electrons and holes during the thermal
stimulation, the calculations are based on a simplified energy level scheme in the different
phenomenological theories. The differential equations are usually solved in an approxi-
mate way with the assumption that the density of the free carriers is small compared
with that of trapped carriers during stimulation. However, even in the simplest model
consisting of a single trap level and a recombination level, the analytical solutions seem
to be reasonable only for TL. The shape of TSC has also been calculated in some cases,
however, by the introduction and variation of additional parameters such as non-radiative
transitions or additional thermally disconnected traps.
An exact solution has shown that neither of these additional assumptions are necessary.
The simplest model is sufficient to explain the observed phenomena. As a consequence,
the influence and magnitude of such additional effects cannot be concluded from TL and
TSC measurements alone. Only if these measurements are related to studies on other opti-
cal, electrical and magnetic properties of the sample will the experimental results provide
a reasonable basis for a discussion of the electronic processes in solids. The present and
probable future importance of the studies of TL and TSC depends on a strong inter-
relation with other branches of solid-state physics.
Theory 37
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Applied Thermoluminescence Dosimetry. Eds M Oberhofer and A Scharmann
1981 ECSC, EEC, EAEC, Brussels and Luxembourg
3
Instrumentation
H W JULIUS
3.1. Introduction
This chapter deals with the instrumentation used to evaluate thermoluminescence
dosemeters. The basic phenomenon of thermoluminescence dosimetry, i.e. the stimula-
tion of light by heating the phosphor after it has been exposed to radiation, takes place
in the reader instrument.
The method of reading a TL detector is simple and straightforward. In a relatively
short time (usually ranging from a few seconds to a few minutes) the TLD is heated from
ambient temperature to some 200-300 C, and the emitted light is measured quantita-
tively. Thus the reader consists essentially of two basic parts:
(i) a heating device, and
(ii) a light detecting system.
Constructing a reader instrument would therefore be easy if there were not so many
pitfalls in the TLD method, such as:
(i) The method is a destructive one, i.e. the radiation energy absorbed in the detector
(or at least most of it) is lost during the readout procedure. Care should therefore be
taken not to lose information.
(ii) The behaviour of a TL detector (such as its sensitivity and fading characteristics) is
substantially dependent on its thermal history. This means that especially when no
post-read (pre-irradiation) anneal is applied the response of a TLD after re-use is
influenced by the heat treatment during the previous readout.
(iii) Thermoluminescence dosimetry is a relative method, and therefore attention
should be paid to high stability, combined with frequent calibration.
(iv) Because of surface-related phenomena, the light emitted tends to be contaminated
with non-radiation-induced signals (chemiluminescence) which, when not suppressed,
restrict the lower limit of detection.
The TLD method has a wide range of applications, many of which have special
requirements as far as the evaluating instrument is concerned. Some fields of application
are:
(a) personnel monitoring (requiring badges),
(b) environmental dosimetry (requiring high sensitivity),
(c) patient dosimetry in radiotherapy and x-ray diagnostics (requiring wide dose ranges),
(d) age determination (requiring relatively large amounts of TL material),
(e) military dosimetry (requiring special dosemeters and the use of portable instruments),
etc.
40 H W Julius
These subjects are dealt with in detail in the corresponding chapters in this book.
In general, different requirements hold for instruments used for research purposes (i.e.
for the investigation of TL materials) and large-scale routine dosimetry. In the first case
the recording of the light output as a function of temperature (or time) ('glow curves')
will be made, requiring well-controlled temperature/time profiles, while speed is of no
importance. In the second case the primary concern is high-speed operation (thus fast
heating and preferably automatic loading and processing of detectors is needed), to
provide a large throughput.
Some systems are specially designed to cover special applications, while others are less
or more versatile. A large number of TLD systems have been developed in recent years,
partly by industry, partly by laboratories and organisations for their own use (of which
some are commercially available). Although not all of them can be mentioned, some
systems are reviewed, after the principles of TLD instrumentation have been discussed.
3.2. The heating system
3.2.1. General
One of the essentials in heating a TL detector in the reader is that there should be
optimal thermal contact between the heating medium and the detector. Insuffi-
cient thermal contact tends to lead to irreproducible results. The way a TL detector
follows the temperature of the heating medium depends on the thermal capacity
and the thermal conductivity of the detector material. Loose powder, extruded ribbons
or rods and sintered or compressed materials have, in general, good thermal conductivity.
Materials of this kind usually have well-defined geometrical shapes, so that they can
easily be brought into good contact with the heater. In contrast, detectors made of
phosphors embedded in Teflon (PTFEI"), such as LiF-Teflon discs and rods, have low
thermal conductivity. These materials tend to crinkle or curl up during heating. Good
thermal contact is then more difficult to achieve, especially when they are heated in a
tray, so that special precautions are needed (see 3.2.2.1 and 4.2). This is even more
important when glow curves are taken for research purposes, because large temperature
gradients tend to blur out details in the light output as a function of temperature.
Often the total heat treatment of a TL detector is considered as being split up into
three different steps:
(a) The pre-read heating, applied in order to remove completely the low-temperature
peaks in the glow curve, i.e. to empty the low-energy traps (the release temperature
of the electrons being at or below about 100 C, and hence being subject to fading).
(b) The readout procedure itself.
(c) The post-read (or pre-irradiation) anneal, applied either to remove all residual signals
from the dosemeter and/or to restore the trap distribution in the lattice in order to
restore the original TLD properties (sensitivity and fading characteristics).
These three steps are frequently performed separately, using ovens (see 4.10) for
(a) and (b). They can, however (and sometimes are), combined in one single read-anneal
f Polytetrafluoroethylene.
Instrumentation 41
cycle in the reader instrument, which therefore must be equipped to perform a flexible,
programmable heat cycle, so that it can be adapted to various materials.
As far as the pure readout cycle is concerned, several philosophies and approaches have
been developed.
In the early days a linear temperature rise was applied in most TLD readers used for
both scientific purposes and routine measurements. This method (which is still in use)
permits glow-curve analysis, the light output being plotted against time, and hence
allowing the various peaks to be associated with temperature. In most cases the (variable)
temperature ramp is followed by a plateau, the height and duration of which can be set
on the reader panel. Response measurements can often be done by choosing a distinct
temperature (or time) interval for the integration of the luminescent signal (figure 3.1).
For large-scale routine measurements, this method tends to be too time-consuming. A
rapid rise in temperature usually not linear against time is then preferred (figure 3.2).
-PLATEAU
-LIGHT
INTEGRATION
ti t
2
t
3
TIME
Figure 3.1. Linear heating, combined with a plateau. The temperature (or time) interval
during which the light output is measured can be varied. (I) temperature, (II) light output.
- IU sec
Figure 3.2. Non-linear heating. Maximum temperature and measuring time are variable.
(I) temperature, (II) light output.
42 HW Julius
As long as the characteristics of the dosemeter are not adversely influenced, there is
only one requirement for the 7X0 function: that it should be highly reproducible.
Generally, it is not easy to select a special integration interval, as the luminescence
begins too quickly. A pre-read heat treatment can, if necessary for a large number of
dosemeters, be performed in an oven. The same holds, of course, for the post-read anneal.
Figure 3.3 shows the multiple plateau heating method, in which the three steps (a), (b)
and (c), mentioned earlier, are combined.
LJ
3
I
<
CE
Ld
Q.
UJ
i
PREHEAT
300
210-
L
100
I S
' I "
I
<.ooc I
I
27 0 C j
!
-150C \l/\
-J\J
READ
I
I
I
1 -
1 /
w
f
Vin
^*,
ANNEAL
" 1
1
1
1
'/
I )
COOL
v
\
\
3
Q-
I
o
X
o
TIME
Figure 3.3. Preheat, read and anneal are combined in one single programmable heat cycle.
The various plateaux can be reached either linearly or non-linearly. (I) temperature, (II) light
output.
As pointed out earlier (3.1), the thermoluminescence response may be contaminated
by spurious (non-radiation-induced) signals, due to excitation of impurities at the surface
layer of the detector (chemiluminescence). This effect can be suppressed by heating the
TL detector in an inert-gas atmosphere, for which purpose pure dry nitrogen gas
( 0.5-1 lmin~')is most commonly used (see also 4.3).
3.2.2. Heating methods
This subsection deals with various methods of heating thermoluminescence dosemeters.
For the sake of simplicity they are discussed under different headings, although combina-
tions are encountered in versatile instruments.
3.2.2.1. Controlled planchet heating
The most common method of heating is still the one using a low-thermal-capacity (hence
thin) metal planchet (tray), on which the dosemeter is placed (see also chapters 4 and 7).
The heating power is generally provided by a low voltage-high current transformer. The
planchet can be heated indirectly (see below) but it generally acts as the heater element
itself, in which case it is connected across the transformer secondary winding, closing the
circuit with some 10 mD. after it has been brought into the readout position. Therefore,
the tray is placed in a drawer assembly by which it can be pulled out and pushed into
the reader for (un)loading and reading, respectively (figures 3.4 and 3.5). The shape of
Instrumentation
43
TL D -
PLANCHET
SAMPL E D RAWER/
TEMPERATURE
SENSOR
-LIGHT DETECTOR ( PM )
OPTICAL SYSTEM
( INCL . L ENSES, MIRROR
AND FIL TERS )
LIGHT SOURCE
* - I NERT GAS
TRANSFORMER HEATER CONTROL
Figure 3.4. Schematic set-up of a conventional type of TLD reader with controlled planchet
heating and sample drawer system. This principle is encountered in a number of commercial
instruments.
Figure 3.5. Example of a sample drawer with planchet and TLD chip.
the planchet car. be adapted to the form and size of the TLD. Both solid forms and loose
powder can be used.
Because of the low thermal capacity of the heater planchet, it is relatively simple to
control its temperature versus time profile, just by controlling the generating voltage.
A thermocouple is used to give a negative-feedback signal to the voltage control unit. A
practical problem is to obtain good contact between the thermocouple junction and
the heater element. Welding the thermocouple to the planchet itself gives adequate
contact but makes the tray less easily interchangeable. When the thermocouple is simply
mechanically pressed against the planchet, thermal contact is not reliable and hence
heating is not reproducible. A solution for both problems has been found in heating the
tray indirectly by means of a separate heater element which can be brought into close
contact with the planchet. The thermocouple is then welded to the heater element.
44 HW Julius
Instead of thermocouples, infrared sensors, mounted underneath the planchet, have
been used. Although thermal contact problems are avoided, this technique is not entirely
satisfactory, because the sensitivity of the sensor can change, due to obstacles in the
optical pathway (dust) or changes in the IR emitting property of the planchet.
The low-thermal-capacity heating method is very suitable for programmable heating
cycles (see figures 3.1 and 3.3), so temperature ramps, plateaux, time intervals (ranging
from about 20 s to over 1 min), etc can be set on the instrument, so that for each
TL material the optimal readout procedure can be chosen (by trial and error). Although
this seems to be an ideal situation, one should keep in mind that, if low residual dose
and satisfactory fading characteristics can be achieved with a simple readout cycle and
they often can reproducibility of the heat treatment is the most essential parameter to
focus on, to obtain reliable results.
A substantial problem associated with the planchet method is to get sufficient and
reproducible thermal contact between the heater and the detector. This is especially true
for large PTFE disc-type dosemeters and even more so for thin ones. To hold the TLD tight
against the tray, various techniques have been used, most of them applying some device
on top of the dosemeter, so that the detector is 'sandwiched' between two layers. Springs,
meshes, cruciform apertures, rings and quartz glass discs are used for this purpose. In
some instruments these devices are made part of the heating system, so achieving lower
temperature gradients. Obviously, these prevent a fraction of the emitted light from
reaching the light detector. This is acceptable, provided this fraction is reproducible. An
alternative solution is to hold the detector in place by suction.
Several TLD readers use a lens system to focus the TL light on to the cathode of the
PM (see 3.3). Reproducible positioning of the detector is then of greater importance.
Care should be taken to keep the surface of the planchet clean, since changes in its
reflectivity result in changes in effective light output of the TLD, in particular when
transparent materials are used (see 7.2.1).
IR light emitted by the tray when reaching the maximum readout temperature can
add a spurious signal to the emitted TL light. This will lead to high and usually irrepro-
ducible background signals, which of course limit the lower detection threshold.
3.2.2.2. The heater block method
An analogous method for heating the TLD uses a metal block ('hot finger'), held at
a constant sufficiently high temperature by a resistive heater element, which is brought
into contact with the detector. Some advantages of this method are fast heating rates
(hence short cycle times; some 10 s are typical) and simple and reliable construction.
Because of the lack of flexibility, this technique is obviously not suitable for research
purposes, but is quite popular in personnel monitoring systems. Since an appreciable
amount of electric power is dissipated in the reader, cooling the photomultiplier tube is
unavoidable in practice.
The way in which the TLD is brought to or held in its readout position depends on the
design of the dosemeter holder. Sometimes the detectors are stuck on an adhesive Kapton
tapef, while in other systems they are mounted in a metal plate, either sandwiched
between two thin Teflon foils, or fitted by a clamping ring. An individual monitoring
f Polyimide film with a pressure-sensitive silicone polymer adhesive on one side.
Instrumentation 45
system has been developed which uses dental-size TLD plaques (Teflon embedded with
phosphors). Different areas of the dosemeter can be read by applying local heating with
blocks (see also 4.2).
The hot finger method can also be used to read loose solid TLD and powder, in which
cases thin platinum trays are used.
3.2.2.3. Hot gas heating
In the late 1960s the idea was born of using nitrogen gas applied in most TLD readers
to reduce chemiluminescence to heat the dosemeter (figure 3.6) [12]. The obvious
advantage of this method is the almost perfect thermal contact between the detector
and the heating medium, independent within certain limits of the form and shape
of the dosemeter. The TLD, generally brought into the heating cavity by means of a
vacuum needle, is heated by one or more hot nitrogen gas jets. In the first case only small
TLD (up to 6 mm in diameter) can be read, while the latter can also read the larger disc-
type dosemeters (12.7 mm diameter). Other advantages of hot nitrogen heating are a
short heating cycle (about 10 s), low background signal, excellent reproducibility, easy
loading procedures (which make automation a matter of course) and high versatility
(ribbons, discs and rods can be read without interchanging instrument devices).
Disadvantages are similar to those of the hot finger system: the heating cycle does not
lend itself to programming (the gas temperature rigorously being kept constant), and thus
the method can be used only for routine measurements.
FRONT VIEW
1 - FURNACE
2 - THERMOCOUPLE
3 - BRASS TUBE
t - PYREX GLASS READOUT CHAMBER
5 - EXTRUDED TLD LiF
6 - VERMICULITE INSULATION
7 - WATER-COOLED JACKET m^zj
8 - LISHT TRAP " ^ *
9 - REMOVABLE BRASS CARTRIDGE
10- ROTATING STAGE
11 - ESCAPEMENT
12 - ELEVATOR
13- VACUUM HOLDING PROBE
U - MOTOR
15 - LENS SYSTEM
16- VACUUM LINE
17 - CAM FOLLOWER
16 - PM TUBE
19- MAIN DRIVE MOTOR
2 0 - FLOWMETER
SIDE VIEW
Figure 3.6. An example of a TLD reader, using hot nitrogen gas to heat the detector (after
Petrock and Jones [12]). Variations on the theme have been utilised by others.
46 H W Julius
Instrument parts in the immediate vicinity of the heating cavity get warm, so that
cooling (for instance, of the PM tube) is necessary. Obviously, powder cannot be handled
unless it is sealed in small glass bulbs. In this case, there is no direct contact between the
heating medium and the phosphor, so that hot air can be used instead of nitrogen.
3.2.2.4. RFheating
A TLD system has been designed which uses RF heating [5]. The thermoluminescent
material is sealed on to a graphite tray using silicone resin adhesive. The dosemeter is
brought (by a drawer system) to above a flat, water-cooled RF coil (1 MHz), where it
reaches its maximum temperature (300C) in about 10 s. In principle, this heating
method allows the collection of the light emitted from both sides of the dosemeter.
Using a specially designed dosemeter and two photomultipliers, both surface and pene-
trating doses can then be measured simultaneously. (The author is not aware of whether
this has in fact been done.) Disadvantages of the RF method seem to be the large amount
of RF power necessary, and the difficulties of controlling the heat cycle.
3.2.2.5. Optical heating
Several years ago a projector bulb was used to heat the TLD [2], The method was
abandoned because of problems associated with spurious light from the heater. Recently,
new life has been given to the method. In a TLD system, specially designed for personnel
Figure 3.7. Examples of glass bulb TL doscmeters with built-in heater elements, (a) Phosphor
directly bound to the heater, (ft) Phosphor fixed on to the outer surface of a hollow cylinder
indirectly heated by a filament, (c) Extruded or hot-pressed phosphor in close contact with
the heater element.
Instrumentation
47
dosimetry, detectors are used consisting of a thin layer of crystalline phosphor, bound to
a polyimide film, which on the back side is coated with a light- and iR-absorbing carbon
layer. By irradiating the latter with a pulsed IR beam, the detector can be heated in 0.6 s.
The TL light is emitted and measured within 1.5 s (figures 3.27 and 3.28).
3.2.2.6. Built-in heater element
Although this method has less to do with instrumentation than with the design of TL
dosemeters, it will briefly be discussed here. Examples of dosemeters with built-in heater
elements are usually in the form of a subminiature evacuated radio tube or a fuse-type
glass bulb. Within the bulb the phosphor may either be directly bound to the resistive
heater or fixed on to the outer surface of a hollow cylinder which is indirectly heated
by a filament. A third option is to bring the solid TL detector into close contact with the
Figure 3.8. Drawer assembly for glass bulb TL dosemeter insertion.
Contact pi r . sv^
Figure 3.9. Glass bulb TL dosemeter adapter for dosemeter types (a) and (c) shown in
figure 3.7.
48 HW Julius
wires of a built-in heater element (figure 3.7). By introducing the dosemeter into the
reader instrument, the contact pins (or caps) are connected to the heater voltage supply
(figures 3.8 and 3.9).
Some advantages of these dosemeters are good thermal contact between the phosphor
and the heater element and consequently good reproducibility, and sturdiness of the
dosemeter assembly (which is of greater importance in military applications).
Some disadvantages are a low-energy cutoff due to the glass encapsulation, self-
irradiation (which, however, can be minimised by using glass with low potassium content
[11]), and high cost. Moreover, most types are fairly bulky.
3.3. The light detecting system
3.3.1. General
The technique of light detection is well known and not specific to TLD. The light measur-
ing system does not affect the TL detector during readout as the heating system does
and therefore this part of the reader has less to do with the pitfalls of thermoluminescence
dosimetry. Nevertheless it should be given attention because of the large dose range to be
covered (from a fraction of a millirad to several kilorad or even megarad) and the
precision (and hence stability) required in radiation dosimetry.
The general task of the light detecting system is to convert the light emitted by the TL
detector into an electronic signal (charge, current, voltage), which can be measured and
used to activate output devices (meter, scaler, printer, chart recorder, computer, etc).
The light detecting system can be thought of as being divided into three parts:
(i) The light collecting system,
(ii) The light detector and signal amplifier,
(iii) The signal conditioning system.
In figure 3.10 a schematic diagram of the light detecting system is shown.
CURRENT TO FREQUENCY
C0NVERT0R
ELECTRO METER
PHOTON COUNTING
HIGH VOLTAGE
POWER
SUPPLY
LENS
I AND/ OR MIRROR)
TLD OR LIGHT SOURCE
HEATING SYSTEM
SIGNAL
CONDITIONING
SYSTEM
LIGHT DETECTING
SYSTEM
LIGHT COLLECTING
SYSTEM
INITIAL
SIGNAL
Figure 3.10. Schematic diagram of the light detecting system of a TLD reader.
Instrumentation 49
3.3.2. The light collecting system
In order to achieve maximum detection efficiency, the first aim is to concentrate as
much luminescence light as possible on the sensitive layer of the light detector. It would
in principle be most efficient to bring the TLD into direct contact with the photocathode.
However, because of the temperature sensitivity of the photocathode, thermal separation
is necessary. To achieve this, several methods have been applied, using lens systems, heat
filters, water layers, vacuum layers, light pipes, etc. Easy thermal separation is attained
when the light detector is placed beside the heating system instead of above it in order to
avoid heat transport by hot air (a mirror system can then be used).
The optical system is preferably designed in such a way that light collection is
minimally affected by changes in the position of the dosemeter.
Optical filters are frequently applied in order to prevent infrared radiation emitted
by the heater elements or the TLD itself reaching the light detector.
Sources of error in the light measuring system are introduced by obstacles (dust) in the
light path or changes in reflectivity of the heater planchet or parts of the optical system.
3.3.3. The light detector and signal amplifier
The light emitted by a TL detector after being exposed to 1 mR is of the order of
10"
I3
lm. Up to now solid-state photodetectors are not sensitive enough to allow the
measurement of such low levels and therefore only photomultiplier (PM) tubes are
considered to be applicable in TLD. They combine high sensitivity and large dynamic
range (l(T
13
-10~
6
im).
A PM tube is chosen for optimal cathode sensitivity, matching the wavelength typical
of the TL material under consideration. As an example, LiF emits in the blue-green
region, whereas Li
2
B
4
0
7
emits in the red. For optimal results, these materials require
different PM tubes. A low response to other wavelengths, especially IR, is preferred.
Figure 3.11 gives an example of PM tubes with various spectral responses.
Sensitivity and signal-to-noise ratio are affected by a number of parameters. Some of
them are now dealt with briefly.
Dark current is the signal which is generated by the PM while light is absent. The
phenomenon is mainly due to thermal emission of electrons from the cathode layer.
PM tubes, even of the same type, may show large variations in dark current, a reason
why they are preferably selected for low noise. The remaining dark current is kept as
low as possible by operating the tube at low temperature (Peltier cooling is generally
used).
Temperature effects. Changes in temperaure affect the overall sensitivity of the PM
(approximately 1%C
_1
). The tube should therefore be kept at constant temperature.
Fatigue effect. If the PM is exposed to large light intensities, its sensitivity decreases,
while the dark current increases. The effect of PM fatigue gradually vanishes over a period
of hours. Errors may be introduced if reference light sources of high intensity are used.
Aging effects. After long use the gain of the PMT gradually decreases. In addition to
long-term gain drift, a slow shift in spectral response may occur. If the sensitivity is cali-
brated with a reference light source, the spectral emission of which deviates significantly
from the wavelength of the luminescent light, errors can be introduced. (See also
3.3.5.)
50 HW Julius
^ x ^ ^
^ \ ^
\
, - 5- 20
r S-20
k 96S&
\ L- EXTENOED
L \ \
s
"
20
\ V-s-io\ \ \
\\ V
s
"\\ \
\ \ I
s
" " \ \ \ \
0.5 0.6 0.7 0.8
WAVELENGTH MICRONS
Figure 3.11. Typical spectral response curves for PM photocathodes (EMI, 50 and 30
diameter tubes).
Magnetic fields may affect the PMT sensitivity due to changes in focusing. In this
respect, magnetic fields generated by the heating power are often the culprit, especially
when DC currents are used. These effects can be reduced by using a cylindrical mumetal
screen, surrounding the PM tube, which is kept at cathode potential.
Discharges, mostly resulting from toohigh tube voltages, may cause charge bursts at
the anode, due to light emission associated with the discharge. As a result the background
signal is affected in an unpredictable way.
High tension variations have substantial influence on the PM sensitivity: 1% change in
high tension may cause some 10% change in gain.
Current leakage which may occur at various locations in or at the surface of the PM
tube may cause apparently high dark currents. Cleaning the connector pins may some
times redress the problem.
3.3.4. The signal conditioning system
The signal conditioning system essentially serves to convert the PM signal into a quantity
which can be measured quantitatively. The PM signal (which is typically at the picoamp
level) generally needs further amplification. For the next step two methods can be
applied.
3.3.4.1. Peak height measurement
The height of the peak with maximum amplitude in the glow curve is taken as the
relevant signal. It is measured by converting the PM current into a voltage by which a
capacitor is charged. The (maximum) charge of the capacitor is then measured. Because
the height of the glow curve main peak depends strongly on the heating rate of the dose
Instrumentation
51
meter, this method requires extremely reproducible heat cycles (see figure 3.12). How
ever, the improved signaltonoise ratio is a real advantage in the case of low dose
measurement. Moreover, the lowtemperature peaks, which are subject to fading, are
omitted. Nevertheless, the method is seldom used.
200
150
100
50
y
y\
/L
/ ~ ^ ~
/
/
/
* INTEGRAL READING METHOD
x PEAK HEIGHT READING METHOD
i i i I
z
<
CD
<
4 5 6 7 8
FILAMENT VOLTAGE
Figure 3.12. Peak height and integrated peak area as a function of the heating rate for
CaF
2
: natural (after MBL E).
3.3.4.2. Peak area measurement
This is the method most often applied in thermoluminescence dosimetry. The PM signal,
having been digitised by a chargetopulse converter, is fed into a counter. The number of
pulses at the end of the readout time is proportional to the integral light output of the
dosemeter. A ratemeter, connected to the converter output, provides the signal used for
plotting glow curves. As can be seen from figure 3.12, this method is less affected by
changes in the rate at which the TL D is heated during readout.
As an alternative technique for measuring the integrated light sum, the method of
photon counting has also been (and is still) used. Although one would expect a better
signaltonoise ratio, theoretical and experimental investigations [10] have shown that
improvement by a factor of 1.4 is the maximum achievable.
3.3.5. The reference light source
The many sources of error discussed in the previous subsections make frequent sensitivity
checks of the entire system a matter of necessity. The safest way to do this is with TL
detectors, irradiated to a precisely known exposure (or dose). Both the light detecting
system and the heat cycle are tested in this way.
For more frequent checks of the sensitivity, a reference constant light source is
generally employed. It is placed at or near the normal position of the TL D (figure 3.4
shows an example). This can be done before each reading or at suitable intervals, either
by the operator or as dictated by an automatic control system. If correctly applied, this
method of system 'calibration' may trace changes in the optical pathway, changes in PM
52 H W Julius
sensitivity and malfunction of the electronic circuitry. Reference light source measure-
ments have been used for automatic checks of the overall system sensitivity.
Light sources are usually made of long-lived radio-isotopes (
14
C or '"Sr) embedded in a
scintillation material. Light emitted by the source should preferably have the same spec-
tral composition as that of the TLD material in use. It should be noted that most light
sources have outputs which are temperature-dependent. Errors may be introduced due to
changes in the light source itself or variations in the spectral response of the photo-
multiplier tube. The heating system remains unchecked. For more information on light
sources and the errors encountered with them, see 4.4, 7.2.1 and 11.4.
3.4. Special items
In the previous subsection only the two basic parts of a basic TLD readout instrument
have been discussed. Modern instruments, however, are usually equipped with, or can be
connected to, additional devices which extend their capabilities. Some of them are now
briefly reviewed.
3.4.1. Glow-curve plotting
As has already been pointed out, the analysis of the light output as a function of time or
temperature is essential if one wishes to investigate thermoluminescent phosphors. For
this purpose many TLD readers are provided with a special output of the ratemeter signal,
to which an X,Y or X,t recorder (plotter) can be connected. It is sometimes convenient
to use a pulse height analyser to record the (pulsed) TL signal against time, because the
digitised glow curve can more easily be prepared for (computer) calculations. The glow-
curve signal can also be fed directly into a computer for pattern recognition, which has
been suggested as being useful in routine dosimetry.
3.4.2. Output writing and response handling
Almost all TLD readers can be equipped with an output recorder, such as a simple printer,
teletype or similar device. Printing calculators can also be used. Some readers have built-in
electronic devices which can, for instance, subtract a predetermined background or can
multiply the response by a calibration factor (in order to give the output in terms of dose
or exposure). More sophisticated systems in particular the automatic ones sometimes
have the capability of setting a lower and an upper level (by thumbwheels or keyboard)
with which the response can be compared. The result of the comparison may cause an
alarm signal or a prolonged heating time, or can be used to select automatically detectors
with uniform sensitivity. Because such installations which are intended for large-scale
measurement are generally computer-compatible, all data handling and instrument
control is therefore preferably done by a minicomputer (or microprocessor).
3.4.3. Automation
After the method of thermoluminescence dosimetry proved to be successful in radiation
dosimetry, its applications developed explosively. Consequently, there is a growing
tendency towards automation.
Instrumentation 53
Two groups of automatic instruments can be distinguished:
(a) Systems particularly designed for personnel monitoring purposes. They are, in
general, merely capable of processing some special kind of TLD badge and no other
forms can be accepted. Badge handling includes identification decoding and reading
the dosemeter(s) in the holder, which may be controlled by a microprocessor or large
computer system for dose calculation and record-keeping of individual dose data.
The variety in the degree of sophistication, possibilities and approaches is so enor-
mous that they cannot be dealt with in any detail in the context of this chapter.
Some rough information can be found in 3.5.
(b) Systems particularly designed for automatic readout of loose solid TL detectors. At
the moment only a few systems of this kind exist (see 3.5). They all use a rotating
disc type of sample changer to present the TLD to the reader. Transportation of the
TLD to and from its readout position is done either by a built-in manipulator (such as
is used in hot gas readers) or by a separate device. It should be noted that the con-
ventional type of reader with a drawer mechanism can quite easily be transformed
into a semi-automatic instrument: a vacuum needle, mounted at the end of the
swinging arm, can take a TLD from a turntable and put it on the planchet (and vice
versa). The drawer is then closed and opened by a suitable device, operating in con-
junction with the loading system.
A TLD system has been developed which combines both reader types (a) and (b) in
the same instrument. For each application the proper sampling device should be chosen.
It is generally stated that the use of automatic readers is only justifiable when very
large numbers of dosemeters are to be evaluated. Although this might be true from the
point of view of financial investment, it should be emphasised that automation usually
improves accuracy considerably. Those who are familiar with TLD are aware of the many
pitfalls of the method and the fact that most of them are associated with manual
operation of the equipment and handling the dosemeters, which introduce irreproduci-
bilities in the procedure. Automation can, to a large extent, overcome these problems.
As was said before, the heat treatment of a TLD has a decisive influence on its future
behaviour. This holds true in particular for the post-read anneal. The greatest repro-
ducibility is therefore obtained by performing no annealing whatsoever and using a
single optimum heat treatment in an automatic reader.
3.5. TLD readers and systems
This chapter would not be complete without some review of available equipment. It is
obvious, however, that a complete compilation cannot be given. While preparing the
text, the author contacted all the TLD firms he knew of, in order to collect technical
data.
Reactions were very divergent, ranging from no answer at all to abundant information.
Both categories are represented in the following pages, where a short list of available TLD
equipment is given together with some technical information which is only indicative.
Performance data are strictly omitted. Further information should be obtained from
the manufacturers. The address list is given in 3.6.
54
HW Julius
3.5.1. Systems for the evaluation of loose TL detectors
3.5.1.]. Harshaw Model 2000 TL analyser
The system consists of two components: the Model 2000-A TL Detector and the Model
2000-B Automatic Integrating Picoammeter (figure 3.13). The system uses heater
planchets mounted in a sample drawer. The planchet temperature can be controlled,
providing various temperature profiles, which are divided into three steps:
(a) a rapid pre-heat, ranging from 50 to 400 C, followed by
(b) a linear increase of temperature, adjustable from 4 to 25 C s
_1
, for readout, followed
by
(c) a maximum temperature plateau (50-400 C).
Figure 3.13. Harshaw Model 2000 TL analyser.
The total integrating period can be chosen as either 10, 30, 60, 100 s or infinity.
The TL signal is measured as the integrated area under the glow peak, represented by
the total charge delivered by the PM tube during the read cycle (digital counter with
automatic ranging circuitry, showing three significant figures). The picoammeter has
output connections to drive recorders for glow-curve plotting.
The system is capable of reading powder, ribbons, rods and other forms of solid detec-
tors. A number of modifications (such as TL integration between two predetermined
temperatures) are optional. Various accessories are available.
3.5.1.2. Teledyne Isotopes Model 7300 TLD reader
The Model 7300 TLD reader (figure 3.14) is a manual instrument using the conventional
sample drawer system to insert the detectors. The dosemeters are heated by means of
interchangeable metal trays which follow a controlled temperature profile, which is
Instrumen tat ion
55
Figure 3.14. Telcdync Isotopes Model 7300 TLD reader.
divided into four steps:
(a) a pre-heat cycle of 7 s (150 C),
(b) a readout cycle of 12 s (linear ramp to a plateau),
(c) an anneal cycle of 20 s (310 C),
(d) a cool period of 18 s (down to about 100 C),
The user may either make a selection from three pre-fixed temperature programmes,
each adapted to a special dosemeter (of the phosphor-Teflon type manufactured by
Teledyne Isotopes), or use the manual mode (maximum readout temperature adjustable
from 150 to 350 C). Sensitivity, calibration, background (automatic subtraction),
exposure range and nitrogen flow are set by manual controls (all protected by a door in
the front panel to avoid inadvertent changes). A serial binary code decimal ( BCD) output
of the display on the front panel and a print command are provided.
3.5.1.3. Pitman Toledo Model 654 TLD reader
The basic principle of the Toledo reader (figure 3.15(a)) is the same as in the two
previous instruments. The dosemeter, when put in a metal tray, is shifted towards its
readout position by means of a drawer system. In contrast to other readers, the tray is
heated indirectly by a separate heater element which is brought into contact with the tray
after the drawer has been closed.
Two interchangeable modules are available to control the heat cycle. The standard
module has a preprogrammed three-step temperature profile (of which the pre-heat and
anneal cycles can be switched off). With the research module the programme can be
widely varied by the user (two to four steps - which include controlled cooling - and
eight variables). The Toledo uses a feedback circuit to stabilise the sensitivity, using an
internal reference light source. This system compensates automatically for HM gain drift,
changes in the signal conditioning system and the light collecting system.
The reader is also equipped with systems for background subtraction and sensitivity
adjustment, both controlled by thumbwheels.
56 HW Julius
^Sf WWW
(a) (b)
Figure 3.15. (a) Pitman Toledo Model 654 TLD reader. (6) Pitman automatic sample
changer attached to the Model 654 TLD reader (by courtesy of D A Pitman Ltd).
The manufacturer has various accessories available, among which is an automatic
sample changer for up to 30 dosemeters (readout time 30-40 min) (figure 3.15(b)).
3.5.1.4. TNO hot gas automatic TLD reader
This instrument (figure 3.16) uses three hot nitrogen gas jets to heat the dosemeters. Solid
TLD (of any form) are brought into the heating cavity by a vacuum needle, mounted in a
motor-driven manipulator (figure 3.17). The detectors can, for example, be presented to
the reader by a turntable (maximum content 200 TLD), placed underneath the balcony,
through which the vacuum needle protrudes. Evaluated TLD can be unloaded and new
ones loaded during continuous operation. Readout time (normally 10 s) and (constant)
gas temperature can be adjusted. Typical total cycle time is about 18 s. When operating
in automatic mode, the reader checks all relevant parameters (gas temperature, nitrogen
flow, sensitivity, vacuum) continuously and stops if one of them is outside the range.
Responses can be given in terms of net dose or exposure by automatic background
subtraction and multiplication by a calibration factor. The proper values are introduced
by means of a keyboard. Values for lower and upper levels (also keyed in) may be used
for special functions, such as automatic anneal and selection of dosemeters with uniform
sensitivity (two-way ejection). Output connections are available for control by teletype,
(micro)processor or other devices.
3.5.1.5. Harshaw automated TL analyser system (ATLAS)
The ATLAS consists of a Model 2000-D TL Detector, a Model 2000-B Automatic Inte-
grating Picoammeter, a vacuum pump and a printer. A heated laminar flow of nitrogen
gas is used to heat the TLD elements (chips). A turntable disc, which can accommodate
50 elements, is inserted into the Model 2000-D unit and the cover closed. The TLD are
brought into the readout position by a vacuum probe which protrudes through holes in
the turntable and lifts the detectors into the reading chamber. One 50 element sequence
Instrumentation
57
. ^MWW******M*V
COOLING
( O)
TL D
N2 OUTL ET
NEED L E
PISTON
D RUM
CUBIC BOX
( EMERGENCY EXIT)
TL D - HOL D ER
SAMPL E CHANGER
(6)
Figure 3.16. Schematic diagram of the TNO automatic hot gas TLD reader, (a) TLD
exposed to three hot nitrogen jets, (b) Manipulator, mirror and PM tube.
Figure 3.17. TNO automatic TLD reader with sampling mechanism for loose detectors
with automatic chip loader.
58 HW Julius
is completed in approximately 12 min. Key parameters are monitored continuously and
will stop the system and prevent further operation if a fault is detected. The system
sensitivity may be checked whenever the system is not processing dosemeters by using an
internal reference light source. The instrument is shown in figure 3.18. The mechanical
set-up is based on the one shown in figure 3.6.
Figure 3.18. Harshaw automated TL analyser system (ATLAS).
3.5.1.6. Therados TLD- 10 system
This system (figure 3.19) is designed specifically for in vivo dosimetry at the therapeutic
level. It uses probes made of
6
LiF-Teflon enclosed in Teflon tubes of various lengths.
For readout the tubes (a number of which can be connected up to a maximum length of
2 m) are put in a magazine, from which they are transported with constant speed towards
the readout position. Heating takes place in two sequential steps (pre-read anneal and
readout) by two separate ovens through which the tubes are led. The individual TLD are
separated by steel balls which are sensed by an inductive element by means of which
sequence numbers are generated. The system is equipped with a special calibration source
(175 mCi ^Sr) by which the tubiform dosemeters are irradiated.
3.5.1.7. Victoreen 2810 TLD reader
This is a versatile manual instrument (see figure 3.20) capable of reading hot-pressed
chips and rods, glass-encapsulated rods and glass bulbs (specially meant for environmental
dosimetry). Readout cycles are built-in for both LiF and CaF
2
: Mn dosemeters. Cycles
for other TL materials are programmed using auxiliary controls. The calcium fluoride glass
bulb dosemeters are heated by constant current. The optical system has a conical
reflector which collects 90% of the luminescent light. The instrument uses both peak
height and integral readout methods. The dynamic range covers over seven decades,
displayed on a 3 \ digit autoranging scaler.
Instrumentation
59
Figure 3.19. Therados TL D10 system for therapeutic dosimetry (by courtesy of Instru
ment AB Therados). . ' ; ' . . " '
Figure 3.20. Victoreen 2810 TL D reader (by courtesy of Victoreen, Inc).
3.5.2. Personnel dosimetry systems
At present there are a number of systems for personnel dosimetry, most of them being
more or less automatic. Except for one, all of them are socalled closed systems, i.e. they
are designed to handle only one special type of personal TL D badge (eventually in various
configurations) as supplied by the manufacturer. From the point of view of individual
monitoring, the heart of each system is the badge itself, a discussion of which, however,
would go far beyond the subject of this chapterf. From an operational point of view,
degree of automation, speed, versatility, etc and hence the instrumental aspects are
of great importance. It will be clear that a careful description of individual dosimetry
systems cannot be given without a detailed discussion of both personal dosemeters and
the evaluation system, which would require a separate article (or several) for each of
them. As a consequence, and because an incomplete description would not do any system
justice, the author has decided to provide only a short list.
f For more information the reader is referred to chapter 10.
60
HW Julius
3.5.2.1. Harshaw 2271 automated personnel monitoring TLD system (figure 3.21)
Dosemeter
TLD card ( 3x4 cm
2
) with two chips, sandwiched in Teflon foils, BCD punched hole
identification. The card is worn in a holder. Cards are stacked in a magazine for read-
out or inserted by hand.
^TL D CARD LOADER
TLD CARD RECEIVER
Figure 3. 21. Harshaw 2271 automated personnel monitoring system.
System components
Detector/dosemeter identifier
Automatic integrating picoammeter
Card loader and cartridge
Card receiver and cartridge
Digital comparator
Heating method
Hot finger
Badges are stacked in a magazine.
3.5.2.2. Harshaw 2276 microprocessor-controlled TLD system (figure 3.22)
Dosemeter
TLD card ( 3x4 cm
2
) with four chips, sandwiched in Teflon foil. Identification by
bar code with Arabic numeral equivalent. Cards, worn in a holder, are stacked in a
magazine for readout.
System components
Transport module
Logic module (microprocessor)
Automatic integrating picoammeter
Heating method
Hot finger
Instrumentation
61
Figure 3.22. Harshaw 2276 microprocessor-controlled TLD system.
3.5.2.3. Teledyne Isotopes 9100 automatic TLD reader (figure 3.23)
Dosemeter
'Radi-guard' multi-area phosphor embedded in Teflon ( 3x4 cm
2
) with four readout
areas and four backup areas. Identification by Arabic numbers printed on the detector
surface, TLD plaque, wrapped in a plastic envelope, is worn in a holder with filters.
Bare TLD are stacked in a holder for readout.
Figure 3.23. Teledyne Isotopes 9100 automatic TLD reader.
System components
Badge sampler, decoder, readout system and electronics in one desk-type unit.
Heating method
Three-stage heating by blocks.
3.5.2.4. Pitman 605 automatic TLD reader (figure 3.24)
Dosemeter
Two elements (phosphor-embedded Teflon discs) in metal plate containing identifica-
tion (punched holes). The dosemeter, wrapped in a plastic envelope, is worn in a
62
H W Julius
Figure 3.24. Pitman 605 automatic TLD reader.
plastic holder containing the filters. The plates are stacked in a magazine for automatic
readout.
System components
All in one cabinet.
Heating method
Metal blocks.
3.5.2.5. Studsvik automatic TLD reader 1313B (figure 3.25)
Dosemeter
Plastic holder with insert, containing identification (punched holes and corresponding
Arabic number) and up to four pellets (4.5 mm diameter) or chips. This unit is worn in
a plastic holder with clip. Dosemeters are loaded in a container for readout.
System components
All in one unit.
Heating method
Hot nitrogen gas.
3.5.2.6. TNO automatic TLD system (figure 3.26)
Dosemeter
May, within technical restrictions, be made by the user. A badge is provided, consisting
of a plastic holder with up to six TLD (at choice of the user, maximum 12 mm
diameter). Identification by OCR- A figures. No holder needed. Dosemeters are loaded
in two magazines or manually inserted for readout.
Instrumentation
63
m
I
f ;
Figure 3.25. Studsvik automatic TLD reader 1313B.
Figure 3.26. TNO automatic TLD system for personnel dosimetry.
System components
Badge sampler and reader are separate devices.
Heating system
Hot nitrogen gas.
3.5.2.7. National Panasonic automatic TLD system (figures 3.27 and 3.28)
Dosemeter (see 3.2.2.5)
Four elements in a plastic holder, containing the identification (punched holes plus
printed label).
System components
All in one unit.
64 H W Julius
Figure 3.27. National automatic reader UD-710 AG TL badge system.
INFRA-RED RAY BEAM
OPTICAL GUIDE
PM-TUBE ^ i
THERMOLUMINESCENCE
DOSIMETER ELEMENT
UUL
VOLTAGE APPLIED
TO LAMP
LAMP
SILICON FILTER
Figure 3.28. Schematic diagram of the optical heating system of National Model 710 AG
automatic TLD reader.
Heating system
Optical (IR) heating by a lamp in combination with photon counting.
3.6. Address list
Aloka Co., Ltd
6-22-1, Mure, Mitaka-shi 181
Japan
Central Research Institute for Physics
of the Hungarian Academy of Sciences
Felelos kiadd: Feher Istvan
Peldanyszam: 210 Torzsszam: 74-9876
Keszult a KFKI sokszorosito iizemeben
Budapest, 1974 majus ho
Dai Nippon Tokyo Co., Ltd
Phosphor Division
Shin Tokyo Bldg, 3-3-1, Marunouchi
Chiyoda-ku, Tokyo
Japan
Desmarquest & CEC SA
Division 'Oxydes Frittes'
Zone Industrielle No. 1
F-27000 Evreux
France
Instrumentation 65
D A Pitman Ltd
Jessamy Road
Weybridge, Surrey KT13 8LE
England
Eberline Instrument Corporation
PO Box 2108
SanteFe,NM 87501
USA
Instrument AB Therados
Dalgatan 15
S-752 28 Uppsala
Sweden
National Panasonic Matsushita
Electric Trading Co., Ltd
Head Office
PO Box 288
Osaka 541
Japan
POLON
Sales Office
Bielariska 1
00-086 Warszawa
Poland
SAPHYMO-SRAT
Services Commerciaux
51 Rue de l'Amiral Mouchez
F-75-Paris-13
e
France
Studsvik Energiteknik AB
S-61182Nykoping
Sweden
Teledyne Isotopes
50 Van Buren Avenue
Westwood, NJ 07675
USA
The Harshaw Chemical Company
Crystal & Electronic Products Department
6801 Cochran Road
Solon, Ohio 44139
USA
VEB RFT Messelektronik Dresden
Fetscherstrasse 70
DDR-8016 Dresden
German Democratic Republic
Radiation Detection Company
385 Logue Avenue
Mountain View, California
USA
Victoreen Instrument Division
10101 Woodland Avenue
Cleveland, Ohio 44104
USA
Radiological Service TNO
Utrechtseweg310
N-Arnhem
The Netherlands
V/O 'Licensintorg'
31 Kakhovka St
Moscow, B-420
USSR
References and further reading
1 Becker K 1973 Solid state dosimetry (Cleveland: CRC Press)
2 Cameron J R, Suntharalingam N and Kenney G N 1968 Thermoluminescent dosimetry (Madison:
University of Wisconsin Press)
3 Frank M and Stolz W 1969 Festkorperdosimetrie ionisierender Strahlung (Leipzig: BSB B G
Teubner Verlagsgesellschaft)
4 Robertson M E A 1975 Identification and reduction of errors in thermoluminescence dosimetry
systems (Weybridge: D A Pitman)
66 HW Julius
5 Brunskill R T et al 1970 A sealed thermoluminescent dosemeter employing RF heating for routine
individual monitoring Proc. IAEA Symp. on Advances in Physical and Biological Radiation Detec-
tors, Vienna, November 1970 pp 67-76
6 Julius H W et al 1974 A versatile automatic TLD system under development Proc. 4th Int. Conf.
on Luminescence Dosimetry, Krakow, Poland, 27-31 August vol 2 (Krakow: Institute of Nuclear
Physics) pp 675-89
7 Kartha M 1971 An automated thermoluminescence dosimeter reader Int. J. Appl. Radiat. Isotopes
22 131-4
8 Portal G et al 1977 A new automatic reader for big scale routine of TL personal dosimeters Proc.
5th Int. Conf. on Luminescence Dosimetry, Sao Paulo, February 1977 (Giessen: I Physikalisches
Institut of the Justus-Liebig Universita't) pp 257-61
9 Schlesinger T et al 1971 Photon counting as applied to thermoluminescence dosimetry Proc. 3rd
Int. Conf. on Luminescence Dosimetry, Danish AEC, Riso, October 1971. Riso Rep. No. 249,
pp 226-36
10 Spanne P 1974 Comparison of photon counting and charge integration as signal registration
methods in low dose TL measurements Proc. 4th Int. Conf. on Luminescence Dosimetry, Krakow,
Poland, 27-31 August vol 2 (Krakow: Institute of Nuclear Physics)
11 Oberhofer M 1968 Inherent background reduction for the EG&G model TL-IL CaF
2
(Mn) thermo-
luminescent-dosimeter Health Phys. 15 156-8
12 Petrock K F and Jones D E 1968 Hot nitrogen gas for heating thermoluminescence dosimeters
Proc. 2nd Int. Conf. on Luminescence Dosimetry, Gatlinburg, Tenn., September 1968. USAEC
Rep. CONF 680920, pp 652-69
Applied Thennoluminescence Dosimetry. Eds M Oberhofer and A Scharmann
1981 ECSC, EEC, EAEC, Brussels and Luxembourg
4
Accessory instrumentation
M OBERHOFER
4.1. Introduction
A complete TLD system consists, besides the basic readout instrument, of several addi-
tional accessories, such as spare heating planchets, light sources, powder dispensers,
tweezers, sieves, ultrasonic cleaners, annealing furnaces, annealing stands and irradiators.
These accessories are dealt with in this chapter, which also contains some hints for their
proper use.
Some items have already been mentioned earlier as part of the readout instrument,
such as heating planchets (see 3.2.2.1) and light sources (3.3.5). Some more remarks
will be made with regard to them.
4.2. Heating planchets
As was mentioned in 3.2.2.1 the most common way of heating TL phosphors is the
one using low-thermal-capacity metal planchets. Some of the planchets used with the
Teledyne Isotopes TL readers Model 5100, 7100 and 7300 are reproduced in figure4.1(a).
Planchet type A is intended to be used with TL phosphors in powder form. The
recessed circle helps keep the powders in place. For extruded chip dosemeters this
planchet has four metal posts for keeping the chips securely centred (planchet type B).
Micro-rod dosemeters are read in planchet type C. Here the rods are held in place between
two metal rods. Planchet type D was designed for reading disc dosemeters measuring
9 mm or more in diameter and 0.4 mm thick. The discs are held firmly in place by four
metal prongs. However, one prong would do in the case where the dosemeter extends into
the centre of the planchet, thus simplifying planchet loading. To prevent thin (0.13 mm)
or ultra-thin (20 im) discs bending upwards or warping during the readout process
planchet type E may be used with advantage. With the help of an insertion strip (F in
figure 4.1(a)) the dosemeter discs are inerted under a metal mesh panel (figure 4.1(b)).
In the case shown the mesh is fixed in the direction of the current. With some planchets
of this type the mesh is point-soldered at right angles to the electric current direction.
In this way current also flows through the mesh and consequently heats up the discs
from above, giving a more homogeneous temperature increase throughout the dosemeter
material. To reduce the fraction of light absorbed by the mesh, a hole may be punched
into the mesh with a diameter that still allows the disc to be held down along its peri-
meter. A 60% open area is normally chosen to obtain the best results. In all the mesh type
planchets care has to be taken not to scratch the disc surfaces as this would certainly
result in triboluminescence and a deterioration in accuracy.
68 M Oberhofer
(fl)
(b)
Figure 4.1. (a) Some planchets used with the Teledyne Isotopes dosemeter system. A,
planchet with recess for TL powder use; B, planchet for extruded chip dosemeters, measur-
ing gin X | i n X 0.035 in; C, planchet for micro-rod dosemeters; D, planchet for disc dose-
meters measuring 9 mm or more in diameter and 0.4 mm thick; E, planchet for ultra-thin
and 0.13 mm thick disc dosemeters; F, insertion strip, (b) Detail of a planchet for disc dose-
meters showing insertion of TL disc dosemeter.
How the reading accuracy may be improved by proper planchet design has been
impressively demonstrated by some authors. They describe a planchet version for a disc
dosemeter, where part of the screened region is overlaid with a solid nichrome cover to
reduce and/or prevent curling of the dosemeter during readout, which apparently was
responsible for observed readout deviations of between 5 and 10% [1 J. With the improved
planchet these variations are reduced by 0.16-2.8%, averaging around 1.11%.
Accessory instrumentation 69
As already indicated in 3.2.2.1 and shown in 7.2.1 (figure 7.4) the surface properties
of the planchets substantially influence the TL signal and therefore the material from which
they are made needs careful attention with regard to its light emissivity and reflectivity and
the changes with continuous usage. From the very beginning a planchet type is desirable
with a minimum emissivity in the visible and infrared. Both generally increase with
temperature (incandescent light). Low planchet emissivity gives low 'zero readings' with-
out a TL detector and consequently zero-reading variations which may have a negligible
influence on the TL detector readings. This is of particular importance when low
phosphor emissions from low radiation exposure have to be measured. In connection with
the emissivity of planchets it should be remembered that some materials with low emissi-
vity in the visible may have high emissivity in the infrared. Although the emissivity of
a planchet should be low, its reflectivity ought to be large so as to reflect as much as
possible of the light emitted by the TL detector during its heating up into the light
collecting and detecting system. The light reflection should not vary with time or with
repeated use of the planchet. Reflectivity changes are observed with materials whose
surfaces easily oxidise with time or with successive heating cycles. Consequently non-
oxidising planchets should be used, such as platinum. Inert-gas (nitrogen or argon) flow
helps to reduce the oxidising effect. Where materials other than platinum are used
silver-plated heater planchets, for example oxidising is likely to some degree even
with inert-gas flushing, and cleaning of the planchets or replacing them by new ones
may change their reflectivity with considerable TL signal changes as a consequence.
Some attention is required here.
Trouble is also often caused by organic contamination of the planchet, such as finger-
prints. The planchets therefore should not be touched with the fingers and should be
cleaned frequently with tissue wetted with alcohol, acetone or trichloroethylene.
In connection with heating planchets another tip may help to obtain more reliable
results. Often the cooling-down period in a heating cycle is too short to allow the
planchet to be brought back to a sufficiently low temperature before starting a new
reading cycle. This is particularly true for built-in heater elements, which sometimes cool
down rather slowly because of their high thermal capacity if no forced cooling is
provided. In this case temperature build-up often occurs, with reading trouble as a
consequence. The optimum cooling-down period has to be determined experimentally
for each instrument type. Several minutes (2-3) will do in most cases.
4.3. Gas flushing
According to 3.2.1 use is made of inert gas in most of the commercial TL reader systems
to suppress spurious luminescence from oxygen effects and combustion phenomena. The
gas should be turned on 15-20 min before taking the first readings. To obtain optimal
quenching of spurious luminescence the gas flow needs to be adjusted properly by means
of a pressure reduction valve attached to the gas bottle. The flow is usually indicated by a
gas flow meter. The gas flow and its fluctuations are not too important, commonly
between about 0.5 and 11 min
-1
, but it should, if possible, be kept at the same value after
a certain flow has been decided upon. The gas should be pure and dry. Therefore the gas
should be passed through a gas dryer bottle to remove moisture or through a purifier.
70 M Oberhofer
The background reduction with N
2
or other gas flushing should always be verified
before taking a series of measurements or at least when using a new gas bottle for the first
time to avoid surprises.
4.4. Reference light sourcesf
Some instrument manufacturers supply reference light sources with different light intensi-
ties (figure 4.2) and with different light colours matched to the light colour of the TL
emission from the phosphors to be used (blue for LiF, orange for lithium borate and
green for calcium fluoride and calcium sulphate).
Figure 4.2. Teledyne Isotopes standard light sources of
14
C mixed with a luminescent
phosphor for use in day-to-day checking of instrument stability.
In some instances for instrument stability checking and calibration the light sources
are inserted into the drawer in place of the TL detector and brought under the photo-
multiplier tube by pushing the drawer into the instrument. In this case it is important to
make sure that the sources are all inserted in the same way, as the light source reading
may sometimes depend on the source direction with respect to the PM tube position.
External light sources have the disadvantage that they are normally exposed to
environmental light and in most cases show some additional light emission as a conse-
quence of light excitation which, although it fades away exponentially in the dark, may
be troublesome. It may take some minutes before the light-induced phosphorescence has
decayed away to negligible intensity levels. In any case, before a check or calibration with
an external light source one must ensure that the light source has been sufficiently long
in its final position within the reader and that it yields average readings with an accept-
ably low standard deviation, say less than 2%. It should be borne in mind that the light
source output is subject to internal source fluctuations of the order of 0.4 up to 0.6%
and that the light output can be influenced by ambient temperature (see also 7.2.1 and
11.4). In one case of a plastic scintillator light source 0.05% K
_1
light intensity varia-
tions were found and in a case of a Nal (TL) scintillator light source the value was
0.3%K"
1
[2]. Age may also affect the light output. So, for example, for some Na(Tl)
t See also 3.3.5.
Accessory instrumentation 71
scintillator light sources a time-dependent decrease in light intensity of 3% yr
1
was
observed as a consequence of their
210
Pb content, which decays with a half-life of 19.4 yr
or with - 3. 1% yr"
1
[2];
All these error sources were recently the subject of detailed studies [1]. According to
these studies nitrogen affects plastic scintillator light sources, which may suffer reader
response variations up to 5% during a working day. This is one reason for being careful
with nitrogen gas flushing when using certain light sources for instrument checking and
adjustment.
4.5. Powder dispensers
Where weighing of TL phosphor powder is too cumbersome in routine dosimetry, for
example powder dispensers are employed.
In this case identical powder aliquots are prepared volumetrically. Figures 4.3 and 4.4
show schematically two commercially available powder dispensers. In both cases the
metered volume is defined by a small hole (funnel) through a slide or a rotating metal
plate. In its filling position the metered volume is just underneath a powder reservoir,
from which it is filled. In its discharge position, reached in the first case by withdrawing
the dispensing plunger from the device until a limit stopper prevents further movement
and in the second case by rotating the metal plate around its axis towards a stop, which
for reasons of simplicity is not shown in the figure, the powder is released through a
discharge tube on to a planchet or into a pan or also into a dosemeter capsule. Repro-
ducibility is improved considerably by shaking the dispenser with a vibrator, which may
be timed. The dispenser is vibrated for a few seconds during the filling cf the metered
volume and a few seconds during discharge. As a vibrator, either an electric engraving
tool or a DC relay operated on alternating current, so as to produce a chattering motion,
can be attached to the dispenser, if it does not already have a vibrator. In figures 4.5 and
4.6 the photographs of the powder dispensers shown schematically earlier are reproduced
together with their vibrators. Figure 4.6(b) shows another version of the Harshaw
HANDLE
POWDER RESERVOIR
METERED VOLUME
DISPENSING
PLUNGER
LIMIT STOPPER
DISCHARGE TUBE
PLANCHET
Figure 4. 3. Tclcdyne Isotopes phosphor dispenser, schematically represented.
72 M Oberhofer
NUT FOR TIGHTENING
OF DISPENSER
ASSEMBLY
PLANCHET
Figure 4.4. Harshaw flat-ptfte powder dispenser, schematically simplified. In the actual
device the handle, powder reservoir and discharge hole are not located in the same plane,
as can be seen from figure 4.6.
"1
Figure 4.5. Teledyne Isotopes (formerly CON-RAD) phosphor dispenser with automatic
vibrator feature.
dispenser with vibrator (here a DC motor-driven eccentric) manufactured by D A Pitman
Ltd.
How reproducibility can be improved with a vibrator is demonstrated by an example.
In table 1 data are compiled which were obtained with a vibrator produced by Eberline
Instrument Corporation (Model PB-1 Powder Dispenser) together with LiF powder from
The Harshaw Chemical Company, varying the time settings of the vibrator. The powder
weight is the average of 10 aliquots.
Accessory instrumentation
73
(a) (b)
Figure 4.6. (a) Harshaw powder dispenser with electrically (push-button) operated vibrator.
(6) Model 624 vibrator powder dispenser of Pitman Instruments.
Table 4. 1. Influence of vibrating times on the reproducibility of powder sample weight for
samples prepared with a powder dispenser.
Vibrating
time setting
(s)
6
9
15
21
Average
powder
weight
(mg)
31.916
32.610
33.311
34.125
Standard
deviation
(%)
0.94
0.06
0.15
0.18
Maximum
weight
(mg)
32.01
33.02
33.52
34.97
Minimum
weight
(mg)
29.39
32.23
33.12
33.45
Maximum weight
deviation
(%)
8.5
2.4
1.2
4.4
From this table it is evident that the optimum vibrator time setting for the automatic
vibrator used is 15 s which yields the lowest weight deviations between single samples and
also a sufficiently low standard deviation (0.15%) for the average weight.
Most phosphor dispensers are designed for 80-200 mesh phosphors, which include LiF
and li
2
B
4
0
7
:Mn. The much finer CaS0
4
: Mn and CaF
2
: Mn powders do not dispense
readily. Weighing or a simple volume sampling should be used with such phosphors.
The following hints are given to avoid difficulties with dispensers of the types
described here.
First of all, the dispensers must be clean, dry and free running. In a humid climate
such as in the tropics, the transfer chambers of the slides and the charge and discharge
tubes may be obstructed by humidity or humid corrosion products if the dispenser is not
made out of non-corrosive material (high-quality stainless steel, for example). In this case
cleaning of the disassembled parts of the dispenser should be done with acetone, possibly
74 M Oberhofer
making use of a pipe-cleaner, and the dispenser parts should be thoroughly dried after-
wards with a hot air blower. To reduce malfunctioning of the dispenser it is recom-
mended that it should always be kept in a dry atmosphere if not in use. In most cases
it will be sufficient to keep it in a plastic bag with silica gel. From time to time the
dispenser should be checked by weighing successive samplings and by determining their
standard deviation, which should be the same as before. Of course, the phosphor must
also be dry. If the powder shows a tendency to lump together, it should be stored in a
desiccator. If the phosphor for one reason or another has become quite lumpy because
of humidity, it must be dried at no more than 80 C. For optimum precision, powder
should be dispensed only when the reservoir contains appreciably more than one single
metered volume of powder.
There may be some uncertainty as to the accuracy of the first aliquot from a newly
filled dispenser. It is therefore advisable to put the first aliquot back into the hopper of
the dispenser and begin measurements with the second aliquot.
Another hint may be useful in operating a dispenser successfully: care should be taken
to prevent cross-contamination if the dispenser is used to dispense phosphor irradiated to
various doses or phosphors of different radiation sensitivity.
Low-dose measurements can be greatly disturbed by contamination of the low-dose
phosphor with a few grains of a material which has received high doses or has a much
higher TL yield. To prevent this inconvenience, either the dispenser should be washed
before re-use with, for example, acetone, or a separate dispenser for low-dose measure-
ment only should be used. If the dispenser is washed, it must be dried carefully before it
is used again.
Where more than one dispenser is used, it is necessary to check for differences in the
metering volume. In an experiment the average weights of samples prepared with each
vibrator should be compared and, if necessary, correction factors applied for each powder
dispenser.
4.6. Mechanical tweezersf
Rods, chips and discs may be handled by stainless steel tweezers. Care has to be taken
that in utilising them the dosemeters are not scratched, as scratching them normally leads
to phosphor excitation and light emission upon heating with unpredictable readings. To
avoid scratching the tweezer tips should be covered with some soft coating which can
easily be cleaned and/or exchanged.
4.7. Vacuum tweezersf
For rapid and simple dosemeter handling without squeezing or abrading, vacuum tweezers
are advantageous. Such tweezers may be acquired from Pitman Instruments, for example
(see figure 4.7(a)), or made with a small vacuum or suction pump, some small diameter
tube and a connecting rubber hose to the pump. Air is sucked into the tube with which
the dosemeter is to be picked up. The dosemeter stays fixed to the tube end by means of
the vacuum created at its surface. For discs the tube may have at its end a rubber or
plastic sucker. Figure 4.7 demonstrates such a device schematically. Dosemeter release is
t See also 7.26.
Accessory instrumentation
75
k- k,
- J .
t t *
(a)
(6)
Figure 4.7. (a) Pitman vacuum tweezers for easy dosemeter handling (courtesy of D A
Pitman Ltd), (b) Operating principle of vacuum tweezers, a Dosemeter pick-up, b dosemeter
transfer, c dosemeter release.
effected by letting air enter into the vacuum within the most simple device just by
stopping the pump or by releasing the finger tip from the tube top.
4.8. Sieves
Where powder material is used for dosimetry it is necessary either to produce material
with a grain size within a certain range, say from 80 to 200 mesh, or to make sure that
the grain size corresponds to that specified or desired or to re-sieve it for cleaning. These
sieves are available in chemists' shops in sets, allowing sieving for various average grain
sizes and grain size spreads. For grain size spreads of 80-200 mesh no particular problems
are encountered in sieving, pre-supposing that the material is dry.
Difficulties due to agglomeration may arise, for example for LiF, when trying to sieve
powders ground to very small grain sizes.
4.9. Ultrasonic cleaners
If one wants to perform precise TLD measurements cleanliness is of the utmost importance,
as dirt either within the reading system or on the dosemeter surface may cause spurious
readings which give erratic results. Dirt also reduces the usable life of the dosemeter due
to the burning into the surface of dirt and grease during the annealing process required
before re-use, or even during the read cycle itself.
For cleaning the dosemeters ultrasonic cleaners are recommended. Ultrasonic cleaning
may increase the life expectancy of the dosemeters considerably. For phosphor-Teflon
dosemeters it was found that the introduction into the re-use cycle of a short ultrasonic
cleaning period on average doubles the life expectancy, provided they are not exposed
to doses in excess of 10
4
R, when radiation damage becomes important.
76 M Oberhofer
Ultrasonic cleaners are available in various sizes from different manufacturers.
Normally the tank and generator are combined in a single unit. They are supplied with
perforated stainless steel trays to hold the dosemeters and also with tank covers. The
dosemeters are placed loosely into the perforated tray supplied with the cleaner and
lowered into the cleaning solution for a period of 5-15 min with the instrument in
operation.
The dosemeters are then removed, rinsed thoroughly in methanol, for example, and
allowed to "dry on a lint-free surface before annealing. A solid tray is used instead of a
perforated one if the dosemeters are micro-rods. For more information on dosemeter
cleaning the reader is referred to 7.2.7.
4.10. Annealing furnaces
Annealing of the dosemeter material in many cases (LiF, for example) is performed in
ovens. Often two ovens are used, one with a maximum temperature up to 400 C, which
is sufficient for all dosemeters in common use, and one up to 150C. Emphasis should be
put on good temperature control and constancy of the preselected temperatures by
means of a precision temperature control regulator over extended periods of time. This
latter feature is of importance in particular for ovens of low maximum temperature. LiF,
for example, needs to be kept at 80 C for over 24 h after high-temperature baking, if the
standard annealing procedure is followed. If other procedures are followed with shorter
anneal times the temperature constancy may be even more important (see also 7.2.5).
Forced convection is desirable since there are then no temperature gradients within the
oven and identical annealing temperatures are guaranteed for all dosemeters, independent
of their position within the oven. It is convenient to have C0
2
cooling for controlled
cooling-down of the dosemeter material.
In figure 4.8(a), (b) and (c) photographs of a number of 'conventional' ovens are
reproduced, selected by Teledyne Isotopes as most suitable for TL dosemeter anneal. Any
of the ovens should be brought up to the preselected temperature and allowed to stabilise
well before dosemeter insertion. Balancing by adjusting the temperature frequently is
difficult and is not recommended.
In order to avoid contamination of the annealing ovens with some material which
might also contaminate the TL dosemeters later on the ovens should be set aside exclusively
for dosemeter anneal.
Ultimately some other 'advanced' oven types came on to the market specially designed
for dosemeter anneal. Their construction makes use of 'thermoplatesj which contain the
heating elements and the associated thermocouple temperature sensors. One example
(figure 4.8(G0) shows an oven unit offered by D A Pitman Ltd, which consists of a heated
well lid, suitable for top loading of several special annealing blocks made of aluminium
with holes to hold the dosemeters and a hole for inserting a stem thermometer. Thermal
gradients through the system are extremely low due to the high thermal conductivity of
aluminium.
Similar ovens with sample cassette plates are produced by Aloka Co, Ltd. This
company also offers heater pans to be heated up by means of infrared light from a
halogen lamp.
Accessory instrumentation
77
(a) (b)
<*.
^**rxX.X^iyU*Z.1?:!&V'
i w ^ - ? ^ ^ ^ * - ^ ^ ^ ! ! . - - . - ^ : ^ - . - - . . ^ , .
(c)
(d)
Figure 4.8. (a) Annealing oven for hightemperature anneal. This compact muffle furnace
has a temperature range (up to 1093C) that makes it highly suitable for annealing
phosphor powders. Designed for maximum efficiency, the control circuitry is exactly
matched to the size of the heating chamber (courtesy of Teledyne Isotopes), (b) Annealing
oven for mediumtemperature anneal. This practical compact oven is ideally suited for
annealing of CaS0
4
: Dy dosemeters. Amply insulated, the heating chamber has damper
controlled induced air circulation and two adjustable shelves (courtesy of Teledyne
Isotopes), (c) Annealing oven for medium and lowtemperature anneal. This highquality
forced convection oven offers a temperature range (from 40 C up to 300 C) that makes it
ideal for most annealing purposes. The forced convection design combines with a sophisti
cated proportional temperature control system to assure easily controlled, constant
temperatures (courtesy of Teledyne Isotopes), (d) D A Pitman L td programmed thermo
plate annealing facility. Oven unit left, control unit right (courtesy of D A Pitman L td).
4.11. Annealing stands
Difficulties in obtaining identical thermal treatment of a whole batch of dosemeters may
be overcome sufficiently well by the use of heater stands or other devices for the same
purpose. Such a stand is shown in figure 4.9. where for example, disc dosemeters are
placed between an aluminium or nickel plate of 3 mm thickness. To ensure good thermal
78 M Oberhofer
%
Figure 4.9. Doscmctcr annealing stand with phosphor-Teflon disc dosemeters. Top plate
has been taken off to show how the dosemeters are arranged (courtesy of Tcledyne
Isotopes).
contact the surface may be anodised black. For rod dosemeters plates with machined
grooves are used which hold 100 micro-rods at one time. The depth of the grooves is such
that the micro-rods project slightly and, by laying another flat plate over the top, the rods
are held in good thermal contact with the surface along three lines. As many as five of
these trays may be used at one time on the annealing stand, enabling 500 micro-rods to be
annealed simultaneously. Four legs eliminate thermal gradients due to conduction of
heat to or from the floor of the oven. The plate efficiently distributes the heat to the
dosemeters. Another device, the cross section of which is given in figure 4.10, may be
utilised with good results for annealing isothermally at least 50 disc dosemeters, if air
exchange is possible by means of one or several holes. Severe coloration and consequently
loss of sensitivity of the dosemeters is observed if air exchange is not possible [3].
END CAP TEFLON DISC
DOSIMETERS
COMPRESSING
SPRING
-TEFLON PLUGS
Figure 4.10. Cross-sectional view of an annealing tube for Teflon disc dosemeters.
Experience has been good with the annealing device shown in figure 4.11. This
annealing stand consists of 13 plates interleaved with spacers. Each plate has 18 circular
cut-outs, which will accept discs up to 12.7 mm diameter from ultra-thin up to 0.4 mm
thick. The plates and spacers are made out of anodised aluminium and are stacked on a
centre bolt so that a total of 234 discs can easily be assembled in a single unit of high
packing density and good thermal conductivity. A stand-off base raises the main assembly
approximately 2.5 cm above the oven floor so that thermal gradients due to conduction
are minimized.
Accessory instrumentation
79
Figure 4. 11. DA Pitman Ltd TLD annealing stand with 234 disc compartments.
4.12. Irradiators
For dosemeter calibration, portable irradiators are available, in one case (Teledyne
Isotopes) being a device which contains ' "Sr/^Y as the radiation source and which was
designed for use with Teflon disc dosemeters. The device is offered for activities of 2, 10,
50 and 100 mCi with maximum dose rates of 5, 24, 120 and 240 rad min"
1
, respectively.
The discs are inserted into the irradiator by means of a drawer. A highly reproducible
dose is also obtained with the Reference Dose Irradiator of Studsvik Instrument AB
(figure 4.12), which can be varied within a wide range from 20 mrad well up into the
kilorad range. The radioactive source here is also '"Sr/^Y (standard: 1 mCi, with options
of 0.3, 3, 10 and 30mCi), placed in a heavy nickel-plated brass shield. The dosemeter to
be exposed, which may have dimensions up to 30x40mm
2
and a thickness of 4 mm
maximum, is rotated within the irradiator by means of a synchronous motor which gives
a well-defined speed, resulting in a constant dose per revolution (70 mrad for the standard
Figure 4.12. Studsvik reference dose irradiator 6527 B (courtesy of Studsvik).
80
M Oberhofer
version). The instrument can also be set in a way that the dosemeter remains stationary
under the source. The time of irradiation in the stationary mode can be set from a few
seconds up to 12 h, which corresponds to a dose of between about 50 mrad to 1 krad per
mCiof
90
Sr/
90
Y.
Another irradiator version is shown in figure 4.13, which is produced by D A Pitman
Ltd. This automatic irradiator is principally characterised by two opposed 1 mCi ' "Sr/^Y
sources (matched in activity to within 5%) with sliding shutter assemblies and a turntable
with 30 apertures around its circumference into which thin Kapton trays with TL dose-
meters (discs, chips, micro-rods) can be placed and which is aligned to carry the dose-
meters between the sources. With the standard gearbox per revolution a dose in the order
of 10 mrad (4-14 mrad according to speed) is administered to the dosemeters. The expo-
sure reproducibility obtainable is better than 2% standard deviation.
Figure 4.13. DA Pitman Ltd Model 623 dosemeter irradiator (courtesy of D A Pitman
Ltd).
In some instances the calibrators are part of the TL reader system, for example in the
Therados TLD- 10 system shown in figure 3.19 or in the Harshaw Model 2271 Detector
and L Card Loader System.
4.13. Literature
In the following some literature is listed which is exclusively dedicated to TL or TLD or where this
subject is treated as a whole among other solid-state dosimetric methods.
1967 Luminescence Dosimetry. Proc. Int. Conf. on Luminescence Dosimetry, Stanford University,
June 21-23. 1965. USAEC Division of Technical Information AEC 8, Symp. Ser.
Cameron J R, Suntharalingam N and Kenney G N 1968 Thermoluminescent Dosimetry (Madison:
The University of Wisconsin Press)
1969 Solid State Dosimetry. Proc. NATO Summer School, Brussels, September 4-16, 1967 ed
S. Amelinckx, B Blatz and R Strumane (New York: Gordon and Breach)
Accessory instrumentation 81
1969 Proc. 2nd Int. Conf. on Luminescence Dosimetry, Gatlinburg, Tenn., September 1968. USAEC
Rep. COW 680920
Frank M and Stolz W 1969 Festkorperdosimetrie Ionisierender Strahlung (Leipzig: B G Teubner
Verlagsgesellschaft)
1971 Proc. 3rd Int. Conf. on Luminescence Dosimetry, Danish AEC Research Establishment, Riso,
October 11-14. Riso Rep. No 249, part I, II and III
Becker K 1973 Solid State Dosimetry (Cleveland: CRC Press)
Oberhofer M 1974 Termoluminescence Dosimetry, Lecture notes of a course given at the Bandung
Reactor Centre, Bandung, Indonesia, June-October 1973 (Bandung, Indonesia: Pusat Reaktor Atom
Bandung) PRAB: 335/HP-40/73
1974 Proc. 4th Int. Conf. on Luminescence Dosimetry, Krakow, August 27-31 Vol I, II and III
(Krakow: Institute of Nuclear Physics)
Becker K and Scharmann A 1975 Einfuhrung in die Festkorperdosimetrie, Thiemig Taschenbuch vol
56 (Miinchen: Verlag Karl Thiemig)
1975 Technical Recommendations for the Use of Thermoluminescence of Dosimetry in Individual
Monitoring for Photons and Electrons from External Sources. Radiological Protection 3 (Commission
of the European Communities) EUR 5358 e
Robertson M E A 1975 Identification and reduction of errors in Thermoluminescence Dosimetry
Systems (Weybridge: D A Pitman Ltd)
1977 Proc. 5th Int. Conf. on Luminescence Dosimetry, Sao Paulo, February 14-17 (Giessen: I
Physikalisches Institut of the Justus-Liebing Universitat)
Nambi K S V 1977 Thermoluminescence: Its Understanding and Applications (Sao Paulo: Centro de
Protecao Radiologica e Dosimetria, Instituto de Energia Atomica) Informacao IEA 54.CPRD-AMD 1
1979 Thermoluminescence: Dosimetry and Applications, Bull. Radiat. Protection 2 No 4
1980 Proc. 6th Int. Conf. on Solid State Dosimetry, Toulouse, April 1-4. Nucl. Instrum. Meth. 175
No 1 (September)
References
1 Matthews R J and Stoebe T G 1980 Precision thermoluminescent dosimetry using CaSQ,: Dy
Teflon dosimeters Proc. 6th Int. Conf. on Solid State Dosimetry, Toulouse, April 1-4. Nucl.
Instrum. Meth. 175 No 1 (September)
2 Burgkhardt B and Piesch E 1979 Systematical and statistical errors of the TLD-reader calibration
with reference light-sources Report presented at 11th Meeting of the Working Group 'Assessment
of Doses- caused by External Radiation Sources' of the Fachverband fur Strahlenschutz e.V.,
November 29-30, Karlsruhe
3 Verhagen H W, Petten ECN private communication
Applied Thermoluminescence Dosimetry. Eds M Oberhofer and A Scharmann
1981 ECSC, EEC, EAEC, Brussels and Luxembourg
5
General characteristics OF TL materials
G BUSUOLI
5.1. Introduction
TL materials are at present widely used in many fields of dosimetry due to their properties
that are now known from other classical dosimetry systems. This chapter deals with the
general characteristics for TLD; special characteristics for certain applications (such as
personal, environmental and chemical dosimetry) are discussed in the corresponding
chapters.
5.2. Linearity
For many applications it is generally preferred to have a linear dose-TL signal relation-
ship, i.e. proportionality between the TL signal and the dose, from D = 0.
The form of this function is determined by the TL yield Y
Th
, defined as the quotient
of the energy emitted as light E
TL
, the mass of the detector m and the absorbed dose D:
Y
TL
= E
TL
/mD.
In the range where Y
JL
is constant, the dose characteristic is linear and one can write:
Q
TL
= a
T
Y
TL
D
where a
t
is a proportionality factor and Q
TL
is the thermoluminescent signal from the
phosphor.
Figure 5.1 shows a typical curve for the /th glow peak. On the y axis the thermo-
luminescent signal is plotted (the zero dose signal being subtracted) while on the x axis
the dose is plotted.
If a phosphor presents a glow curve with several maxima at different temperatures,
either the integrated light emitted by every peak, or its height, or the whole of the light
emitted by the phosphor as the sum of the contributions from the different peaks present
a linear dose characteristic. Every curve will be characterised by a different light yield.
As can be seen from the figure, the dose characteristic is linear up to a maximum value
D
m
after which 'saturation' occurs or 'supralinearity' starts.
Table 5.1 gives the dose ranges within which detectors show a linear behaviour [1].
Both the lower and upper dose values are very different for each detector.
The data presented in the table demonstrate that for all of the phosphors shown the
deviation from linearity is due to the presence of supralinearity. The origin of this
84 G Busuoli
W
z
o
a.
UJ
/
/
/
/
/
/ LINEAR
RANGE'
J
\
Dm D
s
DOSE
Figure 5.1. Example of a linearity curve
Table 5.1. Linearity ranges.
TL material Linearity range for
60
Co gamma rays
(order of magnitude) (rad)
LiF : Mg, Ti
Li
2
B
4
0
7
: Mn
CaF
2
: Mn
CaF
2
: Dy
BeO
10"
2
-10
2
KTMO
2
10- MO
3
1CT
5
-10
3
l ( T
2
- l u
2
phenomenon is not yet well known. As an example, in figure 5.2 the dose characteristic
for BeO (Thermalox 995) irradiated with ^Co gamma rays is given [2]. In this case, as is
clearly shown in the figure, supralinearity is present for doses of the order of 50 rad.
For an explanation of the phenomenon, different hypotheses have been put forward,
such as the creation of new traps as an effect of the irradiation [3] or an increase of the
intrinsic TL efficiency, etc.
Even if the sensitivity of the TL detector increases in this region, the accuracy of the
measurements made in the supralinearity range is lower than that for the linear region.
This comes from the necessity of introducing correction factors that generate further
errors.
The supralinearity can be a function of the linear energy transfer (LET) of the radiation
and the dose limit at which supralinearity becomes evident is larger for high LET particles.
Moreover, supralinearity influences the various TL peaks of the detectors in different
ways. Figure 5.3 is an example of this behaviour; the figure gives the curves for the main
peaks of LiF (called the first peak) and for the peak at about 280 C (called the second
peak) for irradiation using ^Co gamma rays (low LET) and using slow neutrons (high
LET) [4]. The figure clearly shows the influences mentioned above.
Attention should be paid to the fact that if the supralinearity region is reached, the TL
detector maintains the new sensitivity even after the readout process. This fact is a
General characteristics of TL materials 85
~ 1 0
A
u
m
'o
3
Q.
3
O
10'
5 10
1
10'
10"
10"' 10
c
10' 10'
1111
'
-,3 ,
n
4
10
J
10"
EXPOSURE (R )
Figure5.2. BeO TL response plotted against
60
Co gamma ray exposure.
=> 10
5
or
<
CD
<
b 10-
D.
I
o
60
r
J PEAK I
\ . PEAK II
SLOW frPEAK I
NEUTRONS I PEAK II
10'
D OSE ( rod )
Figure 5. 3. Total light output plotted against dose for the two main peaks of LiF for
60
Co
gamma rays and slow neutrons.
problem for those detectors that are re-used, as in the case of personnel dosimetry or,
more likely for the dose levels present, in the case of clinical dosimetry. If a detector has
been irradiated in the supralinearity range, in order to restore its previous sensitivity it
will be necessary to perform a complete annealing cycle and not just a simple readout.
Care must be taken on this point in order to avoid errors in the dose assessment.
Beyond the supralinearity range, due to the decrease in the number of available traps,
the saturation effect of the phosphor becomes apparent. The saturation effect auto-
matically determines the upper dose limit for each detector, which is usually taken as
86 G Busuoli
20% below the saturation value. Measurements made in the proximity of the saturation
value are affected by larger errors and it is recommended that TL detectors not be used
in the presence of such high doses. Moreover, attention must be paid to the fact that even
a complete annealing of the phosphor does not completely restore the initial properties
of the material due to the large amount of damage suffered by it.
Finally, another interesting point to discuss is the lower dose limit or threshold dose.
For a given combination of TL material and readout device, the lower limit of detection
is essentially determined by the variability of the signal obtained by the reading of non-
irradiated detectors.
The detection threshold, which can be defined as the smallest dose that can be distin-
guished significantly from a zero dose, can be taken as three times the standard deviation
of the zero-dose reading, expressed in units of absorbed dose. It must be emphasised that
the uncertainty of a dose, in the region of the detection threshold, may be of the order of
100%.
The zero-dose reading is calculated from the signal obtained when a non-irradiated
detector is read. This signal may be due to triboluminescence and chemiluminescence,
stimulation of the detector by visible and ultraviolet light, infrared emission of the
heating element and dark current fluctuations of the photomultiplier tube and residual
signals due to previous irradiations.
5.3. Response to photons
If a TL material is to be used for any dosimetric applications in the field of photon radia-
tion, one of the main characteristics that must be known is its energy response. For the
purpose of this subsection, energy response is defined as follows: the energy response is a
measure of the energy absorbed in the TL material used in comparison to the energy
absorbed in a material taken as the reference, when irradiated at the same exposure.
(Normal reference materials in dosimetry are air and tissue.)
The energy response is therefore characteristic of each TL material and a direct
measurement is obtained when the material is under electronic equilibrium conditions
[5]. Energy response is not so easily measured, but its theoretical value is very helpful in
selecting a particular TL material for any special applications.
The energy response can easily be calculated as the ratio between the mass energy
absorption coefficients of the detector and of air respectively, in the energy range up
to 3 MeV, i.e. where exposure is still defined. Calculations can also be performed for high
energies but in practice they have no meaning as electronic equilibrium no longer exists
[6].
Air is normally taken as the reference medium because a well-defined quantity, the
exposure, can easily and accurately be measured for it and because the ratio between
absorbed dose and exposure for air is a constant.
If S(E) is the energy response one has (where d stands for 'detector')
_ , . (Men/P)d
(^en/P)air
This formula is simply derived from the Bragg principle applied to large cavities.
General characteristics of TL materials 87
Since Oj
e
n/p)d commonly refers to a compound or a mixture of different elements,
the additivity rule must be used to calculate it at every energy value [7]:
- (Men/P)d = (Men/P)l ^ 1 + (Men/p)
2
W
2
+... + ( / i
e n
/ p) / W
t
+ . . .
where (p
en
lp)i is the mass energy absorption coefficient of the ith element and Wi is its
fraction by weight.
In a practical calculation dealing with phosphor doped with or containing various
impurities, these must be considered on account of their high Z values.
The simple formula used for energy response calculations is valid under the following
conditions [5]:
(a) electronic equilibrium;
(b) no self-absorption in the detector;
(c) light yield per rad independent of the LET.
Moreover, the formula does not take into account the fluorescent x-radiation created
in the material itself. Of course, more sophisticated calculations are possible.
In figure 5.4 some examples of energy response calculations are given [6].
1 - CaF
2
: 3.0 7. Mn
2-CaSOi:0.217. Dy
- Co SOi :0.22V. Tm
0.1 1.0 10 100
ENERGY ( MeV )
1-METAPHOSPHATE GLASS
0.3 V. Mn
2- AI
2
0
3
(a)
0.1 1.0 10 100
ENERGY ( MeV)
(b)
1.5
O
Q_
01
05
1
- 1
l-L iF( TL D -IOO] .
0 0.9V. ; Si 0.3 V. ;
Mg 0 03V. ; P 0.025V.
2-L i
2
B
4
0
7
: Mn 0.34V.
L 3-BeO - Thermalox 995
( c)
0.1 1.0 10 100
ENERGY ( MeV )
Figure 5.4. Examples of calculated energy
dependence for several TL detectors.
88 G Busuoli
For dosimetric purposes a material with an energy response which is as constant as
possible over the energy range of interest is desirable. This can be achieved by choosing
materials with a low effective atomic number Z. For special applications, however, high Z
materials coupled with filters can be used. In this case the energy response of the detector
is modified by the dosemeter design and must be determined experimentally. The factors
to be used to correct for dosemeter response at a given energy level can be obtained from
the ratio of the dosemeter reading at the energy in question and at some reference energy
which is commonly taken to be that for "'Co gamma rays.
A particular practical example of calculated energy response compared with measured
energy response is reported in figure 5.5 for BeO [2]. In this case the discrepancy between
calculation and experimental data is not only due to the previously reported factors but
also comes from something substantial and perhaps intrinsic to the material itself. For
this special case a satisfactory explanation of the phenomenon has not yet been given; a
hypothetical presence of high Z impurities has been demonstrated as being invalid from
chemical analysis performed on the material.
2.0
o
Q.
if)
W 1.5
a:
ID
>
< 1.0
I
LU
rr
_i i i _
_i i '
10 100 1000
ENERGY ( keV )
Figure 5.5. Calculated energy dependence and measured energy response for BeO discs.
Sometimes, for special applications, a large energy response can be useful for deter-
mining the energy components of the radiation field. In fact, by using several detectors
with different filtrations, TL responses that are different in the presence of different
radiation energies are obtained. Of course, if detailed information on the different
energies is needed a large number of detectors should be used. In this case the dosemeter
will be very complicated; moreover, it will be more likely to introduce large errors into
the evaluation. Therefore the solution of using too many detectors in the same dosemeter
is to be carefully considered.
5.4. Response to beta rays
TL materials are sensitive to beta rays and, theoretically, can also be used in the design of
dosemeters for this radiation. However, due to the large dimensions of the grains, as in
the case of a powder, or to the thickness of the sample, as in the case of a compacted
General characteristics of TL materials
89
detector, it will be impossible to satisfy cavity theory. Consequently any detector
employed for beta measurements shows a response decreasing steeply in the low-energy
range.
Figure 5.6. shows the relative response of LiF as a function of the mean beta energy
of various sources [8]. Curve (a) refers to powder (0.15 mm average grain diameter)
exposed at the surface of special beta sources; curve (b) is for 1 mm diameter LiF-Teflon
rods at the surface of a container of the emitting solution; curve (c) is for LiF-Teflon
immersed in a solution of the nuclide.
LU
LO
z
o
0-
LO
LU
o n
LU
>
LU
a:
0.02
0.02 0.1 1
MEAN BETA ENERGY (MeV)
Figure 5.6. Relative response of TL in Li F: Mg, Ti as a function of the mean beta energy of
various emitters: (a) with powder (0.15 mm average grain diameter) exposed at the surface
of a gelatine mould; ( i ) with 1 mm diameter LiF-Teflon rods, at the surface of a container
of the emitting solution; and (c) immersed in a solution of the nuclide (after [8]).
Figure 5.7 is a further example for LiF chips and three different sized BeO discs [9].
From this figure it can be seen that in the range from 0.5 MeV up to ^Srj^Y, the dose
in skin taken at a depth from 5 to 10 mg cm
-2
can be determined with an uncertainty
of a factor of 2. If greater accuracy is required, either the use of thinner detectors or the
use of several detectors in order to obtain some information on the energy of the beta
rays would be necessary.
The problem of beta dosimetry with TL materials is now being widely studied in
various European laboratories and some comparisons are in progress as part of a programme
by the Commission of the European Communities.
5.5. Response to neutrons
In many situations it is necessary to measure photon and electron doses in the presence of
neutrons and it may be necessary to correct the results for the sensitivity of the detector
to neutrons. On the other hand, for several applications and particularly for personal
dosimetry, it is necessary to have detectors sensitive to neutrons in order to assess the
dose equivalent of people working in the surroundings of nuclear power plants.
90 G Busuoli
Q
LU
or
o
o
1X1
>
10'
LU
or
LU
in
z
o
0_
to
_
J
V
/
/
1
Jk
oL iF CHIPS
.BeO ( A)
* BeO ( B)
* BeO ( C)
i
0.1 5 1.0 5 10
Ep ( max) ( MeV) AT CALIBRATION POINT
Figure 5.7. Energy dependence for beta rays (after [9]).
An example of gamma detection in the presence of large amounts of neutron radiation
is in the case of accident dosimetry. Measurements performed in an experimental reactor
show that the biggest errors in gamma dose assessment come from the presence of
thermal or slow neutrons and from the sensitivity of the TL detectors to these radiations
[10].
The sensitivity to neutrons of TL phosphors depends on their isotopic composition and
to some extent on the content of different impurities. For example, LiF and Li
2
B
4
0
7
can
be manufactured without any difficulty with different abundances of
6
Li and
10
B, thus
increasing markedly the slow neutron sensitivity (see also chapter 12).
Theoretical calculations and very accurate measurements in order to assess the
sensitivity of different TL phosphors to slow and fast neutrons have recently been
published [11-14].
Table 5.2 gives some published values for the response of a number of TL materials
to a fluence of 10
10
thermal neutrons cm
-2
in terms of an equivalent exposure to ^Co
gamma rays [1].
Table 5.2. Slow neutron sensitivity.
Material Response (10
10
cm
2
)/Response (R of
60
Co gamma rays)
LiF (TLD 100)
Li
2
B, 0
7
: Mn
LiF (TLD 600)
LiF (TLD 700)
CaF
2
: Mn
CaSO: Dy
BeO
350
310
1930
1.5
0.6
0.5
0.3
General characteristics of TL materials 91
The neutron response depends upon the sample thickness, the isotopic content of the
material and the irradiation conditions. Moreover, the neutron sensitivity will also depend
on the material surrounding the detectors. Therefore the values in table 5.2 can only be
used as a rough indication of the thermal neutron sensitivity of the listed materials.
As can be seen from the table (apart from other considerations) one of the most useful
materials for performing gamma measurements in a mixed neutron-gamma field seems to
be BeO due to its low response. Conversely
7
LiF shows a rather high response to neutrons
and therefore corrections must be applied to this detector when used in a neutron dose-
meter employing two detectors (
6
Li and
7
Li) in order to discriminate gamma rays from
neutrons.
Similar considerations apply to the sensitivity of TL phosphors to fast neutrons (see
chapter 12). As an example table 5.3 shows the response of LiF and BeO to fast neutrons
[15]. In this case the equivalent responses are rather low and if fast neutrons encountered
in personal dosimetry have to be measured, it would be necessary to use some converters
in front of the TL detectors in order to obtain greater sensitivities.
Table 5.3. Fast-neutron sensitivity.
Energy (MeV)
Response
BeO
(10' cm
2
)/Rcsponse (R of
60
Co)
LiF
0.5
1.0
2.7
4.2
15
Fission (critical assembly)
0.6
1.0
3.3
3.9
20
1.0
0.2
0.3
1.2
1.7
10
0.4
5.6. Fading
The release of electrons and holes from their traps and consequently their recombination
is a statistical phenomenon, the probability of which is a function of temperature.
This probability is given by:
P = Sexp(-E/kT)
with P = transition probability, S = vibrational factor characteristic of the centre,
E = activation energy, k = Boltzmann's constant, and T = absolute temperature.
The half-life of the phenomenon is given by
T = 0.693 P'K
Table 5.4 gives the temperature of the different peaks and information on the stability
of the carriers in the corresponding traps at 20C for some phosphors [10]. When this
information is not available in the table, an estimate of the loss of the signal during the
period for a storage temperature of 20 C is reported within parentheses. These values are
only qualitative, as they are taken from different authors who have not necessarily used
the same experimental parameters.
92 G Busuoli
Table5.4. Glow peak temperatures and halflives for different TL phosphors.
TL material
L iF : Mg
CaF
2
: Mn
CaF
2
: Dy
BeO
L i
2
B
4
0
7
: Mn
Peak
number
I
II
III
IV
V
VI
I
I
II
III
IV
I
II
III
IV
I
II
III
IV
Emission
temperature (C)
70
130
170
200
225
275
260
120
140
200
240/
70
160
180
220/
50
90
200 1
220/
Halflife
5 min
10 h
0.5 yr
7yr
80 yr

1% per day
25% per month
0% per 5 month
10% per 2 month
As is well known, the unintentional loss of the latent information is called fading.
Temperature is normally responsible for this loss, but other quantities such as light can
greatly influence the latent information in the TL material.
In table 5.5 the thermal fading measured for the most commonly used TL materials
is given [1]. As can be seen, the majority of the listed materials do not have a large degree
of fading; one exception is CaS0
4
: Mn as it presents a peak at a relatively low tempera
ture. Therefore this material cannot be used over such long periods of time as those
normally accepted for routine personnel dosimetry.
Concerning thermal fading, the shallow traps will fade more rapidly than deep ones
due to a larger transition probability. This fact can produce large errors in dose assess
Table 5.5. Fading characteristics.
TL material
L iF : Mg
L i
2
B
4
0
7
: Mn
CaF
2
: Mn
CaF
2
: Dy
BeO
CaS0
4
: Mn
Thermal fading (25 C)
~ 5 % in 1 year
10% in 2 months
~l %i n 1 day
~ 13% in 1 month
~ 8% in 3 months
5085% in 3 days
Optical fading
Weak
Weak

Strong
Strong

General characteristics of TL materials 93


ment and in order to avoid them the shallow traps can be emptied intentionally by a post-
irradiation heat treatment either in a separate oven or in the reader as part of the readout
process. This thermal treatment, when applicable, will increase the stability of the latent
information even over very long periods.
Table 5.5 also gives some qualitative indications of optical fading, i.e. the modification
due to artificial light or sunlight [1]. In fact, electron transitions may be stimulated by light
(particularly near-uv light) giving rise to two effects that can take place simultaneously:
(a) the creation of a spurious signal, and
(b) the loss of the latent dose information.
The two effects can be equally important; for example, for IiF-Teflon spurious doses
of the order of several millirad have been observed for discs exposed to sunlight for
several hours. At the same time irradiated LiF kept near a uv source for about one day
had a reduction of the recorded dose of the order of 35%.
However, the sensitivity of different detectors to light is not a big disadvantage as it
can be avoided by simply wrapping them in a light-tight envelope.
5.7. Annealing procedures
For each TL material used in dosimetric applications, it is extremely important to know
the procedure for restoring its basic conditions after an irradiation. This procedure is
called annealing and has two aims: the first is to empty the traps of the phosphor com-
pletely after the irradiation and readout cycle; the second is to stabilise the electron
traps in order to obtain, within narrow limits, the same glow curves even after repeated
irradiations and thermal treatments. The annealing procedure is similar for every TL
material and, in some cases such as LiF, it is very critical because if the procedure is not
strictly the same, one can obtain significantly different results from repeated irradiations
to the same exposure.
In table 5.6 are summarised the annealing procedures for several TL materials used in
practice. As can be seen, the heat treatment needed to anneal LiF (TLD 100) and to
stabilise its response is somewhat complex and it must be performed in a very rigorous
and reproducible way.
The different annealings given in the table are necessary in order to empty all the traps
(shallow and deep) of the phosphor. Many TL materials also have different peaks at low
Table 5.6. Annealing procedures.
TL material Annealing procedures Pre-read annealing
LiF (TLD 100) l h a t 4 0 0 C + 24ha t 80C 10mi na t l 00 C
(or 2 ha t 100C)
Li
2
B
4
0
7
: Mn 15 min at 300C 10 min at 100C
BeO 15 min at 600 C
CaF
2
:Dy (TLD200) l h a t 4 0 0 C
CaF
2
:Mn (TLD 100) l h a t 4 0 0 C
LiF (PTL 700) 240-250 C in the reader Performed in the reader
94 G Busuoli
temperature; these peaks are likely to be emptied even at room temperature (particularly
peaks below 100C) so in many cases it is necessary to perform a partial annealing before
the reading in order to avoid a significant loss of information. This procedure is known as
pre-read annealing and, in table 5.6, these treatments are also given.
Of course, the annealing procedure makes the evaluation time longer so that, in many
cases, new materials have been studied in order to avoid a long heat treatment. This is the
case, for example, for LiF (PTL 710) [16].
Finally, in order to perform a quick assessment of the dose recorded by the TL detec-
tors, particular set-ups have been introduced in the readers for obtaining, in a simple
and rapid way, the reading of TL light and, afterwards, the annealing of the detector, its
reproducibility remaining the same. This procedure, however, can only be applied when
the radiation dose is not too high and the residual signal is comparable to or lower than
the background signal of the non-irradiated phosphor.
In the case of high irradiation it is therefore necessary to perform a high-temperature
anneal of the TL detector.
5.8. Stability and reproducibility
The term stability here means physicochemical stability. A phosphor used for dosimetric
purposes should not undergo any physicochemical changes during the repeated annealing
processes and repeated exposures. This means that the glow curve, as well as the non-
radiation-induced light emission and TL yield, must not change during extended storage
of the material, repeated irradiation and reading. If these conditions are fulfilled the TL
material can be used for dosimetric applications.
Several materials can be re-used many times without any noticeable changes in the
material as long as it is not exposed to high doses.
As a consequence of the stability of the phosphor one can evaluate the reproducibility
of each material to a certain dose level by calculating the standard deviation of a repeated
set of measurements under the same exposure and reading conditions. As a practical
example of reproducibility, table 5.7 gives some experimental data obtained with two
different kinds of detectors irradiated at 1 R using ^Co gamma rays [9]. In this case the
readings were performed in an automatic apparatus which uses hot nitrogen as the heating
medium. At this dose level the readout cycle was sufficient to anneal the different
phosphors.
Table 5.7. Reproducibility of four types
BeO
(9.5 mm
diameter)
Standard deviation 3.6%
(over 6 d)
of detectors.
BeO
(9.8 mm
diameter)
9.8%
BeO
(6.3 mm
diameter)
1.0%
LiF
( TL D 100)
1.1%
General characteristics of TL materials 95
5.9. D ose rate dependence
The dose rate dependence of LiF, Li
2
B40
7
:Mn and BeO was studied by exposing these
detectors to an x-ray beam which emits very short pulses of high intensity [17]. The pulse
duration was 10~
7
s. The results obtained have shown that:
(a) the response of LiF is not modified up to an exposure of 1.5 x 10
11
R s
_1
;
(b) the response of BeO is not modified up to 5 x 10
11
R s
_1
;
(c) the response of Li
2
B
4
0
7
is independent of the dose rate up to 10
l 2
Rs
_1
.
The non-dependence on dose rate is an important requirement that demonstrates the
possibility of using the TL detectors for measurements near installations delivering photons
in very short pulses.
It has demonstrated that for radiological protection purposes the dose rate dependence
of TL materials can be taken as insignificant.
5.10. Tribothermoluminescence (or triboluminescence)
Triboluminescence is a spurious signal that should be avoided, as otherwise it would be
included in the measurement, thus increasing both the detection threshold and the error
in the dose assessment.
The mechanism of this phenomenon is not well known: it is believed to be produced
by the mutual friction of the crystals. The surface tensions so created release their energy
as light during the heating process.
The triboluminescence depends on the physical state of the detector. Microcrystalline
powder presents a larger triboluminescence in comparison with extruded or single-crystal
detectors. For LiF, for example, the light emitted due to tribo-phenomena can be
approximately equivalent to 1 rad or 20 mrad, depending on the physical state of the
detector.
In order to eliminate this phenomenon, an experiment was carried out [18] which
showed that it is sufficient to heat the sample in the absence of oxygen. Very good results
can be obtained by putting the detector in an atmosphere of inert gas such as argon or
nitrogen. No theoretical explanation has been given for this influence of the gas in
eliminating triboluminescence.
Of course, the triboluminescence is more or less important depending on the dose
received by the detectors. So in the case of dose measurements at therapy levels (doses of
the order of several hundred rad) it is not important to use inert gas during the readout
process. Conversely, in routine personnel dosimetry where the dose is not known a priori,
it is essential to heat the detector in the presence of the inert gas (normally nitrogen).
References
1 1975 Technical Recommendations for the Use of Thermoluminescence for Dosimetry in Individual
Monitoring for Photons and Electrons from External Sources. Commission of the European Com-
munities Doc. EUR 5358
2 Busuoli G, Rimondi O and Vicini G 1973 Commission of the European Communities Doc.
CEC(73)9
3 Cameron J R, Zimmerman D and Blond R 1967 Proc. 1st Int. Conf. on Luminescence Dosimetry,
Stanford University, June 1965. USAECDiv. Tech. Inf. AEC 8
96 G Busuoli
4 Busuoli G, Cavallini A, Fasso A and Rimondi O 1970 Phys. Med. Biol. 15 673
5 Attix F H 1968 Health Phys. 15 49
6 Bassi P, Busuoli G and Rimondi O 1976 Int. J. Appl. Rad. Isotopes 27 291
7 Morgan K Z and Turner J E 1967 Principles of Radiation Protection (New York: Wiley)
8 Becker K 1973 Solid State Dosimetry (Cleveland, Ohio: CRC Press)
9 Busuoli G and Julius H W 1977 Proc. 5th Int. Conf. on Luminescence Dosimetry, Sao Paulo, 14-17
February (Giessen: I Physikalisches Institut of the Justus-Liebig Universitat)
10 Portal G 1975 Rep. CEA-R-4697
11 Spumy F, Medioni R and Portal G 1975 Rep. CEA-R-4687,CEA-R-4688
12 Horowitz Y S, Freeman S and Dubi A 1979 Nucl. Instrum. Meth. 160 313
13 Horowitz Y Setal 1979 Nucl. Instrum. Meth. 160 317
14 Viragh E and Zsolnay E M 1980 Proc. 6th Int. Conf. on Solid State Dosimetry, Toulouse, 1-4
April. Nucl. Instrum. Meth. 175 No 1 (September)
15 Tochilin E, Goldstein N and Miller W G 1969 Health Phys. 16 1
16 Portal G, Francois H and Blanchard P 1969 Rep. CEA-R-3476
17 Goldstein N 1972 Health Phys. 22 90
18 Schulman J H, Attix F H, West E J and Ginther R J 1960 Rev. Sci. Instrum. 31 1263
Applied Thermoluminescence Dosimetry. Eds M Oberhofer and A Scharmann
1981 ECSC, EEC, EAEC, Brussels and Luxembourg
6
Preparation and properties of principal TL products
G PORTAL
6.1. Introduction
This chapter furnishes detailed information about the production, physical and dosi-
metric properties of the most commonly used TL phosphors. The phosphors treated here
are activated lithium fluoride (LiF), lithium borate (IJ2B4O7), magnesium borate
(MgB
4
0
7
), beryllium oxide (BeO), calcium fluoride (CaF
2
), calcium sulphate (CaS0
4
) and
aluminium oxide (A1
2
0
3
).
6.2. Lithium fluoride
First studied by Daniels [18,19] who used crystals intended for optical applications, LiF
was abandoned for other materials which do not present low-temperature traps. Studies
were resumed by Cameron [11, 12] who conceived the systematic regeneration of LiF
and encouraged the commercial production by The Harshaw Chemical Company (in the
following just referred to as Harshaw) of products known as TLD 100, TLD 600 and
TLD 700 depending on their preparation from natural lithium or lithium enriched with
6
Li or
7
Li (LiF TLD). A similar quality LiF, stabilised with sodium, was studied in France
by Portal [45-47] and commercialised by Desmarquest & CEC, SA under the name of
PTL 710, 716 and 717 (LiF PTL). These products do not necessitate systemic regeneration
before each usage.
6.2.1. Preparation of LiF
The preparation of LiF is delicate. Only well equipped laboratories with trained staff can
produce a material of good quality. It is generally more convenient to use commercial
products. '
6.2.1.1. Preparation of LiF TLD powder
Two methods were described in the Harshaw [33] patent.
6.2.1.1.1. Solidification method. The following materials are mixed in a graphite
crucible:
Lithium fluoride 1000000 parts by weight
Magnesium fluoride 400 parts by weight
Lithium cryolite 200 parts by weight
Lithium titanium fluoride 55 parts by weight
98 G Portal
After having obtained a homogeneous fusion of the mixture in vacuum the product is
slowly cooled, pulverised and graded between 60 and 200 /im.
6.2.1.1.2. Single-crystal method. The mixture mentioned above is placed in a vacuum or
inert-atmosphere oven in which a single crystal is drawn using the Czochralski method
[17]. The graphite crucible is placed in a zone where the temperature is sufficiently high
to obtain a homogeneous fusion mixture. It is then slowly moved to a zone of lower
temperature which allows progressive solidification (about 15mmh
_1
). After cooling,
this material is also pulverised and graded between 60 and 200 /mi.
This method, which takes more time to produce TLD grade l i F, allows preparation of
more sensitive products than the solidification method described under 6.2.1.1.1.
In both cases the TLD powders are annealed at 400 C for some hours and at 80 C
for 48 h.
6.2.1.2. Preparation of compressed LiF TLD
The LiF powder mixture is placed in a neutral-atmosphere press at a carefully chosen
pressure and temperature, e.g. 3500 kg cm"
2
and 700 C. The piston of the press pushes
the mixture through a hole which acts as a die. The bar so obtained is then sectioned to
provide pellets of uniform thickness. The faces of the pellets are polished. The extruded
dosemeters exhibit the same TL properties as the powder. The mixture undergoes a
crystallisation, very likely due to the combined effect of temperature and pressure, for
which the result is similar to that obtained by the Czochralski method.
6.2.1.3. Preparation of sodium-stabilised LiF PTL
The following compounds are added to LiF powder [46]:
(i) 200 PPM magnesium fluoride,
(ii) 1-2% by weight of sodium fluoride.
The powdered mixture is homogenised. It is then put in an aluminium oxide crucible
and held at the crystallisation temperature for about 3 h in a nitrogen flow oven. The
temperature is then progressively reduced to 60 C in 45 min, the sample taken out of the
oven and cooled rapidly. The product is finely pulverised, then subjected to an identical
treatment. It is finally repulverised and graded between 60 and 200 /jm.
Annealing is carried out to encourage the creation of stable traps. An ordinary oven is
made use of for this purpose with no nitrogen flow. 500 C is used as the annealing
temperature over 72 h. Cooling of the crystals is obtained by pouring them on to a cold
metal plate. The final product has a sensitivity equivalent to the LiF TLD produced by the
Czochralski method.
6.2.1.4. Preparation of LiF PTL pellets
PTL TLD powder is finely sieved, compressed at about 5000 kg cm"
2
in the desired form
and then placed in a nitrogen gas oven. The chosen temperature is slighdy lower than
the fusion temperature. Under these conditions a new fusion of microcrystallites is
obtained. The pellets can be used after a simple annealing at 500 C.
Preparation and properties of principal TL products
99
6.2.1.5. Preparation of LiF-Teflon dosemeters^
The production of LiF-Teflon (PTFE) dosemeters was first described by Bjarngard [4].
The commercial rights are protected by patents (e.g. British Patent Specification
1140028). Patent holders are Teledyne Isotopes Inc. The material is also produced,
under licence, by D A Pitman Ltd.
The production technique is based on a thorough mixing of LiF powder of grain size
less than about 80 /urn with fine Teflon powder; the average l i F grain size is about 10 im\.
Both components need to be dry in order to avoid clogging. The optimum mixing time
depends upon the design of the mixer and amount of mix. Too short a time results in an
uneven phosphor distribution, whereas too long mixing times lead to the separating out
of phosphor grains coated with fine Teflon powder. The mixture is either moulded into
bars of, typically, 5-15 mm by compressing it into a mould, sintering at 365 C for about
1 h and slow cooling, or extruded, typically as a 1 mm rod. For moulding, the highest
content of LiF is about 30% by weight. Higher concentrations would deteriorate the
mechanical properties of the dosemeters. For extrusions, the maximum loading is about
10%, with 4% being the normal loading. The moulded or extruded material is cut into
dosemeters of the desired shape. Discs are made from bars by parting off on a lathe or,
for very (ultra) thin discs, on a microtome. Tape is fabricated by shaving the sides of a
bar.
6.2.2. Physical properties of LiF
6.2.2.1. TL glow curve
The TL glow curve of LiF is quite complicated because of its complex trap dynamics,
as can be seen in figure 6.1.
The main peak normally used for dosimetric purposes, called the dosimetry peak, is
peak V at a peak temperature of 225 C. The corresponding trap level is very stable. The
C/1
z
L iF TLC
IV
III
II
- 1 0 0
V
z
t
Z
I
1
_!
I
TEMPERATURE (C) TEMPERATURE (C ]
f This subsection has been inserted by the editors.
Figure 6. 1. Glow curves of LiF TLD 100
(Haishaw [33]) and LiF PTL 710 (Des-
marquest [22]), no particular annealing
treatment.
100 G Portal
low-temperature peaks I, II and III are relatively unstable and must be suppressed by a
thermal regeneration process.
In the case of LiF TLD this process consists of a heat treatment at 400 C for two
hours followed by a rapid cooling (figure 6.2). This thermal treatment restores the initial
height of peak V and reduces the heights of peaks I, II and III. They are completely
suppressed by a further heat treatment at 80 C for 24 h. This treatment (standard
anneal) is to be repeated before each exposure, since during the reading the effect of the
thermal treatment is lost.
100 200 300 400 500 600 700 800
TEMPERATURE ( C)
Figure 6.2. Peak heights of LiF TLD 100
(peaks I-V) as a function of annealing tempera-
ture for a 2 h anneal and rapid cooling.
For sodium-stabilised LiF PTL annealing is generally unnecessary with the reader
operated in the proper mode (use of a preliminary heating plateau at about 160C).
As can be seen in figure 6.1, peaks I and II are feeble and peak III is practically non-
existent. In these conditions the same sample can be re-used repeatedly without regenera-
tion. Nevertheless, regeneration is necessary for heavily irradiated samples. Figure 6.3
shows that the best value for peak height V/peak height II is obtained with an annealing
at 500 C for half an hour and rapid cooling.
Figure 6.4 gives an idea of the stabilising effect of sodium on the TL glow curve. The
glow curve for LiF without sodium is totally degraded after a thermal treatment at
210 C over 15 s. This is the temperature up to which the phosphor is heated during one
heating cycle. The height of peak II is increased considerably, reaching that of peak V at
around 30 s.
The LiF PTL system is definitely more resistant.
Figure 6.1 also shows that there is a peak at a temperature of 275 C corresponding to
a high-energy trap level in the phosphor. This peak shows up with relatively high absorbed
doses (about 100 rad) and is more pronounced with exposure of LiF to high LET
particles, such as the alpha particles produced by thermal neutrons in the
6
Li(n, a)
3
H
reaction. Some more high-energy trap levels with corresponding TL emission peaks exist
up to 500 C. They are not discussed here.
Preparation and properties of principal TL products 101
Figure 6 J . Peak heights of L iF PTL 710
(peaks IV) as a function of annealing tempera
ture for a 3h anneal followed by rapid cooling.
100 200 300 400 500 600
TEMPERATURE (C)
~ 100
1/1
3
cL
\_
m
or
<
1
o
HI
I
I
X-
<
90
80
70 -
60 -
50
40
30
20 -
10 \
0
Li F TLD 700 PEAK
J A ^
j N . i F TLD 700 PEAK I I
J
- f -
15
+
Li F PTL 710
PEAK Y
LiF PTL 710
PEAK I I
+
30 60 120
TIME OF HEAT- TREATMENT ( s)
Figure 6.4. Effect of a 210 C heat treatment on the peak heights of L iF TL D 700 and
L iF PTL 710.
6.2.2.2. Trap characteristics
The emission maxima of LiF occur at the temperatures given in table 6.1. The halflives
of the corresponding traps at 20 C are summarised in table 6.2.
One can state that, as a rule, the first two levels are unstable. They must not be used
for long integration times. Level III only presents difficulties for integration times
exceeding several weeks. Levels IV, V and VI are sufficiently stable for most dosimetric
applications [49].
102 G Portal
Table 6.1. LiF peak temperatures.
Type of ph
LiF TLD
LiF PTL
Table 6.2.
Type of ph
LiF TLD
LiF PTL
osphor Peak
I
II
III
rv
V
VI
I
II
V
VI
no. Peak temperature (C)
(maximum)
65
120
160
195
210
275
80
130
220
280
Half-lives of the LiF trap levels.
osphor Peak
I
II
III
IV
V
I
II
V
VI
no. Half-life
5 min
l Oh
0.5 yr
7yr
80 yr
20 min
80h
1.3 XlO
7
yr
not measured
6.2.23. Emission characteristics
The maximum emission wavelength of LiF is 400 nm for both LiF TLD [29] and LiF
PTL [48]. All traps give an identical emission. The intrinsic TL efficiency (TL yield),
defined as the ratio of energy emitted in the form of light per unit of phosphor mass and
absorbed dose, is 0.04, a low value if compared with the majority of TL materials used.
This explains the low sensitivity of LiF in general.
6.2.2.4. Model
At present there is no completely satisfactory model. It is certain that magnesium plays an
essential role in the creation of traps. Claffy [15] showed that, if LiF contains less than
1 PPM of magnesium, it is not thermoluminescent.
Magnesium has an atomic diameter (0.065 nm) close to that of lithium (0.060 nm)
and can therefore easily substitute the latter. This has two consequences:
(i) It favours the creation of electron traps. With magnesium being divalent, a local
excess positive charge is produced.
(ii) It favours the creation of electron holes, because in compensating the excess
positive charge of the divalent magnesium ions substituting the monovalent ions of
lithium, alkali ion valencies appear in the crystal lattice.
Preparation and properties of principal TL products 103
+ - +
- (fK- + - + - + vti> -
- + - + - \ +* ) - + - + - '<*+/-
+
* \ + - +"- vf+K- + -/|j) - "^
-\(1) - + - + -\-) - (*/- + -\+f>
D IPOLE D IMER TRIMER
n=1 n = 2 n = 3
Figure 6.5. Model for trap formation in LiF, dipoles and complexes (ffl = ion vacancy).
Grant and Cameron [30] showed, by dielectric measurements, that trap level II is due
to the creation of Mg
2+
-n dipoles (figure 6.5,n = 1) and Harris and Jackson [32] showed
that trap levels II and III are due to dipole coupling or dimers (figure 6.5, n = 2). Stoebe
et al [61], following results of ionic conductivity measurements on samples annealed at
different temperatures, provided the hypothesis that grouping of three dipoles (trimers)
is responsible for trap levels IV and V (figure 6.5, n = 3). Claffy [15] explains the forma-
tion of trap level VI by the regrouping of groups of dipoles. In some recent work Nink
and Kos [43] show that F centres are involved in TL peak V. According to the authors the
migration of Nig
2
* and Mg
+
to F centres leads directly to the formation of so-called Z
centres:
Mg
2+
+ FMg
2+
F = Z
3
Mg
+
+ FMg
2+
F' = Z
2
.
The Z-centre concentration is enhanced when an increased concentration of isolated
magnesium impurities is present (Z
2
-Z
3
model). The creation of Z centres from F centres
and isolated Mg ions and their reciprocal conversion leads to a probable explanation of
Z
2
centres to be responsible for TL peak V of LiF:Mg, Ti. According to Rossiter et al
[53] the luminsecent centres are due to the presence of titanium and/or aluminium.
6.2.3. Dosimetric properties
LiF is the most commonly used TL material. It provides a good compromise between the
desired dosimetric properties (see chapter 5). Its effective atomic number is sufficiently
near to that of tissue (Z
e
f
f
(
LiF
) = 8.14,Z
e
ff(
tissue
) = 7.4) so as to provide a response which
varies only slightly with photon energy: it varies by about 30% between 3.0 keV and
1.2 MeV (see figure 6.6 [48]) and one says that it is tissue equivalent.
Although its sensitivity is lower than certain other TL materials (see later subsections)
it allows dose measurements from 10 mrad, which is a detection limit sufficient for most
current dosimetric applications.
Figure 6.7 shows the dose characteristic of LiF. Supralinearity starts at 300 rad with
more recent samples and at 100 rad if the reader is set in a way to eliminate the
influence of peak VI of the glow curve. With earlier industrial LiF products, supra-
linearity was observed starting at 800 rad. If LiF is pre-irradiated with a dose of 10
4
rad
104 G Portal
THEORETICAL CURVE
( Q) 0"/. NQF
( b) 2V. NQF
+ 3/. NaF
EXPERIMENTAL CURVE ( L iF PTL -717)
10 1CT 10
J
PHOTON ENERGY ( keV)
Figure 6.6. Energy dependence of the response of LiF.
10*
Figure 6.7. Dose characteristic of LiF. (a) Original
material, (b) pre-irradiated (KVrad) material.
DOSE ( r od )
[24] its sensitivity increases by a factor of 2-3 and its linearity extends up to 10
4
rad.
Thermal regeneration reduces the effect of this treatment.
Samples which have received doses of 10
s
rad and more since their fabrication cannot
be regenerated any longer by thermal treatment. LiF containing
6
Li is sensitive to thermal
neutrons. Table 6.3 (from EUR 5358) summarises the results of LiF TLD dosemeter
exposures to a thermal neutron radiation of 10
10
n^cm"
2
. The material was standardised
using a ^Co source. The data are expressed in roentgen-equivalents.
Preparation and properties of principal TL products 105
Table 63. Sensitivity of LiF TLD to
thermal neutrons (from [68]).
Phosphor Sensitivity
TLD 100
TLD 600
TLD 700
328
1360
1.1
Table 6.4. Sensitivity of LiF PTL to thermal neutrons
(from [48]).
Type of neutrons PTL 710 PTL 717
Thermal
2S2
Cf
Pu-Be
14.7 MeV
450
0.16
2.5
9.5
2.5
0.73
1.9
7.2
Table 6.4 [48] gives the sensitivity of LiF PTL to neutrons of different energies. Again
the results are expressed in roentgen-equivalents.
Figure 6.8 [66] shows the relative response of LiF (peak V) for various LET radiations.
This response decreases with increasing LET of the ionising particles (protons, alpha
particles, etc). According to this figure the TL yield for a particles from the reaction
6
li(n, a)
3
H, the average LET of which is 140keV/um
_1
, amounts to 0.22, a rather low
sensitivity value. In contrast, trap level VI (peak VI) is particularly sensitive to a particles.
For example, the ratio peak height Vl/peak height V is 0.015 for ^Co gamma rays and
0.175 for thermal neutrons. This difference in behaviour allows one to monitor the
presence of thermal neutrons in a mixed radiation field (for more on neutron sensitivity
of TL phosphors, see chapter 12).
w
1.0
o
Q.
i/i 0.8
111
CZ
UJ 0.6
>
< 0.4
_i
LU
a
0.2
ENERGY ( MeV)
1000 200 50 20 10 5 3
T
- r
T" T T
0.1 1.0
LET (keW/um )
Figure 6.8. Relative response of LiF as a function of LET and/or particle energy. A, protons
of 720 MeVjO, a particles; *, a particles from
6
Li (n, a)
3
H reaction (from [66]).
106 G Portal
6.3. Lithium borate
6.3.1. Manganese-activated lithium borate
Schulman [59, 60] studied the preparation and properties of different borates activated
with manganese. One of the most interesting borates turned out to be lithium tetraborate
IJ2B4O7 +0.1% Mn. More recent work by Christensen (see [5]) resulted in materials
which show improved air and tissue equivalence and higher stability with respect to air
humidity.
6.3.1.1. Preparation
The preparation of li
2
B40
7
:Mn is relatively straightforward. Kirk et al [37] proposed a
mixture of 32.5 g of lithium carbonate and 108.96 g boric acid. The mixture is added to
a 5 ml aqueous solution of 75 mg MnCl
2
4H
2
0 which is heated at 100 C for 12 h.
The product is placed in a platinum crucible, heated up to 950 C and then rapidly
cooled. The crystalline mass thus obtained is ground and graded between 75 and
175 im. Botter-Jensen and Christensen [5] added 0.25% by weight of silica to reduce the
influence of humidity on the lithium borate which is very hygroscopic. The material can
be sintered at 900 C to prepare solid detectors or diffused into a plastic carrier such as
Teflon or silicone rubber.
6.3.1.2. Physical properties
The TL glow curve of Li2B
4
0
7
:Mn (figure 6.9) is composed of two groups of distinct
peaks:
(i) one series of unstable peaks between 50 C and 90 C,
(ii) a double peak, the first of which appears at 200 C at low doses and the second of
which appears at 200 C for doses in excess of 50 rad. Another peak appears with
high LET radiation at 350 C.
Only the double peak is suitable for dosimetric purposes due to its stability. However,
this peak is less favourable than the dosimetry (210C) peak of LiF because of its fading
20 l 100
50
TEMPERATURE C O
400
Figure 6.9. Glow curve of Li,B
4
0,:Mn at 3.4, 8.6, 27.3,
69.2 and 960 min, respectively, after irradiation [59].
Preparation and properties of principal TL products 107
characterstics. In fact, Li
2
B
4
0
7
:Mn loses 10 and 37% of its information in 2 and 13
months, respectively, when kept at ambient temperature. Christensen et al [14] showed
the effect of humidity on fading. The addition of Si0
2
(0.5%) to the phosphor reduces
fading notedly.
In contrast to LiF the reading procedure does not change the distribution of traps in
Li
2
B
4
0
7
:Mn. Therefore this phosphor can be used without regeneration. If regeneration
is necessary, for zeroing the phosphor after high doses for example, it is sufficient to
reheat the material at 300C for 35 min.
The wavelength of the light emitted from Li
2
B
4
0
7
:Mn (main peak) is about 600 nm
[29]. From this it follows that with the photomultipliers normally mounted in com-
mercially available TL readers the sensitivity of Li
2
B40
7
:Mn is low: 1/8 of that of LiF
with an S 11 photocathode and 1/2 of that with an S20 photocathode and this in spite
of the fact that the intrinsic sensitivity (TL yield) of Li
2
B
4
0
7
:Mn is a factor of 1.83
higher than that of LiF (0.04). Brunskill [8, 9] used an SbCsO photocathode. In this case
the sensitivity reached a higher level. Christensen, on the other hand, used a photo-
multiplier tube with an S photocathode. He found similar sensitivity for Li
2
B
4
0
7
:Mn
and LiF. Attempts were made to modify the emission wavelength. Replacing manganese
by silver, Moreno et al [41] obtained a uv emission which, though making the spectral
distribution of the emitted light more favourable, enhanced its light sensitivity, an un-
desirable feature.
6.3.1.3. Dosimetric properties
The apparent sensitivity of Li
2
B
4
0
7
:Mn depends upon the characteristics of the reader
used, as mentioned earlier.
In their preliminary work, Schulman et al [59] observed background noise, which
limited the minimal detectable dose to lOOmrad. More recently reports by Christensen
[13] and Brunskill [8] showed that it is possible to measure doses down to 10 mrad with
sintered detectors. Christensen studied the influence of the manganese concentration on
Li
2
B
4
0
7
:Mn properties. He concluded that samples prepared with 0.4% by weight of Mn
presented the best compromise between sensitivity, energy dependence and humidity
resistance. The samples he prepared had a linear response up to 300 rad and were supra-
linear up to 3 x 10
6
rad (figure 6.10). Kirk et al [37] obtained a material linear from 1 to
10
s
rad following a pre-irradiation of 10
s
rad. This material is four times more sensitive
but exhibits a background noise which limits the minimal detection of doses around
l rad.
Li
2
B
4
0
7
:Mn is light-sensitive. This creates a background equivalent to about 15 mrad.
Li
2
B
4
0
7
:Mn is the TL material which presents the least variable response with photon
energy. Jayachandran et al [34] showed that the energy dependence of the response of
Li
2
B
4
0
7
: Mn is equal within 3% to that of air and/or water with a 0.34 and/or 0.1%
by weight content of manganese.
With the presence of
6
Li and
10
B the phosphor is very sensitive to thermal neutrons.
Wallace and Ziemer [64] reported that a sample exposed to a dose equivalent of 1 rem
yields a response to thermal neutrons equal to that of a sample exposed to 67 R y radia-
tion. Christensen found 42 R rem
-1
under slightly different conditions. Li
2
B
4
0
7
:Mn is
therefore slightly more sensitive to thermal neutrons than is LiF TLD 100.
108
G Portal
10 10
1
10* I0
3
10' I0
5
ABSORBED DOSE ( r od)
Figure 6.10. Li
2
B0
7
:Mn TL output as a function
of absorbed dose.
Wallace et al studied the response of Ii
2
B40
7
:Mn to fast neutrons from a Pu-Be
neutron source. They obtained 0.01 R rem
-1
.
Figure 6.11 demonstrates that the relative response of Ii2B
4
07:Mn as a function of
LET is quite different to that of LiF.
10 10 10
1
10
2
10'
LET ( keV/ pm)
Figure 6. 11. Relative response of LiF,
BeO and LijB
4
0
7
:Mn as a function of
LET of charged particles [62].
6.3.2. Copper-activated lithium borate
Takenaga recently proposed a new sintered TL phosphor activated with copper.
6.3.2.1. Preparation
To raw Li
2
B
4
0
7
powder a solution of CuCl
2
in acetone or alcohol is added and the
mixture is then stirred and dried. The U2B4O7 powder containing the activator compound
is heat-treated in air in a platinum boat for about 1 h at a temperature between 900 and
913 C, which is just below the melting point (917 C) of Li
2
B
4
0
7
.
By the heat treatment clear crystals, having an almost spherical form, are produced
from the raw powder of Li
2
B
4
07, which is porous and opaque. The heat treatment causes
Preparation and properties of principal TL products 109
diffusion of the activator into the Li
2
B
4
0
7
crystal as well as recrystallisation and sintering
due to diffusion, vaporisation and deposition.
6.3.2.2. Physical properties
Li2B
4
0
7
:Cu phosphor exhibits two TL peaks. One is a small and rapidly decaying peak
at about 120 C and the other a dominant and stable peak at about 205 C.
It has been found that the stoichiometric phosphor (lLi
2
0-2B
2
03) shows minimum
absorption of humidity. In this case the loss in sensitivity due to the effect of humidity
is 10 and 25% respectively after two and six months of storage.
6.3.23. Dosimetric properties
The sensitivity to y rays is about 20 times higher than that of Li
2
B
4
0
7
:Mn produced by
the Schulman method. One of the factors contributing to this relatively high sensitivity
is the favourable spectral location of the TL emission which peaks at 368 nm.
Some other dosimetric characteristics of the stoichiometric phosphor were also in-
vestigated, (i) Linearity: the TL output is linear with exposure to about 10
s
R, above
which it is sublinear by colouring, (ii) Fading: the dominant peak at 205 C fades less
than 9% in intensity at 25 C and 30% at 50 C after 60 d in the dark, (iii) Light-induced
fading: the TL output fades less than 10% after exposure to room lighting at 1000 lx for
3h.
63. 3. Magnesium borate activated with dysprosium or thulium
This product was recently introduced by Prokic [51]. It contains a little amount of
yttrium used as a sensitiser of the TL emission. The material is produced in the form of
sintered dosemeters.
The wavelengths of the TL emission spectra for MgB
4
0
7
:Dy/Tm are typical of that for
dysprosium or thulium atoms, which show emissions in the green-yellow band for Dy
and emissions in the blue band for Tm. The influence of the co-activator reflects only on
the relative emission efficiency of the basic activator, but the spectral distributions
mainly stay unchanged for the Dy activator. However, the co-activator changes the
emission in the Tm-activated material into green-yellow light.
MgB
4
0
7
:Dy/Tm has a sensitivity about seven times higher than LiF TLD 100. Its
effective atomic number for photoelectric absorption is similar to the effective atomic
number of LiF.
The material does not require annealing before irradiation and after read-out. Fading
amounts to under 10% during the first 60 d after irradiation when the appropriate post-
irradiation annealing is applied similar to LiF or after applying a corresponding
read-out procedure with a preheating in the reader.
Magnesium borate TLD are not hygroscopic or light sensitive. With a Harshaw Model
2000 TL analyser this material detects exposures of 1 mR with 25 mg samples.
6.4. Beryllium oxide
BeO, like other oxides of calcium and magnesium, exhibits TL properties. It is the very
small quantities of impurities always present in these materials which are responsible for
110 G Portal
the TL. Moore [40] was one of the first to study the TL properties of BeO. Jones et al
[35], Tochilin et al [63] and Scarpa [54] studied its dosimetric properties.
6.4.1. Preparation
Only specialised laboratories are capable of producing BeO. It is commercially available
in microcrystalline powder form. However, dispersed in air as a fine powder, this material
is extremely toxic and therefore only specially equipped laboratories can use it in this
form. Sintered pellets are also available which are used as transistor bases in the electronics
industry. In this form the material presents no danger as long as abrasion of the surfaces
and therefore production of powder and dust is avoided. These sintered materials contain
sodium to increase their sensitivity.
6.4.2. Physical properties
The TL glow curve varies with the origin of the product. Scarpa [54] noted that the
temperature of the main peak varies between 180C and 280 C and that some samples
contain unstable traps.
The product chosen by Tochilin et al [63] showed two stable neighbouring peaks at
180C and 220 C, respectively. The second peak appears with relatively high doses and
becomes preponderant about 1000 rad. Most samples show another peak at 350 C. The
stability of the main peak varies, according to different authors, from 0% in five months
to 7% in two months. This variation probably depends upon the material chosen for
study, the pre-reading treatment and the storage conditions.
Mandeville and Albrecht [39] observed that the TL light emission extends into the
ultraviolet.
6.4.3. Dosimetric properties
With measurements carried out on a TL reader equipped with a standard photomultiplier
the apparent sensitivity of BeO is low (about seven times less than that of LiF). However,
with a reader equipped with a photomultiplier with a quartz window also permitting light
with a short wavelength to pass, a sensitivity results which equals that of LiF. BeO
containing sodium is very sensitive and allows the measurement of doses down to 1 mrad.
However, the phosphor must be kept in the dark as a consequence of its high sensitivity
to light. Fluorescent light accelerates fading by optical stimulation. Scarpa [55] noted
that a sample placed 1 m from a fluorescent lamp of 80 W loses half of its information
within 1 h.
The dose response curve is linear up to 50 rad. The following supralinear range extends
up to doses of 5 x 10
5
rad after which saturation occurs. These values are variable with
LET.
BeO is a rather good tissue-equivalent material (Z
ef
[ = 7.13). It is 60% more sensitive
to 10-50 keV photon radiation compared with
60
Co y rays. Agreement between experi-
mental and theoretical energy dependence curves for the response is not too good. This
anomaly seems to have to do with a linear energy transfer effect of the radiation on the
detector response [63].
Preparation and properties of principal TL products 111
BeO is 2-3 times more sensitive to fast neutrons than is LiF, but it is much less sensitive
to thermal neutrons. It is this property which sometimes makes BeO preferable to other
phosphors. In fact, subjected to a radiation of 10
10
neutrons cm
-2
BeO exhibits a response
equivalent to 0.2 R of
60
Co photon radiation, which is a response three times less than
that of calcium fluoride. In contrast to LiF and Li
2
B40
7
: Mn, BeO exhibits an increased
response with increasing LET (figure 6.11). This is quite unusual and may be used for
identifying the type of incident radiation.
The dosimetric properties of BeO make it interesting for its application in the field of
personnel dosimetry.
6.5. Calcium fluoride
CaF
2
exists in nature as fluorite. Its TL properties were studied by Wiedemann and
Schmidt [65] and later by Kossel in 1954 and Houtermans in 1957.
Grogler et al [31] used it for dosimetry of ionising radiation. Ginther [25-27] studied
the preparation of synthetic CaF
2
activated with manganese (CaF
2
:Mn). Harshaw
recently commercialised a CaF
2
activated with dysprosium (CaF
2
:Dy). CaF
2
is not tissue-
equivalent (Z
e
ff = 16.57). It is a factor of 15 more sensitive to 30 keV photon radiation
than to the photon radiation from
60
Co. It is therefore necessary to use appropriate
filters for energy compensation or reserve its use for the dosimetry of high-energy photon
radiation.
CaF
2
has two important advantages over LiF in certain applications:
(i) it is considerably more sensitive: the minimum detectable dose is about 10 times
less;
(ii) it has a larger linear dose response range.
6.5.1. Natural calcium fluoride
Natural CaF
2
has been used predominantly by the Belgian company Manufacture Beige de
Lamps et de Material Electronique SA (MBLE). Its dosimetric properties were analysed in
detail by Schayes [56, 57]. The most commonly found impurity activators in the natural
products are the rare earths (Gd, Dy, Er, Tb) in bi- or trivalent states and trivalent
uranium.
The TLD glow curve exhibits several peaks with a predominant stable peak at 250 C
(figure 6.12). The lower-temperature peaks are rather unstable. The peaks at higher
temperatures corresponding to deeper trapping levels (not shown in figure 6.12) may be
used for information storage from previous exposures and may be evaluated at a later
date. By means of uv stimulation one can encourage trap-to-trap migration and refill the
traps which correspond to the 250 C peak.
Adam and Katriel [1] analysed the trap depths of the MBLE material and obtained
the results shown in table 6.5.
The half-lives of the trap levels are 3 months, 5 yr and 2 x 10
5
yr, respectively, making
the phosphor very suitable for long integration times, as long as the trapped electrons in
the first trap level are released beforehand.
Increasing interest in natural CaF
2
has been shown recently. This material is abundant
in nature and production costs are low [42,44].
112 G Portal
100 200 300
TEMPERATURE C O
Figure 6.12. Glow curves of some TL products
[23]. (A) CaSO:Mn, (B) LiF:Mg TLD 100, (C)
natural CaF
2
, (D) CaF
2
: Mn.
Table 6.5. Trap depths and frequency factors for natural CaF
2
.
Emission Trap depth Frequency
temperature (C) (activation energy) (eV) factor
110
175
263
1.2
1.65
1.71
4X10'
S
6 X1 0 "
4 X1 0 "
20 100
200 250 300 400 500
TEMPERATURE C O
Figure 6.13. TL glow curves from different
natural fluorites [58]. 1, 8, 9, S: sample
designation.
Natural CaF
2
phosphors exhibit different dosimetric characteristics depending upon
their origin. Quite different glow curves are obtained. Figure 6.13 [58] gives an example
of this variation. The TL emission of natural CaF
2
is at a wavelength of 375 nm (see
figure 6.14). It is therefore easy to distinguish between black-body emission and TL. This
is advantageous for the measurement of low doses. With an appropriate TL reader the
minimum detectable dose lies between 0.1 and 1.0 mrad. The sensitivity can be up to 50
times greater than that of LiF.
Preparation and properties of principal TL products
100
113
3500 4000 4500 5000 5500 6000
WAVEL ENGTH ( n m)
Figure 6.14. Light emission spectrum of some TL products [29]. (A) CaSO:Mn, (B) LiF
TLD 100, (C) natural CaF
2
(260C peak), (D) CaF
2
: Mn.
Linearity is observed up to 5 x 10
3
rad, saturation between 10
4
and 10
s
rad.
The phosphor must be protected from light. If not, one may observe a diminution of
the TL signal or the appearance of a pre-dose due to the emptying of deeper traps.
Sensitivity to both fast and thermal neutrons is low. The experimental results of
Tochilin et al [63] showed that CaF
2
is half as sensitive to thermal neutrons as is LiF
TLD 700. The sensitivity to 10
10
neutrons cm"
2
with neutrons of 2.5 MeV and 14.5 MeV
is 1 R and 4 R equivalents, respectively.
6.5.2. Manganese-activated calcium fluoride
Manganese-activated (3%) CaF
2
is prepared by co-precipitation of CaF
2
and MnF
2
from a
solution of CaQ
2
and MnCl
2
in ammonium fluoride (NH
4
)F. The precipitate is dried and
heated in a neutral-atmosphere oven at 1200C, powdered and graded. It may be pressed
or sintered in the same way as described for LiF. It can also, like all TL microcrystallites,
be diffused in a plastic material such as Teflon, as was already shown for LiF. The TLD
glow curve apparently consists of a main peak at 260 C. Actually this peak is a combined
peak which results from several trap levels located very close to each other. High-
temperature peaks also exist which turn out to cause evaluation difficulties, when the
phosphor is exposed to high doses. A sample subjected to a high dose must be re-heated
to empty the higher trap levels before being used for low-dose measurements.
An initial diminution of the signal of about 10% in the first few hours which decreases
to 1% per day, was observed. Ginther [28] noted that this problem may be eliminated
using slow heating rates (1 C s"
1
).
The light emission at 500 nm is characteristic of the presence of manganese (figure
6.14).
The intrinsic sensitivity of CaF
2
:Mn is excellent: 0.44 compared with 0.04 for LiF.
Synthetic manganese-activated CaF
2
, although less sensitive than the natural products,
is 3-5 times more sensitive than LiF. It allows measurements of doses in the order of
some (1-2) millirad only. Certain commercial products, however, contain non-negligible
amounts of radioactivity which make them unsuitable for low-dose assessment. The
response of CaF
2
:Mn is linear up to 2 x 10
s
rad, saturation occurs at 10
6
rad. This
114 G Portal
extraordinarily long linearity of response with dose is the main reason why CaF
2
:Mn is of
so much interest. Sensitivity to neutrons is low. Blum et al [7] usedCaF
2
:Mn for measure-
ments in mixed radiation fields. According to calculations a thermal neutron radiation of
10
10
neutrons cm
-2
yields a roentgen equivalent of 0.77 R. Due to the presence of im-
purities in the phosphor an actual value of 1.05 R was measured by Prokic [51]. With
10
10
neutrons cm"
2
of 14 MeV neutrons a roentgen equivalent of 3.54 is obtained. Com-
pared to LiF the sensitivity of CaF
2
: Mn to 2-5 MeV a particles is a factor of two higher.
Based on Schulmann's work CaF
2
:Mn was produced commercially by the US
company Edgerton, Germeshausen & Grier, Inc (EG&G), which had marketed a variety
of dosemeter types.
6.5.3. Dysprosium-activated calcium fluoride
Harshaw markets, under the code TLD 200, a dysprosium-activated calcium fluoride
(CaF
2
:Dy) which is considerably more sensitive than CaF
2
:Mn. Its properties were
studied by Binder et al [2].
The glow curve of this phosphor actually consists of six peaks which are difficult to
separate (figure 6.15). This holds true for the unstable peaks at 120 C and 140Caswell
as for the stable peaks at 200 C and 250 C. Two higher-temperature peaks appear at
340 C and 400 C. CaF
2
: Dy is not a stable dosemeter material. It shows strong fading.
A thermal treatment of 10 min at 80 C has been proposed which reduces the fading from
25 to 13% per month [2].
10
9 -
8
7
6
5
U
3
2
1
i r
CaF
2
: D y, 1C/sec
AFTER EXPOSURE
40 80 120 160 200 240 2 80 320 360
TEMPERATURE C O
Figure 6.15. Glow curve of CaF
2
:Dy [16].
The TL emission of CaF
2
:Dy shows three maxima at 460,483 and 576 nm. The latter
maximum is detected with a variable efficiency depending upon the photomultiplier
used.
With commercially available readers the sensitivity of CaF
2
:Dy is 15 times greater
than that of LiF. With an S20 photocathode this factor is doubled.
Due to the presence of the numerous peaks in the glow curve, which develop following
different laws, the dose response curve is complicated and only measurements based on
light integration make sense.
Preparation and properties of principal TL products 115
Supralinearity may be eliminated by mepns of a thermal treatment at 600 C for 2 h
before exposure. The response is linear then up to 10
5
rad with saturation at 10
6
rad.
This treatment, however, favours the second glow peak at 140 C which is relatively un-
stable and diminishes the sensitivity of the phosphor by a factor of two.
The presence of dysprosium gives the material a non-negligible sensitivity to thermal
neutrons.
CaF
2
:Dy serves mostly for the measurement of low doses but is increasingly being
replaced by calcium sulphate activated with dysprosium which is more stable.
6.6. Calcium sulphate
Calcium sulphate (CaS0
4
) was first used for dosimetry by Wiedemann et al in 1895. The
first synthetic CaS0
4
prepared by Watanabe in 1951 was activated with manganese
(CaS0
4
: Mn). Since then a number of materials with different activators have been
prepared and studied. CaS0
4
is one of the most sensitive TLD products used in dosimetry.
6.6.1. Manganese-activated calcium sulphate
The glow curve of CaS0
4
:Mn shows a single low-temperature peak at 90 C. For this
reason the information stored in the phosphor is lost very soon and dosemeter readings
need to be made shortly after exposure. Depending on the product and its fading
characteristics, the TL readings for some standard exposure may vary from 15 to 60% in
the first 10 h and from 40 to 85% in the first 3 d after exposure.
CaS0
4
: Mn has been used by Bjarngard [3] for detection of doses as low as 20 /irad.
6.6.2. Samarium-activated calcium sulphate
CaS0
4
:Sm [38] is about 2.5 times more sensitive than CaS0
4
:Mn and has a glow peak at
200 C with the wavelength of the emitted TL being at 600 nm. The material has low
fading at ambient temperature but is very light-sensitive.
6.6.3. Dysprosium- or thulium-activated calcium sulphate
CaS0
4
: Dy and CaS0
4
: Tm are the latest and most interesting phosphors in the CaS0
4
phosphor series, since their response is considerably more stable. The phosphors were first
prepared by Yamashita et al [67].
6.63.1. Preparation
75 mg of powdered dysprosium oxide (Dy
2
0
3
) or 80 mg thulium oxide (Tm
2
0
3
) are
dissolved in 250 cm
3
concentrated sulphuric acid (H
2
S0
4
). The solution is poured into a
crucible, heated up to 250C and 34.4 g of calcium sulphate (CaS0
4
-2H
2
0) added. The
solution is then evaporated at 300 C until crystals of calcium sulphate are obtained. The
crystals are pulverised and graded between 75 and 200 nm. Finally, the microcrystalline
powder is heated at 750 C for 2 h in an aluminium oxide crucible in air, followed by a
final heat treatment at 400 C for 15 min.
The US company, Teledyne, markets CaS0
4
:Dy/Tm embedded in
T
eflon.
116 G Portal
6.6.3.2. Physical properties
The TL glow curve of CaS0
4
: Dy/Tm is similar to that of CaS0
4
: Sm. The main peak
(peak III) is found at 220 C and two lower-temperature peaks (peaks I and II) at 80 C
and 120C (see figure 6.16). These latter peaks are rather unstable. A higher-temperature
peak (peak IV) appears at 250 C for doses in excess of several hundred rad for CaS0
4
: Tm
and for doses of several thousand rad for CaS0
4
: Dy. It is necessary to eliminate the first
two peaks by a pre-heating procedure either in an oven or within the reader itself. The
stability of the trap levels corresponding to the peaks III and VI varies according to dif-
ferent authors. According to Yamashita et al [67] fading is 7% in 6 months, but according
to Mejdahl it is 30%.
l
UJ
C0.SO4 :TmJlII\ 10 R
CaSO^iD yf
Uy
0 100 200 300 400
TEMPERATURE C O
Figure 6.16. TL glow curve of CaSO:Dy and
CaSO,:Tmat 10 R.
Peak no.
HI
IV
Table 6.6. Trap level characteristics for CaS0
4
: Dy (from [50]).
Emission Trap depth Frequency
temperature (C) (activation energy) (eV) factor
220 1.4 2.07 X10'
4
260 1.54 3.25 X10
14
Half-life
at 20C( yr )
120
20300
By applying isothermal annealing, trap level characteristics were obtained for the trap
levels III and IV of CaS0
4
:Dy (table 6.6) [50].
CaS0
4
:Dy and CaS0
4
:Tm are light-sensitive. The background reading can be equiva-
lent to as much as several tens of rad and the fading may be as much as 30% in 5 h in
sunlight [67].
The luminescence spectrum of CaS0
4
:Dy presents two peaks at 478 nm and 571 nm.
That of the Tm-activated sulphate exhibits a main peak at 452 nm and less important
structures at 360,470 and 520 nm.
6.6.3.3. Dosimetric properties
CaS0
4
: Dy and CaS0
4
: Tm are equally more sensitive to photon radiation than is LiF.
The lower detection limit is about 0.1 mrad.
The tribothermoluminescence noise is low.
Preparation and properties of principal TL products 117
The dose response of CaS0
4
: Tm is linear up to doses of 300 rad. Saturation starts
at 10
4
rad. The dose response of CaS0
4
:Dy is linear up to doses of 3xl 0
3
rad and
saturation occurs at 10
s
rad. Regeneration is necessary for heavily irradiated phosphors
and can be effected by annealing at 400 C for 15 min.
The relative response of CaS0
4
as a function of photon energy is shown in figure 6.17
together with that of aluminium oxide (A1
2
0
3
). The effective atomic number of CaS0
4
:
Dy/Tm is 15.6, compared to 16.6 for CaF
2
. The response to 30 keV photon radiation is
11 times superior to that obtained with the photon radiation from
60
Co (16 for CaF
2
).
i i i
10'
Figure 6.17. Photon energy dependence of
CaSO (O) and A1
2
0
3
(A) response. ,
theoretical; , experimental.
ENERGY ( keV)
Table 6.7. Neutron sensitivity of CaS0
4
: Dy/Tm (from [48]).
Neutron source
and/or energy
Thermal
2
"Cf
Pu-Be
14.7 MeV
Roentgen equivalent
per 10
10
neutrons cm
0.6
0.3
1.1
6.87
The sensitivity to neutrons is given in table 6.7 with the sensitivity expressed as
roentgen equivalent for a neutron radiation of 10
10
neutrons cm
-2
[48].
Both phosphors are suitable for low-dose measurements. Blum et al [6] used CaS0
4
: Tm
for 7 dosimetry in neutron fields.
118 G Portal
Recently Prokic [51] prepared sintered TLD from a mixture of CaS0
4
:Tm powder
and a few per cent of a particular component, which plays an essential role during the
sintering process and simultaneously acts as sensitiser.
6.7. Aluminium oxide
Aluminium oxide (A1
2
0
3
) is interesting because it is available at low cost due to the large
industrial production of ceramic and heat resistant materials made out of it.
A1
2
0
3
has been used for a long time in radiation dosimetry. In 1954 Daniels and
Rieman [20] used a personal dosemeter containing sapphire crystals fixed in a silver
chloride base. However, in spite of all the research undertaken on sapphires and rubies,
so far little use has been made of A1
2
0
3
. Kenney and Cameron [36] used a combination
of Al
2
0
3
with LiF to measure the effective energy of some x-ray beams.
Rieke and Daniels [52] tried to explain the catalytic properties of alumina. They
studied the influence of the crystalline lattice and its impurities on its TL properties and
analysed samples baked at different temperatures representing different crystalline states.
Kelly examined the TL glow curve of pure and magnesium-activated aluminas. More
recently Portal [46] used a commercial alumina (corindon) for dosimetry in areas with
criticality risks. Various diamond spars with impurity ions are suitable as TL phosphors:
(i) red sapphire containing iron,
(ii) blue sapphire containing iron, titanium and lithium,
(iii) gilt sapphire containing nickel and magnesium,
(iv) ruby containing aluminium and chromium.
6.7.1. Physical properties
6.7.1.1. Glow curve
Figure 6.18 shows the glow curve of A1
2
0
3
. It exhibits four peaks referred to as peak I,
II, III and IV. The first three peaks are merged, whereas the fourth peak is well separated.
1 -
>
\-
0.5
100 200 300
TEMPERATURE ( C )
Figure 6.18. Glow curve of A1
;
0
3
.
Preparation and properties of principal TL products 119
Rieke and Daniels [52] observed TL peaks at the following temperatures (heating rate
25 C mm
-1
): 103 C, 123 C, 164 C and 236 C.
The relative importance of the trap levels corresponding to these peaks varies con-
siderably with the crystalline structure and impurity content. The first three glow peaks
(I, II and III) seem to be correlated to imperfections in the crystalline lattice rather than
to the presence of impurities. The 260 C peak (IV) appears with bakes at temperatures
greater than 1000C when alumina is completely dehydrated. Its height is proportional
to the sodium ion concentration. The sodium ions act as impurity.
Rieke and Daniels concluded that the 123C peak corresponds to partially hydrated
centres (Al(OH)
2+
), while the 164C peak, which appears at higher baking temperatures,
corresponds to an A10
+
-type centre. The 236 C peak should be due to sodium ion
trapping centres. Portal [46] measured the half-lives of trap levels I, II and III, which are
1 h, 140 h and 115 d, respectively. Trap level IV corresponding to peak IV is very stable
(half-life at 20 C = 1.8 x 10
7
yr).
The TL glow curve of A1
2
0
3
is not affected by the heating cycle during the read-out
process. The material can be regenerated by annealing it at 500 C for 1 h. Once irradiated,
A1
2
0
3
should be stored away from light.
6.7.1.2. Spectral emission of alumina
Corindon exhibits a double emission which is the same for all four trap levels [48]:
(i) a strong emission in the 650 nm region which is difficult to distinguish from black-
body radiation,
(ii) a weaker emission between 390 and 550 nm.
It is the latter emission which is more interesting because it can be detected with an
ordinary commercial TL reader. For suppressing emissions above the 450-500 nm region,
a filter is needed. In practice the filters used for LiF are also suitable for alumina.
6.7.1.3. Dosimetric properties
In figure 6.19 the glow curves of A1
2
0
3
(curve a) and LiF (curve b) are reproduced for
comparison reasons. The ratios between the heights of peaks III and IV of alumina
and that of the main peak of LiF are 0.2 for peak III and 0.12 for peak IV.
b) Al
2
0
3
(6 rad)
c
. , , _
c J
Figure 6.19. Comparison of the glow curves of
7Y-, | , A l ^ (b) and LiF (a) (from [48]).
TEMPERATURE ( C )
120
G Portal
If phosphor reading is effected shortly after exposure it is advantageous to perform
light sum readings over peaks II, III and IV. In this way a sensitivity of about 30% of that
of LiF is obtained and one is able to measure down to doses of about 50 mrad. If the
reading is effected some time later after exposure it is preferable to analyse glow peak
IV only avoiding decay corrections. The lowest detectable dose under these circum-
stances is about 100 mrad as long as the readings are performed with N
2
flushing. Without
N
2
flushing triboluminescence is responsible for an increase of the lower detection
threshold to about lOrad. Figures 6.20 and 6.21 demonstrate that Al
2
0
3
has no linear
dose characteristic for either glow peak (figure 6.20) or the total light sum (figure 6.21).
Calibration curves must therefore be used. Saturation prevails at 10
6
rad.
From figure 6.19 [48] it follows that alumina is less photon-energy-dependent than
CaS0
4
.
100 500 1000
ABSORBED DOSE ( r ad )
Figure 6.20. Dose characteristic of A1
2
0
3
.
Figure 6.21. Dose characteristic of A1
2
0
3
(total
light integration).
10
J
W 10= 10
ABSORBED DOSE ( r ad )
Preparation and properties of principal TL products 121
The sensitivity of alumina to neutrons is summarised in table 6.8. Alumina shows a
very low sensitivity to thermal neutrons.
Table 6.8. Sensitivity of alumina to neutrons.
Neutron source Roentgen equivalent
and/or energies per 10
10
neutrons cm"
2
Thermal neutrons 0.5
J52
Cf 0.38
Pu-Be 0.35
14.7 MeV 12.1
References
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Danish AEC)
2 Binder W, Disterhoft S and Cameron J R 1969 Proc. 2nd Int. Conf. on Luminescence Dosimetry,
Gatlinburg, Tenn., September 1968. USAECRep. CONF 680920, p 43
3 Bjarngard B E 1962 Aktiebolaget Atomenergie
:
Stockholm AE-118
4 Bjarngard B E 1965 Proc. 1st Int. Conf. on Medical Physics, Harrogate
5 Botter-Jensen L and Christensen P 1972 Acta Radiol. Suppl. 313 247
6 Blum E, Bewley D K and Heather J D 1912 Phys. Med. Biol. 17 661
7 Blum E, Bewley D K and Heather J D 1973 Phys. Med. Biol. 18 226
8 Brunskill R T 1968 UKAEA-PG Rep. 837(W)
9 Brunskill R T 1970 Proc. 2nd Conf. IRPA, Brighton IRPA/2/P62
10 Busuoli G 1973 private communication
11 Cameron J R, Zimmerman D, Kenney G N, Buch R, Bland R and Grant R 1964 Health Phys.
10 25
12 Cameron J R, Daniels F, Johnson H and Kenney G N 1961 Science 134 333
13 Christensen P 1969 Proc. 2nd Int. Conf. on Luminescence Dosimetry, Gatlinburg, Tenn., Septem-
ber 1968. USAEC Rep. CONF 680920, p 90
14 Christensen P, Botter-Jensen L and Majborn B 1973 Regional Conf. on Radiation Protection,
Jerusalem
15 Claffy E W 1967 Proc. 1st Int. Conf. on Luminescence Dosimetry, Stanford University, June 1965.
USAECDiv. Tech. Inf. AEC 8, p 74
16 McCurdy D E, Schiager K J and Flack E D 1969 Miners, Health Phys. 17 415
17 Czochialski Z 1917 Z. Phys. Chem. 92 219
18 Daniels F 1950 Rep. 4th Symp. on Chemical Physics and Radiation Dosimetry, Edgewood,
Maryland pl 48
19 Daniels F, Boyd C A and Saunders D F 1953 Science 117 343
20 Daniels F and Rieman W P 1954 University of Wisconsin, Final Rep. No 7
21 Dean P N and Larkins J H 1963 LAMS 3034, p205
22 Desmarquest & CEC Zone Industrielle no 1, 27000 Evreux, France
23 Fowler J L and Attix F H 1966 Radiation Dosimetry vol II, ed F H Attix and W C Roesch (New
York: Academic) p272
24 Frank M and Edelmann B U 1966 Kernenergie 7 228
25 Ginther R J 1954/ . Electrochem. Soc. 101 248
26 Ginther R J and Kirk R D 1956 USNRLProg. Rep. September, pi 2
27 Ginther R J and Kixk R D 1957 J. Electrochem. Soc. 104 365
28 Ginther R J 1965 CONF650637, p l l 8
29 Gorbies S G 1967 Proc. 1st Int. Conf. on Luminescence Dosimetry, Stanford University, June
1965. USAEC Div. Tech. Inf. AEC 8, p 167
122 G Portal
30 Grant R M and Cameron J R 1966 J. Appl. Phys. 37 3791
31 Grogler N, Houtermans F G and Stauffer H \95SProc. 2nd Int. Conf. on Peaceful Uses of Atomic
Energy, Geneva 21 (New York: UN) p226
32 Harris A M and Jackson J H 1969 Br. J. Appl. Phys. 2 1667
33 Harshaw Chemie NV, Strijkiertel 95, De Meern, Holland
34 Jayachandran C A, West M and Shuttleworth F 1969 Proc. 2nd Int. Conf. on Luminescence Dosi-
metry, Gatlinburg, Tenn., September 1968. USAECRep. CONF-680920, pi 18
35 Jones D E, Petrock K F and Denham D H 1966 UCRL Prog. Rep. No 25
36 Kenney G N and Cameron J R \963 Prog. Rep. TID 19112
37 Kirk R D, Schulman H J, West E J and Nash A E 1967 Proc. Symp. on Solid-State Chemistry and
Radiation Dosimetry (Vienna: IAEA) p91
38 Krasnaya A R, Nosenko B M, Revzin L S and Yaskolko V 1961 Atomnayia Energyia 10 630
39 Mandeville C E and Albrecht H O 1954 Phys. Rev. 94 494
40 Moore L E 1957 J. Phys. Chem. 61 636
41 Moreno A, Archundia C and Salsbery L 1971 Proc. 3rd Int. Conf. on Luminescence Dosimetry.
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42 Nambi K S V, Kathuria S P and Sunta C M 1969 Radiation Monitoring Thermoluminescent
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43 Nink R and Kos H 1977 Phys. Stat. Solidi a 41 K157
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45 Portal G, Francois H and Blanchard Ph 1969 C.R. Congr. Europ. IRPA, Menton 9-11 October p79
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48 Portal F 1975 CEA Rep. No R^1697
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52 Rieke J K and Daniels F 1957/ . Phys. Chem. 61 629
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56 Schayes R and Brooke C 1963 Rev. MBLE 6 24
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68 Technical Recommendations for the Use of Thermoluminescence for Dosimetry in Individual
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Applied Thermoluminescence Dosimetry. Eds M Oberhofer and A Scharmann
1981 ECSC, EEC, EAEC, Brussels and Luxembourg
Operational aspects
D F REGULLA
7.1. Introduction
The requirements of modern dosimetry for high local resolution of radiation fields, for
ruggedness of the detector, an extended detection range, independence of detector
response from dose rate, etc, can often not be fulfilled by conventional dosimetry tech-
niques, such as ionisation chamber dosimetry. To a certain extent solid-state
techniques, particularly thermoluminescence dosimetry (TLD), can cover these require-
ments. The question is whether TLD can provide an accuracy of <10% (preferably
<5%), and this with an uncertainty of 2-3% from the reference dosemeter already
included. Considering the precision of data from the literature, one finds coefficients of
variation as low as 1% or even less (figure 7.1), which indicates that high enough accuracy
can, in principle, be provided for most applications.
However, it must be realised that these data from the literature have been obtained
under laboratory conditions and by skilled personnel knowing about the various error
sources. Therefore, both the newcomer to the field of TLD and the expert should
o
<
Q
cr
<
Q
Z
<
LU
10
1 1
\
\
\
\
o
-
1 1
1 r
uniformity
1 1
CaF
2
: Dy
within 10 detectors
precision ^
for one detecto
i i
o
r
1 1
O
1
_
"
-
0.1
1 10 10
2
10
3
EXPOSURE (m R)
Figure 7.1. Precision for one detector and uniformity within ten detectors depending on
exposure. Detector material is CaF
2
: Dy.
124 DFRegulla
anticipate higher variations under practical conditions. The following selected items may
demonstrate the possible variability of error sources, a situation which will not change
significantly in the near future if TLD technology is not seriously improved [1].
7.2. Parameters affecting precision
Any review of error sources in TLD must consider instability of the read-out instrument
and of the influence quantities and performance parameters during irradiation, storage,
reading and annealing (figure 7.2).
IRRADIATION
a) Temperature
bl Incidental Direct
cISec.Particle Equilib
Pre Irr Storage :
a) Temperature
bl Light
J
\
Pre Irr. Annealing:
a) High Annealing Temp.
b)Cooling Rate
c)Low Annealing Temp.
EVALUATION
a)Heating Rate
b)Max. readout Temp.
dCooling Rate
Post Irr. Storage.
a) Temperature
b) Light
Post Irr Annealing:
a) Temperature
b)Annealmg Time
Figure 7.2. Influences on-TLD precision within the measuring cycle.
7.2.1. Read-out instrument
The TLD read-out instrument should be operated at constant room temperature. A
temperature increase was found to cause a reversible decay of the reference light source
reading (figure 7.3) which in practice would erroneously be compensated for by in-
creasing the voltage. For common TLD readers, the ambient temperature should not
exceed 25 C to avoid trouble from the electronics.
Unidentified errors from the electronics have been found due to spontaneous changes
in light source readings up to 2% on different days or due to effects of dry nitrogen,
which is recommended as an inert gas (see later in this chapter) and which gave rise to an
increase in PMT dark current by up to a facte, of 30 (see also 3.3.5 and 4.4).
An important error arises from the fact that the TLD reader sensitivity is mainly con-
trolled by means of a reference light source which is characterised by a certain emission
spectrum. This spectrum is modified by the spectral transmission factor of filters and
Operational aspects
125
15 25 35
ROOM TEMPERATURE (C)
Figure 7.3. Temperature dependence of reference light source reading. Curve A, Harshaw
2000 (Regulla, GSF Munich); curve B, Teledyne 7300 (Roenick, IRD Rio de Janeiro).
lenses in the optical path before it reaches the PMT. Since the spectral transmission factor
is non-stable and will change in the course of the instrument's use due to surface
contamination from dust or combustion products, the reference light source reading
will decrease. Usually this is compensated for by increasing the high-voltage setting of the
PMT. This procedure, however, will be correct only for those detectors with a TL emission
spectrum comparable to that of the reference light source but may cause a major error
for all detectors with a different emission spectrum. The reason is that the transmission
factor does not change linearly over all the spectrum but selectively.
It should be noticed that the spectral response of most photomultipliers will shift
with the change of voltage so that the calibration should be repeated. Moreover, the
sensitivity check of the TL read-out instrument using a reference light source does not
cover the heater planchet and its optical properties.
Influences on the TL signal due to the optical properties of the heater planchet are
surface-related. Some tens of per cent of the TL light reaching the PMT photocathode
may result from the planchet due to reflection. This figure can change with the change
in reflectivity properties of the planchet surface during use (figure 7.4) (see also
3.2.2.1 and 4.2). The error can be kept small by using permanent planchets, e.g.
planchets made of noble metals such as platinum. To avoid this error, a different heating
(") (b) (c) (d) (e) (/)
Figure 7.4. Appearance of silver-plated heater planchets in course of use (a-d) and of
platinum planchets, (e) virgin and (/") frequently used.
126 DFRegulla
technique has to be used, e.g. hot gas. In this way, a geometrical error of up to 10% or
more which arises from the positioning of the TL detector with respect to the planchet
could also be kept small. All these figures were determined with a Harshaw Model 2000
TLD analyser.
As a precondition for low-level measurements, the read-out of the TL detectors is most
often done under an atmosphere of inert gas. This provision reduces or eliminates effects
of non-radiation-induced but thermally stimulated chemoluminescence at the surface of
the detector or heater planchet. In addition it was found that the location of the glow
curve when plotted versus the temperature (figure 7.5) as well as the achieved measuring
precision in the case of multiple use (table 7.1) depend on the read-out atmosphere
chosen. As a consequence, for example, an increased maximum read-out temperature
would be necessary for read-out under dry argon gas if compared with dry nitrogen gas.
t, 6-
o
X
2 -
LU
-
-
r\^-^"
a i r
f i ^ - d r y nitrogen
t l V" ^
a r
9
o n
f >
f i
11
ll
i
l
i
I
i
J i
\
I
4 -
Figure
200 400 600
TEMPERATURE ( C)
7 J . Influence of the readout atmosphere on the glow curve of LiF detectors.
Table 7. 1. Influence of the reading atmosphere on the precision of
LiF : Mg,Ti extruded rods and on the PMT dark current. 24 uses in each
atmosphere. Exposure 20 R.
Reading Standard Dark current Dark current
atmosphere deviation (%) at 250 C( pA) at 300C( pA)
Air
Nitrogen
Argon
Oxygen
5.3
2.7
2.4
6.7
12
3
30
3
Operational aspects
7.2.2. Irradiation
127
Usually, irradiation of thermoluminescence dosemeters is performed at room tempera-
ture. Relatively extreme temperatures will occur only in restricted areas, e.g. in reactor
and space research. To clarify the effect of temperature during exposure on TL sensitivity,
LiF : Mg,Ti detectors were irradiated in Perspex containers in liquid nitrogen ( 196 C)
and in water maintained at 0 C, 20 C, 50 C and 90 C after having reached temperature
equilibrium with the ambient medium (figure 7.6).
-200 0 50 100
TEMPERATURE DURING EXPOSURE ( C)
Figure 7.6. TL output of Li F: Mg,Ti as a function of irradiation temperature. Curve A,
Sunta and Watanabe 1976 Health Phys.; curve B, Regulla.
The measurements revealed that for irradiation at 196C TL sensitivity drops to
about 80% when normalised to 20 C. For irradiation between 0C and 50 C, TL sensi-
tivity remained approximately constant. At 90 C, however, TL sensitivity increased by
about 14%. The elevated TL sensitivity remained constant over a period of 10 d while
stored at room temperature.
To understand better the effect of irradiation temperature the glow curves of the
detectors irradiated at the above-mentioned temperatures were recorded (figure 7.7). It
is seen that the irradiation at 90 C favours an additional electron trapping in a high-
temperature peak around 260 C besides the main TL peak at 210 C. The high-tempera-
ture peak does not appear in the case of low-temperature exposures at 196 C.
A further error may arise from different irradiation geometries between calibration
and measurement in an unknown radiation field, TL detectors show a non-negligible
change of response depending on the direction of radiation incidence (figure 7.8).
Evidently, the magnitude of this effect depends on detector geometry and material as
well as on the radiation quality.
128 DFRegulla
300
100
~ 30
LiJ i n
/
/
1
1,
1
1
1
ll
II
1
1
1
1
ll
ll
ll
1
1
1
ll
1
1\
1*
H
1 I'
1 *
I ll
\
V y
/
/ '
/
/
> /
M
/
Figure 7.7 Glow curves of L i F: Mg,Ti after
irradiation at different temperatures: ,
90C; , 50C; . . . , 20C; , 196 C;
. , background. Heat rate 2 C s"'.
100 200 300
TEMPERATURE ("CI
&> 90
90/0 1180
0.5 1.0 1.5 HVLImm Al )
10 29 43 50 50 kVp
1Be 0.6
0 3AI
1
mm TOTAL FILTRATION
Figure 7.8. Directional dependence of TL D chips (3 X 3 X 0.9 mm
3
) for low photon energies.
, CaF
2
:Dy; , L iF:Ti, Mg.
7.2.3. Storage
Between irradiation and readout, the signal intensity can be influenced by the storage
conditions and by light. The effect of storage temperature can, in general, be kept small
by a proper annealing procedure at an elevated temperature before readout. Even for
storage for one week at 70 C using CaF
2
: Dy, which is subject to substantial fading even
at room temperature, this fading can be almost totally eliminated by a proper preread
out annealing procedure (figure 7.9), e.g. 15 min at 130C (see also 7.2.4).
The effect of light on the TL output is twofold. Besides a reduction of the TL signal
depending on light intensity, wavelength (uv!) and duration of light exposure, a stimula
tion of thermoluminescence was found (figure 7.10). The latter effect, simulating a ^Co
Operational aspects 129
Figure 7.9. Magnitude of fading of CaF
2
: Dy
for different storage and prereadout annealing
temperatures.
STORAGE TIME (min
100
<
o
LU
o 60
<
o
LU
20
LU
- - '
~~~^4o)
[b) /
/
s*
/
s
^ + '


r

^ . -
10<
uv EXPOSURE TIME (min)
<
z
o
iOO
8
200 w
LU
o:
Z)
(/)
o
CL
X
10'
Figure 7.10. Effect of UV light (Philips mercury lamp HG 8; 9A; source distance 15 cm) on
(a) irradiated and (ft) unirradiated L iF: Mg.Ti.
gamma exposure signal of up to several hundred milliroentgens for LiF : Mg,Ti or several
roentgens in the case of CaF
2
and CaS0
4
, refers to a glow curve different from the one
after ^Co gamma exposure and should be ascribed to surface physics (figure 7.11). In
practice, a superposition of both lightinduced fading and stimulation of the TL signal has
to be expected.
In figure 7.12, results of a fading experiment at 70 C storage temperature with the
presence of daylight are reported for different types of TL materials. The decay be
haviour of all detector materials was different from reference probes also stored at
70 C but in the dark. Obviously, fading correction factors obtained from experiments
in the dark should be applied very carefully in cases in which detectors might have been
exposed to light during storage.
Thermoluminescence dosimetry is generally said to be independent of humidity. This
wellknown statement is, however, not true at least for lithium borate chips Li
2
B40
7
:Mn,
130
DFRegulla
60
20
/
1 /
1/
/]
/ /
^ Ugh
A j.
\
t exposu
30 mm
JOOr
\ irra
\
\
A
1
nR.Co
60
lout pre
diation -
s \ ^ ^
- and post-
annealing
100 200
TEMPERATURE I t )
300
Figure 7.11. Comparison of LiF:Mg,Ti
glow curves induced by
60
Co 7-rays and
ultraviolet light.
0.5h1h 3h 1d 3d 2w3w
STORAGE TIME (min)
Figure 7.12. Comparison of fading behaviour of different TL materials after storage at 70 C
(a) in the dark and (6) with access of daylight (h = hour, d = day, w = week).
which in the course of a four week fading experiment at 50 C and 70% relative humidity
became unnaturally transparent and blew up during subsequent read-out (figure 7.13). As
a consequence the detectors were destroyed. It is beyond doubt that any application of a
TL detector material under conditions of increased humidity requires that the test pro-
gramme should be carefully performed under these conditions.
7.2.4. Pre-read-out annealing
The purpose of pre-read-out annealing is to remove any existing low-temperature glow
peaks ^> 100 C that are thermally unstable even at room temperature and are responsible
for spontaneous signal losses after irradiation (thermal fading). Low-temperature peaks
Operational aspects
131
Figure 7.13. Appearance of L i,B.,0
7
: Mn chips. Left: new detectors; middle: after storage at
50 C and 70% relative humidity; right: with subsequent readout.
are typically present in CaF
2
; Dy, and in L iF: Mg,Ti which has not been annealed con
ventionally (see figure 7.15).
To optimise the prereadout annealing in the case of L iF: Mg,Ti, i.e. eliminating the
lowtemperature peaks without significantly reducing sensitivity, the detectors were
subjected to different prereadout annealing temperatures between 20 C and 175C
for 10 min annealing time, respectively (figure 7.14). As a result, fading at room tempera
ture was completely eliminated by about 15 min prereadout annealing at 100 C, while
the sensitivity loss was only about 15%. The glow curve so achieved is shown in figure
7.15.
To find the optimum duration of temperature treatment at 100 C, the LiF detectors
were subjected to prereadout annealing for different periods of time (figure 7.16). From
these results it is obvious that sensitivity losses become significant only if the detectors
~ 1.00
>
i
i
(/)
z
LU
1/1
LU
>
LU
0.50
1 15V.
0 100 200
TEMPERATURE (C)
Figure 7.14. Influence of the magnitude of temperature during prereadout annealing on
the TL sensitivity of L iF : Mg.Ti. Annealing period 10 min.
132
120
80
40
DFRegulla
.
/
/
/
/
/
/
*t ,'
I '
Re-usi
I
1 1
1
1 /
thK C/
w ithout
1
1 A.
1 /
\ /
V
A'
any ann
' ' A
' 1
ealing
100 200
TEMPERATURE lCJ
300
Figure 7.15. Comparison of glow curves of
LiF : Mg.Ti used after annealing at 400 "C with
and without pre-read-out annealing (see 7.2.6).
are stored at 100 C for extended periods, e.g. TL loss becomes about 50% after one day
of storage at 100 C. Additionally recorded glow curves revealed that after this extended
heat treatment only the 210 C glow peak is present. Johnson et al [2] observed that the
pre-read-out annealing procedure can be applied before or after exposure without
affecting the TL sensitivity. However, recent findings on this subject show that major
research is still necessary to achieve the relevant information [3].
1.2
>
0.8
> 0.4
UJ
cr
n l i i l l i
10 10' 10
J
TIME Imin)
Figure 7.16. Influence of pre-read-out annealing time at 100 C on TL sensitivity of
LiF : Mg.Ti normalised to the TL output after 5 min at 100 C.
1 1 11
M M
1 1
i 1 1 1
1 Hour
, , i
i i
i i
i 1 1 1
i i n
lOoy
7.2.5. Read-out process
In most commercial TLD instruments the maximum read-out temperature is preset and
controlled by a simple scale indication. If the temperature indication is incorrect for
some reason, e.g. faulty contact between heating planchet and thermocouple or wrong
reference temperature, then the preset read-out temperature may not be sufficient. The
resulting errors were studied for LiF: Mg,Ti detectors by measuring the TL output for
Operational aspects 133
various maximum read-out temperatures at constant evaluation time (figure 7.17). If
the temperature is lower than or equal to the main glow-peak temperature (210C) the
TL sensitivity decreases markedly, for instance to 60% for 200 C if compared with com-
plete read-out at > 250 C. This is due to only partial release of the trapped electrons. For
temperatures well above the main glow peak all traps are emptied which results in
constant TL sensitivity of the detector.
P 0.8
z
LU
l/l
LU
> 0.4
<
_ j
LU
cr
O D
150
250
TEMPERATURE lC)
350
Figure 7.17. TL sensitivity of LiF : Mg.Ti as a function of maximum read-out temperature.
The TL output also depends on the holding time at maximum read-out temperature.
This is shown in figure 7.18 for two different heating rates. The sensitivity drop at shorter
holding times is due to the fact that there is no temperature equilibrium between heater
planchet and detector. For a fast heating rate, e.g. 50Cs
_1
and 300C maximum read-
out temperature during 5 s holding time, 93% of the TL signal is integrated. If measured
with a 250 C maximum read-out temperature for the same holding time and heating
rate, only 90% of the TL signal is collected. Therefore, a 250C maximum read-out
temperature, a heating rate of 50Cs
_1
and at least 15 s read-out time appears useful
for fast routine evaluation.
1.00
0.90
0.80
300'cy/
7
250"C
o i. 15C/se
: SSO'C/se
c
c
0 5 10 15
TIME AFTER REACHING THE PRESELECTED
MAXIMUM TEMPERATURE ( s)
Figure 7.18. TL sensitivity of Li F: Mg,Ti as a
function of the holding time at maximum read-
out temperature. Parameter: heating rate.
134 DFRegulla
In figure 7.19 the effect of heating rate during read-out on TL eutput of LiF: Mg,Ti
is shown. This effect is different for different phosphors, even for the so-called integral
measuring technique. Obviously, one should choose a different heating rate for the read-
out of, for example, LiF: Mg,Ti or CaF
2
: Mn, in order to minimise the effect of heating
rate fluctuations on TL output. These fluctuations probably arise from changes in the
thermal contact between planchet and detector. As also shown in figure 7.19, the peak
height measuring technique is significantly more dependent on the heating rate than the
integral method and is therefore restricted to very special dosemeter assemblies.
0.8
0-
. 0. 4
1 3 6 10 30 6010
2
300 60010
3
HEATING RATE |C mm"')
Figure 7.19. Influence of heating rate during
read-out on TL output for peak height and
integral reading.
Studies of the influence of dry nitrogen gas flow on TL output revealed no effect of
flow rates between 1 and 15 1 min
-1
. Hence, for economic reasons a flow rate of
1-2 1 min
-1
seems to be sufficient even in cases of fast routine evaluation (see 4.3).
7.2.6. Post-read-out annealing
In order to erase the residual TL signals completely, the TL detectors must be annealed
prior to re-use. This procedure is called pre-irradiation annealing or post-read-out anneal-
ing. Cameron et al [4] proposed a standard annealing technique based on a high-
temperature treatment at 400 C for one hour followed by a long-term low-temperature
treatment at 80 C for 23 h in the case of LiF: Mg,Ti. While the aim of the high-
temperature treatment is to erase all previous dose information from the detector, the
aim of the low-temperature annealing is to restore the original shape of the glow curve
and thus reproduce the TL sensitivity.
The following results concern the effect of the upper post-read-out annealing tempera-
ture on the TL sensitivity. For this purpose two groups of LiF detectors were subjected
to temperatures between 300 C and 600 C for periods of 15 min and l h prior to
irradiation. These detectors were then exposed and read out. The results for both groups
are shown in figure 7.20. For annealing at temperatures around 400 C the TL sensitivity
Operational aspects
200
135
400
TEMPERATURE ( C)
600
Figure 7.20. Relative sensitivity changes of LiF:Mg,Ti due to non-constant high post-
read-out annealing temperature. Parameter: annealing time. Normalisation to maximum
sensitivity.
remains roughly constant. Annealing for more extended periods and at temperatures
above 450C reduces the sensitivity significantly, e.g. a one hour treatment at 600C
diminishes the sensitivity by about 30%. Hence, 15min annealing at 400 C appears
sufficient to reset the LiF detector sensitivity which, moreover, yields roughly the same
sensitivity as a one hour treatment at 400 C.
The reproduction of the upper post-read-out annealing temperature is of even greater
importance for LiF of the French CEA. There, the prescribed 485 C must be reproduced
to within 5 C in order to avoid serious changes of the TL sensitivity.
Besides the upper annealing temperature, the cooling rate during the subsequent
cooling phase has a major influence on TL sensitivity and, hence, on precision, particu-
larly for LiF: Mg,Ti. Varying the cooling rate from the 400 C level down to room
temperature revealed that a fast cooling rate produces a higher TL sensitivity because of
low-temperature glow-peak formation. The difference in TL sensitivity between cooling
rates of 3Cmin
_1
and 3000Cmin~' were found to be up to a factor of four (figure
7.21). Therefore, for precise TL dosimetry with LiF:Mg,Ti, one should make every effort
to reproduce the cooling rate as well as possible between calibration and measurements. It
should be noted that for other TLD materials the cooling rate does not influence the TL
sensitivity so much.
The low-temperature post-read-out annealing (usually 80 C) subsequent to the high-
temperature annealing, as mentioned at the beginning of 7.2.6, is intended to eliminate
low-temperature glow peaks and therefore fading for LiF: Mg.Ti. However, this low-
temperature annealing does not provide a simple cut-off of the glow curve, but changes
the distribution of the glow curve due to a dynamic trap mechanism in LiF: Mg,Ti
(figure 7.22). Subjecting LiF: Mg,Ti which has been annealed at 400 C for 15 min to a
low-temperature post-read-out annealing in the range 20-300 C for a duration of one
hour, the TL sensitivity is influenced as shown in figure 7.23. From the steep decay of the
curve it becomes evident that good reproducibility of the low post-read-out annealing
temperature is an important precondition for high-precision measurements with LiF: Mg,Ti.
136 DFRegulla
LQQ
200
n
I i l l
i i i i
I i l l
i I I I
I i l l
i I I I
i I I I
y^ 1
i I I I
1 10 10
2
10
3
10*
COOLING RATE lC mirf
1
)
Figure 7. 21. TL sensitivity to LiF:Mg,Ti as a function of cooling rate.
Figure 7.22. Dynamics in the glow-curve
structure of LiF: Mg,Ti as a function of
post-read-out annealing time at the low-
temperature level of 80C [5]. Annealing
time in hours.
Again it should be noted that the trap dynamics at low post-read-out annealing tempera-
ture is particular to LiF : Mg,Ti and must not be considered for other TLD materials.
The above-described annealing technique proposed by Cameron et al [4] for LiF: Mg,Ti
certainly reveals high precision but is inconvenient, because of the annealing periods
needed of over 20 h. Therefore, a 'fast-annealing' procedure which is applicable even for
LiF : Mg,Ti has been proposed by Regulla [6]. It consists of a short post-read-out anneal-
ing (5 min) at a temperature of 400 C and a 10 min pre-read-out annealing at 100C to
eliminate fading by suppressing the low-temperature glow peaks but without trying to
restore the original glow-curve shape. The glow curve thus resulting for LiF: Mg,Ti is
given in figure 7.15.
Operational aspects 137
100 200
TEMPERATURE |C)
300
Figure 7. 23. Influence of a nonconstant low postreadout annealing temperature on the
TL sensitivity of L i F: Mg,Ti. Annealing period 60 min. Insets: glow curves taken after
annealing at the indicated temperatures.
The precision attainable with the 'fastannealing' technique [6] is strongly dependent
on the accuracy with which the 100C temperature level is controlled. Data on repro
ducibility achieved by this method are given in figures 7.1 and 7.24. The measurements
were made with LiF:Mg,Ti TL D 100 chips of dimension 3 x 3 x 0.9 mm
3
.
~ 2
3 0
< 1
>
1- 2
LU
o
u.
z 0
o
5
>-2
(JJ
Q
C
:
4

b
</\
1 -
" '
.____.
5 \
'--J J
y

S
!>
c
1
s
-
i
) " ^ ^
,!

,
>'
k
?
\
~~J J
|
( t >)
U 6
NUMBER OF USE
10
Figure 7.24. Reproducibility measurements with L i F: Mg.Ti using a 'fastannealing' tech
nique according to Regulla [ 6] . (a) O, single detector; , corrected with group tendency.
(b) Mean of group (10 detectors).
The furnace used in the present investigations was purposebuilt and operated with an
accuracy of (100 2.5) C. The reproducibility of results can still be improved further
by using a precision temperaturecontrolled furnace. Meanwhile, coefficients of variation
as low as 0.5% and better could be realised by an improvement in technology. These
figures clearly demonstrate the usefulness and high practical value of the 'fastannealing'
138 DFRegulla
procedure for laboratory and routine TLD application. At least 10 repeated measurements
a day can be performed with the 'fast-annealing' technique compared with one measure-
ment with the conventional 24 h annealing process.
In figure 7.24, the usefulness of a 'calibration detector group' is also shown. The
detectors of this group are subjected to the same annealing programme as the detectors
used for the measurement in the unknown radiation fields, but they are always exposed
to a known exposure under calibration conditions. In this way, the influence of slight
changes in the annealing procedure or of the read-out equipment and their effect on the
precision of the measuring detectors can be avoided by evaluating a correction factor
as the mean value from the results of the 'calibration detector group'. The scatter of
readings from the 'measuring detectors' can thus be reduced.
7.2.7. Detector handling
The physical size of TL detectors is usually very small, which is an advantage. Tweezers
must be used to handle them. It seems that frequently handled TL detectors lose sensi-
tivity when handled with normal mechanical tweezers. This effect is due to microscopic
scratches and other damage to the detector surfaces and edges. Figure 7.25 shows that
the sensitivity loss may reach up to 20% after a 50-fold use in the case of LiF: Mg,Ti
chips [7]. When 'vacuum tweezers' are used the sensitivity loss is almost negligible (see
also figure 7.25). Therefore, handling with 'vacuum tweezers' appears to be strongly
recommended in operational TLD.
In dosimetric practice, one cannot avoid crystals serving as TL detectors getting dirty
in the course of their use. This is due to inorganic and organic detector contaminations
baking on to and diffusing into the surface layer. As a result the TL sensitivity is reduced.
This effect may amount to several tens of per cent. Careful handling of the detectors will
help to limit the surface contamination. Once contaminated, most detectors can to
a certain extent be cleaned again according to the washing procedure given by the
manufacturer.
Instructions on cleaning procedures are available from, for example, Harshaw for
extruded TL detectors: '(a) Between normal uses, the detectors should be rinsed with
analytical grade methanol, (b) Detectors which seem extremely dirty or are touched with
40 60
Figure 7.
tweezers
40 60 20
NUMBER OF USES
.25. TL sensitivity of LiF : Mg,Ti chips after repeated handling with (a) mechanical
and (b) vacuum tweezers [7].
Operational aspects 139
the hands should be rinsed with warm trichlorethylene followed by the methanol rinse'.
The application of an ultrasonic bath will increase the efficiency of the cleaning
procedure. The ultrasonic treatment does not affect the TL signal if its duration does not
exceed several minutes.
However, from experience, cleaning should usually be avoided. Regular cleaning, e.g.
as part of the measuring cycle, affects the reproducibility and, hence, the precision of
measurement markedly. This may be due to changes of the crystalline surface structure
which can be observed under the microscope after the cleaning procedure. The changes
in the detector surface are particularly pronounced if detergents (even in low concentra-
tion) are used. While the cleaning effect may be remarkable (see figure 7.26), a permanent
loss of TL sensitivity may be found at the same time. This apparently has to do with the
partial dissolution of detector material in water which is strikingly demonstrated in figure
7.27. This figure compares the surfaces of two TLD 700 chips magnified by a factor of
1800 using an electron microscope. The chips had been deposited in double-distilled
heavy water for 43 h.
Figure 7.26. Surfaces of two TLD 700
chips [11]. Left, virgin; right, after 43 h in
double-distilled D, 0.
Figure 7.27. Microscopic view of the two chips shown in figure 7.26, magnification X 1800
[11]. Left, virgin; right, after 43 h in double-distilled D
2
0.
140 DFRegulla
Obviously, it is the solubility which must be carefully considered when cleaning TL
detectors over extended periods of time even in pure water. The solubility is also the
reason why TL detectors should, in general, not be implanted into tissue without being
wrapped in an appropriate cover. Dettmer et al [8, 9] report changes of surface properties
and TL sensitivity of detectors which had been implanted uncovered; three weeks after
implantation the detectors could not even be found. Obviously, the detectors had been
dissolved by the inter-cellular fluid. Besides, tissue reactions were observed which lead
one to consider also the biological toxicity of TL materials in cases of implantation.
For the operator of thermoluminescence dosimetry the question may arise of whether
or not TL materials are toxic and should be handled with special care. Except for
beryllium oxide, the considerable toxicity of which is recognised, there is no particular
information in the literature. At least, Dettmer et al [10] conducted a pilot study using
the drinking water of young rats saturated with LiF (solubility 0.27 g LiF per 100 cm
3
cold water). From the results they strongly recommended that LiF should be handled
with at least as much caution as other toxic fluorides.
Along with the toxicity of detector materials one should also consider a probable
health risk from chemical solvents and detergents used for detector cleaning. Trichlor-
ethylene, for instance, has an acute toxic effect on the human liver and central nervous
system. It handling, if allowed at all, should be done with due care and using a hood.
7.3. Conclusion
A precondition for precise thermoluminescence dosimetry is the appropriate equipment,
i.e. a short- and long-term stable read-out instrument and regulated annealing facilities.
This requirement is not trivial, since such equipment is not at present fully available to
the necessary quality. Hence, in the author's opinion, for high dosimetric reliability
thermoluminescence dosimetry still requires a good deal of technological improvement.
Besides, as long as the measuring cycle is not automated, any precision TLD will demand a
'precision operator' who can control the equipment and the different influence quantities
and parameters while following the processing instructions exactly. This calls for long-
term knowledge of the subject under consideration; book-learning is helpful but cannot
replace operational experience. In the present situation, an overall accuracy of 10%
should be achievable with TLD in practice, e.g. in radiation therapy. The question is
whether this accuracy corresponds to what is needed.
References
1 Regulla D F 1980 Remarks on the present state of thermoluminescence dosimetry, Proc. 6th Int.
Conf. on Solid State Dosimetry, Toulouse, April 1-4 1980. Nucl. Instrum. Meth. 175 98
2 Johnson T L, Attix F H and Booth L F 1971 Health Phys. 21 22
3 de Planque G, Julius H W and Verhoef C W 1980 Effects of storage intervals on the sensitivity and
fading of LiF TLD Proc. 6th Int. Conf. on Solid State Dosimetry, Toulouse, April 1-4 1980. Nucl.
Instrum. Meth. 175 177
4 Cameron J R, Zimmermann D W, Kenney G, Buch R, Bland R and Grant R 1964 Health Phys. 10
25
Operational aspects 141
5 Zimmermann D W, Rhyner C R and Cameron J R 1966 Health Phys. 12 525
6 Regulla D F 1971 Experience with the LiF TLD system and recommendations for its practical
application. GSF-Rep. S-124
7 Cox F M, Lucas A C and Kapsai B M 1976 The reusability of solid thermoluminescent dosemeters
and its relation to the maintenance of TL standards, Health Phys. 30 135
8 Dettmer C M and Galkin B M 1969 The toxicity of thermoluminescent phosphors, Proc. 2nd Int.
Conf. on Luminescence Dosimetry, Gatlinburg, Tenn., September 1968. USAEC Rep. CONF
680920
9 Galkin B M, Dettmer C M and Suntharalingam N 1969 Sensitivity changes in solid thermo-
luminescent dosemeters after subcutaneous implantation, Proc. 2nd Int. Conf. on Luminescence
Dosimetry, Gatlinburg, Tenn., September 1968. USAEC Rep. CONF 680920
10 Dettmer C M, Galking B M and Hanna H J 1967 Phys. Med. Biol. 12 577
11 Guarducci D 1978 Studio della risposta dei dosimetri a TL alia radiaiione beta di bassa energia di
tritio. Thesis Universita degli Studi di Milano, Facolta di Scienze Fisiche
Applied Thermoluminescence Dosimetry. Eds M Oberhofer and A Scharmann
1981 ECSC, EEC, EAEC, Brussels and Luxembourg
8
Precision and accuracy O/TLD measurements
G BUSUOLI
8.1. Introduction
This chapter describes the precision and accuracy with which TL measurements can be
performed and those parameters that can influence precision and accuracy. As some
confusion exists with the terms precision and accuracy, they must be defined in order
that they should be used in the right way.
8.2. Definitions
8.2.1. Precision
Precision is a term related to the random uncertainties associated with the measurement,
i.e. the uncertainties that have been derived by statistical methods from a number of
repeated readings. In order to define the precision of a set of measurements, the standard
deviation may be used. 'Low precision' means that random uncertainties are very high.
8.2.2. Accuracy
Accuracy is a statement of the closeness with which a measurement is expected to
approach the true value. Accuracy includes the effect of both systematic and random
uncertainties. The value of a quantity is understood to be considered as 'true' either by
theoretical considerations or by comparison with a fundamental measurement. The
indicated value is the value of a quantity as indicated by the relevant measuring device,
sometimes also called 'reading' or measured value.
'High accuracy' means that the indicated and the actual values are nearly the same.
8.3. Assessment of random and systematic uncertainties
8.3.1. Random uncertainties
If the measured value of a quantity is represented by a parameter Y then, for a normal
distribution, the probability of Y having a value lying between Y and Y + d7 is given by
P(Y)dY= exp - p - \ d Y
oy/{2v) \ 2a
2
/
where ju is a constant, equal to the value of Y at the maximum of the distribution curve,
144 G Busuoli
and a is a measure of the dispersion or width of the curve. The quantity a
2
is called the
variance of the distribution. The quantity a can be estimated from an analysis of the
observations and this estimate, together with the number of degrees of freedom, are used
to derive the random uncertainties.
If n measurements of the same quantity are performed, the best estimate of the
constant \x of the distribution is given by the mean value Y:
_ 1 "
n ,
= l
and the best estimate of the variance a
2
of the distribution is given by the variance
S
2
(Y):
1
S\Y) x Vi-ry
n - 1 , fi
The quantity S(Y) is called the standard deviation of the measurements.
Because any mean value Y comes from a limited number of measurements, repeated
determination of Y will produce a series of different values. These, for a large n, will have
a distribution close to normal, whatever the distribution of Y. The standard deviation
of this distribution can be determined and it is called the standard error of the mean
5(F), given by
1 _ , S\Y)
S\Y) = X (V, - Y)
2
= - ^ .
n(n - 1) ,= ! n
In many circumstances experiments consist of measurements that involve several
quantities. Therefore, the value 7 of a physical quantity is linked to other separate
physical quantities by the relationship Y=f(a, b, c,...) with the variances of the single
quantities S
2
(a), S
2
(b),....
The estimated variance of Y is given by
S
2
(Y) = (bY/da)
2
S
2
(a) + (dY/bb)
2
S
2
(b)+(dY/bc)
2
S
2
(c) + ....
The same holds true for Y = f(a, b, c,...).
83. 2. Systematic uncertainties
Whereas in the treatment of random uncertainties a straightforward statistical procedure
can be applied, for systematic uncertainties this is not possible, since the probability
distribution is not known.
If the value Y of a physical quantity is a function of a number of measurements
a, b, c,... of separate physical quantities, i.e.
Y=f{a,b,c,...)
then, if the measurements are all independent, the systematic uncertainty (AY)
a
of Y,
due to the systematic uncertainty Aa on a, is given by
(AY)
a
=\dY/da\Aa.
Precision and accuracy of TLD measurements 145
In practice there are two methods used to combine the different components in order to
give the overall systematic uncertainty AY. The first is by a simple arithmetic addition:
AY=(AY)
a
+(AY)
b
+ (AY)
c
+ ...
ay
da
Aa +
dY
db
Ab +
dY
Ac +.
dc
The second is to combine them in quadrature:
AY
2
= (AY)* + (AY)
2
b
+ (AYf
c
+...
/bYf /dY\
2
/ ay\
2
= )Aa
2
+ )Ab
2
+ Ac
2
+ .
\?>a/ \db/ \dc/
The first method probably overestimates the total systematic uncertainty, while the
second tends to underestimate it. Therefore, in stating the systematic uncertainty of a
physical quantity the component parts should be listed, together with the actual value of
any constants and correction factors used; the method of summing the component parts
should also be indicated.
8.4. Sources of errors in TLD
From the publication EUR 5358 'Technical recommendations for the use of thermo-
luminescence for dosimetry in individual monitoring for photons and electrons from
external sources', we can derive a list of commonly encountered sources of errors that
affect the precision and accuracy in determining the dose under identical geometrical
conditions.!
These errors will depend on the detectors, the reader and the evaluation procedure, the
thermal history and the sensitivity of the detectors to neutrons.
8.4.1. Errors due to the detector
Variability of transparency and other optical properties of the detector.
Variability of the optical properties of any covering material, if this remains in position
while the detector is read.
Temperature influences in excess of those taken into account by the calibration pro-
cedures.
light effects.
Effects due to the energy and directional dependence of the dosemeter response.
Contamination of the thermoluminescent material (not radioactive contamination).
Ineffective and non-reproducible cleaning procedures applied to the detector.
Variability of the mass of the thermoluminescent material in the detector.
f Commission of the European Communities Document.
146 G Busuoli
Where the use of powder is concerned, the distribution of the powder in the tray of the
reader.
Changes in the detector sensitivity due to radiation damage.
8.4.2. Errors due to the reader and evaluation procedure
Instability of the functions of the read-out device and the peripheral equipment.
Instability of the reference light source, due to intensity and spectral changes, with time
and temperature.
Non-reproducibility and variability of the rate of inert-gas flow.
Non-reproducibility of the detector position in the reader and of the heat transfer
between heater and detector.
Variations in the zero-dose reading.
Non-consistency of the thermal read-out cycle during calibration and measurement.
Changes in the optical properties of the read-out device, in particular due to variations in
the reflectance of the heater element.
8.4.3. Errors due to the thermal treatment
Non-reproducibility of the pre-irradiation annealing procedure.
Non-reproducibility of the post-irradiation heat treatment.
Non-reproducibility of the thermal treatment during read-out.
The above list consists both of systematic and random errors and the loss of precision,
introduced by these sources, can be minimised by carefully performing the whole
measuring cycle with the TL dosemeters.
8.5. Precision of TL measurements
(a) Precision obtainable with one single dosemeter. If a single dosemeter is repeatedly
irradiated with the same dose and is read keeping the different parameters constant,
variations in the measured TL signal are observed.
These variations determine the precision with which a certain dose can be measured
with the dosemeter. There are several sources of these variations and they are amongst
those previously listed. Their relative weight on the precision of the results will depend,
to some extent, on the dose value to be measured. One of the most important causes of
variations comes from the detector's zero reading (or background signal), determined
from repeated measurements on unirradiated dosemeters. This is particularly important
a low doses, while with increasing doses the background and its variation become less
and less important and finally can be neglected.
A further source of variation is due to the instrument instability determined through
repeated readings of the light source normally placed inside the instrument. The contribu-
Precision and accuracy of TLD measurements 147
tion to standard deviation which originates from the instrument conditions normally does
not amount to more than 0.3%.
Assuming that the dose is exactly the same in the different series of exposures, the
total variance in a series of measurements at any dose level with one single dosemeter is
given by the following equation:
Here cr
s
is the percentage standard deviation of measurements when background effects
are negligible, D is the dose, in millirad, and a^ is the variance of the readout of un
irradiated dosemeters in equivalent absorbed dose, here in millirad..
As an example, table 8.1 gives the standard deviations as measured in practice for
different TL detectors exposed to 0.1 R of
60
Co gamma rays. The figures for the standard
deviations reported in table 8.1 are representative of both the reproducibility of the
detectors and the stability of the readers, whose setting remained unchanged during the
entire experiment.
(b) Precision obtainable with several dosemeters of the same type. This is the normal
situation encountered in practice; in fact the calibration curves are made with dosemeters
which are not those used routinely, even if they belong to the same batch. In this case
therefore, some more sensitivity variations among the dosemeters affect the precision
obtainable. The variations of sensitivity are mainly due to the following reasons:
(a) variation in the amount of phosphor;
(b) variation in the size of the compact dosemeters;
(c) variation in the grain size;
(d) variation in the optical density of some types of dosemeters due to the temperature
during the production process, as in the case of Teflon dosemeters.
These variations are normally reduced to a minimum by the producer himself either by
putting the dosemeters into groups of equal sensitivity or by assigning to every dosemeter
its sensitivity factor.
For the standard deviation of a group of dosemeters of the same type, the same
formula holds as before:
Ui'M
where, in this case, a
s
is the percentage standard deviation of the group irradiated to the
doseZ).
The percentage standard deviation is given by
\ 2 / \ 2- | l / 2
D
()&)]
which shows that the standard deviation depends on the dose to be measured and by
increasing this dose it decreases to a constant value which depends on the variation in
sensitivity.
-1^
oo
CTi
Table 8.1. Reproducibility test at the 100 mR exposure
readings). o(%)
Participant
TLD material
1
2 repeated
3 exposures
4
5 100 mR
6
7
8
9
10
X(10 readings)
<7(%)
e level for single detectors and 5 re-uses. X
= relative standard deviation for X(10 detectors)
1
Li
2
B, 0
7
n c
X
0.99
1.00
1.01
1.01
1.00
1.01
1.03
0.98
1.00
0.97
1.00
1.7
<7(%)
4.0
5.2
1.2
2.1
3.9
0.9
1.1
6.9
4.8
3.7
2
LiF
c
X
0.99
0.98
0.97
1.02
0.98
1.05
0.94
1.03
0.94
1.09
1.00
4.8
<r(%)
2.0
2.6
1.8
1.8
6.0
1.0
3.2
3.4
1.6
1.4
3a
LiF
c
X
0.97
0.98
1.01
1.02
1.00
1.02
1.01
1.00
1.00
0.99
1.00
1.6
<7(%)
1.8
1.5
1.4
4.0
3.4
2.6
2.7
2.3
0.8
1.4
).
3b
CaF
2
c
X
0.98
1.01
1.01
1.01
1.00
0.97
0.99
1.01
1.01
1.01
1.00
1.5
o(%) X
1.8
1.0
0.9
1.4
1.8
0.8
0.9
1.0
0.9
1.2
4
Li F
n c
o(%)
5
Li F
n c
X
1.03
1.16
1.05
1.02
0.90
0.95
1.02
0.96
0.98
0.93
1.00
7.4
(%)
16.5
10.9
11.8
10.4
9.3
10.1
23.2
10.5
10.7
15.2
= X(10 detectors)/.?(10 detectors and 5
6
Li F
c
X
1.00
1.01
1.01
0.99
1.00
1.00
0.98
1.00
1.00
1.01
1.00
0.9
o(%)
6.0
5.3
3.8
3.6
3.8
3.3
1.7
4.2
3.5
5.4
7
LiF
c
X
1.02
1.01
1.02
0.98
0.98
0.98
1.06
0.99
0.99
0.98
1.00
2.6
a(%)
1.4
1.4
3.5
3.3
1.7
1.9
2.2
1.0
3.1
2.3
8
BeO
X
1.04
0.86
1.07
1.04
1.01
0.92
0.93
1.02
1.06
1.05
1.00
7.0
o(%)
6.5
5.3
4.5
8.0
9.1
5.2
6.2
9.8
4.8
10.0
to
K
C
Q
j ^ .
c, commercial; nc, non-commercial.
Precision and accuracy of TLD measurements 149
Typical values for o
s
are 2% and 3% for l i F powder (43 mg) and IiF-Teflon discs
(0.4 mm thick) respectively. Corresponding background values in equivalent exposure of
(8 1) mR and (31 3) mR are found.
From these data and the previous formula for the percentage total standard deviations,
it is possible to calculate the data given in table 8.2 for the precision at different dose
levels.
Table 8.2. Precision
levels.
LiF powder
LiF-Teflon discs
of TLD
10 mR
12%
30%
measurements
lOOmR
2.5%
4.0%
for different dose
1 R 2 R
2% 2%
3% 3%
If after use there is no change in sensitivity due to the thermal treatment or to the
irradiation, a calibration factor or sensitivity factor can be assigned to each dosemeter and
used to correct responses. In this case the precision obtainable can be of the order of 1%
or even less.
8.6. Accuracy of TL measurements
As reported in the above definition, the accuracy of a particular dose measurement is
defined by the difference between the measured value of the dose and the true dose with
which the dosemeter was irradiated.
The most important variables that influence the accuracy are associated with the
calibration of the dosimetric system and with the behaviour of the dosemeter when
exposed to different kinds of radiation, i.e. energy dependence, dose rate dependence,
etc.
To avoid, for example, inaccuracies due to the energy dependence, it would be
desirable to perform the calibration of the dosemeters with the same radiation quality
as the control. In many practical situations this is not achievable because the value of the
energy is unknown a priori since the dosemeters have been exposed to a mixed x- and
gamma ray field as in the case of routine dosimetry. In this case a systematic error is
unavoidable even if very sophisticated techniques for energy correction have been
applied. As an example, figure 8.1 gives a typical energy response curve for a practical
dosemeter in which a filter is used so that a flat energy response within a large range can
be obtained. If the energy varies from 80 keV to
60
Co, the systematic error, introduced
because the calibration is carried out at a well-defined energy value, will be of the order
of about 5%. If, however, the radiation field contains mainly low-energy x-rays, as in
the case for many practical situations, the error will be much higher.
Another example of systematic uncertainty comes from the inaccurate positioning
of the dosemeter in the heating tray; this is particularly true for powder dosemeters if
appropriate care is not taken.
150 G Busuoli
10
1
>
<
LU
0.1
o
Q_
LU
cr
0.01
10
** S *-
100 1000
ENERGY ( keV)
Figure 8.1. Example of the systematic
uncertainty due to energy response. ,
CaF
2
: Mn (filtered); A, CaF
2
: Mn (unfiltered).
8.7. Accuracy in low-dose measurements
One of the recent applications of TL materials is for the measurement of low doses such
as in the case of environmental monitoring around nuclear power plants.
For this application, the signal which is obtained is in many cases comparable with the
background signal, even if using high-sensitivity materials. Therefore special attention
must be given during calibration.
Reproducibility will be determined by giving one TLD repeated exposures equal to that
resulting from an exposure rate of 10//Rh"
1
during the field cycle. The responses will
have a relative standard deviation of less than 3.0%.
Uniformity will be determined by giving TLD from the same batch an exposure equal
to that resulting from an exposure rate of 10 /nR h"
1
during the field cycle. The response
obtained will have a relative standard deviation of less than 7.5%. If the level of uni-
formity specified above is not obtained, a selection of TLD or an individual calibration
will be necessary.
As for the accuracy, 95% of the final corrected values (after all appropriate corrections
to the measured values are applied, including those for errors expected under field con-
ditions) will differ from the true exposure value by less than 30% of the true exposure
value.
Applied Thermoluminescence Dosimetry. Eds M Oberhofer and A Scharmann
1981 ECSC, EEC, EAEC, Brussels and Luxembourg
Reference to other solid-state methods
E PITT AND A SCHARMANN
9.1. Introduction
The subject of this book is thermoluminescence dosimetry. Some other solid-state effects
are also known which are useful in dosimetry. This chapter is designed to give a brief
survey of them.
The basic absorption mechanisms of damaging radiation in a solid-state material are
first summarised (figure 9.1).
INCOMING RAD I ATI ON
(a)
ABSORBING MATERIAL
(>)
Figure 9.1. Scattering of ionising radiation, (a) Charged particles, e.g. c, p, a, etc; (b) neutral
particles, e.g. n, 7, etc.
Two types of basic mechanisms must be distinguished:
(a) Directly ionising radiation consists of charged particles such as electrons, protons,
positrons, a-particles, etc. The atoms of the absorbing material are directly ionised
by Coulomb interaction.
(b) Indirectly ionising radiation consists of neutral particles such as neutrons, x-rays,
7 photons, etc, which primarily create charged particles by inelastic collisions or
nuclear reactions. These charged particles ionise secondarily as described under
(a). (The direct ionisation of neutral particles is negligible.)
The main effect on biological tissue is the ionisation and disturbance of molecules.
Several effects are known which indicate ionisation products in solids. Only those effects
152
E Pitt and A Scharmann
which are of interest in dosimetry are considered. In every case it is required that ionisa-
tion causes a reaction in the solid which is easily observed directly or indirectly and which
can be used to measure the absorbed dose or dose rate. Linearity over several orders of
magnitude is also required.
The most important effects for solid-state dosimetry are specified in table 9.1. Scintilla-
tion dosemeters are used for dose ratemeters, whereas the other effects are used for the
integration of the dose absorbed during a certain period.
Table 9. 1. The most important effects used in solid-state dosimetry.
Effect
Radiophotoluminescence
Coloration
Photographic effect
Exoelectron emission
Track detection
Neutron-induced defects
Scintillation
Measured quantity
Luminescence
Optical density
Optical density
Number of electrons
Number of tracks
Change of resistance
Luminescence
Dosemeter material
Glass
Crystal, glass
Film
Ceramics (BeO)
Organic film
Semiconductor (Si)
Crystal
Radiation types
measured
7
7, n
7, n
7, n, (3, a
n
n
7
The electronic processes which follow the ionisation are in general explained in the
energy band diagram. A simplified model is illustrated in figure 9.2. During excitation
electron-hole pairs are created. The holes move in the valence band and some of them
can be trapped at recombination centres. The electrons diffuse in the conduction band.
From there direct recombination with holes, sometimes by preference at special re-
combination centres, is possible. A fraction leading to scintillations is counted by a
photomultiplier. This mechanism is observed during and immediately after the excitation.
It is therefore only useful for dose rate measurements. In the case of all other effects the
second step after the excitation is the already mentioned trapping of electrons. The trap
depth and the resulting emptying temperature are responsible for the stability of an
integrating dosemeter. For routine dosemeters it is usually not less than 200 C. The
CONDUCTION BAND
( o) 16)
( c)
*--
'fo r/,. %'//X7/ %////%, '/,/. w /////,
SURFACE -
VALENCE BAND
Figure 9.2. Mechanisms of solid-state
dosemeters in the simplified energy band
diagram, (a) Scintillation, (b) RPL,
coloration, (c) TL, (d) TSEE.
Reference to other solid-state methods 153
electronic processes taking place in these integrating dosemeters are described in the
following subsections.
9.2. Radiophotoluminescence (RPL)
Silver (Ag
+
)-doped phosphate glass shows the optical behaviour described by figure 9.3.
Approached from short wavelengths, the lattice absorption decreases and vanishes at the
band gap energy. At longer wavelengths the defect absorption band of Ag
+
centres arises
followed by the corresponding emission of light, the so-called photoluminescence, at still
longer wavelengths. This electronic excitation and relaxation is observed in most
crystalline solids at impurity centres.
arb
units absorption-
c
o
c/i
m

c
o
o
in
<
Ag* Ag*
Ag
Ag
Conduction Band
trap
Ag*
Ag - Jt
Valence Band
200 300 400 500 600 700 nm
Wave Lengt h
Figure 9.3. Optical behaviour of an RPL glass (left) and RPL mechanism (right).
After exposure to ionising radiation two additional bands are found, both situated on
the long-wavelength side of the original Ag
+
bands. A new radiation-induced photo-
luminescence centre has been created by the recombination of Ag
+
ions and electrons
released to the conduction band. The concentration of these neutral Ag centres (figure
9.3) is proportional over a wide range to the ionising radiation dose. Their luminescence,
the radiophotoluminescence, is measured after selective excitation of the RPL absorption
band only.
Figure 9.4 shows the block diagram of a commercial RPL reader. The light of a uv
source is focused on the RPL glass. An optical filter selects the excitation wavelength of
the RPL band. The emission is observed through a second filter by a photomultiplier.
Trap centres, capturing some of the conduction electrons for a certain time after the
absorption of ionising radiation, enhance the build-up of the RPL centres. This process
can be accelerated by heat treatment for some minutes.
RPL exhibits a specific advantage over TLD. Dose read-out does not cause annealing
of the radiation-induced effect. Therefore the loss of information by mistakes and errors
154
E Pitt and A Scharmann
UV source l ens-
optical C
filters
RPL glass
photomultiplier
Figure 9.4. Principles of an RPL reader.
at any point of the reading procedure is avoided, whereas a repetition of the read-out is
impossible for TLD. Another advantage of this effect is the possibility of registration of
small doses over extended periods of time (~year) with a dosemeter for short duration
monitoring (~day or month), which may be read several times without annealing.
The lower detection limit of about 100 mrad for commercial RPL systems is too high
for personnel dosimetry. This limit is not due to the read-out system, but rather to the
so-called pre-dose. This is the dose reading which is already monitored without excitation
by ionising radiation. It stems from the luminescence of internal or surface defects and
impurities of the glass rod. The luminescence mechanism has therefore been studied in
detail. It was found that the luminescence decay may be described as a sum of three
exponentials. One of them depends on the ionising radiation. Its decay time is about
3 /xs, whereas the two other components decay with a longer and a shorter time,
respectively.
This behaviour leads to a modified RPL reader. The continuous light source is replaced
by a nitrogen laser, which can be built easily and cheaply. Its emission wavelength of
337 nm corresponds to the excitation maximum of the RPL band. The pulse width of the
laser flash is 8 ns. The intensity of this very simple laser varies over a range of 30%. Thus,
normalising each measured luminescence value to the laser intensity is necessary.
Figure 9.5 shows the block diagram of the evaluation device. It exists only as a labora-
tory model. The glass rod is'irradiated by the laser pulse. The luminescence is registered
by a photomultiplier (RPL). A part of the laser intensity is deflected by a quartz slice
to a second photomultiplier (laser), which measures the laser intensity for normalising.
The two light intensities are integrated and the data analysed by a microcomputer. At the
right-hand side of the figure the corresponding curves of the laser pulse, the luminescence
pulse and the voltage pulse at the first dynode of the multiplier are plotted. 2 jus after the
ultraviolet flash a large fraction of the pre-dose luminescence has decayed. Then during
a period of 8 ids the ratio of radiation-induced to pre-dose luminescence shows a
maximum, even for low x-ray doses. During this time the voltage pulse at the first dynode
sensitises the photomultiplier. The registered luminescence is integrated and stored.
Better accuracy is achieved by repetition of the procedure and calculation of the average
value by a microcomputer based on a microprocessor unit, which also controls the
measurements. In this way the lower detection limit of an RPL dosemeter is about
10 mrad. At higher doses a deviation of the linearity between dose and dose reading is
observed. In this range the visible colouring of the glass is used as a measure for the dose
and the absorption of the glass is registered by a third photomultiplier.
Reference to other solid-state methods
Quartz Slice RPL Glass
155
N
;
Laser | ~ ~ \ ^
v-
PM
Transmiss
Opt Filters
Integration
Storage
Trigger
EH
PM
RPL
Integration
Storage
Laser Pulse
Luminescence Pulse
Integration
Storage
Microprocessor
B
Voltage Pulse
at the first Dynode
1
i
-^ r~
T
2
Printer
Figure 9.5. Block diagram of an RPL reader.
9.3. Colouring
As mentioned in the preceding subsection, a heavily irradiated glass exhibits an absorp
tion in the visible range. This effect is well known from the investigations of colour
centres in alkali halides (figure 9.6). Electrons lifted into the conduction band during the
excitation process are trapped at anion defects in socalled F centres. The corresponding
cation defects with trapped holes are denoted as Vj centres. Both are excited by visible
light. This energy absorption gives rise to the colouring of the glass. Similar effects are
known for nearly all transparent materials. They can be used for dosimetry.
00000
0 O, Q0 0
0
v
)0 O
0 0
O00
0 > 0 0
0000
000
F centre
Figure 9.6. Colour centres.
V, centre
An absorption reader consists mainly of a light source and a detector for the trans
mitted light. The transmission of the unirradiated dosemeter is only slightly decreased by
ionising radiation doses, which are of interest in personnel dosimetry, since the concentra
tion of the created colour centres is small. Thus the relative change of the light intensity
is too small for sufficient sensitivity. Doses of 10
2
rad up to 10
7
rad and more are
detectable by absorption dosemeters.
These basic considerations show that a dose reader for practical use should measure
an effect which is absent in the unirradiated dosemeter and which is generated at high
156 E Pitt and A Scharmann
sensitivity by the ionising radiation. Otherwise a developing procedure is necessary which
amplifies the effect as in film dosemeters.
9.4. Photographic process
Most dosemeter films consist of silver bromide crystals in a gelatin layer. These films
were the most commonly used personnel dosemeters for a long time since their handling
is easy and the processes are sufficiently well known from optical photography. The
elementary processes are illustrated in figure 9.7.
conduction band
5r
excitation
^
Ag
+
Ag Ag * " ^ Ag
+
valence band ;
(a) (6)
Figure 9.7. Elementary processes in an AgBr film.
By high-energy excitation an electron-hole pair is created and both particles are
captured in deep traps (a). Then a rather mobile Ag
+
ion migrates to a trapped electron
and recombines to produce a neutral Ag atom (b). This represents a deep trap for another
Ag
+
ion. The Ag so formed is again a trap for an electron. By the alternate capture of
electrons and Ag
+
ions metallic silver grains grow in the gelatin layer and can be
registered.
The film dosemeter no longer meets the standard required although it is still often
used. The main reason is the lack of stability during storage in a warm and humid
atmosphere. As a consequence one expects dosimetric and material changes, such as:
(a) changing sensitivity,
(b) the gelatin becomes sticky and the film is destroyed,
(c) the unirradiated film exhibits a fog,
(d) destruction of the gelatin by microbiological reactions,
(e) high fading up to 70% at 80% humidity.
But even if the film is used under optimal climatic conditions there are some dis-
advantages compared with other personnel dosemeters:
(1) The relative energy response for 7-rays from 30 keV to 1 MeV covers a range of
1-30 as a result of the high AgBr concentration. Some efforts were made to
compensate for this effect by using several filters and increased AgBr grain sizes
together with special developing techniques.
(2) An error during the developing procedure or the storage destroys the stored
information.
Reference to other solid-state methods 157
(3) The film is also sensitive to normal daylight.
Nowadays film dosemeters are commonly used together with several filters of different
atomic number to determine the composition of the photon energy spectrum.
However, the film dosemeter is of some importance in neutron dosimetry. Filters are
used to absorb 7-radiation which cannot be neglected in usual mixed fields. The neutron
dose can be calculated by comparison of the filtered and the unfiltered parts of a film.
In practice the error in this method is very high since the 7 sensitivity far exeeds the
neutron sensitivity.
A comparison of an actual exposure with the read-out of several developing services
has shown that, in the case of 7 dosimetry, the error of about half of all readings
exceeded 50%.
Although the mentioned sources for errors in film dosimetry are well known, it is
still in use because of its easy handling. The film, together with all necessary filters, can
be placed in a thin badge. The identification mark is easily fixed to the film by applying
pressure. Developing large numbers of films is feasible. The unexposed ones are separated
by visual inspection.
9.5. Stimulated exoelectron emission
As is known from the TL theory, electrons are raised into the conduction band of an
insulator by excitation with ionising radiation. They are then able to recombine directly
with holes or to be captured in traps. A third mechanism is observed at the surface of
some materials: low-energy electrons originating from the conduction band are emitted
after excitation or during heat or light treatment (figure 9.2). They are called exo-
electrons and occur at temperatures below thermionic emission. The exoelectron emission
is a surface process which is competitive with the recombination process and which gives
rise to light emission of spontaneous luminescence or thermoluminescence. Thus, for a
schematic description of the mechanism a modified kinetic model may be used as is
known from TL.
Exoelectron emission is observed not only at surfaces excited by ionising radiation,
but can also be due to surface treatments such as
(i) mechanical deformation,
(ii) desorption and adsorption reactions,
(hi) chemical reactions.
These additional effects are a severe problem in exoelectron dosimetry: each of them
is a source of erratic dose readings. Consequently the dosemeter must be kept clean and
dry. The adsorption of water molecules very strongly influences the emission of most
exoelectron dosemeters.
In general all laboratories use their own instrumentation for exoelectron dosimetry.
Figure 9.8 shows a reader for thermally stimulated exoelectron emission based on a pro-
portional gas flow counter. According to the diagram of figure 9.9 such a reader consists
of a heater with the sample, in front of which is situated a cylindrical methane-filled gas
tube. Emitted exoelectrons are accelerated in the electric field between the sample and
the steel wire. They ionise gas molecules. The resulting electron current is collected at
the wire. A corresponding voltage pulse at the exit of the gas tube is amplified and
158 E Pitt and A Scharmann
Figure 9.8. High-temperature TSEE gas flow proportional counter built at the Radiation
Protection Division of the Joint Research Center of the European Communities, Ispra
Establishment, showing water-cooled sample slide with oven withdrawn.
gas outlet
gas outlet
high voltage
amplifier supply
s
sample
bridge
spring rested
heater
water cooling
thermocouple
Figure 9.9. Diagram of a cylindrical TSEE gas flow proportional counter.
registered. Metal oxides, especially BeO, are used as a personnel dosemeter. BeO has a
low effective atomic number and therefore exhibits an energy dependence nearly equal
to that of human tissue. Its main peak is about 200 C, so that it is stable at room
temperature. A typical exoelectron curve of BeO is shown in Figure 9.10. Recently BeO
thin-film detectors evaporated on graphite substrates have been developed. They are
superior to the formerly used ceramic BeO with respect to an improved dose stability
against mechanical and humidity influences.
The standard deviation of a certain exoelectron dosemeter can reach 20%, caused by
the sensitivity to other surface treatments. Nevertheless exoelectron dosemeters are
superior to other systems in some special cases. This is especially true in the low dose
Reference to other solid-state methods
t7) A
159
r r
i -
ii
m
<
>-
i -
ii
LU
LU
LU
CO
400
200 250 300 350
TEMPERATURE ( C)
Figure 9.10. TSEE curve of BeO. 1500 A BeO on graphite heated in wet nitrogen at
1000C.
range, where it is possible to detect microrad doses with a reasonable expenditure of
effort. Although the surface character of exoelectron emission makes this method sensitive
to disturbing mechanisms which cannot occur in the case of bulk effects such as TLD or
RPL it offers some favourable properties too. Since the dose information originates only
from a thin surface layer exoelectron emission enables a sensitive detection of nuclear
particles which deposit their energy close to the surface, such as a-rays or low-energy
/3-particles. For instance, radon concentrations of a few tenths of a picocourie per litre
have been measured after an exposure time of only 1 d. After 1 h exposure insoluble
tritium gas at a concentration of 2 x lO^jLtCimr
1
can be detected. Because of the
increasing number of nuclear power stations tritium dosimetry may become one of
the main applications of the exoelectron method. In principle, the detection of fast
neutrons is also possible if the dosemeter is covered by a polyethylene radiator which
generates recoil protons.
Since exoelectron emission is an electronic process like TL emission the repeated use of
the same dosemeter after annealing is possible.
9.6. Track detection
In the preceding chapters some dosemeter materials and methods have been described
which are sensitive to 7-rays and sometimes additionally to neutrons. One of the main
problems of personnel dosimetry is the detection of neutron doses in mixed 7-n fields
because it is difficult to find a sensitive neutron detector which is also not sensitive to
7-radiation. Often a combination of two detectors is used, one monitoring the mixed-
field dose and the other one monitoring the 7 dose. Nevertheless neutron dosimetry is
an unsolved problem and in some nuclear research centres a neutron dose has never been
registered with these personnel dosemeters.
Nuclear track detectors are selective fast-neutron detectors. They consist of organic
films of high hydrogen content such as cellulose nitrate. The elastic energy transfer of
160 E Pitt and A Scharmann
fast neutrons penetrating into a solid depends on the atomic weight of the stopping
nuclei. It exhibits a maximum for hydrogen atoms. These nuclei are released and also
stopped in the solid. During this stopping process of neutrons and protons a latent track of
destroyed material is generated. Some etchants are known whose etching rate is higher
in the latent track than at the surface of the film. By this procedure the tracks become
visible. KOH is a typical etchant proposed by the producer of cellulose nitrate detectors.
The dose reader counts the tracks generated. Computer-operated image analysing
systems are used, which count the tracks automatically. This method is expensive, very
complicated and the operating speed is rather slow. Under optimum conditions an
area of 1 mm
2
, necessary for a lower detection limit of 0.5 rad, is investigated in 15 min.
The sensitivity is limited by non-radiation-induced tracks which result from production
defects, handling, etc. Evidently this system is not suitable for evaluations of large
numbers of detectors.
For routine dosimetry a fast reader was developed based on spark counting (figure
9.11). The latent tracks of thin foils are etched through. The foil is placed as a dielectric
between the electrodes of a capacitor. A ramp voltage is applied and the sparks occurring
are counted. To avoid multiple counting of the same hole an aluminised polycarbonate
foil is used as one of the electrodes. The aluminium in the environment of the hole is
burned away. This reader is cheaper than the optical image analyser and the reading time
is shorter. Using automatic devices reading times of about 1 min for one foil are feasible.
When counting an area of 2.5 cm
2
the sensitivity is 5 mrad for 14 MeV neutrons. For
thermal neutrons n-a converters have to be used for the generation of the latent tracks.
HV +
H Z Z h
R
COUNT
D ISCHARGE =
CAPACITOR C
-PRESPARK
c
^
mmmmrn
2 COUNTER
i
Figure 9.11. Block diagram of a spark counter. 1, high-voltage electrode; 2, detector foil,
3, aluminised polycarbonate film.
The track detection technique is applied not only in neutron dosimetry, but also for
heavier particles, up to the heaviest atoms. In this case glass or crystal detectors of higher
atomic numbers are used, corresponding to the higher weight of the incoming particles.
In recent years a new material called CR39 has been developed which shows an
excellent contrast of the etched track. With this detector it may be possible to reach even
lower dose ranges, especially at lower neutron energies. The energy response of CR 39
fits the rem curve fairly well.
Reference to other solid-state methods
9.7. Change of resistance in silicon diodes
161
One more neutron dosemeter of practical use is the silicon diode. Fast neutrons produce
reversible defects in semiconductors; in the case of silicon, especially vacancies and
Frenkel defects. These defects strongly decrease the conductivity by trapping carriers.
The main advantage of this fast-neutron dosemeter is the small size, of the order of some
cubic millimetres. But, as mentioned in the subsection concerning absorption dosemeters,
low sensitivity is expected due to the reading procedure: a forward voltage is applied to
the diode. The corresponding current decreases after irradiation. The reader shows the
voltage change of the diode at a certain diode current. The relative change is small at
small doses. Figure 9.12 shows typical characteristics of commercial diodes.
Figure 9.12. Forward current as a func-
tion of forward voltage for unirradiated
and neutron-irradiated silicon diodes [5].
A higher diode current seems to sensitise the system. The simultaneous warming-up
of the diode during the reading procedure increases the annealing probability of the
defects and thus the reader error increases.
Another disadvantage of the silicon diode detector is the low stability. Thermal
annealing at room temperature leads to a fading of up to 10% during 10 d. Apart from
this disadvantage, the dosimetric data of silicon diodes from a single production run
vary over a wide range. Therefore the accuracy at 10 rad is about 10%. After individual
adjustment a lower detection limit of 1 rad is achieved at reasonable accuracy with high-
sensitivity diodes. The useful range is about three orders of magnitude. For less sensitive
diodes the upper detection limit is 10000 rad. These properties show that the diode
is interesting only for reactor, accidental or military dosimetry, but not for personnel
monitoring.
Thermally stimulated 7: 10"
s
- l 0" rad
exoelectron emission (TSEE) n: 10~
4
-10
4
rad
10keV-30MeV
>l Me V
High sensitivity, surface resolution Strong influence of chemical or
mechanical treatment
Track detection n > 0.1 rad 1 keV-20 MeV Tissue equivalent, low sensitivity to
7, x, j3 background
Destruction by over-etching,
sensitive to mechanical treatment
Photographic effect
50 mrad-10
3
rad 40 keV-3 MeV Repetition of the reading is possible, no
fading after developing
Destruction by wrong developing,
strong fading, strong energy
dependence
Coloration 7: 10M0
7
r ad 15 keV-3 MeV Easy reading, important in high-dose
dosimetry
Low sensitivity
Neutron-induced resistance n: 1-10" rad
change
>0. 4 MeV Simple reading, small volume Individual calibration necessary,
strong fading, non-linear reading
t o
h]
Table 9.2. Properties of solid-state dosemeters.
Dose range
TLD
Energy range Advantages Disadvantages
7: 1 mrad-10
4
rad 10 keV-30 MeV
Radiophotoluminescence 7: 10 mr ad- l Cr ad 15 keV-30 MeV
1% fading/month, low costs, storage
unlimited, low energy dependence
Low fading, low costs, low energy
dependence, storage unlimited, repeated
monitoring possible
Annihilation of stored informa-
tion by evaluation
Thick dosemeter badge
a
a.
sh
ft
s
Reference to other solid-state methods 163
9.8. Scintillation dosemeter
One of the main requirements mentioned for a dosemeter is the storage of the absorbed
dose information. Here a differential dosemeter is briefly mentioned, which does not
meet this requirement and which therefore can only monitor the dose rate.
The scintillation mechanism is as follows (figure 9.2): electron-hole pairs are created
by exciting radiation. Both electrons and holes migrate separately or together to activator
centres consisting, in general, of dopants. At these centres the luminescent recombination
takes place. A photomultiplier registers the emitted light. This detection system is well
known from nuclear physics. It is used only in laboratories and not in routine dosimetry
because of its large size. Therefore only this brief description is given.
Several scintillators of practical interest are known, mainly inorganic crystals like alkali
halides, organic crystals and plastics. By selection of the atomic number of the absorbing
material it is possible to measure approximately air-equivalent or tissue-equivalent doses.
Photon as well as particle radiation is detectable. Especially in clinical dosimetry the small
size of the absorber itself is interesting. It can be placed far away from the light detector
if connected by a light pipe.
9.9. Conclusions
Besides the well-known TLD some other dosemeter methods are interesting for practical
use. Solid-state materials are principally qualified because information is easily stored
for a longer time as a consequence of solid-state properties. This holds for radiophoto-
luminescence, thermally stimulated exoelectron emission, film, track detector and
coloration as well as for TLD. TLD is the best-developed system since much money was
spent in its investigation. Nevertheless, each of the other systems has its advantage in
special applications. The main features are compared in table 9.2. The limits given here
are valid only for commercial systems. Some larger nuclear research centres have built
their own systems with better results.
References and further reading
1 Attix F H, Roesch W C and Tochilin E Radiation Dosimetry (New York: Academic)
2 Frank M and Stolz W Festkorperdosimetrie (Weinheim: Verlag Chemie)
3 Becker K Filmdosimetrie (Berlin: Springer-Verlag)
4 Becker K and Scharmann A Einfiihrung in die Festkorperdosimetrie (Munchen: Verlag Karl
Thiemig)
5 Becker K Solid-State Dosimetry (Cleveland: CRC Press)
6 1976 Proc. 5th Int. Symp. on Exoelectron Emission and Dosimetry, Zvikov ed A Scharmann
(I. Physikalisches Institut, Universitat Giessen)
7 1977 Proc. 5th Int. Conf. on Luminescence Dosimetry, Sao Paulo ed A Scharmann (I.
Physikalisches Institut, Universitat Giessen)
8 1979 Proc. 6th Int. Symp. on Exoelectron Emission and Applications (University of Rostock)
P
art II: Applications
Applied Thermoluminescence Dosimetry. Eds M Oberhofer and A Scharmann
1981 ECSC, EEC, EAEC, Brussels and Luxembourg
10
Application ofTLD to personnel dosimetry
E PIESCH
10.1. Introduction
Personnel monitoring is based on the international recommendations of the ICRPf. The
primary objective of individual monitoring for external radiation is to assess, and thus
limit, radiation doses to individual workers. Supplementary objectives are to provide
information about the trends of these doses and about the conditions in places of work
and to give information in the event of accidental exposure [1]. Depending on the kind
of radiation hazard, the ICRP recommend maximum permissible dose (MPD) values.
These are the maximum dose equivalent values which are not expected to cause
appreciable body injury to a person during his lifetime. With respect to the various MPD
values, the following quantities should be measured in personnel monitoring:
(a) skin dose or the surface absorbed dose to assess the dose equivalent to the basal
layer of the epidermis at a depth of 5-10 mg cm
-2
, if only non-penetrating
radiation has to be considered (x-rays < 15 keV, /3-rays);
(b) whole body dose or the dose equivalent at a depth of 400-1000 mg cm
-2
below the
surface of the body to assess or over-estimate the effective dose equivalent or the
average dose equivalent in the critical organs for the case of penetrating radiation
and whole body irradiation (x-rays > 15 keV, 7-rays, neutrons);
(c) extremity dose to assess the maximum value of the dose equivalent (skin dose) in
tissue to any part of the hands, forearms, feet or ankles.
In contrast to film dosimetry, approximately tissue-equivalent TL detectors of small
size and high precision in measurement are available which may serve as an ideal
extremity dosemeter and as a basic dosemeter for the dose estimation of photons in the
energy range of interest as well as for the detection of /3-rays and neutrons. In addition,
a multi-detector badge offers practical possibilities for short-term and long-term
monitoring periods, for separate indication of skin dose and body dose and finally for the
estimation of radiation quality.
The role of TLD for an individual monitoring service is based on the following features:
(a) TL phosphors are available in solid form as chips, extruded ribbons or in a Teflon
matrix; the dose reading of some materials is approximately tissue-equivalent and
largely independent of the angle of radiation incidence;
(b) the dose reading is practically independent of dose rate up to 10
11
rad s"
1
and pro-
portional to the dose up to several hundred rem;
f International Commission on Radiological Prolection.
168 EPiesch
(c) in some TL materials the fading at room temperature is so small, especially after a
post-irradiation annealing, that they can be used for issue periods of up to 1 yr;
(d) TL detectors are convenient to wear, suitable for postal service, flexible in issue
period, can be evaluated in less than 1 min and can be re-used, although a regenera-
tion procedure prior to re-use is often necessary;
(e) TLD lends itself to automation; with an on-line computer the calibration factor for
individual dosemeters can be stored and also the shape of the glow curve may be
checked to verify the radiation-induced TL;
if) for the reassessment of the dose recorded, a redundant detector can be included in
the badge design.
TLD, the most advanced and most intensively studied integrating dosemeter system,
has now reached the stage at which it may replace or supplement film dosimetry.
Primarily for applications in personnel monitoring, various suppliers offer a number of
commercial TLD systems with manual or automatic evaluation systems (see chapter 3).
10.2. Performance specifications
According to the 'Technical Recommendations for Monitoring the Exposure of
Individuals to External Radiation' [2], three kinds of dosemeters are discussed and
recommended by the Commission of the European Communities:
(a) the non-discriminating basic dosemeter is mainly recommended for the group of
low-risk persons to measure the dose without obtaining information on the radia-
tion field;
{b) the discriminating basic dosemeter recommended for the group of high-risk persons
should offer additional information on the radiation field;
(c) the extremity dosemeter is worn in addition to the basic dosemeter if the results
from the basic dosemeter are not representative of doses received by the body
extremities.
For the application of TLD systems in individual monitoring, Euratom has published
technical recommendations [3] which should serve more or less as an indication of what
is generally regarded as good practice and for assistance in avoiding the common sources
of error. For the performance of the basic TL dosemeter only general figures are discussed
(table 10.1).
Performance specifications and test procedures for the application of TLD systems in
personnel monitoring are discussed in additional papers which are all still in the draft
stage:
(a) the PTBf draft 'Requirements of the PTB for the type approval of TLD systems for
radiation protection measurements' 1976;
(b) the ANSIf draft 'American National Standards Criteria for Testing Dosimetry
Performance'N13.ll, 1978;
(c) the HPSSC WG/15 draft 'Proposed Standard Criteria for Testing Personnel Dosi-
metry Performance' 1977;
f Physikalisch Technische Bundesanstalt.
J American National Standards Institute Inc.
Health Physics Society Standards Committee.
Application of TLD to personnel dosimetry 169
Table 10.1. Recommended performance of basic thermoluminescent dosemeters after EUR
5358.
Basic property Nondiscriminating Discriminating
Dose range (photons) ]
m
_
l Q 3 t Q lQ4nd
Dose range (electrons) J
Energy range (photons) 0.0150 MeV
Energy range (electrons) 0.550 MeV
Information on photon radiation Not required Necessary in the range
quality 10200 keV
Overall uncertainty For doses <50 rad: 30%,+50% or 50 mrad
(whichever is the greatest)
>50r ad: 20%, +25%
Precision 2 a < 10% at 1 rad
Photon energy dependence for body 2 0 %+ 40% 15%
dose at 1 cm depth (over energy
range given above)
Dependence on environmental conditions Insignificant
Photon angular response 30% [32]
Fading <5% over the monitoring period at 25 C
(see 6.2)
(d) the ISOf draft 'Personal and Environmental Thermoluminescence Dosimeters'
1979;
(e) the 'Standard Test Programme' recommended as a performance test to establish
a solidstate dosemeter system in the lower dose range [9].
The PTB draft presents more detailed performance criteria. The requirements for the
type approval fix the components of a TLD system, which consists mainly of one or
several TL elements in a badge, of the TL readout instrument (heating and indicating
system) and of additional devices for calibration and annealing. For each quantity of
interest a 'nominal minimum range' is given by definition. With respect to the provided
application of TL D systems, the following minimum ranges and reference energies for
photons are given:
1060 keV, reference energy 30 keV
30200 keV, reference energy 150 keV
1001300 keV, reference energy 662 keV.
The maximum permissible errors for the type approval of TL D systems are presented in
table 10.2. BattelleNorthwest conducted a study to compare and evaluate the four
performance standards existing in the USA and recommended the HPSSC standard for
use in establishing performance criteria for personnel dosimetry [4].
The Naval Research Laboratory participated in a personnel performance testing pilot
study on the basis of the new ANSI and HPS draft. Comments on the testing methods
and procedures are given and recommendations are made for their improvement [27].
The standard test programme was organised from the Fachverband fur Strahlenschutz
[9] as well as in the European Community to study TL D systems in the lower dose range
[28]. The experimental procedure of the interlaboratory test programme (see chapter 11,
table 11.3) provides that measurement runs be carried out by each laboratory with a
f International Organization for Standardization.
170 EPiesch
Table 10.2. Maximum permissible variations of influence quantities and dose reading
according to the PTB requirements (second draft).
Quantity Reference value /max (%)
Photon energy range
Direction of radiation incidence
Temperature (detector)
Humidity (detector)
Temperature (TL reader)
Dose rate
Light sensitivity
Fading after exposure
Operation voltage
Table 10.3. Some properties of thermoluminescent phosphors after EUR 5358.
Thermoluminescent Z
e
ff Main Environmental Number of Dose range
material glow maximum (nm) maxima (rem)
30keV
150keV
662 keV
Of priority
20 C
65% RA
20 C
Indication by manufacturer
Indication by manufacturer
15 minat (20 t 2) C
Indication by manufacturer
+ 30
30
+ 30
20
10
+ 10
2
10
+ 5
5
2
Li F: Mg, Ti
Li
2
B0
7
:Mn,
Li
2
B
4
0
7
:Mn
Li
:
B, 0
7
: Cu,
CaF
2
:Dy
CaF,:Mn
CaF
2
: natural
CaSO:Mn
CaSO<:Dy
CaS0
4
: Tm
BeO
A1
2
0
3
Si
Ag
8.3
7.3
7.3
7.3
16.3
16.3
16.3
14.4
14.4
14.4
7.1
10.2
230
220
185
215
260
260
100
180
300
400
665
368
500
500
380
500
350
699
6
2
2
3
1
6
1
1
2
10
2
-10
4
l O' MO
6
10"
2
-10
6
10
s
- 10
6
10" MO"
10 MO
6
io-
5
-io*
10"
4
-10
s
io-"-io
5
10- M0
5
l O' - l O"
batch of 10 dosemeters taking 10 readings for each dosemeter or repeating the measure-
ment cycle 10 times. The dose range has been related to a multiple of the lowest
detectable dose Z)
ldl
defined here as three times the standard deviation (3a value) of the
zero-dose reading a
u
of unirradiated dosemeters after subtraction of the dark current
reading ao- According to the recommended test procedure every laboratory tests their
own dosemeter systems with respect to zero-dose reading, the lower detection limit, the
standard deviation as a function of exposure, long-term stability of the system and
temperature effects during storage at 70 C.
10.3. D etector materials and specific requirements!
10.3.1. TL materials and detectors
From the TL materials listed in table 10.3 mainly LiF, U2B4O7, CaS0
4
, BeO and A1
2
0
3
doped with appropriate activators are in use which are commercially available as single
f For general requirements, see Chapter 5.
Application of TLD to personnel dosimetry 171
crystals, as hot-pressed or extruded elements, as powder embedded into a Teflon matrix
or in glass capillaries or fixed in thin layers of about 20 mg cm"
2
on a metal or plastic
foil. Generally, most of the TL phosphors are suitable for personnel monitoring but
preferably tissue-equivalent detectors are used. For LiF or U2B4O7 encapsulated in glass,
one has to consider the loss in response in the low photon energy range. For automatic
read-out, the detector chips are encapsulated between two Teflon foils in dosemeter
cards.
Besides the most commonly used LiF: Mg,Ti from Harshaw, the new commercially
available French LiF: Na,Ti (PTL 717) reduces the low-temperature glow peaks, resulting
in a better fading characteristic [6]. Nink [7] published data for an experimental pre-
doped LiF (instead of a Ti0
2
activator, Ti-doped LiF was directly used for adding) and a
Ti-doped LiF. Both materials enhance the main peak, evidently showing excellent fading
and reproducibility results [8]. National produces II
2
B
4
0
7
: Ag,Cu detectors of20mgcm"
2
thickness for automatic read-out [25]. Further TL materials and thin detectors developed
for P dosimetry are described in 5.1.
Sintered MgB
4
0
7
: Dy(Ti) was recently four. J to be a new highly promising TL material
which, in the future, may replace LiF: Mg,Ti in personnel monitoring [46]. Compared
to LiF : Mg,Ti this material shows only a single glow peak, higher sensitivity and precision
(<1%) and a similar energy dependence and fading characteristic; compared to IJ2B4O7
no effect of light sensitivity and hygroscopy has been found.
For the choice of TL materials different aspects and properties with respect to routine
monitoring should be considered:
(a) the dosemeter properties of the detector including dose range, energy response,
reproducibility, uniformity within a batch, energy response and fading;
(b) the requirements for a monitoring service including performance specifications and
type approval, the necessary precision and accuracy of the TLD system, the com-
plexity of the annealing procedure, the type of service, i.e. national or decentralised,
and the degree of automation.
The accuracy of dose measurement is significantly limited by the uniformity in
response within the group of detectors of the same type. The group of detectors should
have the same sensitivity according to the PTB requirements within a highest permissible
variation of 10%, according to Euratom with a 2a value of < 10%. Experimental results
of the variation in sensitivity within a detector group are presented in figure 10.1 for
different TL systems [9]. On the basis of calibration exposures individual calibration
factors can be applied to each dosemeter, for example, by an on-line computer in a fully
automated system.
10.3.2. Energy dependence
Since most of the TL detectors are not tissue-equivalent, the response of TL materials is
a function of photon energy. The energy dependence of the response depends on the
detector's thickness and encapsulation. The lowest dependence on energy was found for
Li
2
B
4
0
7
detectors (figure 10.2). The most commonly applied LiF:Mg,Ti is approxi-
mately tissue-equivalent, resulting in an over-estimation of + 40% for low-energy photons
in the 30 keV range and in an under-estimation of 40% for high-energy photons in the
172 E Piesch
"


3
: 1
6
7
' 5 ;
i \
! '
28
36
35
33
2U
17
15
12
8
7

3
1 0 VALUE OF 10 DETECTORS
11
TLD
ra RPL
jy
31
24
22~1
13
23
21
19
11
27
20
18
K
5
2
30
26
25
11
16
10
1
-hi .
Figure 10.1.
a batch.
Variation in sensitivity within
BATCH UNIFORMITY 0 VALUE IN !.
PHOTON ENERGV IN keV
Figure 10.2. Energy dependence of L iF:Mg,Ti and L i
2
B
4
0
7
: Mn.Si dosemeter systems
compared to the FD1 phosphate glass in the spherical capsule.
10MeV range. BeO detectors show an unexpectedly high overestimation of about
+ 60% at lOOkeV [19].
HighZ materials such as CaF
2
and CaS0
4
with an overestimation of about a factor of
12 at 50 keV are therefore used in personnel monitoring mainly as a supplement to nearly
tissueequivalent detectors in order to estimate radiation quality.
The relatively low directional dependence of the dose reading of tissueequivalent
detectors becomes worse, especially for lowenergy photons, if the detector is worn
inside a plastic encapsulation.
Additional changes in the energy dependence arise due to backscattering and
absorption of the radiation in the body of the wearer as shown in figure 10.3 for LiF.
A further description of the energy dependence is given in chapter 5.
10.3.3. Fading
According to Euratom's recommendations, the uncertainties introduced into the results
due to the application of corrections for instability of latent information (e.g. fading)
should not exceed 5% during the regular monitoring period. The fading characteristics
Application of TLD to personnel dosimetry 173
>-
2.0
> 1.0 -
t/>
LJ 0.5 -
CC 1/1
10
_L
LiF DOSIMETER
HARSHAW RIBBONS TLD 100
0.125'x 0.125"x 0.035
i
J_
' i
20
1000 50 100 200 500
QUANTUM ENERGY ( keV )
Figure 10.3. Energy dependence of the dosemeter reading of an L iF dosemeter irradiated in
free air (a) and on the front side of an Alderson human dummy (b), without secondary
electron equilibrium for 1.2 MeV.
of some TL materials are presented in table 10.4 and figure 10.4 as a function of storage
period. Most of the TL materials show a fading lower than 5% for monitoring periods up
to 3 months. No corrections are therefore necessary to fulfil the recommendation. A
preheating before evaluation may significantly reduce the fading for some TL materials
[6, 26] (see also chapter 11).
Table 10.4. Fading characteristics of some common thermoluminescent materials after
Eur 5358.
Thermoluminescent Thermal fadingf (25 C) Optical fadingt
material
L iF:Mg
L i
2
B<0
7
:Mn
CaF
2
:Mn
CaF
2
:Dy
CaS0
4
:Mn
CaSO:Dy
CaSO:Tm
BeO
A1
2
0
3
Very weak ~ 5% in 1 yr Weak
Weak ~ 10% in 2 months Weak
Average ~ 1% in 1 d
Weak ~ 13% in 1 month Strong
St r ong 50 85% in 3 d
Weak ~ 12% in 1 month Weak
Weak ~ 12% in 1 month Weak
Weak ~ 8 % in 3 months Strong
Very weak Strong
f These data are taken from the literature and should be regarded as
an indication of the magnitude of the effect. Fading can be minimised
by applying appropriate lowtemperature annealing procedures.
t Due to sunlight: at the present time information of a more specific
nature is not available.
10.3.4. Reproducibility and re-use
The reproducibility of a TL D system depends on the detector type, the zerodose reading,
the batch uniformity in response and zerodose reading, the readout technique and the
individual reader quality. Reproducibility curves of various TL D systems presented in
figure 10.5 result in a characteristic shape which decreases for low doses as a function of
exposure and reaches a constant value for higher doses. The standard deviation may vary
significantly for TL D systems in use [9, 28]. No significant difference has been found
174 E Piesch
STORAGE TEMPERATURE 25 C
LiF Mg.Ti
CaF
2
:Dy
CaS0< Dy TEFLON
Li ^O, Mn TEFLON
FADI NG OF TLD SYST EMS
PREHEATI NG TOO X j 20mm
Figure
10 100 1000
STORAGE PERIOD I N DAYS
10.4. Fading results of different TL materials for storage at 25 C.
100
o
5
Si
0.1
CnSIUm LiF Moji Li,BA:Mn LiF:Mg.Ti
0.1
LijB.O^Mn
:
CaS0
l
:Tm/(JoF2:Dy
! LiF:Mg;Ti
1
10
J
10' 10 10'
EXPOSURE IN mR
Figure 10.5. Reproducibility of dose measurement plotted against exposure for different
TLD systems [28]. Is value of 10 dosemeters.
between manual and automatic read-out systems. The relative standard deviation versus
exposure curve of TLD systems can be described by a two-parameter fit:
s = (l/D)(2s
2
u
Dl+s?y
/2
taking into account the actual exposure D, the zero-dose reading D
u
of unirradiated dose-
meters, the s values of the zero-dose reading (s
u
) and of the reference dose reading (s
T
).
For more details see 11.4.2 and [29].
For re-use of TL detectors the constancy and reproducibility of the dosimetric
properties is of general importance. As the response and the zero-dose reading often
change with the thermal and irradiation history of the detector the user can adopt one
of the following techniques:
(a) Prior to re-use, a special thermal treatment (pre-irradiation treatment) for each
detector is recommended from the manufacturer or can be found experimentally
by optimising the temperature-time characteristic of annealing to obtain repro-
ducible results. For LiF: Mg.Ti, for instance, an annealing at 400C/lh and
100C/3 his applied.
Application of TLD to personnel dosimetry
175
{b) External annealing procedure in an oven may be replaced by an extended thermal
treatment during or immediately after the read-out cycle. Here the detector is
measured once at, or slightly above, the maximum read-out temperature for a
period of some tens of seconds.
Automatic read-out systems mostly apply an internal annealing procedure in the
reader below 400 C. Detectors embedded in or covered with Teflon can be annealed
only up to 300C, resulting in a significant zero-dose reading after high pre-exposure.
Detectors previously exposed to high doses should therefore be separated from those
exposed to low doses only. This should be taken into account for TLD systems with fully
automatic read-out procedures where the detectors are mostly covered by Teflon foils.
The PTB requirements for TLD systems allow maximum variations in the response of
5% from the mean value of the batch, if the same detector has been exposed to a
reference dose and re-used 20 times. Experimental results of a test programme with
different TLD systems are presented in figure 10.6, showing the standard deviation of the
response for 10 dosemeters which have been exposed and re-used 10 times without recali-
bration of the reader [9].
6
2
1
20
36
26
21
21
19
12
6
3
35
33
17
6
7
32
31
29
11
11 TLD
r i RPL
27
9
7
5
3
2 < | B | | | | 25| |, e
REL STANDARD DEVIATION 1I a VALUE ) IN V.
Figure 10.6. Variation in response of TLD systems after 10 times of re-use.
10.3.5. Residual reading
In the milliroentgen dose range the zero-dose reading of TL detectors defines the lower
detection limit as well as the reproducibility of the dose readings. The dose readings of
unirradiated detectors are caused by:
(a) triboluminescence, visible and ultraviolet light stimulation;
(b) the infrared emission of the heating element;
(c) the dark current fluctuation of the PM tube;
(d) residual signals due to the annealing and irradiation history of the dosemeter.
If optimal annealing procedures are not applied, previous irradiations are mainly
responsible for an uncontrolled build-up or a time-dependent change of the residual
reading. Test procedures which normally apply a repeated programme of exposure and
read-out cannot correctly simulate the actual exposure conditions because the exposure
176 E Piesch
frequency and the dose received may vary significantly in practice. The residual reading
of an automatic system is presented in figure 10.7 for repeated exposures to doses of
250 mR and a standard annealing at 380C/lmin resulting in an increase of the residual
reading up to approximately 3 mR [10].
_ 2 -
as
t u
00 LU
9 o
00 r
LU X
Q- LU
' '
I
J I ' I I
STANDARD
ANNEALING j
380Cl mi n _^
i
100 200 500
I 2 5 10 20 50
EXPOSURE READING (CYCLE)
Figure 10.7. Residual dose per exposure as a function of exposure-reading cycles;
exposure for each cycle is at 250 mR [10].
the
The residual dose reading mainly depends on the TL material and the irradiation
history of the individual detector and has been found to be of the order of 0.03% up to
6% of the pre-exposure without taking into account the reader-dependent fraction of the
zero-dose reading (figure 10.8) [11].
8 I
Sio
:

10
U^O,-. Mn.Si
10 10" 10 10" 10'
GAMMA EXPOSURE IN R
Figure 10.8. Relative dose reading at second evaluation
After high exposure a second read-out of the dosemeter may be applied to re-assess
the dose. A uv photo-transfer technique was recently developed for the re-assessment of
the exposure in LiF [32] which results in an increase of the intrinsic response by a factor
of five. The uv re-estimation is independent of y or n radiation [33].
Application of TLD to personnel dosimetry 177
10.4. Personnel dosemeter systems!
10.4.1. General aspects
In mixed beta-gamma radiation fields, it is sufficient to estimate the dose equivalent to
the skin and the whole body [2]. To meet these requirements, such a dosemeter should
contain two tissue-equivalent TL elements with different shieldings, for instance, covered
by a tissue-equivalent material of about 7 mg cm"
2
and 500 or 1000 mg cm"
2
, respec-
tively. In most cases, it is known that the major part of the dose received will always be
due to penetrating radiation (x-rays, 7-rays) or to non-penetrating radiation (low-energy
7-rays or x-rays), so it may be sufficient to use a basic dosemeter containing only a single
tissue-equivalent TL element. In practice, however, the response curves of LiF and
Li
2
B
4
0
7
are only approximately tissue-equivalent, as can be seen in figure 10.2 [5].
The discriminating basic dosemeter recommended by Euratom should provide
additional information on the radiation quality and, if possible, an indication as to
whether the dose has been received predominantly from in front of or behind the wearer.
TLD does not lend itself to the provision of information on the radiation field. Informa-
tion on the quality of photons can be obtained in the energy range 10-200 keV by using
special techniques and additional dosemeters, for example:
(a) at least two elements and a filter system similar to the film badge design which,
however, would lead to a marked angular response; or
(b) two different TL materials, one tissue-equivalent and one with a high-energy
response characteristic, for instance LiF and CaS0
4
.
10.4.2. Practical dosemeter systems
After early applications in nuclear research centres and at nuclear power reactor stations,
mainly in the United States, and also until now centralised services in Austria, Denmark,
Sweden, the Netherlands and recently in France, the United Kingdom, Germany and Fin-
land automatic read-out systems in personnel monitoring are already being used or are in
preparation [23, 24, 30]. On the other hand, a number of smaller monitoring services
with some thousands of dosemeter evaluations per month are still using non-automatic
instruments, besides personnel monitoring mainly for application in extremity and
environmental dosimetry.
The most important aspect for the large-scale use of TLD systems in personnel
monitoring is the application of an automatic TLD system. The main properties of some
automatic readers are presented in table 10.5. The different automatic read-out systems
now commercially available make use of multi-element dosemeters with two, three or
four detectors or detector fields within a badge with at least one unfiltered detector
(detection of skin dose) and one filtered (detection of whole body dose).
Some of these systems are mentioned in chapter 3 together with the types of personal
dosemeters used with them. Figure 10.9(a)-(e) shows five commercially available personal
dosemeter badges. Figure 10.9(/) shows some multi-element dosemeter cards produced
by Harshaw, figure 10.9(g) the multi-element dosemeter cards produced by the Institute
of Radiation Protection, Helsinki, and figure 10.9(h) the multi-element badge of National
Panasonic.
t See also 3.5.2.
178
E Piesch
Table 10.5. Properties of automatic TLD readers [12].
Heating principle
Detector
Number of detectors
Reading (s)/detector
Badges per hour
Working days for
10 000 badges
Harshaw
2271
Hot finger
LiF: Mg, Ti
chip
2
35
100
12
National
UD510
Hot air
BeO: Na thin layer
CaS0
4
: Tm glass
capillary
3
33
110
11
Studsvik
1313A
Hot nitrogen
Li
2
B
4
0, :
disc
4
40
90
14
Mn, Si
Teledyne
9100
Hot element
LiF : Mg.Ti
Teflon matrix
4
47
75
16
French
CEA
Hot plate
LiF: Na, Mg
disc
4
8
450
3
The TLD detectors used in the multi-element dosemeters for automatic read-out are:
(a) LiF : Mg,Ti or CaF
2
: Dy chips covered on both sides by Teflon foils inside the
dosemeter card produced by Harshaw (figure 10.9(f));
(b) LiF: Mg,Ti and Li
2
B
4
0
7
: Mn,Si chips not fixed and movable inside the holder,
made by Studsvik (figure 10.9(A));
(c) LiF and CaS0
4
embedded in Teflon (Teledyne Isotopes) and sealed in a black
plastic foil to avoid light exposure and contamination (figure 10.9(c));
(d) U2B4O7: Cu,Ag and CaS0
4
:Tm in a layer of about 20 mg cm
-2
cemented on a
plastic foil and coated on both sides by thin foils of 10 mg cm
-2
inside the dose-
meter card of National Panasonic (figure 10.9(h)).
Instead of Teflon protection foils two Teflon rings are also used from both sides to
fit the rectangular chips on the edges inside the dosemeter card [31] (figure 10.9(f)).
Because of the interest in automatic read-out instruments, results of a standard test
programme are presented in table 10.6 for seven TLD systems using automatic evaluation
[9]. By definition, the dose at the lower detection limit D
m
was found experimentally
as the 3 a value of the zero-dose reading of unexposed dosemeters. The long-term
variation of the dark current of the zero-dose reading and of the results for repeated
exposures to lOOD^ were investigated over a monitoring period of 10 d. The reproduci-
bility of representative TLD systems is presented in figure 10.5 as a function of exposure.
The s values are high for low doses caused by the a
u
value of the system but decrease
with increasing dose and result in a constant value for doses above 100Z>i
d
i- For a longer
period or other systems the reproducibility may vary (figure 10.10) depending on the
quality of the detector batch, of the individual reader and the read-out technique applied
[29]. This is demonstrated in figure 10.11 taking TLD 700 and TLD 600 systems as examples.
On the basis of experimental standard deviation versus dose curves the different error
sources of TLD systems can be interpreted qualitatively. The reproducibility of dose
reading is improved in the low dose range by using a quick, instead of a slow, read-out
technique for peak no 5 + 6 (factor 2.6) or only an evaluation of peak no 5 instead of
peak no 5 +6 (factor 2). On the other hand, higher s(D) values have been found for new
TLD 700 batches compared to old ones manufactured in 1974 (a factor of 2.5 for low
Application of TLD to personnel dosimetry
179
ia)
Si
(e)
E5780Q9t
n
115148780267 |
150780866
(?)
(/O
Figure 10.9. (a) Thermoluminescence dosemeter of the Austrian Atomic Energy Research Organization
Ltd. (b) Studsvik TL dosemeter type 6541A. (c) TLD badge developed and used by the Swiss Public
Health Department, Section of Radiation Protection (Swissbadge). Detector: Teledyne Isotopes Radi-
Guard multi-area dosemeter. (d) Nuclear station badge produced and distributed by R S Landauer Jr &
Co, Division of Technical Operations, Inc (by courtesy of R S Landauer Jr & Co), (e) TLD badge with
coded insert designed by the National Radiological Protection Board (NRPB) Harwell with plastic
dome-shaped filter (700 mg cm
- 2
), produced by D A Pitman Ltd (courtesy of D A Pitman Ltd).
(/) Harshaw multi-element TLD cards, a Two-element card with binary code decimal (BCD)
identification (see also figure 9(c)). b Three- and four-element cards with bar code (Codabar ). Left
card used with Model 2276 microprocessor-controlled TL dosimetry system. Right card used with
Model 2271L automated TLD system, (g) Multi-element TLD cards without protection layers, pro-
duced by the Institute of Radiation Protection, Helsinki. (/;) National Panasonic composite TL
dosemeter.
180 E Piesch
Table 10.6. Performance of automatic TLD read-out systems.
Reader type Harshaw 2271 National UD 510 Studsvik 1313A
TLdetector TLD 100 TLD 100 Li
2
B
4
0
7
: Ag,Cu CaSO:Tm TLD 700 Li
2
B
4
0, :Mn, Si
Annealing No No Internal Internal No No
TL D 2 0 0
400 C
1.5 h
Z>ldi (mR)t 1.2
Dark current:):
a
0
(mR) 0.7
o(%) 26
Zero dose %
a
u
(mR)
o (%)
Reproduci-
bility
l a value (%)
lOODidi 1.7
30 mR 3.9
0.9
1.3
2
2.6
40.5
7.9
6.3
5
2
62.5
4
44.2
2.6
16.8
2
-
-
3
14.6
1.1
3.0
2.0
0.55
8.1
2.4
24.5
1.3
4.1
1.2
3.5
6.5
1.8
29.3
1.3
2.3
0.08
0.06
8
0.1
23
2.2
1.3
t Z>idl dose at the lower detection limit equal to 3 a value of zero dose a
u
of unirradiated dosemeters.
$ Long-term stability during 10 d, variation of mean value for 10 readings per day.
doses), between TLD 700 and TLD 600 (a factor of 5 for low doses) as well as after
annealing 60 times at 400 C (a factor of 3 for high doses).
The application of automatic TLD systems in personnel monitoring requires micro-
computer control of the automatic read-out functions and the data processing and
recording. This technique is described in detail by Duftschmid [35] for an automatic
computerised TLD personal monitoring service.
The properties of different commercial TLD systems were discussed under the aspect
of data security and service availability with respect to a large-scale or a decentralised
monitoring service [12, 39]. Laboratories with large-scale TLD monitoring also apply an
individual calibration of each chip and the loss of dosemeters has been found to be of
the order of 2% yr"
1
[39]. As a supplement of the performance test of TLD systems by
means of the standard test programme [9] the report of an inquiry about the experience
with read-out systems [36] discusses the reliability of the reader, mechanical, electronic
and automatic dosemeter identification as well as the malfunctions and service experience
of 38 different read-out systems in 24 different laboratories. Compared to readers with
manual evaluation, additional malfunctions have been found from the automatic trans-
port of the dosemeter card. But there are more administrative and economic reasons, as
well as the lack of international recommendations for the layout of detectors or reading
equipment, which are responsible for the fact that the application of TLD systems as a
film replacement will come somewhat later than expected some years ago [13].
Application of TLD to personnel dosimetry 181
BATCH
TLD 6 0 0 ^
FACTOR 5
QUALITY IN ZERO DOSE
READING
TLD 7 00
. x^
a
10 10 10
EXPOSURE IN mR
100
10
1
\
FA
READ-OUT TECHNIQUE
>v TLD 700
\ \ P E A K No 5.6
PEAK N o s \ ^ ^ N .
CTOR 5 b
Vf 10
3
EXPOSURE IN mR
(a) (b)
ANNEALING
\
FACTOR 3
HISTORY
TLD 7 00
ANNEAL 6 0 -
d
(c)
EXPOSURE IN mR
(d)
BATCH UNIFORMITY IN
RESPONSE
10' 10'
EXPOSURE IN mR
Figure 10.10. Reproducibility of TLD 600 and TLD 700 dosemeters as a function of exposure repre-
senting the following error parameters: (a) batch quality in zero-dose reading, (b) read-out technique,
(c) annealing history, (d) batch uniformity in response.
w 10-

t
2
7
5

2
1
29
20
15
10
7
6
3
6
36
35
26
17
12
8
1
f1 TLD
T^\ RPL
3
33
32
19
11
5
28
24
9 27 1 18 1 16 | 25 1
REL.STANDARD DEVIATION ( 2o VALUE ) IN V.
Figure 10.11. Frequency distribution of reproducibility for different TLD and RPL systems
exposed to 100 times the lowest detectable dose D\$\. Number of system according to the
standard test programme [9].
182
E Piesch
10.5. Special applications
10.5.1. ^-radiation and extremity dosimetry
High-energy /3-rays may contribute significantly to the depth dose in tissue. In such
/3-radiation fields it is therefore recommended to measure both skin dose and whole body
dose by using two separate tissue-equivalent dosemeters. For |3 energies below 1 MeV the
response changes significantly with the energy distribution dependent upon the thickness
of detector and shielding. For the dose measurement of non-penetrating radiation, ideally
the skin dose should be measured with a tissue-equivalent detector of 5 mg cm"
2
thickness covered by a layer of tissue-equivalent material 5 mg cm"
2
thick. Usually some-
what thicker detectors are used which under-estimate the dose of low-energy /3-rays by
up to 50%. For a detector with an actual thickness of about 150 mg cm"
2
or 200 mg cm"
2
,
the energy threshold achieved in practice is about 0.6 MeV or 0.8 MeV (figure 10.12).
100
50
M
o
a.
if)
UJ
t r
_ i
i
?n
10
b
d
c
I I I I
Al DISC
76 mm )
m )
CaF
2
: Mn CHIP ( 0.75mm)
CaF
2
: Mn ROD ( 1 mm)
_i J i i l _
200 500 1000 2000
MAXIMUM BETA RAY ENERGY ( keV )
Figure 10.12. Sensitivity to beta radiation [15].
5000
To improve the sensitivity for low-energy 0-ray emitters, different techniques have
been adopted:
(a) a thinner detector as well as a 'window' is more suitable;
(b) non-transparent detectors are suitable to discriminate the TL light output from the
surface and deeper layers;
(c) a multi-element dosemeter may provide information on j3- or 7-ray energy so that
corrections for self-absorption can be applied.
Thin UF-Teflon detectors of 0.2-0.02 mm thickness show high j3 sensitivity but are
expensive, fragile and difficult to incorporate in a dosemeter. For non-transparent
graphite-mixed l i F and JJ2B4O7 investigated at Riso [16], the energy threshold of 0-rays
was found to be in the range of 0.2 MeV for detectors having a content of 5-10%
Application of TLD to personnel dosimetry 183
LIF WITH AND WITHOUT GRAPHITE ^^/f
_
10V. /
ov.
/ /
/ /'
* //
//,
y^s//f
> < / / / /
's //'
^ ///
/'/
/ O
7
.
FRONT SIDE
BACK SIDE
'
L12B4O7 Mn WITH AND WITHOUT
GRAPHITE
0.02 0 05 0.1 0.2 0.5 1.0
AVERAGE BETA ENERGY ( MeV)
D.02 0.05 01 02 05
AVERAGE BETA ENERGY (MeV)
(a) (b)
Figure 10.13. (a) Energy response curves of LiF dosemeters with 0, 5, 10 and 15% content of
graphite exposed to beta irradiation [16]. (b) Energy response curves of Li
2
Bj0
7
:Mn dosemeters with
0, 0.5, 1, 2, 4 and 8% content of graphite exposed to beta irradiation [16].
graphite (figure 10.13). Similar TLD 100 Harshaw chips containing graphite show a
response of the order of 30% for
204
T1 ("
max
= 0.23 MeV), a sensitvity of 0.2 compared
to transparent LiF and a zero dose of the order of 0.1 R.
A new approach at the Berkeley Nuclear Laboratories uses ultra-thin bonded discs
(U T B) composed of 6 mgem"
2
(U T ) LiF-Teflon or CaS0
4
:Dy-Teflon discs which have
been thermally bonded to thick Teflon bases [17]. A limitation of UTB is their light
sensitivity which gives rise to a high zero dose of 500 mR. Thin CaS0
4
:D y layers of
about lOmgcm"
2
fixed to an aluminium disc also show a high /3-sensitivity up to
0.2 MeV (figure 10.14) [15]. For application in mixed /3-y fields a three-element dose-
200 500 1000 2000 5000
MAXIMUM BETA RAY ENERGY (KeV)
cc
E
cc
UJ
Q.
U J
in
z
2
1/1
U J
cc
(b)
.
- . Ca S0
4
-^K
. I
-
Dy
,JS
^ o L i F ( l )
^ ^ 0 ^ _ c v
- J
-
" "
V /
^ <^ . Li F( 1) / Li F( 2)
, ,i i rTTT-rrn-o
- - 08
50 100 500 1000
EFFECTIVE PHOTON ENERGY ( k e V )
cc
E
en
UJ
a.
UJ
i/>
z
o
D.
I/)
UJ
0.4 cc
1.6
1.2
(a)
Figure 10.14. Beta (a) and gamma (b) sensitivity of the three-element finger ring dosemeter
[15] which consists of an entrance window ( l mgc m
- 1
) and a thin CaS0
4
: D y detector
(~10 mg cm"
2
) on an Al disc behind the window. Behind an additional Al shield (1.5 mm)
and a Pb shield (0.5 mm) two detector elements LiF (1) and LiF (2), respectively, are
applied to correct for energy dependence of photons.
meter uses the CaS0
4
detector on the top (skin dose) and two different shielded LiF
elements below the skin dosemeter. If low-energy gamma radiation is excluded, the dose-
meter is suitable for simultaneous measurement of beta and gamma doses.
184 E Piesch
The new dosemeter from National uses a Li
2
B
4
0
7
: Ag,Cu layer of 20mgcnf
2
coated
on both sides by thin foils of about 10 mg cm"
2
and is heated by an ultra-red lamp. The
detector element represents an optimum arrangement with respect to tissue equivalence
and dose measurement of low-energy /3-rays and photons [25].
The sensitivity to /3-rays may be increased by using a window of 1 mg cm
-2
in front of
the TL detector [38] or a boron-diffused surface layer in UF [37] which creates a new
glow peak, also resulting in a better discrimination of photons.
Tissue-equivalent layers in front of a TLD 700 dosemeter of 0.9 mm thickness change
the 0-ray response significantly as can be seen in figure 10.15 for different (3-ray emitters.
The ratio between skin dose (7 mg cm
-2
) and depth dose (500mgcirT
2
) is dependent
upon the /3-ray energy and the contribution of photons and in practice has been found to
be about 3 for
106
Ru or up to a factor of 30 in mixed fi-y fields.
In personnel monitoring the measurement of skin dose is required above all for
extremity dosimetry. For the purpose of measuring finger and hand doses different kinds
of dosemeters have been developed which use IiF-Teflon discs in a black light-proof
polyethylene pouch (figures 10.16(a) and (b)) or LiF, Li
2
B
4
0
7
or BeO chips up to 0.9 mm
thickness inside a steel ring, plastic ring or a bracelet with 'windows' in optimal cases of
1-7 mgcnT
2
thickness (figures 10.16(c) and (d)). A new design of a finger ring and/or
bracelet dosemeter (figure 10.16(e)) is applicable for semi-automatic handling and
reading [40].
Because of the difference in the maximum permissible dose values for skin dose
(30 rem yr
_1
) and depth dose (5 rem yr"
1
) the measurement of skin dose is required only
in ]3-radiation fields or in mixed (3-y radiation fields if a ratio of//(skin)///(depth) > 1 is
expected.
BETA DOSE READING VS. TISSUE D EPTH
TLD 700/0.9mm thick
R/rd tor 7 mg/ cm
2
, 06
Ru 1.0
Sr/
9
Y 0.92
"Tl
"Pm
0.2
"0.02
I 10 100 1000
ABSORBER IN mg / cm
2
Figure 10.15. Beta dose reading of a 0.9 mm thick TLD 700 detector as a function of
shielding.
10.5.2. Low-energy photons
The under-estimation of low-energy photons below 20 keV is dependent upon the thick-
ness and shape of the detector and the self-absorption in the dosemeter badge which may
Application of TLD to personnel dosimetry
185
(c) (d)
()
Figure 10.16. (a) Teledyne Isotopes TL finger and hand dosemeter. The dosemeter consists of an
LiF-Teflon disc in a light-proof (black) polyethylene pouch adhered to a band-aid type tape, (b) Tele-
dyne Isotopes finger and hand dosemeter applied for assessment of the dose to the finger basal layer,
(c) Examples of TL finger ring dosemeters. a Ring developed by the Gesellschaft fur Strahlen- und
Umweltforschung Miinchen mbH and produced by the Physikalische Werksta'tten Dr Pychlau KG,
Freiburg. This ring uses two LiF micro-rods (1 mm dia X 6 mm), one in a Cu filter screw for p and j
discrimination and photon energy estimation, b Ring produced by Heist KG, Germany, allows TL
phosphor discs and chips to be inserted. Mechanical attachment to the ring and protection is achieved
by means of shrink foils, (d) TNO TLD badge (by courtesy of Dr H W Julius), (e) TLD extremity
dosemeter developed by H W Julius (TNO) and G Busuoli (CNEN) (by courtesy of Dr H W Julius).
186 E Piesch
be improved significantly by using thin detectors (see 10.5.1). The type approval draft
of the PTB recommends three different energy ranges and a maximum error of 30% for
the energy dependence and also for low-energy photons (see table 10.2).
The dose reading of l i F is not exactly tissue-equivalent for photons in the x-ray
energy range of lOkeV (see figure 10.2). The over-estimation of about 40% at about
30 keV may be reduced by an adequate filter which, however, causes an under-estimation
of low-energy photons in the energy range of 10-20 keV. The energy dependence of LiF
is the main limiting factor for the overall uncertainty of dose measurements in the lower
energy range and may be changed by applying a suitable filter in front of the detector
(figure 10.17).
IJ2B4O7 is a TL material with the best tissue equivalence, showing, however, the same
disadvantages of self-absorption if no thin detector elements are applied. The energy
dependence of BeO, on the other hand, results in an over-response of 75% in the energy
range of 100 keV [19]. TL materials with a high effective atomic number Z are not
recommended for the low-energy range.
1
V
LiF TLD-100 RibbonsTNObadge
Response relative to
60
Co( tin)
i
/ A/ / / / y^x
I I /s/ / / / / '
0PEN WIND0W
/ i l l / / / /
2 1 0 m m
PLASTIC
/ / / / 6 / / / /
J
1 Smm ALUMINIUM
/ / / / I n / I / I 2 Omm ALUMINIUM
/ / / / I '/ I f S 0.1mm COPPER
/ / / / / 1 / '
s

I mm c
O
p p
E
R
If/ / / / / 7. O.Jmm COPPER
/ / / / / a / / ' '
0 m m T I N
1 // // jf /
8 10mm TIN
, ^r * * ^ . 1 , 1
- C.5
5 10 2 5 100 2 5 1000 2
Eef f lkeV)
Figure 10.17. Energy response curve for LiF TLD 100 chips (Harshaw: 1/8X1/8X0.035 in
3
)
in the TNO badge, covered by various filters [14].
10.5.3. High-energy photons
The response of TL detectors decreases with photon energies higher than 1 MeV, resulting
in an under-estimation of the dose reading which is dependent on the thickness and shape
of the detector and above all on the thickness of the badge shielding.
At reactor sites, for example, 6 MeV 7-rays occur due to the reaction
, 6
0(n, 7)
17
N
in the water used for neutron moderation and core cooling. In table 10.7 results of a
9 MeV calibration of different TL detectors are presented [18]. According to the detector
thickness, LiF and ^ B ^ v chips show a relative response of 0.24-0.63 compared to that
at 1.3 MeV. A better response of 0.78 was found for bulb dosemeters and 1.12 for
CaF
2
:Dy in the perforated tin sphere. As can be seen from the depth dose results in
figure 10.18, the application of a tissue-equivalent filter with a thickness of 3 mg cm"
2
or
Application of TLD to personnel dosimetry 187
Table 10.7. Relative response of dosemeters to 9 MeV photons.
Detector
Manufacturer Shielding (mg cm
2
) Relative
response]
-
LiF: Mg, Ti
in Teflon 6 mm dia X 0.4 mm Teledyne Isotopes
TLD 700 ribbons 3 X3 X 0.9 mm
3
Harshaw
TLD 700 bulb Harshaw
CaF
2
:Dy
TLD 200 ribbons 3 x 3 X 0.9 mm
3
Harshaw
Phosphate glass
8X8X4. 7mm
3
Ionisation chamber
PHY-SEQ 6
LB 14862
Schott u. Gen.
7
7
500
0.27
0.40
0.57
0.78
7 0.37
Perforated tin sphere 1.12
7 0.72
Perforated tin sphere 1.28
La Physiotechnie Pocket dosemeter 0.58
Berthold Pocket dosemeter 0.74
f Response per rad at 9 MeV corresponding to the maximum value at 3 g cm
2
tissue depth
compared to the response at 1.2 MeV.
100 -
O
<
if)
O
Q
I d
CC
50

-
-
-
* ' v PHOSPHATE GLASS DOS. 2\ IN GLASS
/ A PHOSPHATE GLASS DOS. 8J 8 x 8xA.7mm3
/ L i F: Mg, Ti 1
o IONIZATION CHAMBER J
I N P H A N T 0 M
, i . i , i , i ,
Figure 10.
measured
1 2 3 U
DEPTH IN PHANTOM OR GLASS IN g/ cm
2
.18. Comparison of depth dose distribution for 9 MeV photons in beam direction
in the phantom and in a single block of phosphate glass.
Al filter of 1 cm is sufficient for a correct dose reading of tissue-equivalent detectors. In
the high proton energy range non-tissue-equivalent detector material or filters may also
be applied.
10.5.4. High dose range
In the high dose range (see also chapter 17) most of the TL materials show non-linearity
in the dose reading versus exposure curve. Supralinearity of the dose reading starts at
doses of about 100 R and the response at the maximum varies between 1.6 and 3.8
compared to that at 10 R for the TL phosphors investigated (table 10.8). Due to damage
188
E Piesch
Table 10.8. Highdose properties of TL D materials [20].
Detector type Starting Supra Relative Radiation Residual dose (R)
point (R) linearity response damage
exposure at at 100 R 1000 R
maximum maximum
(R)
7
L iF:Mg,Ti
TLD7 0 0
7
L iF: Na, Mg
PTL717
L i
2
B
4
0
7
:Mn,Si
pellets
L i
2
B
4
0
7
:Mn
TLD8 0 0
CaSO:Tm
UD100 MG
CaSO:Dy
Teflon
CaF
2
:Mn
Teflon
CaF
3
:Dy
TLD2 0 0
100
100
200
2X10
3
200
100
200
200
5X10
4
3X10"
10
5
4X10"
5X10
4
5X10"
5X10"
5X10"
3.83
3.52
3.76
2.08
3.58
3.06
1.6
2.62
2X10
3
R
2X10
3
R
No
Damage
Sensitisation

No damage
1
0.03
0.036
2.2
0.6
2.2
6.0
4.8
17
0.3
0.25
2.3
12
44
95
65
effects, mainly LiF shows a reduction in sensitivity after exposures to doses of more than
1000 R (figure 10.19) [20]. The residual dose reading which is found directly after the
evaluation of preexposed dosemeters was found to be proportional to the preexposure
dependent upon the annealing treatment and the irradiation history of the detector (see
10.3.3). Annealing procedures before reuse are necessary to anneal the residual dose
reading. If no external preirradiation annealing can be applied, as for LiF in Teflon or
CaSC. :Tm
Li,B,0,:Mn.Si
* Li,BiCVMn
CaFjtDy . -
Li F:Mg. Ti ~
LiF:Na.Mg _ .
GAMMA PRE-EXPOSURE IN R
Figure 10.19. Change in response after preexposure.
Application of TLD to personnel dosimetry
189
chips packaged in Teflon cards for automatic read-out, a selection and exchange of highly
exposed dosemeters is recommended to avoid measurement errors in the low dose range
(see also 10.3.3).
10.5.5. Neutrons^
In the presence of neutrons it may be necessary to correct the gamma dose results for the
sensitivity of the detector to neutrons. The thermal neutron response depends upon the
thickness and isotopic content of the nuclides and the encapsulation within the badge.
The response to intermediate neutrons is lower by several orders of magnitude.
However, due to the effect of back-scattered neutrons, the detector worn on a body
will receive twice the radiation for incident thermal neutrons and still some percentage
for incident fast neutrons (albedo factor 0.8 for thermal and 0.1 for 1 MeV neutrons).
The response to thermal neutrons therefore only gives a rough indication for the correc-
tion of neutron sensitivity.
Because of the high thermal-neutron sensitivity of LiF, it is recommended to use
TLD 700 detectors for the dose measurement of photons in mixed radiation fields. In
practice, a glow-curve analysis may be helpful in detecting any contribution from thermal
neutrons if no additional neutron detector has been used. In the low dose range below
10 rem, the peak height ratio P
2
/Pi found for photons (0.04) and neutrons (0.4) differs
by a factor of about 10 (figure 10.20) [20].
GAMMA EXPOSURE IN R
GAMMA EQUIVALENT NEUTRON EXPOSURE IN R
Figure 10.20. Peak height ratio P
2
/P
t
for LiF. (a) y exposure (TLD 600 and 700),
(b) neutron exposure (for TLD 600 only).
An albedo neutron dosemeter uses a cadmium or boron shield facing the source to
eliminate incident thermal neutrons and to yield a dosemeter response which is mainly
caused by thermal neutrons back-scattered from the body. Commercially available dose-
f This topic is treated in more detail in chapter 12.
190 E Piesch
NEUTRON ENERGY IN eV
Figure 10.21. Response of the Karlsruhe single-sphere albedo dosemeter | 221
<=3 BORON LOADED PLASTICS
CD PLASTICS
LiF- DETECTOR
(c)
Figure 10.22. (a) Constructional details of the Karlsruhe albedo neutron dosemeter.
(b) Close-up view of the Karlsruhe albedo dosemeter (courtesy of Heist KG), (c) Karlsruhe
albedo dosemeter belt (courtesy of Heist KG).
Application of TLD to personnel dosimetry
191
meter types developed by Harvey et al [47], Hankins [41], Hoy [42], Piesch and
Burgkhardt [21] and Brunskill and Way Wang [43] are presented in detail in chapter 12.
The main properties of albedo dosimetry are the neutron detection without any energy
threshold and, on the other hand, a significant decrease in response above 10 keV, as can
be seen for the Karlsruhe albedo dosemeter in figure 10.21 [22], constructional details
of which are presented in figure 10.22(a) and a close-up view in figure 10.22(A). Figure
10.22(c) shows the same dosemeter on a belt.
Albedo neutron dosemeters of the discriminating analyser type use two or three
different
6
LiF/
7
liF detectors which are positioned, for example, inside a boron-loaded
plastic badge in such a way that incident thermal neutrons (detector a) or incident/back-
scattered intermediate neutrons (detector m) can be indicated separately from the albedo
reading (detector i) in order to correct over-sensitivity to thermal and intermediate
neutron leakage. The application of two albedo dosemeters with a dosemeter belt results
in an approximately directional independence of the dose reading.
In neutron monitoring today the application of albedo dosemeters is based on field
calibrations in the environment of each neutron facility which may be performed, for
instance, by using the rem meter (figure 10.21) with the TLD detector c in the centre as
a phantom for two albedo dosemeters. Figure 10.23 shows examples for field calibrations
at the Heidelberg Compact Cyclotron and at the Karlsruhe Research Reactor FR2. The
effective response /?
e
ff(i) of the albedo dosemeter presented as a function of the reading
ratio i/a may vary by one order of magnitude around one facility caused by local changes
of the thermal radiation and/or the moderation of fast neutrons. The calibration curve
allows the correction of energy dependence for each individual dosemeter reading in
personnel monitoring [44]. The evaluation technique applied in routine monitoring
allows the interpretation of neutron stray radiation fields by the direct use of the graph
presented in figure 10.23 for two neutron facilities, for example, or an on-line computer
FIEL D
CALIBRATION
REL NEUTRON DOSE EQUIVALENT RATIO Hy, / Hn IN 7 .
100 20 10 5 2 1 &5 01
CORRECTION OF THE
LOCAL CHANGE IN
0 1 L THE NEUTRON SPECTRUM
DETECTOR REAOINC RATIO a h l / a ( a )
Figure 10.23. Response of the Karlsruhe albedo dosemeter as a function of reading ratio
i/a on the basis of field calibrations [44].
192 EPiesch
program for data processing and recording to interpret neutron stray radiation fields
in terms of neutron dose equivalent separated for the energy groups 0.4 eV, 0.4eV-10keV
and lOkeV-lOMeV and "
eff
for fast neutrons [22]. In contrast to the multi-sphere
technique the single-sphere albedo technique offers the advantages of a similar field
analysis and the direct measurement of the actual albedo dosemeter response at the
location of interest. This standard technique has been applied for field analysis at
different linear accelerators, neutron therapy facilities, research and power reactors [45].
*
10.5.6. Accident dosimetry
The extended dose range of TL dosemeters applied in routine personnel monitoring also
makes it possible to fulfil the requirements for an accident dosemeter. In the high dose
range the following properties of TL detectors should be taken into account:
(a) after irradiation to high doses the supralinearity above 100 R should be corrected;
(b) after the first read-out the residual dose reading may be used for a second dose
evaluation;
(c) the glow-curve analysis gives information about the contribution of other types of
radiation, above all neutrons;
(d) after high neutron exposure of LiF the intrinsic effect of the neutron-induced
tritium content results in a storage time-dependent increase of the zero-dose
reading which, in addition to the first read-out, may be used to separate photon
and neutron exposures and to estimate the exposure to thermal neutrons [48].
In mixed gamma-neutron radiation fields the gamma dosemeter reading has to be
corrected with respect to the neutron sensitivity of the dosemeter in the neutron energy
range for
t
h, n-
t
and f. The application of albedo dosemeters is limited because a simple
albedo detector does not give information about neutron dose and because of the
relatively high neutron sensitivity. For a moderated fission spectrum linearity is expected
up to a dose equivalent of about 300 rem. Higher neutron exposures result in a gamma-
equivalent dose reading of more than 1000 R and thus in radiation damage of the
detector response. In accident dosimetry albedo dosemeters of the analyser type like the
Karlsruhe albedo dosemeter give sufficient results for the gamma and neutron dose, an
interpretation of the neutron spectrum and the orientation of the person in the radiation
field.
10.6. Future trends
Although most of the users are interested in the application of automatic TLD read-out
systems in personnel monitoring, there is obviously a discrepancy between the properties
of commercial TLD systems and the requirements of highly centralised large-scale
monitoring services. Future improvements of commercial equipment are necessary to
reduce the malfunction rate of the read-out and to perfect the data security, the
availability of tissue-equivalent TLD materials and the service situation.
In personnel monitoring the following future trends can be seen:
(a) because of data storage and service, smaller monitoring services rather than
centralised ones will apply automatic read-out systems;
Application of TLD to personnel dosimetry 193
(b) automatic read-out systems will also be applied for use with extremity dosemeters
and albedo neutron dosemeters;
(c) thin detectors will be produced which will be suitable for 0 and extremity
dosimetry.
The dose reading of tissue-equivalent detectors is practically independent of the
direction of the incident radiation, at least for photon energies above 30 keV. TLD,
however, does not lend itself to information about the radiation quality and the direction
of the incident radiation. For the estimation of radiation quality, two detectors with
different energy responses must be applied. The dose reading ratio of the detector behind
the window and the filtered detector only gives rough information on the radiation
quality, depending on the homogeneity of the radiation field. The accuracy of dose
reading is not only based on the properties of the TLD system adopted but also on the
carefully applied technique of handling, evaluation and annealing treatment. Workshops
or standard test programmes may serve to establish high accuracy in the laboratory and
may stimulate improvements in the read-out cycle.
References
1 1970 Protection against ionizing radiation from external sources ICRPPubl. 15
2 1975 Technical recommendations for monitoring the exposure of individuals to external radiation
CECRep. EUR5287e
3 1975 Technical recommendations for the use of thermoluminescence for dosimetry in individual
monitoring for photons and electrons from external sources CEC Rep. EUR 5358e
4 Nichols L L 1977 A test for the performance of personnel dosimeters Rep. BNWL - 2159
5 Christensen P 1971 Li
2
B
4
0
7
and LiF TL dosimeter for routine personnel monitoring Proc. IAEA
Symp. on Advances in Physics and Biological Radiation Detection plOl
6 Burgkhardt B, Herrera R and Piesch E 1977 Long-term fading experiment with different TLD
systems Proc. 5th Int. Conf. on Luminescence Dosimetry, Sao Paulo, February (I Physikalisches
Institut, Universitat Giessen), p75
7 Nink R and KosM-11980 An improved LiF material for thermoluminescence dosimetry J. Physique
to be published
8 Hahn D and Nink R 1977 Situation and development of solid state dosimetry, from the PTB-point
of view Proc. 5th Int. Conf. on Luminescence Dosimetry, Sao Paulo, February (I Physikalisches
Institut, Universitat Giessen), pl 75
9 Piesch E and Burgkhardt B 1978 RTL Systeme im Bereich kleiner Dosen: Vorstellung eines Test-
programmes und Ergebnisse an 39 Systemen Rep. Fachverband fur Strahlenschutz FS-78-17 AKD
or KfK-2626
10 Miyagawa K et al 1977 An access control system using TLD for radiation monitoring in atomic
power plant Proc. 5th Int. Conf. on Luminescence Dosimetry, Sao Paulo, February (I Physikalisches
Institut, Universitat Giessen), p281
11 Piesch E, Burgkhardt B and Singh D 1977 Properties of TL dosimeters after high gamma irradiation
Proc. 5th Int. Conf. on Luminescence Dosimetry, Sao Paulo, February (I Physikalishes Institut,
Universitat Giessen), p94
12 Regulla D F and Drexler G 1977 Results and discussion of laboratory experiences with different
automated TLD readers for personnel monitoring Proc. 5th Int. Conf. on Luminescence Dosimetry,
Sao Paulo, February (I Physikalisches Institut, Universitat Giessen), p262
13 Becker K 1976 Status and trends in personnel monitoring a worldwide survey Kerntechnik 18
345
14 Julius H W 1976 Introduction of an automated TLD personnel monitoring system and centralized
dose record keeping in the Netherlands Proc. 9th Jahrestagung Fachverband fur Strahlenschutz,
Alpbach Fs-75-12-T, pi 25
194 EPiesch
15 Benco L et al 1977 Thermoluminescent beta dosimetry for routine personnel monitoring Proc.
IRPA Congr., Paris vol 4, pi 261
16 Koczinsky A et al 1974 Graphite-mixed non-transparent LiF and Li
;
B
4
0
7
: Mn TL dosimeters com-
bined with a two side reading system for beta-gamma dosimetry Proc. 4th Int. Conf. on Lumi-
nescence Dosimetry, Krakow, August (Krakow: Institute of Nuclear Physics), vol 2, p641
17 Charles M W 1977 The development of a practical 5 mg/cm
2
skin dosimeter Proc. 5th Int. Conf.
on Luminescence Dosimetry, Sao Paulo, February (I Physikalisches Institut, Universitat Giessen),
p313
18 Burgkhardt B, Piesch E and Schmitt A 1977 Depth dose distribution of 9 MeV photons in a single
phosphate glass compared to phantom results Nucl. Instrum. Meth. 141 141
19 Busuoli G and Julius H W 1977 Possible use of BeO in beta-gamma personnel dosimetry Proc. 5th
Int. Conf. on Luminescence Dosimetry, Sao Paulo, February (I Physikalisches Institut, Universitat
Giessen), p225
20 Piesch E, Burgkhardt B and Sayed A M 1974 Supralinearity and re-evaluation of TLD 600 and
TLD 700 in mixed neutron and gamma fields Proc. 4th Int. Conf. on Luminescence Dosimetry,
Krakow, August (Krakow: Institute of Nuclear Physics), pl201
21 Piesch E and Burgkhardt B 1974 An LiF albedo neutron dosimeter for personnel monitoring in
mixed radiation fields Proc. 4th Int. Conf. on Luminescence Dosimetry, Krakow, August (Krakow:
Institute of Nuclear Physics), vol 3, p l l 2 3 and 1918Proc. IAEA Symp. on Advances in Protection
Monitoring, Stockholm
22 Piesch E and Burgkhardt B 1980 Application of the TLD albedo technique for monitoring and
interpretation of neutron stray radiation field Proc. 6th Int. Conf. on Solid State Dosimetry,
Toulouse, April. Nucl. Instrum. Meth. 175 No 1 (September)
23 Niewiadomski T (ed) 1974 Proc. 4th Int. Conf. on Luminescence Dosimetry, Krakow, August
(Krakow: Institute of Nuclear Physics)
24 Scharmann A (ed) 1977 Proc. 5th Int. Conf. on Luminescence Dosimetry, Sao Paulo, February
(I Physikalisches Institut, Universitat Giessen)
25 Technical Note Development of a new type thermoluminescence dosimeter (Matsushita Electric
Industrial Co Ltd)
26 Burgkhardt B and Piesch E 1978 Nucl. Instrum. Meth. 155 293, 299
27 Luersen R B and Johurson T L 1979 Results of the Naval Research Laboratory's participation in a
personnel dosimetry performance test in pilot study NRL Memorandum Rep. 4048
28 Burgkhardt B, Piesch E and Seguin H 1980 Some results of a European interlaboratory test pro-
gramme for integrating dosimeter systems for environmental monitoring Proc. 6th Int. Conf. on
Solid State Dosimetry, Toulouse, April. Nucl. Instrum. Meth. 175 No 1 (September)
29 Burgkhardt B and Piesch E 1980 Reproducibility of TLD systems - a comprehensive analysis of
experimental results Proc. 6th Int. Conf. on Solid State Dosimetry, Toulouse, April. Nucl. Instrum.
Meth. 175 No 1 (September)
30 Portal G (ed) 1980 Proc. 6th Int. Conf. on Solid State Dosimetry, Toulouse, April. Nucl. Instrum.
Meth. 175 No 1 (September)
31 Toivonen M 1979 Individual TL detector characteristic in automated processing of personnel dosi-
meters Rep. STL-A27
32 McKinlay et al 1980 Photo-transferred thermoluminescence technique and its application to the
routine re-assessment of absorbed dose in the NRPB automated personal dosimetry system Proc.
6th Int. Conf. on Solid State Dosimetry, Toulouse, April. Nucl. Instrum. Meth. 175 No 1 (Sep-
tember)
33 Douglas J A et al 1980 The effect of LET on the efficiency of dose re-estimation in LiF using UV
photo-transfer Proc. 6th Int. Conf. on Solid Dosimetry, Toulouse, April. Nucl. Instrum. Meth.
175 No 1 (September)
34 Regulla D F 1980 Remarks on the present state of thermoluminescence Proc. 6th Int. Conf. on
Solid State Dosimetry, Toulouse, April. Nucl. Instrum. Meth. 175 No 1 (September)
35 Duftschmid K E 1980 The automatic computerized TLD personal monitoring system in Austria
Proc. 6th Int. Conf. on Solid State Dosimetry, Toulouse, April. Nucl. Instrum. Meth. 175 No 1
(September)
36 Burgkhardt B, Moos W and Piesch E 1979 Ergebnisse einer Umfrage iiber Erfahrungen mit Thermo-
lumineszenz- und Phosphatglas-Auswertegeraten Rep. FS 79-19-AKD SI7
Application of TLD to personnel dosimetry 195
37 Christensen P and Majborn B 1980 Boron diffused thermoluminescent surface layer in LiF TLD's
for skin dose assessment Proc. 6th Int. Conf. on Solid State Dosimetry, Toulouse, April. Nucl.
lustrum. Meth. 175 No 1 (September)
38 Uchrin G 1980 A new type of extremity dosimeter Proc. 6th Int. Conf. on Solid State Dosimetry,
Toulouse, April. Nucl. Inst rum. Meth. 175 No 1 (September)
39 Grogan D, Bradley R P and Ashmore J P 1980 Some problems associated with large scale TLD
monitoring and their solutions Proc. 6th Int. Conf. on Solid State Dosimetry, Toulouse, April.
Nucl. lustrum. Meth. 175 No 1 (September)
40 Julius H W and Busuoli G 1980 An extremity (finger ring) dosimeter based on TLD Proc. 6th Int.
Conf. on Solid State Dosimetry, Toulouse, April. Nucl. Instrum. Meth. 175 No 1 (September)
41 Hankins D E 1973 A small inexpensive albedo-neutron dosimeter Los Alamos Rep. LA-5261
42 Hoy J E 1972 Personnel albedo neutron dosimeter with thermoluminescent
6
LiF and
7
LiF
Savanah River Lab. Rep. DP-2377
43 Brunskill R T and Way Wang F S 1980 A personal thermoluminescence dosimeter for the measure-
ment of 0y, y and neutron dose Proc. 6th Int. Conf. on Solid State Dosimetry, Toulouse, April.
Nucl. Instrum. Meth. 175 No 1 (September)
44 Piesch E and Burgkhardt B 1978 The role of an analyser albedo dosimeter in routine monitoring
and the current situation for the calibration technique Proc. 7th DOE Workshop on Personnel
Neutron Dosimetry, Rep. PNL-2807 p25
45 Piesch E and Burgkhardt B 1980 A new technique for neutron monitoring in stray radiation fields
Proc. 5th Int. IRPA Congr., Jerusalem vol III, p 121
46 Prokic M 1980 Development of high sensitive CaS0
4
: Dy/(Tm) and MgB0
7
: Dy/(Tm) sintered
thermoluminescent dosimeters Proc. 6th Int. Conf. on Solid State Dosimetry, Toulouse, April.
Nucl. Instrum. Meth. 175 No 1 (September)
47 Harvey J R, Hudd W H R and Townsend S 1973 Neutron Monitoring for Radiation Protection
Purposes, Symp. Vienna STI/PUB/318, ppl 99-218
48 Piesch E, Burgkhardt B and Sayed AM 1978 Activation and damage effects in TLD 600 after
neutron irradiation Nucl. Instrum. Meth. 147 178-84
Applied Thermoluminescence Dosimetry. Eds M Oberhofer and A Scharmann
1981 ECSC, EEC, EAEC, Brussels and Luxembourg
11
Application ofTLD systems for environmental monitoring
E PIESCH
11.1. Introduction
A significant aspect of environmental monitoring is the limitation of radiation exposure
values in man from the nuclear power fuel cycle. In the case of gaseous radionuclides
released to the environment from a nuclear installation, the acceptable limit of exposure
is based on an annual dose equivalent of 30 mrem, a value about a third that from natural
terrestrial and cosmic radiation. An increasing amount of public interest in environ-
mental monitoring programmes is being focused on the environmental impact of radiation
arising from nuclear power operations and the corresponding detection of slight variations
in the natural radiation background.
TLD systems are widely applied to environmental monitoring programmes near nuclear
installations, TLD systems with high reproducibility in the milliroentgen dose range are
required in order to measure exposures equal to that resulting from an exposure rate of
10 /iR h"
1
during field periods of from several days up to a year.
For the application of TLD systems in environmental monitoring, therefore, special
performance criteria and techniques for selecting, testing, calibrating and using a TLD
system have been established:
(a) The ANSI N545-1975 standard [1] specifies the minimum acceptable performance
of TLD and outlines test methods for compliance. To meet these requirements, each
laboratory has to carry out tests for determining their own limits of error.
(b) On the basis of a standard test programme [41] and an inter-laboratory comparison,
the performance and quality of a broad spectrum of TLD systems can be compared
with respect to variations in the properties of reader, TL material, read-out method
and annealing technique adopted in the laboratories.
(c) Annual control exposures as well as inter-comparison experiments organised by the
ERDAf serve as a valuable way to compare one's own results with the international
level [3].
This chapter reviews the properties of TLD systems and the common techniques used
in the application of TLD in environmental monitoring, taking into account the results
of a test programme and recent investigations of the long-term fading as well as the
calibration technique and the interpretation of experimental results.
f United States Energy Research and Development Administration.
198 EPiesch
11.2. Performance specifications
In contrast to the application in personal monitoring, TLD systems for environmental
monitoring have to fulfil high requirements, such as
(a) good precision and reproducibility of measurement over the exposure range of
interest (10-100 mrem);
(b) low fading over the field exposure period (3-12 months);
(c) insensitivity to environmental parameters, i.e. temperature, moisture, humidity,
light;
(d) approximate tissue equivalence in dose reading;
(e) low self-irradiation due to natural radionuclides in the TLD phosphor or holder;
(/) encapsulation in a plastic holder to provide secondary electronic equilibrium,
shielding against |3-rays and light as well as water tightness;
Q?) calibration techniques for each field cycle to guarantee the highest precision for the
conversion to exposure and to correct for fading, transit exposure and zero-dose
reading.
Up to now only the American National Standard [1] gives performance criteria for
TLD systems used for the measurement of environmental exposure levels. This standard
specifies minimum acceptable performance of TLD used for environmental measurements,
outlines methods to test TLD systems and provides procedures for calibration, field
application and reporting. The performance criteria and specifications for TLD systems
are discussed here on the basis of this standard until such time as other technical recom-
mendations [45] or recommendations of the Commission of the European Communities
are available.
In order to meet requirements for environmental monitoring, tests to determine error
parameters should be carried out at least once a year if a particular TLD system is
adopted. As can be seen from table 11.1, the general testing procedures of ANSI N545-
1975 provide specific tests for uniformity of batch sensitivity, reproducibility, depend-
ence of exposure interpretation on the period of the field cycle, energy and directional
dependence, light and moisture dependence and self-irradiation. The results of tests
should be within the limits given for the errors at the 95% confidence level.
The performance of TLD systems should be determined under laboratory conditions.
Taking into account additional corrections applied to compensate for the errors under
field conditions, the overall error of measurement under field conditions should be less
than 30% at 95% confidence level.
11.3. Properties of commercial TLD systems
11.3.1. TL materials and systems
Typical TL phosphors suitable for monitoring environmental radiation are presented in
table 11.2. The materials indicated in this table have been investigated experimentally
in the past and employed in measurement programmes with varying success. Most of the
TL materials (CaF
2
, CaS0
4
) have been chosen because of their high sensitivity which
allows exposure periods of 1 week to 3 months. Due to the energy dependence of the
Application of TLD systems for environmental monitoring 199
Table 11.1. TL D performance criteria for environmental application (ANSI N5451975).
Testing procedures
Uniformity within field batchf
Reproducibility for one TL Df
Field cycle interpretation}: ratio 7(f)/2/(r/2)
Energy dependence (30 keV3 MeV)
for > 80 keV
for <80keV
Direction dependence during rotation through two
perpendicular planes
L ight dependence}
Moisture dependence}
Selfirradiation}
15%
5%
<0. 9
<20%
Factor of 2
10%
<10%
<10%
10MRr r '
Performance specifications
Test exposure under laboratory conditions! 10%
Correction for field conditions determined from the
testing procedures Factor of 2
Overall measurement error under field conditions 30%
f For an exposure rate of 10 MR h~' during field cycle and at the 95% confidence level.
} For a period t equal to the field cycle.
Table 11.2. Characteristics of thermoluminescence phosphors suitable for environmental
radiation measurements [4].
Phosphor
L iF (TLD 700)t
L i
2
B
4
0
7
:Mn
CaF,:Mn
CaF, : natural
CaF
2
: Dy (TL D200)f
CaSO: Dy
Zeff
8.2
7.4
16.3
16.3
16.3
15.5
Room
temperature
fading
(%/month)
Negligible
<10
5
Negligible
(After preread
out anneal)
<2
Selfirradiation
(MRh"
1
)
Negligible
None reported
722
913.8
Negligible
None reported
Reported
lower
exposure
limit }
(mR)
0.85

1.1
<1
0.5
0.5
Refer
ences
47
48, 49
50, 51
52. 53
54
55
t TL D 100, 200 and 700 are Harshaw Chemical Co designations, but are widely used. TL D
100 (natural L iF composition) and TL D 700 (enriched in
7
L i) have about the same 7ray
responses.
} Lower limits highly dependent on photomultiplier tube used.
reading, these detectors are only suitable for environmental measurements if holders are
used which provide for energy compensation and thus avoid errors up to a factor of
three. Because of the effect of light sensitivity and fading most of these TL materials
200 EPiesch
should be rejected for long-term monitoring. For environmental application, therefore,
mainly chips or high-sensitivity bulb dosemeters of OF, CaF
2
: Dy and CaS0
4
activated
with Dy and Mn are widely used. To complete this review, more-insensitive RPL glass
dosemeters are also applied in environmental measurements. In addition to short read-out
cycles, the low fading characteristic of glasses allows long-term exposure periods of up to
6 yr.
The dosemeter properties of TLD systems may differ significantly due to the individual
properties of the reader, the TL material and the evaluation technique used in the
laboratory. Differences in the dosimetric properties of TLD systems are mainly due to:
(a) the type of reader and the individual properties of the photomultiplier component
in the reader;
(b) the dosemeter material, the activator, the matrix material, the form, thickness and
mounting of the detector, as well as the history of the batch;
(c) the read-out procedure, in particular the heating cycle and the maximum heating
temperature which have been selected;
(d) the thermal treatment of the detector prior to measurement (pre-heating) or the
thermal treatment used prior to re-use (annealing);
(e) the history of the TLD batch, i.e. number of annealings and the amount of pre-
exposure.
Although dosemeter systems with high accuracy may now be applied, the properties
of different TLD readers, even of one type, are not comparable because of variations
either in the PM dark current or in the reproducibility, which may vary by more than a
factor of 100 and a factor of 4, respectively [2]. Results from other laboratories with the
same type of reader or the application of the read-out technique which may be found in
the current literature cannot replace an extended performance test with each reader or
dosemeter system. Compared to the results of an inter-laboratory test programme, single
data reported in the literature or the recommendations in the NCRP Report no 50 [4]
cannot reflect the present technology or the state of the art.
For TLD systems applied in environmental monitoring programmes, therefore, exten-
sive performance tests are required to establish high accuracy, i.e. small random and
systematic measuring errors in the low dose range.
The state of the art may be found in the results of inter-laboratory test programmes
which have recently been organised by the 'Workshop Dosimetry' of the Fachverband fur
Strahlenschutz [2] and the European Communities [41]. Here the properties of 43 and 45
different dosemeter systems, respectively, have been investigated. According to the
recommended test procedure the laboratories tested their dosemeter systems with respect
to zero-dose reading, the lower detection limit, the standard deviation as a function of
exposure, long-term stability of the system and temperature effects during storage at
70 C. The experimental procedure of the inter-laboratory test programme (table 11.3)
provides measurement runs to be carried out by each laboratory with a batch of 10
dosemeters taking 10 readings for each dosemeter or repeating the measurement cycle
10 times. The dose range had been related to a multiple of the lowest detectable dose
>idi defined as three times the standard deviation (3 s value) of the zero-dose reading a
u
of unirradiated dosemeters after subtraction of the dark current reading a
0
.
Application of TLD systems for environmental monitoring
201
Table 11.3. Experimental procedure for the performance of the standard test programme of
TLD systems.
Run Characteristic quantity
no
Number of Test instruction
dosemeters
(measure-
ments)
Zero reading
Dark current
Immediately
70C/ 16h
(10X) Read-out without dosemeter
10 Irradiate new or annealed dosemeters to
300 mR; annealing, read-out
10 Irradiate to 300 mR, annealing, store for
16 h/70C, read-out
4
5
6
7
8
Reproducibility
1-Oldl
30 mR
5D
I d
i to lOOOOidi
Individual sensitivity
Long-term stability
Light source
Dark current
Reference dose
Zero reading
Zero reading 70 C/16h
Influence of temperature
at 70C
10
10
10
10
(10X)
(10X)
10
10
10
10
In each case anneal and irradiate
to 3s value of the zero reading immedi-
ately (=Z3
ldl
)
to 30 mR
to 5, 10, 20, 50, 100 and 1000>i
d
i
to lOOOOidi
Over 10 d per 10 dosemeters/measure-
ments without additional calibration of
instruments
Measure 10 X
Adjust and measure 10 X
Annealing, irradiate to 1000Z)]
d
[, read-out
Annealing, read-out
Store at 70C/16 h, read-out
Irradiate two dosemeters prior to storage
at 70C for 10, 6, 2, 1 d and two reference
dosemeters (storage 2 h/25 C) to
1000>idi, read-out together
11.3.2. Batch uniformity
For TLD of the same batch, the sensitivity of the individual detector may scatter over a
range of the order of 10%. High reproducibility therefore requires an individual calibra-
tion of each TLD in a batch or a selection of TLD by the manufacturer or user, resulting
in a high batch uniformity. The relationship between the deviation in response within a
batch and the resulting reproducibility is presented in figure 11.1 for different dosemeter
systems. By definition, both quantities are identical for a batch calibration showing devia-
tions in the range 3-9% (relative standard deviation), for selected batches also lower than
1%. Individual calibrations of the TLD, which should be considered for an environmental
TLD system, improve reproducibility by more than 3% to better than 1.9% (l a value).
202
E Piesch
m s
INDIVIDUAL CALIBRATION
BATCH CALIBRATION
1 2 3 4 5 6
REPRODUCIBILITY 0 IN 7 .
Figure 11.1. Batch uniformity against reproducibility of dose measurement [2].
11.3.3. Reproducibility
The reproducibility of measurement is a function of detector type, size and sensitivity, of
batch uniformity and reader quality. For each TLD system, a reproducibility test should
be performed in the dose range of interest, starting with an exposure equal to the lower
detection limit D\&\, which may be defined as the 3s value of the zero-dose reading to an
exposure of lOOOZJjdi. Experimental results of the standard deviation as a function of
exposure are presented in figure 11.2 for different TLD systems. The typical shape of the
reproducibility against exposure curve is caused by two parameters, the variation in the
zero-dose reading of the system and its reproducibility in the high dose range which is
explained in more detail with respect to the error of measurement in 11.4.
A constant reproducibility is expected for exposures of about lOCD^, which is equal
to 30 mR and 100 mR, respectively, for most of the LiF systems independent of reader
type and the application of an automatic read-out technique, 0.2 mR and 10 mR for
CaF
2
systems, 5 mR and 100 mR for CaS0
4
and 10 mR and 100 mR for Li
2
B
4
0
7
. The
reproducibility (Is value) achievable in practice is found to be 1-4% for LiF, 2-5% for
LiaE^Ov, 2-6% for CaF
2
and 2-3% for CaS0
4
. To optimise TLD systems for an environ-
mental monitoring programme, field exposure periods of the order of 100D]^ are recom-
mended. The reproducibility for an exposure of 30 mR expected after a field period of
approximately six months is presented in figure 11.3 on the basis of 10 dosemeter readings
per batch. Only one-third of the TLD systems investigated showed relative s values of
about 2%.
11.3.4. Zero-dose reading
The zero-dose reading of a TLD system depends on the PM characteristic, the properties
of the TL material, the annealing treatment and the annealing and irradiation history of
Application O/TLD systems for environmental monitoring 203
(a)
L i j B.O,
NATIONAL
aoi
L ' l Bi O,
STUDSVIK
Caf} STUDSVIK
1 10
DOSE IN mR
1000
10' 10" 10' 10 10
3
10' 10
5
EXPOSURE IN mR
Figure 11.2. (a) Relative standard deviation ( l a value of 10 dosemeters) against exposure
for different TLD systems, LiF systems excluded [2]. (b) Relative standard deviation ( l a
value of 10 dosemeters) against exposure for LiF systems [2]. (c) Relative standard deviation
( l a value for 10 dosemeters) against exposure for LiF automatic systems [2].
204
E Piesch
DOSIMETER SYSTEMS
Figure 11.3. Reproducibility of TLD systems at 30 mR [2].
the batch. The zero-dose reading is presented as the sum of components, the read-out
without dosemeter a
0
and the read-out of unexposed dosemeters a
u
. For highly sensitive
TLD readers, the zero dose a
u
may be much higher than the dark current OQ.
In the lower dose range, the mean value of the zero-dose reading (a
0
+ a
u
) (figure 11.4)
has to be subtracted from the dosemeter reading. By definition, the lower detection limit
Adi is given by the 3s deviation of the zero-dose reading. The results in figure 11.4
demonstrate that the mean value of the zero-dose reading has been found to be smaller
than D
ld
i and, for most of the TLD systems, to be in the range 1 -10 mR.
11 MEAN VALUE | O^' 0,u >
r ^ JBVALUE I D, , ]
Li2Bt 07 CoF2 CQSOJ
u u K ' i a z o T t f t i z i K i i s B Q i T M e k O B n i ] E H a n x > u X B X U
DOSIMETER SYSTEMS
Figure 11.4. Zero-dose reading of different TLD systems [2].
11.3.5. Long-term stability
With respect to the standard test programme, the stability of the system is investigated
over a period of at least 10 d, taking into account a daily check of the dark current, the
Application of TLD systems for environmental monitoring
205
zerodose reading of unexposed dosemeters after repeated measurements/annealings and
the reproducibility of dose reading. For example, for the longterm stability of the reader,
the zerodose reading shown in figure 11.5 may vary between a factor of two and a factor
of ten, especially for systems not applying an annealing treatment. On the other hand,
there are also TL D systems in use showing a low and constant zerodose reading. The
change in sensitivity of the order of 5% can be corrected by an additional reader
calibration taking into account control dosemeters from the same batch and annealing
run.
1.
"Jfto, as*
In
B MEAN AND MAXIMUM VALUES
- \
V
BEADING BEFORE IEST
R REGENERATED BEFORE REUSE
DOSIMETER SYSTEMS
Figure 11.5. Longterm stability (over 10 d period) of zero
dose reading [2].
11.3.6. Energy and directional dependence
The reading of L iF and TJ2B4O7 dosemeters has been found to be sufficiently tissue
equivalent (figure 11.6). If a nontissueequivalent TL material is adopted, the energy
dependence of the dose reading can be improved by using suitable energy compensation
filters (figures 11.7 and 11.8). Perforated tin spheres, for example, are in use to reduce

/
/ /
THER
/ >S
L
'
F
V
1
/DOS I

HOLUMINESC
3.3*Q9mnT> B
Mg.Ti
ENT DOSI METER
HIND 50mg/on> FOR
HWmg/em
1
FOR
It Or Mn.Si
-4 1
-1
PHOSPHATE
PERFORAT
|
GLASS DOSIMETER
1
<0 6MV
>0 6M,V

-OOS2
^
1
-
PHOTON ENERGY IN ktV
Figure 11.6. Energy dependence of LiF:Mg,Ti and Li
2
B
4
0
7
:Mn, Si dosemeter systems.
206 EPiesch
Figure 11.7. Environmental TL dosemeter with 3 mm copper (brass) compensation shield
(filter) for TL phosphor Teflon discs, designed by the Health Physics Institute of the Gesell-
schaft fiir Strahlen- und Umweltforschung Miinchen mbH, produced by the Institute of
Radiation Protection and Dosimetry of CNEN, Brazil.
Figure 11.8. Bulb-type TL dosemeters with energy compensation shields, (a) Harshaw
Bulb TL dosemeter ( O
m i n
: 0.1 mR for the Dy-activated CaF, phosphor dosemeter),
(b) MBLE CaF
2
TL dosemeter type PNP291 {D
mm
: 0.1 mR), (c) Victoreen CaF
2
:Mn dose-
meter Model TL-35 (>
m
in
:
0-
1 m R
if read with Model 2600 reader).
the over-sensitivity of CaF
2
:Dy in the energy range below 100 keV (figure 11.9). In
stray radiation fields around nuclear plants, the compensation filter avoids measurement
errors of the order of a factor of three. The internal directional dependence of the dose
reading should be small in the main direction of the radiation incidence and may be
spoiled by the suspension of the dosemeters on dense objects such as trees, resulting in
directional anomalies or shieldings of the radiation field.
11.3.7. Fading
In environmental monitoring, dosemeters are freely exposed in air up to monitoring
periods of one year during which time the influence of sunshine may cause a relatively
high temperature. The temperature-dependent fading gives rise to a significant loss of
Application O/TLD systems for environmental monitoring 207
CaF2:D y- DOSIMETER
HARSHAW RIBBONS TLD 200
0.125x0.125x0.035"
o 3mm LUCITE
SPHERICAL CAPSULE
2mm AU2mm Sn,PERFORATED
1000
QUANTUM ENERGY IN keV
Figure 11.9. Energy dependence of the dosemeter reading of a CaF
2
: Dy dosemeter with
spherical encapsulation (produced by Heist GmbH, Glottertal, BRD) (open circles) and
without an energy compensation filter (full circles).
signal during exposure and storage before evaluation. Laboratory experiments may result
in the estimation of the fading rate as a function of temperature. Because of changes in
the ambient temperature profile and in the exposure rate during the monitoring period,
the actual fading during each field period should be checked by using pre-exposed control
dosemeters at a representative location.
A long-term fading experiment was recently performed [6, 7] in the temperature range
5-100 C up to storage periods of one year. The fading effects of pre-exposed TL materials
are presented in figures 11.10-11.12 as a function of the storage period. The fading
10 too 1000
STORAGE PERIOD IN D AYS
Figure 11.10. Fading of CaS0
4
: Dy Teflon against storage period related to 1 d storage at
25 C and a post-irradiation treatment at 100C for 20 min [7].
208
E Piesch
i 1000 10 too
STORAGE PERIOD IN DAYS
Figure 11.11. Fading of CaF
2
:Dy Teflon against storage period related to 1 d storage at
25C and a postirradiation treatment at 100C for 20 min [7].
100
90
80
j . 70
? 60
O
z 50
a
2 40
a.
20
10
0
'
"
. i
LiRMg.Ti RIBBONS TLD 700
100 C/ 20mi n
-
v ^
i 1
~ ^ "
- 25 C
* 50C
_
^ ^ v 70 C
- 100 C
1 1000 10 100
STORAGE PERIOD IN DAYS
Figure 11.12. Fading of L iF:Mg, Ti Teflon against storage period related to 1 d storage at
25 C and a postirradiation treatment at 100 C for 20 min [7].
results are based on a postirradiation annealing at 100 C/20 min and on reference dose
meters of the same set that were stored under laboratory conditions and exposed one day
before evaluation.
L iF: Mg, Ti, the TL material most frequently used, shows fading effects of 530% after
more than one year of storage at 25 C and 50 C. For highly sensitive CaF
2
: Dy ribbons
applied in environmental monitoring mainly for short exposure periods, the dose reading
after one year of storage at 25 C was still found to be of the order of 90%. This is the
Application of TLD systems for environmental monitoring
209
result of the post-irradiation annealing at 100C/20min. Without applying any pre-
heating, a similar fading is already found after a storage period of 1 d. The annual fading
at 50 C was found to be 45% compared with 30% for LiF : Mg,Ti.
Further improvements of the fading characteristic may be found by pre-heating at
temperatures higher than 100C or by longer annealing periods in the range of 100 C,
both of which may simulate longer annealing periods at ambient temperature [8]. For
instance, pre-heating at 120C/20 min is sufficient for LiF: Na,Mg to reduce the fading
to practically zero even for storage at 50C/50 d. For LiF: Mg,Ti, on the other hand,
pre-heating at 100C/15 h reduces the fading more effectively than pre-heating at 140 C.
A further increase of temperature does not improve fading results.
The reduction of fading as a function of the pre-heating temperature is presented in
figures 11.13 and 11.14 for LiF:Mg,Ti and CaF
2
:Dy after 20 d storage at 50 C. In
contrast to pre-heating in the reader, an extended pre-heating in the oven may reduce the
fading from 17% and 60% without pre-heating to values of the order of 5% at 130 C/
20 min. An extended pre-heating of CaF
2
: Dy, however, reduces sensitivity in both cases
of the order of 20%.
PREHEATING PERIOD AT 100 *C IN MINUTES
PREHEATING PERIOD AT KO*C IN MINUTES
Figure 11.13. Fading reduction by applying a pre-heating treatment at 100C [8] for
LiF:Mg,Ti (left) and CaF
2
:Dy (right) after 20 d storage at 50 C.
t 0 60 80 100 120 UC
POST-IRRADIATION TREATMENT AT C
40
O
5 30
<
u.
g 20
10
20 tO 60 80 100 120
POST-IRRADIATION TREATMENT AT C
Figure 11.14. Fading reduction by applying a pre-heating treatment at higher temperatures
for LiF:Mg,Ti (left) and CaF
2
:Dy (right) after 20 d storage at 50 C.
210 E Piesch
On the basis of post-irradiation annealing treatment at 100 C/20 min, the long-term
fading at 20 C is sufficient for most of the TL materials investigated. For an application
in environmental monitoring, however, extended pre-heating in the oven but not in the
reader may improve the fading characteristic (see table 11.4).
Table 11.4. Application of pre-heating for fading reduction.
Material Pre-heating
treatment
f Fading after 20 d of storage at 50 C.
Relative
response
Fadingf
(%)
LiF:Mg,Ti
LiF:Na,Mg
Li
;
B
4
0
7
:Mn, Si
CaF
2
:Dy
100C/ 5h
135C/20 min
120 "C/20 min
100C/ 2h
100C/ 16h
130C/20min
0.8
0.62
0.9
0.78
0.3
0.2
3
3
1
20
2
5
The standard test programme makes use of a temperature treatment at 70 C over a
period of 10 d in order to simulate environmental fading effects and to check, more or
less, the post-irradiation annealing technique applied to the system. The high scatter
of the fading results presented in figure 11.15 mainly resulted from variations in the
annealing treatment applied in the laboratories. Discrepancies in published fading data
[21, 38] may be attributed to different TLD systems which may vary in the TL phosphor,
the kind of activator and, above all, the annealing and read-out technique.
For the TLD systems adopted for an environmental monitoring programme the applica-
tion of supplementary techniques for post-irradiation annealing, read-out and calibration
should be provided.
Further fading corrections can be achieved by measuring the fading at the field loca-
tion itself. A good approximation of the time-dependent fading process in the environ-
ment can be found by the Randall-Wilkins theory [9]. In table 11.5, formulae of interest
are presented which can be applied to the different kinds of field and/or control
exposures before or during the field exposure period. In estimating the real fading effect,
uncertainties arise from:
(a) the radiation field, which shows fluctuations of the exposure rate or several short-
term exposures;
(b) the ambient temperature profile during the field exposure;
(c) the knowledge of the fading rate, which is inconstant in Tand t due to several glow
peaks with different functions of \(T) and dependent on the annealing treatment
before read-out;
(d) a constant self-irradiation due to trace radioactivity in materials used for the
encapsulation of the TL phosphor;
(e) the fact that, under practical conditions, no exponential fading function has been
found after longer periods of storage.
Application of TLD systems for environmental monitoring 211
2 ( 6 8
STORAGE PERIOD IN DAYS
2 4 6 8 10
STORAGE PERIOD IN DAYS
z
o
o
Si
K
Ul
Q:
100
80
fin
40
20
n
^ L i
2
B
4
0
7
\ \ \
\v\
V v \
w .
- ^
= 3

0 2 4 6 8 10 0 2 4 6 8 10
STORAGE PERIOD IN DAYS
S T 0 R A S E p E R | 0 D | N

Figure 11.15. Fading of various TLD systems after storage at 70 C [2].
Table 11.5. Formulae for fading correction.
Initial exposure X
0
at time t = 0:
I
t
= aX
0
exp(-A.f) =/ exp(-Xf).
Constant exposure rate X during field exposure:
I
t
= a(X/X)[l - e xp( - Xf ) ] .
Pre-exposure before or during the field exposure period for subgroups
of dosemeters:
I
t
= I
0
exp[ - \ ( f - f,-)] + {aX/\)[\ - exp( - \ f ) ] .
Actual single exposures X, at time t( during the field exposure period:
I
t
= 2 / , - exp[ - \ ( f - r
(
) ] + ( a i / \ ) [ l - e x p ( - W) ] -
i
where I
t
= light intensity at time t, a = conversion factor, X = \(T)
thermoluminescence fading rate dependent on ambient temperature
profile, X = exposure rate during field period.
212 E Piesch
11.3.8. Environmental effects
Environmental agents such as light, friction, moisture and humidity may affect the TLD
signal and the zero-dose reading of unexposed dosemeters in an uncontrolled way. The
creation of spurious TLD signals and the simultaneous loss of the latent dose information
may occur due to:
(a) contamination of the TL phosphor;
(b) tribothermoluminescence;
(c) stimulation of the TLD by visible or uv light;
(d) oxygen atmosphere during read-out;
(e) humidity and moisture.
From the TLD materials of interest, it is mainly LiF which shows the lowest influence
and the best insensitivity to these effects. For example, the TL dirt present in the environ-
ment of Chalk River simulates an apparent exposure to TLD 100 as illustrated in table 11.6.
A few micrograms of dirt may contaminate the TLD and could give rise to signals
Table 11.6. Influence of contaminants on the TL read-out [33].
Contaminant Thermoluminescence (apparent
R mg"
1
)
Sandy
Sub-soil
Top soil
Sand from ash tray
Road sand
0.6-0.7
0.14-0.22
0.2-0.4
2.7-5.2
<
1.0
100 200
100 200 300
too
300 "0
TEMPERATURE CO
Figure 11.16. (Left) Dosemeter response to friction (rubbed with sharp tweezers three times); and
(right) glow curves of different dosemeters for 5 mR exposure taken with Corning 4303 filter and
argon flow [10].
Application of TLD systems for environmental monitoring
213
comparable with those measured in environmental dosimetry [33]. The contamination
effects call for rigorous cleaning before read-out or a dosemeter package which effectively
excludes dirt (see also 4.9 and 7.2.7).
The effect of tribothermoluminescence caused by rubbing the detector with PVC foils
or by sharp tweezers during preparation and handling shows glow peaks similar to that of
radiation-induced TL. Careless handling of the tweezers may increase the background
reading of magnesium silicate and calcium sulphate by a factor of 2-12, arid for LiF by
less than a factor of two (figure 11.16) which may simulate a significant exposure
compared to the flow curves presented for 5 mR [10] (see 4. 6, 4.7 and 7.2.6).
The effect of visible or uv light exposure increases the zero-dose reading of unexposed
TLD (figures 11.17 and 11.19) but may also reduce the signal effectively as is shown for
white plastic shielded CaF
2
: Dy during a three-month field monitoring period (figure
11.18). For environmental application, only a light-tight package (opaque paper and black
polyethylene foil) may protect the TLD against long-term light exposure.
100 200 300
TEMPERATURE C O
Figure 11.17. Glow curves of the dose-
meters exposed to 1 h long fluorescent light
(2000 lx) [10].
100
0 20 10 60
TIME FROM EXPOSURE ( d)
Figure 11.18. Fading of environmental monitoring TLD
(the symbols in parentheses in the key refer to the differ-
ent filters: PI, plastic;Cw, clear plastic, white paper).
214 EPiesch
100
50-
* Mg
2
Si0
4
Tb
CaS0
4
:Dy
LiF.Mg.Ti
Li F- 7
10
^
10
EXPOSURE TIME IN min
Figure 11.19. Increase in the dosemeter background (lower) and fading of 0.1 rad response
(upper) owing to fluorescent light (2000 lx) [10].
In most of the TLD phosphors no significant effects of moisture and humidity were
found for chips and Teflon detectors. The reproducibility of measurement, however, is
highly affected by humidity, resulting in a high scatter [7]. In Li
2
B
4
0
7
:Mn in Teflon the
fading effect .is superimposed by a damage effect which occurs after long-term storage at
high humidities and is strongly influenced by temperature (figure 11.20). An inert-gas
atmosphere is of high importance to quench spurious luminescent signals during low-dose
read-outs. Nitrogen and argon, having an oxygen content of less than 0.1%, are used
resulting in a reduction of zero-dose reading by a factor of 8-16 (figure 11.21) [10].
11.4. Calibration technique for dosemeter batch and reader
Since the relative sensitivity of TLD or the TL response in milliroentgens is a system-
dependent parameter, any variations in the reader conditions, the annealing treatment or
the read-out parameters may cause a significant change in the relative sensitivity. For the
measurement with TL dosemeters, therefore, the reader and each batch of field dose-
meters have to be calibrated individually by additional control dosemeters.
For the use of TLD in environmental monitoring, extensive calibration techniques have
to be applied for sufficiently qualified systems to reach a precision of about 10%. The
procedure for measurement and calibration is illustrated in figure 11.22. In addition to
Application of TLD systems for environmental monitoring 215
423 DAYS
180 DAYS
275 DAYS
423 DAYS
STORAGE AT
o o 50 "t
. 40 C
AFTER
/so
l
DAYS
DAYS
MASON ET AL
"""^.
1974
^ *
TEFLON
POWDER
20 40 60
STORAGE TEMPERATURE IN C
20 80 100
Figure
meters
40 60
REL.HUMIDITY IN V.
11.20. Li
2
B
4
0
7
:Mn fading due to humidity (left) and damage in Li
;
B
4
0
7
:Mn Teflon dose-
due to humidity (right) [7].
E
<
>
D
a
D
O
tr
<
CD
AMg
2
Si0
4
:Tb
L iF:Mg ,Ti
TLD-100
CaS0
4
: D y
20 40 60 80
ARGON FLOW RATE IN l/h
Figure 11.21. Influence of argon flow rate on the dosemeter background investigated with
the integrating reader. Mg
2
Si0
4
: Tb, LiF : Mg,Ti and TLD 100 with the BG-12 filter, reading
temperature 250C; CaS0
4
: Dy without filter, reading temperature 270C [10].
field dosemeters (B
F
), two or more groups of control dosemeters are needed to calibrate
the system (B
c
), to correct for the fading during the field exposure (Bf) and to separate
exposures which the dosemeter batch may receive during transit (B
t
) or storage (B
0
) in
the laboratory. The control dosemeters are shielded in lead at the laboratory over the
whole period (B
c
, B
0
) or after transit to the site during field exposure (B
t
). Both
216
E Piesch
Dosemeter batch B
Pre-irradiation annealing
Encapsulate
Field dosemeters Control dosemeters
Bf B, B
c
B
0
fading transit calibr. zero dose
Travel to site
Field exposure
B
F
B
f
Shield exposure
Bt
Shield exposure
B
c
B
Travel back Calibration
Post-irradiation annealing
Read-out
Figure 11.22. Procedure for TLD calibration and measurement.
environmental and control dosemeters should be pre-annealed, post-annealed and evaluated
together.
For statistical reasons, at least 10 control dosemeters for both B
c
and B
0
are needed
for calibration. Control dosemeters are exposed in the range of 1 R, or 1000 times the
dose of the lower detection limit D
l d
]. The unirradiated control dosemeters B
0
are used to
correct the zero-dose reading which includes the PM dark current, the zero-dose reading
of unirradiated TLD as well as the dose absorbed from cosmic rays and any internal radio-
activity. Additional information about the exposure rate in the shield has to be considered
to enable the estimation of the zero-dose reading and the exposure received during the
storage separately.
The field exposure may be calculated from each TLD reading /, by using the following
equation:
Ci Ii-Io
(11.1)
where D = field exposure in mR, // = read-out of field dosemeter (B
F
), /
t
= mean read-out
of control dosemeters (B
t
) for transit exposure corrected for exposure in the shield,
/j = mean read-out of control dosemeters (B
c
) in the shield exposed to D
x
(calibration
dosemeters), 7
0
= mean read-out of control dosemeters (B
0
) in the shield during field
Application of TLD systems for environmental monitoring 217
exposure, c,- = calibration factor of the single TLD, C
1
= mean calibration factor of control
dosemeters (B
c
).
Here the control dosemeters for the calibration of the batch (c
t
=I>i(/i I
0
)~
l
) are
measured together with the field dosemeters, whereby the individual calibration of each
TLD (Cj = D
2
(l2~A))
-1
) was found before or after the field cycle by an additional
calibration exposure D
2
of the batch.
Individual dosemeter calibration is advantageous if
(a) a permanent identification of individual dosemeters is feasible;
(b) the variation in response within a batch is higher than the variation in response of
a single dosemeter after repeated use (system-dependent parameter);
(c) the variation of response (batch uniformity) is higher than 3%;
(d) only a small number of TLD is involved.
Table 11.7. Properties of light sources in TLD readers.
No. Light source Internal R elative Activity R eading
radioactive light (nCi) time
R eader Scintillator nuclide intensity (s)f
(ncds
- 1
)
1
u i, mnn* Nal (TL) R a.o: 47 , . .
2 Harshaw2000A
N a J ( T L )
^
Q %
^ 100
3 Toledo Plastic "C.p 38.5 5000 0.45
f Light source reading time to achieve a standard deviation of 0.5% (s value from 10
readings).
t Data from the manufacturer Pitman Ltd, UK.
Calculated on the basis of light source 3 as a reference and a statistical error comparison.
For the internal calibration of TLD readers, reference light sources are mainly applied
(table 11.7) which may show significant variations in light intensity and reproducibility
[42, 43] (see also 3.3.5, 4.4 and 7.2.1):
(a) on the basis of a daily check with internal and external light sources the day-to-day
response of the Harshaw 2000 A + B reader was found to overlap the seasonal
fluctuations by about 1% and the Toledo 651 reader of the order of 6% (figure
11.23);
(b) due to nitrogen effects the plastic scintillator in the Toledo reader shows changes
of the reader response of up to 5% during a working day;
(c) the temperature dependence of the light intensity was found to be 0.05% C
_1
for the plastic scintillator and 0.3% "C1 for the Nal (TL) scintillator (figure 11.24);
id) by using the internal light sources, a standard deviation of 0.5% was found after a
reading time of 0.45 s for the Toledo reader and 100 s for the Harshaw reader
(figure 11.25);
(e) due to the
210
Pb content in the Nal (TL) scintillator a time-dependent decrease in
light intensity of 3% yr"
1
was found for the internal light source in the Harshaw
reader.
218
E Piesch
TOLEDO 661 READER
>v^^
/ V v 4
^
HARSHAW 2000 A READER
TEMPERATURE IN HARSHAW 2000 A READER
20
VV^v>
A
f / \ ^
v
A^w/
v
VVW^
T
1977 1978 1979
Figure 11.23. L ongterm fluctuation of external light source check [43].
106
10.
102
j . 100
z
g 98
a
<
UJ
l 96
UJ
or
91
> S T
1
_ i
i
^
K.
. ^
'
1
T |
r-v ii '
1
NaI ( TI | . "c
Nal (TI|.Ro
IN KARS
PLASTIC
HAW READER
SC INT. "C
IN TOLEDO READER
20 30 ( 0
LIGHT SOURCE TEMPERATURE IN t
Figure 11.24. Relative reading of light sources as a function of light source temperature
immediately before readout [43].
The light source calibration of TL D readers may be significantly improved by applying
light sources with a low temperature characteristic, a low standard deviation of the light
intensity and insensitivity to nitrogen gas flow.
Application of TLD systems for environmental monitoring 219
NaI[ Tl ) . Rn ( !
Nal (TI ).
u
C(<> o|
SO 100
Figure 11.25.
time [43].
5 10 20
READING TIME IN SECONDS
Relative standard deviation of the light source reading as a function of reading
11.5. Reproducibility and overall uncertainty of measurement
For a quantitative interpretation of the standard deviation as a function of exposure it is
useful to distinguish between reader- and batch-dependent error sources.
(a) Reader parameters are, for instance, the photomultiplier dark current, the quality
of the heating planchet and deviations in the maximum heating temperature during
the evaluation.
(b) Dosemeter batch parameters are mainly the batch uniformity and the zero-dose
reading dependent on the batch quality and the irradiation/annealing history of the
batch.
A quantitative explanation of the standard deviation against exposure curve was found
by a two-parameter fit given by the following formula:
\ l / 2
(11.2)
1
s(D) = - [2(s
2
0e
+ sl
d
)(D'
u
- D
0
)
2
+ ( 4 + s
2
d
) D
2
)
l/2
(A
1
\"
where s
0e
= relative standard deviation for the dark current a
0
, s
od
= relative standard
deviation for the zero-dose reading of unirradiated dosemeters a
u
= a
u
a
0
, s
rd
= relative
standard deviation for an exposure to 1000>i
dl
(batch uniformity and history), s
re
= rela-
tive standard deviation for an exposure to 1000 D\
d
i (reader properties),/) = exposure in
mR, D
u
= exposure equal to zero-dose reading a
u
of the unirradiated dosemeter batch
after subtraction of a
0
with D
u
= D'
u
D
0
, B = relative standard deviation at high doses,
A = absolute standard deviation at very low doses.
Due to the subtraction of the zero-dose reading the standard deviation is found to be
high for low exposures. The s value decreases as a function of exposure, reaching a
220
E Piesch
z
z
g

100
0.1
V^s,D
ui
l ( D) - 1 0 0
^MJ^T
IV. ]
' for 0-100 D
LDL
s(D)depends on a,b,d
LOWER DETECTION LIMIT
D
uii =
3
"VBu
1
a ZERO D OSE READ ING
b READ-OUT TECHNIQUE
c BATCH UNIFORMITY/CALIBRATION
d ANNEALING/ IRRADIATION HISTORY
- J &2 2
for D-100D
lDl
s(D)depends on b.c.d
io-' 10 10'
&
IO
3
10^
EXPOSURE D IN mR
Figure 11.26. Analysis of the standard deviation against exposure curve [44]; factor of -Jl
only if subtraction of D
u
is based on a single zero-dose reading.
constant value at higher exposures. The exposure range with a constant reproducibility
depends above all on the reader type as well as on the quality of the individual reader.
The test experiment for reproducibility, previously described as a performance criterion
for TLD systems, provides an experimental estimation of the standard deviation in the
dose range of interest (figure 11.26, see also figure 11.2).
In spite of the high uncertainty and scatter in the s values for exposures at the lower
detection limit Djdi the experimental results are sufficiently represented by the theoretical
curve [2, 41, 44].
The uncertainty of measurement can be estimated directly from the statistical error of
the system during the read-out period taking into account the results of field measure-
ments and the read-out of calibration dosemeters. Results of the control dosemeters,
unexposed and exposed to D\, are used to calculate the standard deviations s
u
of the zero-
dose reading and s
r
of the reference exposure Di which should preferably be an exposure
to 1000 D\
A
\.
Instead of using equation (11.2), additional control dosemeters may be directly
exposed to a dose equal or similar to D
t
which is expected from the natural radiation
background at the site during the field exposure period.
The overall uncertainty of measurement is given by statistical and systematic errors
[31, 34-37] which may be estimated for the dosemeter batch and for each monitoring or
read-out period by means of calibration dosemeters. Table 11.8 presents a summary of
error parameters resulting from the performance specifications of dosemeters for environ-
mental monitoring [1, 46] and expected for optimal systems with respect to the measure
of the annual natural background exposure of 70 mR.
Taking into account the experimental results of the standard test programme [2, 45]
the calculated overall uncertainty results in values of 15% or 10 mR related to 70 mR
for the best dosemeter systems (figure 11.27). For the use of n dosemeters at the same
location the statistical error of measurement is reduced by a factor of n
_1 /2
11.6. Interpretation of field exposures
TLD systems are applied to measure time and space variations of the natural radiation
background and to monitor an increase in the background level due to additional
Application of TLD systems for environmental monitoring
Table 11.8. Uncertainty of solid-state dosemeter systems at 70 mR [45].
221
Parameter
Statistical errorst
Dose reading (single dosemeter with
subtraction of zero dose)
Calibration
Single dosemeter
Dosemeter system
Non-linearity
Fading correction
Instability reader/cleaning for glass
Transport dose
Relative error
Permissible
valuef
5
3
5
(3)
3
2
5
(%)
Optimal system
TLD
3
2
1
3
1
3
RPL
5
2
3
3
Systematic errors %
Energy dependence
Direction dependence
Calibration
Fading
Light and humidity influence
Long-term stability
Transport dose, zero dose, etc
Overall uncertainty, Ug
5
%
Statistical ( / R
Systematic (/g
20
tlO
5
5
tlO
5
3
20
29.2
35.3
5
3
5
5
3
3
3
12.9
12
17.6
5
3
5
5
3
5
3
15.7
12.8
20.2
f Requirements for dosemeter systems for environmental monitoring related to a measure-
ment with one dosemeter including calibration.
t Relative standard deviation in per cent.
Maximum measuring errors in per cent.
radiation around nuclear plants or to gaseous effluents released from nuclear power
stations. Two different environmental programmes are generally applied:
(a) monitoring of time and local dependent variations in exposure by using TLD during
short-term field periods of 2 or 4 weeks;
(b) monitoring of local variations in the total annual exposure during field periods of
half a year or a year.
Fluctuations in the background radiation with both time and location are principally
due to changes in soil moisture and surplus water which dilute and shield natural sources
in the ground and have been found to be of the order of 0.7 JLIR h
_1
or 20% of the
terrestrial gamma radiation [11]. Supplementary techniques of calibration and data
correction are applied to eliminate the background component. For the interpretation of
222
E Piesch
30
20
10-
TOTAL UNCERTAINTY U R U S
STATISTICAL UNCERT. UR
LiF:Mg,Ti
H| | H | 1 P | |HA||HA
Li
2
B
4
07
SAMNA
CaF
2
S A MH MH B
CaS0
4
N B
L L L
RPL
[Mil
P PITMAN
S STUDSVIK
N NATIONAL
T TEL EDYNE
A AUTOMAT
B BULB DOSIMETER
35 I 3 1 9 17 IB 26 27 30 28 32 33
DOSIMETER SYSTEM No
Figure 11.27. Calculated overall uncertainty of TLD systems at 70 mR on the basis of
experimental results [2] and data from table 11.8 (after [45]).
TLD data, various approaches [11-15] may be used in order to isolate time-varying
exposures from both components (see table 11.9).
To analyse source fluctuations in the range of 0.1 /iR If
1
, a qualitative estimate of the
exposure is needed, taking into account effluent release, wind frequency direction data
and the stack location distance. For a continuous emission of a noble radioactive gas
mixture from a 100 m stack, the exposure rate decreases approximately with the inverse
of the radius [11].
The assumption of a time- and space-invariant background is not strictly valid because
both the background exposure and its variation may differ significantly from one site to
another and may fluctuate during the seasons. Climatological data have been used with
Table 11.9. Interpretation of environmental measurements.
Source fluctuations
Effluent-wind frequency model
Background fluctuations
Invariance of background with location
Invariance of background with time
Climatic exposure model
Correlation of local exposure to qualitative
estimate using a wind frequency-weighted
1/R model
Exposure changes at reference location equal
to nearby locations
Measure of the total background exposure
prior to or during reactor shutdown
Semi-empirical correction for soil water and
surplus water calculated from local
climatological data
Application of TLD systems for environmental monitoring
223
considerable success to allow for the seasonal fluctuations of the terrestrial gamma
radiation [1, 12, 13, 39].
Long-term field exposure periods of the background radiation result in a mean annual
exposure which significantly compensates for short-term and seasonal fluctuations of the
local exposure.
To determine dose contributions due to the emission of nuclear power stations, the
local individual background dose must be taken into account. For different measuring
stations an average background dose can also form the basis which, by definition, may be
the local dose rate averaged over the area prior to operation of the reactor or a measure-
ment of the local dose at a reference location. Difficulties of interpretation arise, how-
ever, if local fluctuations in the natural background radiation and statistical measuring
errors from both measurements result in calculated negative exposure values.
The measuring uncertainty increases due to subtracting the background dose. The
lowest detectable dose which is found for a difference measurement is thus given by the
amount of the background dose and the quality of the dosemeter system. Figure 11.28
shows the lowest detectable dose which can just be interpreted as a contribution of a
nuclear plant as a function of the difference (Z)
2
/),) where D
2
and D^ are the annual
accumulated dose values at the location of interest and the corresponding background
dose, respectively. For an application in environmental monitoring, therefore, a relatively
high measuring accuracy and reproducibility in the dose range of 10 mrem is required.
Groups of five, three or two dosemeters are used to improve the reproducibility of
measurement at a single field location. The precision of measurements for short-term
exposure periods was found to be better than 3% for 3 mR with LiF by using the average
over five dosemeter results [11]. This permits a quantitative assessment of variations as
small as a few milliroentgens per year in the environmental gamma radiation field.
PERMISSIBLE OVERALL
UNCERTAINTY
OPTIMIZED DOSIMETER
SYSTEMS
DIFFERENCE Dj - D, IN mR
Figure 11.28. Overall uncertainty for a significant increase in the natural background level
of 70 mR.
224 EPiesch
11.7. Practical application
For environmental monitoring, different TLD systems are in use. Generally, there is no
need to differentiate between the soft and penetrating components of the environmental
radiation, if approximate tissue-equivalent dosemeters such as LiF are shielded by
500 mg cm"
2
of plastic. On the other hand, the additional beta sensitivity of unshielded
LiF has to be considered, resulting in an increase of dose reading due to the natural back-
ground radiation, which was found to be (14 + 4)% for a shielding of 50 mg cm"
2
of
plastic and an exposure 2 m above ground.
The energy spectrum from environmental natural 7-rays shows a soft component of
27% of the total photon flux density in the energy range below 100 keV. Therefore, the
dependence of the dosemeter response on energy cannot be neglected if CaF
2
or CaS0
4
detectors are used [16, 19, 22-27, 30, 32]. At Savannah River Plant, CaF
2
dosemeters
are positioned behind a silver and a plastic filter to detect the presence of photons with
energies below 100 keV. For natural background exposure, the average response of the
dosemeters behind the plastic shield was (30 8)% higher than that for the one behind
the silver shield [29]. At Karlsruhe, stray radiation and 'skyshine' from the waste disposal
site near the fence lead to a three-fold over-estimate of unshielded CaF
2
compared to LiF
or CaF
2
shielded by a perforated tin filter [18].
Shielded CaF
2
dosemeters have been used to measure the mean exposure level during
the flight time in different types of aircraft [36]. According to the altitude of the flight,
the exposure level for a DC-10, Boeing 707 or 747 is about five times higher than for a
Boeing 737. The transit exposure of detectors mailed to and from the field site may vary
from between l mR and 100 mR due to contributions from cosmic radiation and/or
additional exposures from radioactive sources during transit [3].
Up to now, different solid-state dosemeters have been used for the monitoring of the
environment of nuclear faculties. At Karlsruhe Nuclear Research Centre, dosemeters
were distributed at more than 250 field sites along the fence and in circles of 1, 2 and
Table 11.10. Measuring accuracy for background measurements in the environ-
ment of Kf Z Karlsruhe.
Dosemeterf
Glass
LiF:Mg,Ti
CaF
2
:Dy
Dose rate meter
Field period
6 month
6 yr
6 month
4 weeks
Direct reading
Mean value of
annual dose (m
5812
644
705.5
594| |
60 6
iR)t
2CJ value
(%)
20
6
9
7
10
+ Glass and CaF
2
: Dy in spherical capsule, LiF: Mg, Ti covered by 50 mg cm"
2
.
t Average of about 80 measuring points along the fence of KfZ with 2a standard
deviation.
Statistical measuring error determined from the deviation of the measured value
of double dosemeters or double measurement at each measuring point.
II Without
41
Ar emission from FR 2.
Application of TLD systems for environmental monitoring 225
3 km diameter. For the interpretation of the dose profile measured at the fence, we have
to consider the emission of
41
Ar from the FR2 reactor in the main direction of the
41
Ar
exhaust air plume, 'skyshine' from the waste storage site and direct radiation from the
Institutes.
The reproducibility found for the measurement of the natural background for the
different dosemeters used is presented in table 11.10. In addition to the TLD, phosphate
glass dosemeters have been in use since 1966 for exposure periods up to 6 yr. Due to the
41
Ar exhaust, an increase of the natural background level has been found to be of the
order of 5 mR yr
-1
at the area boundary and, as expected by calculation, a maximum of
about 20 mRyr"
1
at the northeast corner of the fence. CaF
2
:Dy dosemeters are applied
for short-term monitoring of the fence near the radioactive waste storage site [14, 17, 18].
The reproducibility of dose measurement can be estimated for each individual field
cycle by using the frequency distribution found for the difference in dose readings of two
dosemeters exposed at the same field site.
A comparison of LiF and ionisation chamber results [28, 35] shows that the average
agreement for the total period indicated is within 0.5% and the mean difference for a
4 week measurement period is 2.7%. It is believed that the overall accuracy for these
types of terrestrial 7-ray plus cosmic-ray measurements is about 5% (standard deviation).
The method for analysing TLD data collected fortnightly or monthly makes use of
the frequency plot and log normal probability plot for each location (figure 11.29) [40].
20 30 U) 50 60
SAMPLIN6 PERIOD
2 20 1.0 60 80 98 99
CUMULATIVE PERCENT
Figure 11.29. Frequency and log normal probability plot for a location in the Hanford
environs [40].
226 EPiesch
From the log normal plots the geometric mean (x
g
:50% intercept) and geometric
standard deviation or slope (a
g
: ratio of 84% to 50% intercept) were determined. The 95%
probability intercept of the plotted data means that 95% of all measurements are
expected to be less than this value.
A semi-empirical method for the estimate of the time-varying background exposure
expected at a particular location is based on detailed soil moisture considerations [12,13].
The climatological model takes into account local meteorological and hydrological data.
Variations in the surplus water (difference between precipitation and evaporation of the
water content of the soil) mainly reflects natural background changes. The model agrees
with the TLD results (accuracy 3.5%) within 5% in 75% of the cases, 10% in 94% of the
cases and 15% in all cases [13].
References
1 American National Standard 1975 Performance, testing and procedural specifications for thermo-
luminescence dosimetry (environmental applications) ANSI N545-1975
2 Piesch E and Burgkhardt B 1978 RTL und RPL systeme im Bereich kleiner Dosen: Vorstellung
eines Testprogrammes und Ergebnisse an 43 Systemen Rep. KfK 2626
3 Burke G de P, Gesell T F and Becker K 1977 Second international intercomparison of environ-
mental dosimeters under field and laboratory conditions Proc. 5th Int. Conf. on Luminescence
Dosimetry, Sao Paulo, February (I Physikalisches Institut, Universitat Giessen), p365
4 1975 Environmental Radiation Measurement. NCRP Rep. No 50
5 Piesch E 1974 Solid state dosimetry - 10 years of routine use and development Kerntechnik 16 71
6 Burgkhardt B, Herrera R and Piesch E 1976 Fading characteristics of different thermoluminescent
dosimeters Nucl. Instrum. Meth. 137 41
7 Burgkhardt B, Herrera R and Piesch E 1977 Long-term fading experiment with different TLD
systems Proc. 5th Int. Conf. on Luminescence Dosimetry, Sao Paulo, February (I Physikalisches
Institut, Universitat Giessen), p75
8 Burgkhardt B and Piesch E 1978 The effect of post-irradiation annealing Nucl. Instrum. Meth. 155
293-9
9 Randall I T and Wilkins M E F 1945 Phosphorescence and electron traps Proc. R. Soc. A 184 366
10 Niewiadowski T 1976 Comparative investigations of characteristics of various TL dosimeters, part
II, Low dose measurementsNucleonika 21 1097
11 Burke G de P 1972 Thermoluminescent dosimeter measurements of perturbations of the natural
radiation environment Proc. 2nd Int. Symp. on Natural Radiation in the Environment p305
12 Burke G de P and McLaughlin J E 1974 Performance criteria for environmental radiation monitor-
ing with TLD systems IEEE Trans. Nucl. Sci. NS-21 444
13 Burke G de P and Marcin D G 1973 Interpretability of TLD measurements made in environs of a
nuclear power reactor Trans. Am. Nucl. Soc. November, p537
14 Piesch E 1977 Long-term dosimetry with solid state dosimeters for personnel and environmental
monitoring Kerntechnik 19 27
15 Lindeken CL et al 1972 Geographical variations in environmental radiation background in the
United States Proc. 2nd Int. Symp. on Natural Radiation in the Environment p317
16 Burke G de P and Shambon A 1972 Investigation of thermoluminescent dosimeters for environ-
mental monitoring Rep. HASL-265
17 Burgkhardt B and Piesch E 1972 Use of CaF
2
thermoluminescent dosimeters for measuring the
natural background radiation Kerntechnik 14 128
18 Burgkhardt B, Piesch E and Winter M 1973 Long-term use of various solid state dosimeters for
environmental monitoring of nuclear plants - experience and results Proc. 3rd Int. Congr. IRPA,
Washington p394
19 Shambon A 1974 CaSO:Dy TLD for low level personnel monitoring Rep. HASL-285
Application of TLD systems for environmental monitoring 227
20 Konig LA, Piesch E and Winter M 1974 Die 7-Strahlenbelastung der Umgebung des Kern-
forschungszentrums Karlsruhe Proc. Jahrestagung des Fachverbandes fur Strahlenschutz, Helgoland
p615
21 Becker K 1974 Stability of film and thermoluminescence dosimeters in warm and humid climates
Atomkernenergie 23 267
22 Becker K 1974 Integrating dosimeters for environmental radiation assessment Rep. Conf-741219-1
23 Duftschmid K E1975 Evaluation of CaF
2
:Dy bulb thermoluminescent dosimeter for environmental
radiation monitoring around nuclear facilities Rep. SGAE Ber. no 2462, St-45/75
24 Duftschmid K E and Strachotinsky Ch 1974 Entwicklung und Erprobung hochenergetischer Dosi-
metersysteme in Hinblick auf die Erfassung der radioactiven Umgebungsstrahlung in Osterreich
Rep. SGAE Ber. no 2543, ST-49/75
25 Szabo P P 1975 Investigation of properties of CaS0
4
:Dy thermoluminescent dosimeters Rep.
KFKI-75-1
26 Budd T 1976 The properties of CaF
;
: Dy used as a thermoluminescent dosimeter at low doses Rep.
AERE-R8385
27 Gwiazdowski et al 1974 The comparison of long-term parameter stability of various RTL detectors
used for measurements of natural background radiation Proc. 4th Int. Conf. on Luminescence
Dosimetry, Krakow, August (Krakow: Institute of Nuclear Physics), p 989
28 Lowder W M 1977 Environmental radiation dosimetry with ionizing chambers and thermo-
luminescence dosimeters Proc. 4th Int. Congr. IRPA, Paris vol 1, p59
29 Lorrain S, Piaggio-Bonsi R and Portal G 1977 Stabilite de divers sulfates de calcium RTL destines
aux mesures d'environnement Proc. 4th Int. Congr. IRPA, Paris vol 4, pl 249
30 Vana N, Aiginger M and Erath W 1977 Measurement of doses in the 1 mrad range by means of LiF,
CaF
2
and CaS0
4
dosimeters Proc. 4th Int. Congr. IRPA, Paris vol 4, p 1253
31 Piesch E and Burgkhardt B 1977 TLD and RPL dosimeter performance criteria for environmental
monitoring based on type test and long-term experience Proc. 4th Int. Congr. IRPA, Paris vol 4,
p i 245
32 Toombs G L and Paris R D 1977 Comparative response of thermoluminescent dosimeters in
environmental monitoring situations Proc. 4th Int. Congr. IRPA, Paris vol 2, p525
33 Jones AR 1977 The application of an automatic thermoluminescence dosimetry system to
environmental gamma dosimetry Rep. AECL-T8 35
34 Burke G de P and Gesell T F 1976 Error analysis of environmental radiation measurements made
with integrating detectors Proc. NBS SP456, pl 87
35 McLaughlin J E 1976 Environmental radiation measurements Proc. NBS SP456, p233
36 Kramer R, Regulla D F and Drexler G 1977 TLD environmental radiation monitoring: processing,
experiences and data interpretation Proc. 5th Int. Conf. on Luminescence Dosimetry, Sao Paulo,
February (I Physikalisches Institut, Universitat Giessen), p298
37 Piesch E and Burgkhardt B 1977 Properties of TLD and RPL systems for environmental monitor-
ing Proc. 5th Int. Conf. on Luminescence Dosimetry, Sao Paulo, February (I Physikalisches
Institut, Universitat Giessen), p335
38 Christensen P, Botter-Jensen L and Majborn B 1973 Influence of ambient humidity on TL dosi-
meters for personnel monitoring Proc. Regional Conf. on Radiation Protection, Jerusalem
39 de Planque G 1980 TLD measurements and model calculations of environmental radiation
exposure rates Proc. 3rd Symp. on Natural Radiation in the Environment CONF 780422, vol 2,
p987
40 Fix J J and Blumer PJ 1977 Thermoluminescent dosimeters (CaF
2
:Dy) measurements of the
Hanford environs, 1971-1975 Rep. BNWL-2140
41 Burgkhardt B, Piesch E and Seguin H 1980 Some results of a European interlaboratory test pro-
gramme of integrating dosimeter systems for environmental monitoring Proc. 5th Int. Conf. IRPA,
Jerusalem and Proc. 6th Int. Conf. on Solid State Dosimetry, Toulouse, April. Nucl. Instrum.
Meth. 175 No 1 (September)
42 Nollmann C, Burgkhardt B and Piesch E 1979 Parameters effecting the overall calibration accuracy
in TLD 700 thermoluminescence dosimetry Nucl. Instrum. Meth. 161 449-58
43 Burgkhardt B and Piesch E 1981 Systematical and statistical errors of the TLD reader calibration
with reference light sources Health Phys. 40 549
228 EPiesch
44 Burgkhardt B and Piesch E 1980 Reproducibility of TLD-systems - a comprehensive analysis of
experimental results Proc. 6th Int. Conf. on Solid State Dosimetry, Toulouse, April, Nucl. Instrum.
Meth. 175 No 1 (September)
45 Piesch E 1979 Anforderungen an Festkorperdosimeter zur Messung der integralen Gammadosis in
der Umgebungsuberwachung Proc. Fachgesprdch Uberwachung der Umweltradioakrivitat p84
46 'Technische Empfehlungen fur Festkorperdosimeter zur Umbegungsuberwachung'desArbeitskreises
'Dosismessung externer Strahlung' des Fachverbandes fur Strahlenschutz, in Vorbereitung
47 Shambon A 1972 Some implications of a laboratory study of LiF dosimeters for environmental
radiation measurements Rep. HASL-251 (New York: USAEC)
48 Binder W, Disterhoft S and Cameron J R 1969 Dosimetric properties of CaF
2
Dy Proc. 2nd Int.
Conf. on Luminescence Dosimetry, Gatlinburg, Tenn., September 1968. USAEC Rep. CONF-
680920, p43
49 Becker K 1973 Solid State Dosimetry (Cleveland, Ohio: CRC Press)
50 Burke G de P 1972 Investigations of CaF
2
:Mn thermoluminescent dosimetry system for environ-
mental monitoring Rep. HASL-252 (New York: USAEC)
51 Brinck W, Gross K, Gells G and Partridge J 1975 Special field study at the Vermont Yankee
nuclear power station, Personal communication (US Environmental Protection Agency,
Cincinnati, Ohio)
52 Aitken M J 1969 Low-level environmental radiation measurements using natural calcium fluoride
Proc. 2nd Int. Conf. on Luminescence Dosimetry, Gatlinburg, Tenn., September 1968. USAEC
Rep. CONF-680920,p281
53 Schulman J H 1967 Survey of luminescence dosimetry Luminescence Dosimetry, Symp. Ser. 8
ed. F H Attix (Washington: USAEC), p3
54 Denham D H, Kathren R L and Corley J P 1972 A CaF
2
: Dy thermoluminescent dosimeter for
environmental monitoring Rep. BNWL-SA-4191 (Battelle Northwest Laboratories, Richland, WA)
55 Yamashita T, Nada N, Onishi H and Kitamura S 1971 Calcium sulfate activated thulium or
dysprosium for thermoluminescence dosimetry Health Phys. 21 295
Applied Thermoluminescence Dosimetry. Eds M Oberhofer and A Scharmann
1981 ECSC, EEC, EAEC, Brussels and Luxembourg
12
Applications ofTL materials in neutron dosimetry
J A DOUGLAS
12.1. Introduction
Because of the complex nature of neutron dosimetry some background information is
provided. The two-stage process involved in transferring energy from neutrons to matter
is discussed and the reactions categorised. The choice of appropriate parameters to
monitor the effect of interest is then presented before the terms used in neutron dosi-
metry are defined.
The response of TL materials to neutrons depends greatly on the neutron energy so
the dosimetry of thermal neutrons is dealt with separately from that of intermediate and
fast neutrons. Possible methods of increasing the low response to fast neutrons are
surveyed together with possible applications of these techniques. Finally some of the
possible future developments for fast neutron dosimetry are discussed.
12.2. Neutrons and dosimetry
The dosimetry of neutron radiations is not as simple or as precise as the dosimetry of
gamma radiations because of the numerous energy transfer processes involved and the
variation of the reaction cross sections with energy. The transfer of energy from neutrons
to a medium is a two-stage process involving the production of ionising particles or
radiation either in the medium or in the material adjacent to it. These secondary
radiations dissipate the transferred energy by undergoing electronic and nuclear collisions
in the medium.
12.2.1. Neutron reactions
Neutron reactions producing ionising secondaries can be divided into the following
categories:
(1) Scattering
(a) Elastic: the momentum and kinetic energy are conserved.
(b) Inelastic: the neutron is re-emitted with a reduced energy, leaving the target nucleus
in an excited state. The nucleus returns to the ground state by emitting a gamma-
ray.
230 J A Douglas
(2) Capture
(a) Radiative: the excess energy resulting from the absorption of the neutron is
released almost instantaneously by the nucleus as a capture gamma-ray.
(b) Particle emission: if the neutron energy is high enough a transmutation will occur
with the ejection of a proton or alpha particle, e.g.
6
Ii (n, a)
3
H and
10
B(n, a)
7
l i .
(c) Fission: the neutron is absorbed and the nucleus splits into two fragments plus
neutrons.
(d) Spallation: the nucleus is fragmented ejecting several particles and nuclear frag-
ments. Only significant above 20 MeV.
These reactions can occur either in a TL detector or its environment and will affect its
response. Similarly they can occur in the material being monitored by the dosemeter.
Most chemical and biological effects, for a given type of radiation, are directly related
to the energy absorbed. However, the microscopic spatial distribution of this absorbed
energy is also important, especially in biological material where a high rate of energy
deposition along the track of an ionising particle is more effective at killing a cell than is a
low rate. Thus, in addition to the absorbed energy, the energy spectrum of the incident
neutron is important in chemical and biological systems since this determines the rate of
energy deposition by the recoil particles.
The damage caused by neutrons to materials with a lattice structure is closely related
to the number of atomic displacements resulting from collisions, which in turn is related
to the number of incident fast neutrons. The incident neutron fluence and energy
spectrum are therefore good parameters to specify the damage in this case.
12.2.2. Terminology
The following definitions are mainly taken from ICRUf 26 [44].
(1) Fluence, <$>, of particles is the quotient of dW by da, where djV is the number of
particles which enter a sphere of cross-sectional area da.
(2) Fluence rate, 0, is the quotient of d< by dr, where d<I> is the increment of particle
fluence in the time interval dr.
(3) Energy fluence, ^ , of particles is the quotient of dfl by da, where d
fl
is the sum
of the energies, exclusive of rest energies, of all particles which enter a sphere of
cross-sectional area da.
(4) Absorbed dose, D, is the quotient of de by dm, where de is the mean energy im-
parted by ionising radiation to the matter in a volume element, and dm is the mass
of the matter in that element. (The unit is the rad =100 erg g"
1
. The SI unit is the
gray, 1 Gy = 1 J kg
- 1
= 100 rad.)
(5) Kerma dose, K, is the quotient of dE
ti
by dm, where dE
n
is the sum of the initial
kinetic energies of all the charged particles liberated by indirectly ionising particles
in a volume element and dm is the mass of the matter in that element. The units
are the same as absorbed dose. Note that kerma is independent of the complexities
of the energy transported by charged particles. It also has a defined value for a
f International Commission on Radiation Units and Measurements.
Applications of TL materials in neutron dosimetry
231
sample of vanishingly small size which is embedded in some other material or in
free space. This is not the case with absorbed dose. It is therefore often convenient
to refer to a value of kerma for a specified material in free space or at a point in a
different material. This is the value which would be obtained if a small mass of the
specified material were placed at the point of interest.
Because of the finite range of secondaries, the two steps of energy transfer
energy absorbed from the secondaries (absorbed dose) and the energy transferred
to the secondaries (kerma) take place at different points in the medium. Under
charged particle equilibrium, kerma and absorbed dose are essentially the same.
(6) Dose equivalent, D E, is the risk-related quantity recommended by national and
international bodies for the control of personnel exposed to neutrons. Dose
equivalent is the product of absorbed dose, D, the quality factor, Q F, and other
modifying factors. For external radiation the modifying factors are unity, except
for the eyes. The Q F is also unity for x- and gamma-rays but is related to the linear
energy transfer of the more densely ionising particles and takes into account the
different biological effectiveness. Fluence to dose-equivalent conversion factors at
specific energies and depths in soft tissue have been published [4, 43, 83]. Figure
12.1 is taken from the data in ICRP 21 [42] in which the dose equivalent per
n cm"
2
was based on the maximum dose equivalent in a tissue-equivalent sphere
30 cm diameter with a unidirectional broad beam of monoenergetic neutrons. The
ideal personnel neutron dosemeter would have a fluence response of that shape.
1-7

N
E
< j
E
01
i _
"c
CD
a
>
'u
cr
LU
a>
c/l
o
o
IU
10"
8
10"
9
,
-
-
r ' I i
i i i i i i il
o
i
0
1 1 1 11
001 10 0-1 1
Neutron Energy (MeV)
Figure 12. 1. Fluence to dose equivalent conversion factors [42]. o, Snyder [84].
(7) Linear energy transfer, LET , of charged particles in a medium is the quotient of dE
by d/ where dE is the energy lost by the particle while traversing a distance d/.
The unit is usually keV jum
-1
, or alternatively MeV cm
2
g"
1
.
(8) Lethargy, this is an alternative way of representing neutron energy often used by
reactor physicists. The lethargy C/is defined by the equation
dU=-dQnE) = -dE/E.
232 J A Douglas
Therefore
U=\n(E
0
/E\
E
0
is usually taken as 10 MeV. Lethargy increases as neutron energy decreases, e.g.
Energy Lethargy
10 MeV
Thermal (0.025 eV)
0
l n( 4xl 0
8
) =19. 8
Fluence can be defined per unit lethargy interval, but it is often plotted against
In (energy interval). Figures 12.2(a) and (b) show a \\E spectrum plotted as (a) flux
per unit energy and (ft) flux per unit lethargy.
0001 001 0-1 1 ,u
0
.
0 0 1 0
.
01 0
.
:
T
10
Energy (MeV) Energy (MeV)
Figure 12.2. 1/E spectrum plotted in terms of (a) fluence per unit energy interval,
(b) fluence per unit lethargy interval.
(9) Energy groups. It is sometimes convenient to subdivide neutrons into the following
compartments according to their energy:
(a)
(b)
(c)
(d)
Thermal: Neutrons which are in thermal equilibrium and having a Maxwellian
distribution of velocity with a mean at 0.025 eV. Generally neutrons with
energy < 0.5 eV are called thermal.
Intermediate: 0.5 eV-l 0 keV. Recoil protons < 10 keV are not ionising.
Fast: 10 keV-10 MeV. Mainly elastic scattering in tissue.
Relativistic: > 10 MeV. Inelastic scattering and capture.
12.3. Thermal neutron detectors
Neutrons are usually accompanied by gamma radiation. Two detectors of widely differing
neutron and gamma-ray sensitivities are used to separate them. Table 12.1, which was
compiled by Ayyangar et al [6], is a list of thermal neutron responses of various TL
materials as quoted in the literature. There are many factors which can affect the reading
from a phosphor and may account for some of the apparent discrepancies in the table.
Some of these are listed below:
Applications O/TL materials in neutron dosimetry 233
(a) The read-out system. The glow curves resulting from gamma and neutron irradiations
are not necessarily the same [20]. The relative response thus depends on the basis of the
comparison. Phosphors can be heated either using ramp heating (temperature raised at a
constant rate) or plateau heating (temperature raised quickly to a pre-set value and then
held for a pre-set time at that temperature, and then possibly repeated at one or two
higher temperatures). In the case of ramp heating different results can be obtained by
using peak height or the integrated light output. In the case of plateau heating the use of
a pre-read-out heating phase and its temperature will affect the apparent response. The
type of photomultiplier could also affect the results since the spectrum emitted by a
phosphor may depend on the type of incident radiation (see 12.3.1).
(b) Supralinearity. Deviations from linearity in the light output occur at different doses
for gamma and thermal neutron radiations. How this is allowed for will affect the quoted
response.
(c) Detector self-shielding. Some thermal neutron-sensitive phosphors contain atoms with
a very high cross section (e.g. 945 b for
6
Li). In these cases most of the neutrons will be
absorbed within a short distance of the surface and the rest of a thick phosphor will be
inaccessible. (0.1 mm of TLD 600 absorbs 50% of incident thermal neutrons.) The
thickness of a phosphor thus affects its apparent response. So the neutron sensitivity of
TL material should always be quoted for a 'thin' detector. The neutron response of a
detector will depend on its orientation, unless it is a sphere, since it is the cross-sectional
area with respect to the neutrons, not the volume, which is important.
(d) Batch-to-batch variation. Small changes in the concentration of impurities with high
cross sections (such as the amount of
6
Li in TLD 700) will have a significant effect on the
response to thermal neutrons. In spite of the apparent variations in the reported
responses, it is possible to choose from table 12.1 phosphors of high and low thermal
neutron responses which might be suitable to measure the components in a mixed field.
The following have acceptably high responses to thermal neutrons:
6
LiF either as TLD 600 or TLD 100
Li
2
B
4
0
7
:Mn
CaS0
4
(Mn,
5
Li).
There are many with a low response.
The ideal detector or combination of detectors should have the following
characteristics:
(a) the response to neutron and photon radiations should be independent of energy;
(6) the response should be linear with dose;
(c) the fading should be small;
(d) the sensitivity should be adequate to enable doses to be determined for the separate
components of a mixed field to the required precision;
(e) the phosphors should be easy to use and re-use;
(/) they should be easy to manufacture and cheap.
The characteristics of the three phosphors with the highest thermal neutron responses
will now be examined.
134 J A Douglas
Table 12.1. Comparison of the thermal neutron responses of various TL materials as quoted
in the literature (compiled in [6]).
TL phosphor Thermal neutron response
( R/ 10
, o
ncnr
2
)
Mg
2
Si0
4
:Tb
CaSO : Dy (Harshaw)
CaS0
4
: Dy (DRP)
CaS0
4
: Tm(DRP)
CaSO:(Dy,
6
Li) (DRP)
CaS0
4
: (Mn, Li)
CaS0
4
:(Mn, "Li)
CaS0
4
: Tm
CaF
2
:Mn (Harshaw)
CaF
2
:Mn (EG & G)
CaF
2
:Mn (Conrad)
CaF
2
(MBLE)
CaF
2
(fluorite)
CaF
2
: MnTLD08 (Yugoslavia)
CaF
2
:Mn (Philips)
CaF
2
:Dy TLD 200 (Harshaw)
LiF TLD 700 (Harshaw)
LiF 7 (Conrad)
LiF TLD 100 (Harshaw)
LiF (Conrad)
LiF TLD 600 (Harshaw)
LiF 6 (Conrad)
BeO
Li
2
B
4
0
7
:Mn (Harshaw)
0.21 [6]
0.52 [6]
0.38 [6]
0.21 [6]
6.2 [6]
100 [46]
1050(46)
0.23 [9]
0.6 [6]
0.1-0.13 [76]
0.58 [94]
0.2 [76]
3.5 [1]
0. 16(78]
0.77 (theoretical [73])
1.050.08 (experimental [73])
0.070.01 [75]
0.59 [6]
0. 5-0. 65(76]
1.1(6]
0. 7(81]
0.87-0.96 [76]
1.0(78]
2. 5(25]
1.3 [60]
23 [25]
330 [6]
200(100]
200[99]
220 [81]
535 [76]
310(96]
65( 78]
490( 25]
360[60]
165 [81]
1520 [6]
870[23]
2190(96]
1200-1700(76]
2650 [25]
0.45 [6]
0. 130. 08[79]
0. 20(94]
0. 17-0. 29(79]
0. 2(78]
0. 50. 5[51]
390(6]
230[76]
Applications of Th materials in neutron dosimetry 235
TL phosphor Thermal neutron response
(R/ l O^ncm"
1
)
L i
2
B
4
0
7
:Mn(DRP)
L i
2
B0
7
:Mn (Wallace)
L ijB0
7
:Mn (Christensen)
L i,B
4
0
7
:Mn (Brunskill)
390 [6]
670[96]
300 [60]
420[22]
400500 [17]
12.3.1. Lithium fluoride
Lithium has two naturally occurring stable isotopes,
6
Li and
7
L i, and lithium fluoride is
available with three different isotopic compositions, namely:
natural LiF
enriched
6
IJF
enriched
7
l i F
(Harshaw TL D 100, 7.4%
6
L i)
(Harshaw TL D 600, 95.6%
6
Ii )
(Harshaw TL D 700, ~ 0.010.04%
6
l i )
The main contribution to the thermoluminescence after thermal neutron irradiations
comes from the aparticles and tritons produced from the
6
L i(n, a)
3
H reaction. Because
of the very high capture cross section of
6
L iF for thermal neutrons (945 b compared
with 0.033 b for
7
Ii (n, 7)
8
L i) it has the highest thermal neutron sensitivity of any
phosphor. Figure 12.3 [91] shows that the
6
L i capture cross section is inversely pro
portional to the neutron velocity, V, apart from a resonance at 0.255 MeV. The cross
Energy (MeV)
10
5
10'
10
3
o
m
c
10
2
u
0)
I
2 10
o
4
1
10'
: '
:

r._
-*\
j . ^

=
.
L.
' "
^
10"
8
10"
7
"' I I ' '
A
^>,
1 11
^
^ ^
^-
."I I .
10"
6
) '
/


10"
5
11 I I I I | r
1 ~~~~
1
|l
I
1
l]
1
M
1 1
I |
1 1
1 1
| 1
|
1
s^l
1 ^ ^
V
\
.!>
10"
1 1 l l l l l |
"
3
Cd( n
6
L i ( n
197. ,
Aul n
~-
L
TH
r-rr
10
Tf' cd!
a)
3
H
-
rf^Aui
, , ,
-
_
"

_
:
-
:
-
'.
-
:
;
LLU
10"' 10"
J
1 10 10
2
10"
2
10"
1
Energy I MeV)
Figure 12.3. Neutron capture cross sections of
6
L i, "
3
Cd and ' "Au (after [91]).
236 J A Douglas
sections of cadmium and gold, which are shown for comparison, are also proportional to
1/V for low energies. It can be seen that the energy of the cadmium cut-off is not the
same as the gold resonance and that there is no pronounced cut-off for
6
Li. Although
cadmium shields and gold activation foils are both used to measure thermal neutrons
they do not measure precisely the same spectrum. Some intermediate-energy neutrons
are included in measurements made with gold foils and
6
Li detectors. The cadmium
cut-off is usually taken as 0.5 eV.
The a-particles (2.07 MeV) and tritons (2.74 MeV) from the
6
Ii(n, a)
3
H reaction have
a higher LET than x- and gamma radiations, so the emission spectra, supralinearity and
glow curves are different in the two cases.
Figure 12.4 shows that the optical spectra emitted by
6
LiF after irradiation of a-
particles contains more red light than after beta and gamma irradiations. Since the TL
effect from thermal neutrons is due to a-particles and tritons, the emission spectrum after
neutron irradiation will also contain longer wavelengths than after beta or gamma
irradiations.
100-
(/)
c
CD
c
.c
en
_ i
_ i
1-
0)
>
_^.
a
CD
tr
80
60
40
20
/ / " "V
ft \ .
/ ' >
/ /
II
/ /
/ '
/ /
/ /
/ /
/ /
/ / ' .
/ '
/ ' '
/ / .'
/ / /
/ / /
//.'
/ / .
11/
II:
/ '
II:
II:
//:
1 1
V
\\
\\
\\
V a/
v
\ \ . ' '
\ \
"" Y\
ft\
\ ^
\ \
X. X
^^o^
i i i \ - 1
300 350 400 450 500 550 600 650
Wavelength (nm)
Figure 12.4. Optical emission spectrum of the main TL peak of LiF:Mg,T i after exposure
to different types of radiation.
The departures from linearity of the responses of
6
LiF and
7
LiF to gamma and
neutron radiations are shown in figure 12.5 [70]. The onset of supralinearity in the
response to gamma radiations is different for
6
LiF and
7
LiF. The neutron response of
6
LiF remains constant to a much higher light output. Because the density of ionisations
is high along the tracks of a-particles and tritons, the
6
LiF is effectively operating in the
supralinear region even for very low doses. There is a danger of ambiguity when
expressing the neutron response in terms of apparent -ray dose. Care must be taken to
make it clear whether it is the actual dose of 7-rays which would produce the same
Applications OF TL materials in neutron dosimetry
Thermal Neutron Fluence in n/cm
237
10
c
10
s
10
10
10
11
10
12
10
,13
10
,14
1000
100
lihli|""l ihlili|""l i l i l i l f " ! ! lihli'i""
1
, ,\,\Mf'"\ !hI'IMI
11
"
1
! ,Wilji
10' 10
J
10" 10
3
10 10'
Gamma Equivalent Neutron Exposure in R
0 ' 0 0 1 Ii i i mill i i i mill I i i i null i I i I
10' 10
z
10
J
10
4
10
3
10 10' 10
137
Cs Gamma Exposure in R
Figure 12.5. The variation with exposure of the relative responses of TLD 600 and TLD
700 to neutron and gamma irradiations. , neutron response TLD 600; o, gamma response
TLD 600; A, gamma response TLD 700 (after [70]).
luminescence or whether it is the dose based on the 7-ray response in the linear region
that is used.
Figure 12.6 [58] shows the differences in the glow curves after neutron and photon
irradiations. The positions of the '210 C peaks are slightly different but the main differ-
ence is that the ratio of the height of the '285 C peak to that of the ' 210C peak is
greater after neutron irradiations than after gamma irradiations. This effect has been
noted by many other workers [5, 20, 35, 59]. Attix [3] was the first to suggest the
application of this phenomenon to personnel neutron dosimetry and further studies in
this direction have been made by Nash and Johnson [64] and Budd etal [19]. Nash and
Johnson use linear heating and record peak heights whereas Budd et al use plateau heating
and record the integrated light output. Both systems produce two simultaneous equations
which can be solved for the neutron and 7-ray doses.
Budd et al have also noted that the height of the '285 C' peak relative to the '210 C
peak varies with photon energy. The ratio for 48 keV x-rays is approximately twice that
for radium 7-rays. Uncertainty of the photon energy in a mixed field will increase the
uncertainty of the neutron dose. However, the error in the total neutron plus 7-ray dose
is acceptable for personnel dosimetry.
Fading of the higher temperature peaks is likely to be small. However, departures from
linearity begin at lower doses (at ~30 rad for gamma radiation and ~300 rad equivalent
for thermal neutron irradiation [20] compared with ~300 and ~2000 rad respectively,
for the '210 C peak [70]). These disadvantages are outweighed by the gain in using only
238 J A Douglas
Ti me [ s e e s ) Temperature I C)
Figure 12.6. Glow curves from TLD 600 after gamma and neutron irradiations, (a) Linear
heating (2C s"' ramp), (6) plateau heating [58).
one detector and avoiding the possibility of confusing two detectors of identical appear-
ance. The effect of fast neutrons on the '285 C peak will be briefly mentioned in 12.4.
There has been some confusion in the literature as to whether the effects of neutron
and gamma irradiations are additive. Wallace et al [97] found that vapours were released
in some of the phosphor containers which induced fading and created the illusion of
non-additivity.
The damage to
6
LiF caused by neutrons is cumulative since each
6
Li(n,a)
3
H reaction
reduces the number of
6
Li nuclei available for subsequent neutron reactions. In addition,
there is damage along the tracks of a-particles and tritons due to the high ionisation. This
damage will affect future luminescence only when a new track crosses an old one. The
probability of this happening is small until the phosphor has received a large cumulative
dose(~10
10
ncnf
2
).
12.3.2. Lithium borate
Lithium tetraborate (manganese-activated) was one of the earliest low atomic number
alternatives to LiF [49, 80]. It is simpler to handle as it does not require annealing after
reading and it is more nearly tissue-equivalent for photon irradiation than LiF. How-
ever, it has the disadvantage of being hygroscopic with a consequent high rate of fading.
Christensen et al [22a] report 30% fading after storage in moist air at 25 C for two
months compared with no observed fading after storage in dry air for the same time and
temperature.
Lithium borate can also be activated by silver. Thompson and Ziemer [93] found that
the most favourable energy response was obtained at a concentration of about 0.1%. This
is less hygroscopic than the manganese-activated phosphor and has good stability when
stored in the dark but fades rapidly when exposed to uv light [65, 93].
Applications of TL materials in neutron dosimetry 239
The light emitted from silveractivated borate has maxima at 290 and 365 nm, while
the manganeseactivated phosphor has a broad emission spectrum with a maximum at
600 nm, which makes it difficult to distinguish between the phosphor luminescence
and the infrared blackbody radiation. It should be possible with the appropriate photo
multiplier to detect lower levels of radiation with L i
2
B
4
0
7
: Ag than with L i
2
B
4
0
7
:Mn.
The responses of both silver and manganeseactivated versions are linear for gamma
radiations up to about 10
2
rad and for thermal fluences up to about 10" n cm"
2
[52, 93].
The glow curves after gamma and neutron irradiations are the same in L i
2
B
4
0
7
:Mn, a
simple peak at ~190C [52], but in the silveractivated form there is an extra pronounced
peak at 350 C following exposure to neutrons [87]. The usefulness of this peak for
dosimetry in mixed fields could be beneficially pursued.
The response of activated natural lithium borate is due to the presence of
6
L i and
10
B,
both of which capture neutrons and emit particles. R T Brunskill (private communica
tion) has now produced isotopically enriched
7
Li2
11
B
4
0
7
:Mn in powder form so that
matched neutronsensitive and neutroninsensitive lithium borate detectors are available.
12.3.3. Calcium sulphate
The three main activators which have been used with CaS0
4
are manganese, dysprosium
and thulium. The manganeseactivated phosphor fades very rapidly (~30% in 10 h and
40% in 1 d [14, 32, 54]) and is thus only suitable for short laboratory exposures. The
glow curves for dysprosium and thuliumactivated phosphors are similar with a main peak
at 220 C, which is consistent with the reported low fading rates of 12% in 1 month at
25 C [88, 89, 101]. The thermal neutron responses of CaS0
4
:Dy and CaS0
4
:Tm are
both low (0.38 and 0.23 equivalent rad per 10
10
n cm"
2
, respectively, for 0.05% activator)
[6, 7]. This is because the main TL process is neutron capture by the activators, which are
present in low concentrations. The capture cross sections are 930 and 130 b, respectively.
The response of CaS0
4
:Tm to 7rays and charged particles is ~35 times that of LiF [9]
and that of CaS0
4
:Dy is slightly higher [101]. This high sensitivity plus the low response
to thermal neutrons makes them good detectors of the 7ray component in mixed
neutrongamma fields.
The high sensitivities of CaS0
4
phosphors to charged particles encouraged workers to
mix them with compounds having high thermal neutron capture cross sections to obtain
phosphors with high thermal neutron sensitivities.
6
L i salts are an obvious choice, and
they have been tried with CaS0
4
:Mn [46], CaS0
4
:Dy [6] and CaS0
4
:Tm [9, 45, 89].
Intimate mixtures are essential, so finely powdered phosphors and nonluminous lithium
salts are used. The 7ray sensitivity of such mixtures is essentially proportional to the
concentration of the phosphor. The slight deviation is due to differences in effective
atomic number. The neutron response is a maximum when the proportions are roughly
1:1. Figure 12.7 [89] shows the responses of varying mixtures of CaS0
4
:Tm and
6
L iF.
Mixtures with CaS0
4
:Mn can have a thermal neutron sensitivity about 10 times that
of
6
L iF but the fading rate is still as high as for CaS0
4
:Mn [46].
Ayyangar et al [6] have reported that mixing
6
L i
2
C0
3
with CaS0
4
: Dy transfers energy
from the 210 C glow peak to that at 130 C (figure 12.8). This has the unfortunate effect
of increasing the fading to ~60% in a month. Mixtures of CaS0
4
:Tm with L i
2
S0
4
[9]
and with
6
L iF [89] do not appear to increase the rate of fading. The response of a 40%
240
6
L iF 20 0 60 80
CaSCVTm Content,wt %
CaS0
4
:Tm
Figure 12.7. TL response of CaSO:Tm,
6
LiF mixtures to thermal neutrons (o) and 7-rays
(). , calculated (after [89]).
210C
130C
130C 130C 130C
0% 0 0 1 % 002% 004% 0-3%
Figure 12.8. Glow-curve changes in CaSO:(Dy, *Li) as a function of the weight per cent
of the
6
Li
2
C0
3
content.
Li
2
S0
4
mixture is linear, without phosphor damage, up to a neutron fluence of ~2.5
x 10
14
n cm"
2
and has a sensitivity two-thirds that of TLD 600. By using
6
Li
2
S0
4
Beach and
Huang hope to reach a sensitivity approximately seven times that of TLD 600. The
response of a 50%
6
LiF mixture is linear up to a fluence of only 10' n cm
-2
before phos-
phor damage occurs. The sensitivity of this mixture is approximately six times that of
TLD 600. By using a pair of CaS0
4
:Tm (
6
LiF) and CaS0
4
:Tm (
7
LiF) detectors Takenaga
was able to detect 1 mrem of thermal neutrons with a standard deviation of 4.1% if no
gamma radiation is present rising to 30% in the presence of 1 rad of gamma radiation.
It is possible to adjust the concentrations of these mixtures to obtain the same dose-
equivalent sensitivities to thermal neutron and gamma radiations [6, 7]. More develop-
ment of the CaS0
4
: Tm (
6
Li
2
S0
4
) system should be fruitful.
Applications of TL materials in neutron dosimetry 241
0>
o
c
3
o
10
10" r
(N
- 5 icr =-
E
Q. 3
01
O
S a:
a
>
* 10
LU
o
a
10
-8
"
9
-10
-11
-12
-
-
"
-
1 1 IIMIj 1 1 1 l l l l l j 1 1 1 l l l l l j 1
l ^ W - ^ N
/
x
\ i
A /o
/ s <p
/ *~~
' / o
/ <b

' 1 1 1
* 1 ' ' 1 1
1 1 Mi l l
H
-
_
-
:
~
~
-
-=
;
-
-
-
-
__
:

-
\
-
\
-
: 1 0 "
10"
-7
E
o
c
o
(_
-*-
ai
c
- 1 0 " ' -
10
- 8
1 0
_
" r
^10
- 9
O)
a>
a
E
0)
10
i-2
10" 1 10 10'
Neutron Energy (MeV)
Figure 12.9. The variation with neutron energy of the responses of CaS0
4
: Tm and
BeO:Na. o, CaS0
4
(Tm) (expt) [90]; , CaSO(Tm) (calc) [90]; , BeO(Na) (expt)
[90]; ,BeO(Na)(calc) [90]; A, BeO(Na) (expt) [94]; v, BeO(Na) (expt) [34].
12.4. Intermediate and fast neutron dosemeters
In general, TL phosphors have lower responses to fast neutrons than to equal doses of
beta and gamma radiations because there is enhanced recombination and saturation along
the tracks of high LET particles such as recoil nuclei. In addition, phosphors are non
hydrogenous so that the absorbed dose is less than in tissue, for the same fluence. Because
nuclear collisions are involved in the energy transfer processes, the luminescence will
usually increase with energy. Figure 12.9 compares the experimentally determined
responses for CaS0
4
:Tm [90] and BeO:Na [34, 94] with the values calculated by Tanaka
and Furuta [90]. The responses of
6
L iF and
7
L iF are shown in figure 12.10 [92]. Below
about 100 keV the
6
L i(n,a)
3
H reaction becomes dominant with its 1/F cross section (see
figure 12.3). The sensitivity to 1 MeV neutrons is much smaller than to thermal neutrons
(~2.5 and ~2000 equivalent rad/10
10
ncm~
2
, respectively). The neutron response of the
285 C peak in
7
L iF, which has a higher neutron sensitivity relative to the 7ray sensitivity
than the 210C peak, also increases with energy as shown in figure 12.11 [26].
Various techniques have been tried to increase the neutron response of the main dosi
metry peaks such as (i) using a hydrogenous material to provide recoil protons, (ii) using
a foil of fissionable material and detecting the fragments and (iii) using a moderator to
thermalise the neutrons. These techniques are not unique to TL phosphors and have also
been used, sometimes to greater advantage, with nuclear emulsions, etched foils and
scintillation counters.
12.4.1. Proton radiators
These can be subdivided into two classes as follows: intimate mixtures and sandwiches.
242 J A Douglas
a>
o
c
3
c
o
0)
- E
E
3 c
o
1 - l _
0) - t
Q. ^
Q)
(L C
U ._
o
>
cr
LU
o
O
10"
7
10"
10"
H
=-
10"
10
U
10"" r
: 1 I I I I I H| 1 1 1 I 111 1 1 1 1 11 ll| 1 1 1 l l l l l | 1 1
_
"
r
:
: S
*
S
^s^
-
z
\
r
:

6
Li F
7
Li F
o Exper i ment
Cal cul at i on
^^W^
*>
/ 0
*/
' l '
r' o o
/
1 i i i 1 i i 1 i i i 1 i i
I i ni l
:
'.
-
:
1
-
-
;
-
-
-
10"
5
___
'E
u
10~
6
c
o
1_
"5
<D
C
10"
7
_-
'o>
10"
8
*
a
E
I_
CD
10-
9
*
10"
12
10"
3
10~
2
10"
1
1 10 10
2
Neutron Energy (MeV)
Figure 12.10. The variation of the neutron responses of
6
L iF and
7
L iF with neutron energy
(after [92]).
uu
50
T3
a
0)
a.
0)
w 30
o
Q.
or 20
S?
10
n
-
-
y*252
I
Cf
1
/ A m Be
i i i
^ ^ ^ J 5 M e V
i i
0 2 k 6 8 10 12 U 16
Neutron Energy (MeV)
Figure 12.11. Neutron energy response of the 285 C peak in TL D 100 [26].
12.4.1.1. Intimate mixtures. The hydrogenous compounds which are used must either be
able to withstand the high temperatures of readout and anneal or be easily separated
from the phosphor after irradiation. Readily volatile liquids such as alcohol and water are
natural choices. The difference in response between phosphors exposed wet and dry
indicates the enhancement due to recoil protons.
Applications of TL materials in neutron dosimetry 243
After contact between liquids and phosphors there is a build-up of thermoluminescence
[74, 85], which is probably due to the etching of the surface defects in the phosphor.
Puite delayed exposures for ~100h after mixing CaF
2
:Mn with alcohol to allow equi-
librium to be reached. In the case of LiF in water there is the competing process of
induced rapid fading [85].
Karzmark et al [47] and Wingate et al [99] found that suspending LiF in alcohol
increased its response to 14 MeV neutrons by a factor of 2.5 or 4 depending on whether
the mixture was shaken or not during the irradiation. However, the response is still very
energy-dependent. At 2.9 and 14.9 MeV the responses are 0.17 and 0.66 equivalent
7-ray kerma per neutron kerma in tissue respectively [12]. The variation is due to
the relationship between neutron energy, recoil proton range and the grain diameter of a
phosphor. Reducing the grain diameter will increase the surface area per unit volume and
hence increase the TL from short-range recoil protons. The variation of the response with
neutron energy would thus be reduced. However, the inherent radiation sensitivity of LiF
falls for very fine grains [48].
Alcohol has also been used to boost the fast neutron response of CaF
2
: Mn [74] and
CaS0
4
:Dy [98] which have much higher radiation sensitivities than LiF. It is possible to
detect a fluence of 5 x 10
5
n cm
-2
from a Pu-Be source with a pair of dry and alcohol-
suspended CaS0
4
:Dy dosemeters. Allowance has to be made for the effect of alcohol
on the 7-ray sensitivity. Unruh et al [95] were unable to find a non-hydrogenous liquid
which would produce the same effect on the 7-ray sensitivity of the 'dry' dosemeter.
The big disadvantage of liquid radiators is that stirring or shaking is necessary to
maintain uniform mixing and constant response. Solid matrices, which do not require
such treatment, have been developed incorporating CaS0
4
:Dy [10, 11] and CaS0
4
:Tm
[15]. In the latter case Blum et al encapsulated CaS0
4
:Tm powder in one PTFE tube and
a 3:1 mixture with glucose in another. The glucose was washed out and the phosphor
dried prior to read-out. After irradiation in a cyclotron beam, the TL outputs were in the
ratio of about 4:1 which is sufficient to give good discrimination between the neutron
and 7-ray components in the range 10 mrad to 50 rad. The neutron response changes by
less than 10% when the tube is rotated 90 in the beam.
Becker et al [10, 11 ] have developed a solid matrix which will withstand the necessary
read-out temperatures, thus greatly simplifying the technique. An intimate 1:1 mixture
of finely powdered CaS0
4
:Dy (~4jum diameter grains) and p-sexiphenyl, which has a
melting point of 450 C, is hot-pressed into a pellet 6 mm diameter x 1 mm thick. The
non-hydrogenous counterpart has a PTFE matrix. Table 12.2 shows that a ten-fold
enhancement is achieved at 14 MeV but less at lower energies. This technique could
become as simple to employ as
6
LiF/
7
LiF pairs and will be more precise and less
subjective than nuclear emulsions which are presently employed for personnel fast
neutron dosimetry.
Table 12.2. Fast neutron response of CaSO:Dy embedded in p-sexiphenyl.
Radiation source p-sexiphenyl response/Teflon response Neutron dose (rad)/
(normalised for equal gamma-ray response) gamma-ray dose (rad)
HPRR Reactor 3 7
14 MeV beam 10 25
244 J A Douglas
12.4.1.2. Sandwiches. A simpler type of proton radiator is a sheet of hydrogenous plastic
in contact with a phosphor. Blum et al [16], Sunta et al [87], Spurny et al [86] and
Mohammadi et al [62] have investigated such systems with CaF
2
:Mn in Teflon, TLD 100,
CaS0
4
:Tm, Li
2
B
4
0
7
: Mn, Li
2
B
4
0
7
: Ag, natural CaF
2
and A1
2
0
3
. Table 12.3 shows that
the enhancement is proportional to the hydrogen present in the radiator and that a larger
enhancement is obtainable with A1
2
0
3
than with LiF. However, there is a very pro-
nounced variation with neutron energy and angle of incidence because the range of
proton recoils decreases both with neutron energy and also with increasing angle of
incidence. This severely limits the use of the technique. However, when calibrated at a
particular energy Blum et al [16] found that the discs of CaF
2
:Mn embedded in Teflon
with covers of polyethylene and lead were suitable for clinical use in beams down to
doses of a few rad.
Table 12.3. Effect of proton radiators on the relative response of some thermoluminescent
sintered discs to 14.7 MeV neutrons.
Material Response relative to
60
Co 7-rays with respect to
energy absorbed in wet tissue
Without radiator
(under Al)
PMMA
(9.1% H)
Polyethylene
(14.3% H)
na t
L j F
7
LiF
A1
2
0
3
0.120.02
0.12+0.02
0.170.03
0.290.03
0.300.02
0.65 0.02
0.39 0.04
0.38 0.04
0.960.08
In addition to acting as a dosemeter, a stack of phosphor-loaded hydrogenous discs
can also be a crude spectrometer for neutron beams. The range of a recoil proton is a
function of its energy, so the maximum range is related to the energy of the incident
neutron. Figure 12.12 is a histogram of readings from a stack of epoxy resin discs loaded
<
B 300
0
0 200
R
E
A
D
I
N
G

P
E

8

U MeV NEUTRONS
-
0 500 1000 1500 2000 2500
DEPTH INTO STACK (pm)
Figure 12.12. Histogram of readings from a stack of epoxy resin discs loaded with
CaS0
4
: Sm after exposure to 14 MeV neutrons.
Applications of TL materials in neutron dosimetry 245
with CaS0
4
:Sm which had been exposed to 14 MeV neutrons [30]. At this energy the
TL increases up to a depth of ~2000 fjm when equilibrium is reached, showing that this
is the maximum range of the protons. The magnitude of the luminescence at equilibrium
is proportional to both the hydrogen concentration in the matrix and also to the incident
neutron fluence. The depth at which equilibrium occurs indicates the neutron energy. The
proton range varies very rapidly with energy which means that the method is sensitive,
but ultra-thin discs will be needed at low energies for good resolution. For 1 MeV
neutrons a disc thickness of about 4 /um is required. The use of such a device is naturally
limited to beams.
12.4.2. Fission foils
Ettinger et al [29] have proposed substituting a foil of fissionable material in place of a
proton radiator. This would increase the energy deposited per neutron interaction.
Ettinger used natural CaF
2
powder glued to an aluminium or acetate backing held in
contact with a
238
U foil 0.4 mm thick. The competing (n,p) and (n,a) reactions of ^Ca
and
42
Ca deposit many times less energy than the fission fragments. The range of fission
fragments and the a particles from the decay of
238
U are very similar (~15 /xm in CaF
2
)
and cannot be separated. To obtain maximum discrimination the fission foil should there-
fore be separated from the phosphor after irradiation to reduce the effect of the natural
decay. A neutron fluence rate of ~5 x 10
5
n cm"
2
s
_1
produces the same TL response as the
natural decay of
238
U, which indicates a lower detection limit. Fluence rates of ~10
7
n cm"
2
s"
1
were easily detectable without the need to cool the photomultiplier.
This technique may be useful for calibrating fluences. The performance would be
improved by using a foil of
237
Np instead of
238
U because it has a lower spontaneous
fission rate, lower specific activity and lower energy threshold [13].
12.4.3. Moderators
An alternative method of increasing the energy transferred from fast neutrons to phos-
phors is to thermalise the neutrons and use a phosphor with a high thermal neutron cross
section. Such systems can be sub-divided into (i) moderator surrounding the detector and
(ii) moderator behind the detector. In the latter category the detector responds to back-
scattered or albedo neutrons and will be dealt with in 12.4.4.
Distenfeld et al [23] and Engelke [27] in collaboration with Piltingsrad [72] and with
Israel [28] have developed dosemeters using pairs of
6
LiF and
7
LiF phosphors at the
centre of polyethylene spheres. Figure 12.13 [53] shows the effect of sphere diameter on
the energy dependence. No diameter gives a flat response from 1 to 10
6
eV. Barothoux et
al [8] suggested that a good rad response could be obtained by subtracting 5% of the
response of a 4.2 in sphere from that of a 12 in sphere. More recently Apt and Schiager
[2] have shown that a 10 in diameter sphere has an almost dose-equivalent response for
neutrons up to 7 MeV.
Pairs of
6
LiF/
7
LiF detectors placed along a diameter give information about the
incident spectrum. Figure 12.14 shows that the distance from the surface to the position
of maximum response increases with neutron energy. The ratio of the response at the
centre to that at the surface also increases with energy. Both of these effects can be used
246 J A Douglas
10"
1
-
CD
l/l
C
o
Q.
l/l
dl
cr
10
-2
10'
i-3
3 - - 4
10
,5
10'
10"'
A 8 1
' N \ \ \
\ \
10"' 10 10
1
10
2
10
3
10
4
10
5
10
6
10
7
10
8
Energy (eV)
Figure 12.13. Calculated responses of TL detectors in polyethylene spheres of various
diameters (from [53]).
1 2 3 4 5 6 7 8 9
Distance from Surface of
the Sphere (ins)
10
Figure 12.14. TL output of detectors placed at different depths in a polyethylene sphere,
1 8 in diameter. Normalised to 2 X 10
7
neutron cm"'.
to indicate the effective neutron energy. The latter is used in the 10 in diameter poly
ethylene sphere of Engelke and Israel, which has a pair of
6
L iF/
7
L iF phosphors at the
centre and at 26 points on the surface. The ratio of surface to centre readings enables the
effective energy to be deduced and hence the appropriate calibration factor to apply to
the centre readings to obtain the dose equivalent. In the case of nonuniform fields a
computer is employed to solve the simultaneous equations. The minimum detectable
dose equivalents are 30 mrem of neutrons and 10 mrem of gamma radiation.
Applications of TL materials in neutron dosimetry 247
Pairs of detectors have also been positioned along the axes of cylinders to act as
spectrometers and dosemeters for beams of neutrons. Longworth [55] proposed such a
scheme using a cylinder 41cm diameter x 54 cm long which had an internal thermal
neutron shield. The incident spectrum was unfolded by a computer program. It had a
resolution of ~12% at lower energies improving to 5% at 1 MeV, provided that the
exposure was long enough to allow the fluence to be determined with a precision of 2%.
Singh et al [82] have also developed a spectrometer and dosemeter using pairs of
6
LiF
and
7
LiF detectors at 0.8 cm intervals along the axis of a polyethylene cylinder 25 cm
diameter x 25 cm long. The dose equivalent measured at a depth of 10 cm is almost inde-
pendent of energy. The ratio of the reading at 10 cm to the maximum reading gives the
effective energy. The depth at which the maximum occurs multiplied by the ratio of
maximum reading to the surface reading indicates the thermal neutron content of the
beam.
Spectrometer dosemeters are conceptually good dosemeters because they provide
spectral information in addition to fluence or dose equivalent. Cylindrical versions,
however, can only be used with beams of known direction.
12.4.4. Personal albedo
The human body contains hydrogenous material which moderates and scatters neutrons.
The back-scattered neutrons which re-emerge from the body with lower energy are called
albedo neutrons. Many personnel neutron dosemeters have been designed based on the
detection of the thermal and epithermal albedo neutrons. Unfortunately both the
fraction of neutrons re-emerging with thermal energy and also the neutron fluence to
dose-equivalent conversion factor vary with energy (figures 12.15 and 12.1) in such a
way that the overall response of simple albedo dosemeters is highly energy-dependent.
Various attempts have been made to improve the response by (a) incorporating a
moderator in the dosemeters so that the thermal and epithermal neutron detector will
Energy of Incident Neutrons( eV)
Figure 12.15. Thermal neutron albedo from the body as a function of incident neutron
energy [40].
248 J A Douglas
respond to moderated incident and albedo neutrons and (b) incorporating extra detectors
to provide information about the incident spectrum so that a correction factor can be
applied.
Figure 12.16 [71] shows schematically some of the types of dosemeter which have
been designed. Types (a) [31] and (b) (Burger, private communication) respond to both
incident and albedo thermal and epithermal neutrons, whereas (c) (Preston, private
communication, [37]) responds to neither incident nor albedo thermal neutrons but only
to epithermal plus internally moderated neutrons. Types (d), (e) and (/) [40] have
thermal neutron shields to cut out the direct action of incident thermal neutrons. Types
(g) [18], (h) [41], 0) [21], (k) [50] and (/) [36] distinguish between incident and albedo
response. Type (m) [69] has an additional component which responds to epithermal and
fast neutrons. This allows corrections to be applied to the responses of the other two
pairs of detectors for their responses to fast and epithermal neutrons.
No di scri mi nati on
between i nci dent
and albedo neutrons
D i scr i mi nat i on
agai nst incident
t hermal neutrons
Separati on of
i nci dent and albedo
neutrons
Separation of incident,
thermal and
epi thermal neutrons
6 7
Cd
6 7
CA
e
i rn La
TT?: ^
C d
6 7
fe&
Cd
Cd
^J!3^
6 7
Figure 12.16. Schematic diagram of types of albedo dosemeters (by courtesy of Piesch
[71]).
The response of some of the European dosemeters to monoenergetic neutrons is
shown in figure 12.17 [24]. It can be seen that, apart from the thermal neutron response,
all the curves are the same shape. The findings are in agreement with those of Hankins
[37], who reviewed some American dosemeters, namely:
(1) adding polyethylene to an albedo dosemeter does not change the shape of its
neutron energy response;
(2) including polyethylene increases the dosemeter sensitivity;
(3) dosemeters with no thermal neutron shield are more sensitive to neutrons of all
energies than those which are completely surrounded by one;
(4) variation in neutron energy or spectrum greatly alters the sensitivity of albedo
systems thereby limiting their use.
Some other conclusions of Hankins were:
(5) the sensitivity increases slightly as the body-to-dosemeter distance is increased but
not by much if there is no polyethylene or it has a complete thermal neutron
shield;
Applications ofn materials in neutron dosimetry 249
100p
o Burger
O Piesch Albedo
x Harvey Albedo
A Preston
Brunskill Albedo
(Evaluated by
Brunskill I
0-5 10 1-5
Neutron Energy IMeV)
2 0
Figure 12.17. Responses of various dosemeters
plotted against neutron energy [24].
(6) as the moderator thickness is increased the sensitivity increases rapidly at first and
then remains fairly constant;
(7) most of the response is from the neutrons reemerging from the body;
(8) the thickness of the shield has little effect on the response unless it is on the back
of the dosemeter;
(9) decreasing the dosemeter diameter greatly increases its response to thermal neutrons
but not to fast neutrons;
(10) the thermal neutronsensitive and insensitive TL detectors must be located at the
same or equivalent positions in the dosemeter.
7
L iF probably cannot be used to
determine the 7ray dose.
If a dosemeter is worn on the back as well as one on the front, then the ratio of the
response on the back to that on the front increases with neutron energy. As the neutron
energy increases neutrons penetrate further before becoming thermalised, thus moving
the effective source of albedo neutrons away from the front dosemeter towards the
back one.
Figure 12.18 shows that for the two multicomponent dosemeters investigated by
Douglas and Marshall [24] the ratio of incident to albedo response is independent of
energy, apart from the responses to thermal neutrons. In the case of irradiation by a
neutron spectrum, this ratio would indicate the thermal neutron content of the incident
radiation.
12.4.4.1. Choice and use of an albedo dosemeter. The albedo response of all dosemeters
changes by a factor of approximately 15 in the energy range 0.11.7 MeV. Therefore
a simple albedo dosemeter cannot be used to measure incident neutron dose without
extra information to enable a correction factor to be applied. Three types of working
environment will now be considered: (a) where the neutron spectrum is constant,
(b) where there is one neutron source but varying degrees of moderation and (c) where
there is more than one neutron source and/or type of shielding.
250 J A Douglas
Q)
if)
C
o
Q.
I/)
<D
en
~c
Q)
D
O
C
tt-5,
O
A
Piesch
Brunskil
0
0-5 10 1-5
Neutron Energy (MeV)
2 0
Figure 12.18. Ratio of incident to albedo responses at different neutron energies.
(a) Constant spectrum. In an environment where the spectrum is constant a simple
albedo dosemeter can be used provided either it is directly calibrated in the area or simple
spectrometry is performed in the area to determined the correction factor [40].
(b) Varying degrees of moderation. As a spectrum of neutrons undergoes increasing
moderation by hydrogenous material the mean energy will decrease and the fluence of
thermal neutrons will increase. There will thus be a direct relationship between the
fraction of thermal neutrons present and the mean effective energy. The ratio of incident
to albedo responses of a multi-element dosemeter could thus be used to allow for the
degree of moderation. Piesch [69] and R T Brunskill (private communication) have shown
this to be the case. However, for multi-element dosemeters to work with mixtures of
different degrees of moderation of the same spectrum then the correction factor must be
proportional to the fraction of thermal neutrons in the incident spectrum.
(c) Different neutron sources and/or shields. There will not necessarily be any relation-
ship between the fraction of incident neutrons which are thermal and the mean energy
for different initial neutron spectra. Nor will there be a direct relationship in the case of
different shields around the same neutron source. A metal shield with resonances, e.g.
cadmium or iron, will obviously upset the thermal to mean energy relationship. Therefore
in these cases a multi-component albedo dosemeter is not a solution to the problem. An
alternative approach is to use a single-component albedo dosemeter together with another
dosemeter having a different energy response such as a nuclear emulsion dosemeter on
a fission foil.
12.4.4.2. Effects of angle of incidence. Figure 12.19 shows the variation of response
with angle of incidence for the Harvey dosemeter. For any energy of incident neutrons,
the effect of the angle of incidence on the response is a product of two terms. The first
Applications of TL materials in neutron dosimetry 251
Figure 12.19. Effect of the angle of incidence on the
response of Harvey dosemeters. Elliptical phantom
(20X30 cm
2
): X, lOOkeV neutrons; o, 700 keV
neutrons; , 1.7 MeV neutrons. Cylindrical phantom
(20 cm diameter), v,
25:
Cf source.
Angle of Incidence
relates to the fluence of thermalised neutrons produced behind the dosemeter. This
fluence is proportional to the number of neutrons incident per unit area, which in turn is
proportional to the cosine of the angle of incidence. The second term allows for the
variation with angle of incidence of the distance between this source of thermalised
neutrons and the dosemeter on the surface of the phantom. This distance decreases as
the angle of incidence increases and also as the energy of the incident neutrons decreases.
For low energies of incident neutrons, where the source of thermal neutrons is near
the surface, the predominant term is that of the variation of incident fluence, i.e. cosine
of the angle of incidence. For higher energies the variation with angle of the position of
the source of thermalised neutrons becomes more important and maxima appear in the
response curves.
Most of the energy from incident neutrons is deposited close to the point of entry
into the body. The dose is thus proportional to the number of neutrons per unit area of
body surface, which in turn is proportional to the cosine of the angle of incidence. Hence
a dosemeter, which basically has a cosine response, is acceptable for personnel dosimetry.
The increased response for higher energies at some angles is an extra safety factor.
12.4.4.3. Conclusions. It has been shown that the shape of the energy response curve is
the same for all albedo dosemeters in the range 0.11.7 MeV. Because the response at
0.1 MeV is approximately 15 times that at 1.7 MeV, extra information is required to
correct for the effective energy of incident neutrons. Additional elements in multi
component dosemeters do not provide enough information, except in the restricted case
of varying moderation of one type of neutron source. A singlecomponent dosemeter can
be used in environments with a constant neutron spectrum provided the correction factor
is determined by calibration. A multielement dosemeter (e.g. Piesch) is useful to make
corrections to the calibration for variations in spectrum due to local variations in hydro
genous moderation or backscatter.
252 J A Douglas
12.4.5. Activation
The elements of some TL phosphors form radioactive isotopes after neutron capture. The
radiation subsequently emitted by them doses the phosphor internally. Annealing the
phosphor immediately after exposure removes the direct effect. The thermoluminescence
after a suitable storage period will be proportional to the induced activity which in turn
is proportional to the neutron fluence. This technique has been used by Mayhugh et al
[61] to measure thermal neutron doses using CaS0
4
:Dy, CaF
2
:Dy and natural CaF
2
. By
suitably selecting phosphors containing elements with different energy thresholds for
neutron capture a dosemeter can be obtained which provides information on the energy
spectrum and has complete discrimination against gamma radiation. A system containing
several different phosphors has been extensively investigated by Pearson and Moran [67].
Table 12.4 shows the available neutron reactions in some phosphors.
Table 12.4. Neutron activation reactions in some TL phosphors.
Phosphor
TLD700
(LiF:Mg,Ti)
TLD200
(CaF
2
:Dy)
CaF
2
:Mn
CaS0
4
:Dy
ZnO:Tm
Mg
2
SiO:Tb
Reaction
"F(n, 2n)'
8
F
"F(n, 2n)
18
F
Threshold
12MeV
12MeV
164
Dy(n,
T
)
165
Dy Thermal
"F( n, 2n)
, 8
F
S5
Mn(n,
7
)
56
Mn
32
S(n, p)
32
P
12MeV
Thermal
2.5 MeV
164
Dy(n, 7) ' "Dy Thermal
64
Zn(n, p)
M
Cu
68
Zn(n,7)
69
Zn
24
Mg(n,p)
24
Na
4MeV
Thermal
7 MeV
Capture
cross section
50mbat 14 MeV
50 mb at 14 MeV
2.8 kb
50mbat 14 MeV
13b
250mbat 14 MeV
2.8 kb
200mbat 14 MeV
l b
200 mb at 14 MeV
Decay
r
r
P~
r
r
P~
F
ECB*
<r
f
' mode
0.64 MeV
0.64 MeV
1.3 MeV
0.64 MeV
2.8 MeV
1.7 MeV
1.3 MeV
0.6 MeV
0.9 MeV
2.8 MeV
Half-life
109 min
109 min
140 min
109 min
2.5 h
14d
140 min
12.8h
57 min
15h
Some of the criteria for suitable phosphors are as follows:
(1) The half-lives of the neutron-induced isotopes in a phosphor must be sufficiently
different for the separation of the activities to be possible.
(2) The half-lives must not be very short otherwise most of the induced activity would
decay before annealing is complete (e.g. the t
1/2
of
16
N and
19
0 are 7.2 and 29 s,
respectively, which are too short).
(3) The half-lives must not be very long otherwise the dose rate will not be much greater
than background.
(4) The exposure time must be short compared with the half-life for the induced activity
at the end of the exposure to be proportional to the fluence. (When the exposure is
one tenth or less of the half-life then the activity is proportional to the fluence
within 7%.)
(5) Fading rate must be low.
Applications of TL materials in neutron dosimetry 253
It can therefore be seen from table 12.4 that fluences of thermal neutrons and those of
energy >12 MeV cannot be separated with either CaF
2
:Dy or CaF
2
:Mn. However, using
CaS0
4
:Dy, thermal neutrons can be separated from those of energy >2.5 MeV by
reading after 1 d and again after 14 d. Using ZnO:Tm, Mg
2
Si0
4
:Tb and TLD 700 the
neutron fluences above 4, 7 and 12 MeV, respectively, can also be measured, thus
providing reasonable spectral information.
Because the prompt response of the phosphors is 2-3 orders of magnitude greater than
the delayed response, it is essential that the prompt response is completely and quickly
removed. Pearson achieved this by placing the phosphors in holes in an aluminium block
which was heated in an air furnace at 500 C for 5 min followed by rapid cooling in a lead
block for 2 min. This unfortunately rendered them sensitive to uv light.
The low TL output means that photon counting has to be used in the reader to obtain
reasonable statistics. The thermoluminescence is limited by the number of activations
produced. Therefore the response can be increased by (a) increasing the mass of the
phosphor, (b) using a reaction with a large cross section or (c) using a reaction where the
induced isotope emits beta particles of higher energy (the delayed dose measures the
energy deposited not the number of beta rays).
This is a useful technique for short exposures to relatively high fluence rates such as in
neutron radiation therapy or nuclear accident dosimetry.
12.5. Possible future developments
12.5.1. Use of deeper traps
Lucas and Kapsar [56] are developing a system using the 150C and 240 C peaks in
CaF
2
:Tm. The 240 C peak is mainly sensitive to fast neutrons in contrast to the main
dosimetry peak (150C) which has a low response to neutrons. At this stage it is not
clear whether there is sufficient discrimination against gamma radiation for this to be
useful for personnel monitoring.
12.5.2. Creation of a phosphor by ion implantation
A dosemeter consisting of an intimate mixture of two powders of fine particle size was
investigated at Harwell by Pells and Hughes [68]. One would be a host for luminescence
and the other an activator. Initially the host would be very pure, containing no activator.
Collisions between fast neutrons and activator atoms near the host would implant
activator ions into the host, thus creating a phosphor. The extent of the implantation
would be proportional to the neutron dose. The newly created phosphor could then be
exposed to a known dose of x-rays or electrons and the thermoluminescent output
measured. This would be proportional to the number of injected activator ions and hence
to the neutron dose. It has been shown theoretically [68] that an ideal ion-injection
dosemeter with an ideal reader would have millirad sensitivity. However, there are many
problems in realising this:
(1) fabricating a large interfacial area per unit volume with complete mixing of the
powders;
254 J A Douglas
(2) the dosemeter volume is limited by loss due to self-absorption and scatter. The light
loss perhaps could be reduced if the refractive indices of host and activator were
matched.
More ideas are needed to solve the problems.
12.5.3. Internal proton radiator
Morato et al [63] have diffused hydrogen ions into CaF
2
:Dy and so produced a phosphor
with an internal proton radiator. By this method they claim to have increased the
response to neutrons relative to gamma radiation by a factor of 80. Further work is
required to increase the ion concentration by at least another order of magnitude for the
system to be feasible for routine personnel monitoring.
Although there is no one satisfactory fast neutron dosemeter there is hope for the future.
References and further reading
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Applications of TL materials in neutron dosimetry 255
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256 J A Douglas
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4
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4
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7
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book p63
84 Snyder W S 1971 Dose distributions in a cylindrical phantom for neutron energies up to 14 MeV
Protection against neutron radiation. NCRP Rep. No 38, pp46-84
85 Spumy Z, Novotny J and Hedvicakova L 1971 Thermoluminescent dosimetry using lithium
fluoride in aqueous suspension Phys. Med. Biol. 16 295-301
86 Spumy F, Kralik M, Medioni R and Portal G 1976 A new thermoluminescent dosimeter for
14.7 MeV neutrons Nucl. Instrum. Meth. 137 593-4
87 Sunta C M, Nambi K S V and Bapat V N 1973 Fast neutron response of thermoluminescent detec-
tors with the proton radiator technique Proc. Symp. on Neutron Monitoring for Radiation Protec-
tion Purposes, Vienna IAEA-SM-167/10
88 Szabo PP 1975 Investigation of properties of CaS0
4
:Dy thermoluminescent dosimeters Central
Research Institute for Physics, Budapest KFKI-75-1
89 Takenaga M 1977 Thermoluminescent response to thermal neutrons of mixture of CaS0
4
:Tm and
non-luminous "LiF 7. Nucl. Sci. Tech. 14 292-9
90 Tanaka S and Furuta Y 1974 Neutron responses of thermoluminescent dosimeters, BeO(Na),
CaS0
4
(Tm) and its mixture with
6
LiF and
7
LiF Proc. 4th Int. Conf. on Luminescence Dosimetry,
Krakow, August (Krakow: Institute of Nuclear Physics), pp 1213-28
91 Tanaka S and Furuta Y 1976 Usage of a thermoluminescence dosimeter as a thermal neutron
detector with high sensitivity Nucl. Instrum. Meth. 133 495-9
92 Tanaka S and Furuta Y 1977 Revised energy responses of
6
LiF and
7
LiF thermoluminescence
dosimeters to neutrons Nucl. Instrum. Meth. 140 395-6
93 Thompson J J and Ziemer P L 1973 Thermoluminescent properties of lithium borate activated by
silver Health Phys. 25 435-41
94 Tochilin E, Goldstein N and Miller W G 1969 Beryllium oxide as a thermoluminescent dosimeter
258 J A Douglas
Health Phys. 16 1-7
95 Unruh C M, Baumgartner W V, Kocher L F, Brackenbush L W and Endres CWR 1967 Personnel
neutron dosimeter developments Proc. Symp. on Neutron Monitoring for Radiological Purposes,
Vienna p433
96 Wallace RH and Ziemer PL 1969 Studies on the thermoluminescence of manganese activated
lithium borate Proc. 2nd Int. Conf. on Luminescence Dosimetry, Gatlinburg, Tenn., September
1968. USAECRep. CONF 680920, pp 140-7
97 Wallace R H, Ziemer P L, Kastner J and Oltman B G 1971 The relationship between encapsulation
and apparent fast neutron induced fading in TLD Health Phys. 20 221
98 Weng P S and Chen K M 1974 Response of CaSO(Dy) phosphor to neutrons Nucl. Instrum. Meth.
117 89-92
99 Wingate C L, Tochilin E and Goldstein N 1967 Response of lithium fluoride to neutrons and
charged particles Proc. Jst Int. Conf. on Luminescence Dosimetry, Stanford University, June 1965.
USAECRep. CONF 650637, pp421-34
100 Woodley R G and Johnson N M 1967 Thermoluminescence induced by low-energy alpha particles
Proc. 1st Int. Conf. on Luminescence Dosimetry, Stanford University, June 1965. USAEC Rep.
CONF 650637, pp502-6
101 Yamashita, T, Nada N, Onishi H and Kitamura S 1970 Calcium sulphate activated by thulium or
dysprosium for thermoluminescence dosimetry Health Phys. 21 295-300
Applied Thermoluininescence Dosimetry. Eds M Oberhofer and A Schannann
1981 ECSC, EEC. EAEC. Brussels and Luxembourg
13
Glow-curve analysis
A c LUCAS
13.1. Introduction
Since the beginning of research in thermoluminescence dosimetry, the shape of the glow
curve obtained in heating thermoluminescent materials has been regarded as important
in determining the nature of the material itself and the key to its acting as a suitable
dosemeter. In recent years, the role of thermoluminescence dosimetry in personnel
dosimetry has increased to the point that a large share of film dosemeters have been
replaced. A characteristic of film dosemeters, often lamented as missing in thermo-
luminescence dosemeters, is the fingerprint which may be present after the initial readout.
It may be used in studying the conditions of the exposure of the film. Such a fingerprint
is also present in thermoluminescence dosemeters in the form of the glow curve. In recent
years, the glow curve has been shown to be of importance in a variety of ways as a
support measurement in dosimetry. The. discussions that follow provide a beginning to
analysis of some of the methods which can be used to analyse the glow curve for
dosimetric purposes.
13.2. Recording of glow curves
Glow curves may be recorded in a variety of ways. Each may have advantages or dis-
advantages, depending upon the particular program requirements. The simplest method,
sketched in figure 13.1, is to generate linear glow curves on a strip chart recorder which is
connected to an electrometer amplifier. The method requires range-changing, either
automatic or manual, in order to meet the usual demands for recording data over
ELECTROMETER
Figure 13.1. Simple method for generating linear glow curves.
260 A C Lucas
a wide range of dosemeter exposures. Interpretation of recordings involving range changes
requires some skill and training.
Range changes may be eliminated in strip chart recordings by incorporating
logarithmic electronics in the system. The resulting glow curve may be interpreted some-
what more easily, since the apparent shape is independent of the value of the exposure.
Such systems can be made to operate in the range from 1 pA to 100 /iA without signifi-
cant non-linearity. In such a system, sketched in figure 13.2, faithful recording of glow
curves is possible, over exposures ranging from 1 mR to 500 R.
STRIP CHART RECORD ER
Figure 13.2. Method for generating logarithmic glow curves.
Systems which digitise the anode current from the photomultiplier directly require an
alternative method for driving a strip chart recorder. Figure 13.3 shows a block diagram
of one such method. The pulses from the digitiser are fed to a counting ratemeter circuit
which is in turn connected to the strip chart recorder. The method has a disadvantage
in speed of response, since smoothing must be used to avoid the display of single pulses
at low counting rates.
PMT
CHARGE
DIGITIZER
STRIP CHART RECORDER
Figure 13.3. Method for generating logarithmic glow curves from a charge digitiser.
An alternative system which may be used in conjunction with systems which digitise
the current directly is shown diagrammatically in figure 13.4(a). The system uses
computer memory to store the counts as a function of time during the generation of the
glow curve. The data may then be scaled and summed as desired after accumulation.
Further, the data may be stored compactly using magnetic recording devices, for rapid
recall at a later date. Such a device is shown in figure 13.4(6).
Glow-curve analysis 261
PMT
CHARGE
DIGITIZER
MICRO-
PROCESSOR
MAIN
COMPUTER
DISC
MEMORY
(a)
Figure 13.4. (a) Sketch of a system for storing digitised glow curves, (b) Harshaw Model
2080 digitised glow-curve displayer.
13.3. Measurement of neutron dose equivalent
Deep traps have been shown to exist in both LiF : Mg,Ti and CaF
2
: Tm, which are some-
what more sensitive to neutrons than are the normally instrumented traps. Figure 13.5
shows a sketch of the glow curves obtained for LiF irradiated alternately with neutrons
and gamma rays. While the total amount of light available from the deep-trap measure-
ment is not great, the gamma-ray rejection obtainable using this method is very good.
Care must be taken in arriving at a model for calculating the neutron and gamma-ray
exposures when using such materials in a practical system. Consideration of several
models has led to the following method for analysing LiF data in practical situations.
First, define the variables:
(i) R i is the integral over the main peaks,
(ii) R
2
is the integral over the deep trap,
(iii) Bi is the integral over the main peaks for no exposure,
(iv) B
2
is the integral over the deep trap for no exposure,
(v) g is the response of the deep trap to neutrons divided by its response to gamma
rays, and
262 A C Lucas
100 200 T.C
Figure 13.5. Sketch of the glow
curves obtained for LiF irradiated
alternately with neutrons and gamma
rays.
(vi) / is the response of the deep trap to gamma rays divided by the response of the
main peak to gamma rays.
Now, let the system be calibrated so that it is direct-reading for gamma-ray exposures
and readout of the main peak. Then for the deep trap
(R
2
-B
2
)=fgD
n
+f(R
l
-B
l
)
and for the main peak
(R
1
-B
1
)=D
y
+ kD
n
where h g/10. Now, solving (13.1) for)
n
gives
(R
2
-B
2
)-f(R
l
-B
l
)
D
fg
Substituting (13.3) into (13.2) and letting h = g/10, we obtain
(R
2
-B
2
)
D
y
=l.l(R
l
-B
l
)-
10/
Typically,/has the value 0.005, so that
(R
2
-B
2
)- 0.005(R{-Bi)
D
and
D
y
=l.l(R
1
-B
1
)
0.005^
0.05
(13.1)
(13.2)
(13.3)
(13.4)
(13.5)
(13.6)
Glow-curve analysis
263
100 200 T,C
Figure 13.6. Sketch of the glow curve for CaF
2
: Tm.
Figure 13.6 shows a sketch of the glow curve for CaF
2
:Tm. Because of numerical
differences in the neutron sensitivity and in the amount of light normally emitted in the
readout process, a slightly different approach is used in analysing the readout. Define the
terms R
u
R
2
, B
1
and B
2
as before. In this case, the precision of the method is strongly
dependent upon establishing sensitivities for the two species of trap separately instead of
relying on a common ratio/. The solution is best derived by defining:
(i) S1 as the response of the first peak to gamma rays, and
(ii) S
2
as the response of the second peak to gamma rays.
Further, since the neutron response is relatively small and of the same order of magni-
tude for the two traps, it is as well to treat them separately in the derivation, for clarity.
For the deep trap
(R
2
-B
2
) = S
2
(gD
n
+ DJ
and for the lower-temperature trap
(R
l
-B
l
) = S
l
(hD
n
+D
1
).
Combining equations (13.7) and (13.8) yields
1
/
D
n
=
(x-h)\
R-2 -2 -*M -"1
" )
(13.7)
(13.8)
(13.9)
In practice, the quantity (g - h) is measured directly in neutron calibration using this
equation and S
1
is near unity as a result of gamma-ray calibration. Further, since the
neutron response for the first peak is quite small, we have
0 ,
R
1
-B
1
Si
(13.10)
264 A C Lucas
Typical values for the response g for TLD 600 deep traps is shown in figure 13.7. For
these data, the dosemeter was operated as an albedo dosemeter on a water phantom.
Further, typical values for the response g for TLD 700 are shown in figure 13.8. In this
case, the dosemeter material was placed in a simple polypropylene holder for exposure,
since there is no thermal-neutron sensitivity of consequence.
The response of CaF
2
: Tm, shown in figure 13.9, is principally due to fast neutrons
and has a threshold near 3 MeV. No significant thermal-neutron response was noted.
(TL/RAD)n
(TL/RADJA
1000
100-
TLD-600 WITH 10cm CH
2
Figure 13.7. Energy dependence for the
deep traps in TLD 600 operated as a
neutron albedo dosemeter.
10
1.0
TLD-700
En,MeV
0.1 10
Figure 13.8. Energy dependence for the deep
traps in TLD 700 irradiated with neutrons.
'
-
CALCIUM FLUORIDErTHULIUM
X / d. d
\ /
En,MeV
Figure 13.9. Energy dependence for the deep traps in CaF
2
:Tm irradiated with neutrons.
Glow-curve analysis
265
However, care must be taken to avoid exposure to low-energy x-rays which produce an
effect similar to that of fast neutrons. Further, care should be taken to avoid the effects
of fading of the lower-temperature traps.
13.4. Beta-ray measurement
Laskey and Moran [1] have shown that boron may be diffused into LiF:Mg,Ti in such
a way as to induce thermoluminescence, producing a glow curve at a temperature well
above that at which the normal peaks appear. Figure 13.10 shows their comparison of
glow curves obtained for alternate gamma-ray and beta-ray exposures of a dosemeter.
The data demonstrate that, in principle, it becomes possible to observe the effects of
gamma rays and beta rays independently in a single dosemeter. The method depends for its
operation not only on the separation of the two glow curves but also on the fact that
low-energy beta rays do not penetrate LiF to a great depth.
(O
t -
2
3
>-
tr
<
IT
1-
m
a.
<
A
A f B
/ \ / ^
/ \ / ' i
/ '
/
/
/
/
/
/
300 0 100 200
TEMPERATURE CO
Figure 13.10. Single-crystal TLD 100 with boron diffused into the first 2.0 Mm. Curve A is
response to beta rays from tritium; curve B is response to gamma rays from caesium.
Development of the method for practical dosimetry requires that consideration be
given to the relative contributions to the two separate glow-curve structures by gamma
rays and beta rays. The two separate regions in the dosemeter may be considered to be
two similar dosemeters from the point of view of the gamma rays but thin in one case and
thick in the other when considered from the point of view of the beta rays. A typical
energy dependence for such a case is shown in figure 13.11.
Mathematically, then, the measurement involves the solution to the familiar two-
detector problem. For the thick part
and for the thin part
R
2
= pG + mB.
(13.11)
(13.12)
266 A C Lucas
BETA RAY ENERGY. MeV
Figure 13.11. Sketch of the energy dependence which would be expected for very thin and
very thick dosemeters irradiated with beta rays.
If p is small, then the beta-ray dose is
B=R
2
/m
and the gamma-ray dose is
G = R
t
-kR
2
/m.
(13.13)
(13.14)
While this method has been shown to be feasible, it has not been applied in personnel
dosimetry.
13.5. Fading correction
While many dosimetric materials exhibit little or no fading in routine applications, the
most-used materials, LiF:Mg,Ti and CaF
2
:Dy may exhibit fading under some conditions
of use. In particular, LiF:Mg,Ti is often used in the thermally quenched state in
personnel dosimetry as a matter of convenience. In this state, the lower-temperature
QUENCHED
ANNEALED
100 200 T,C
Figure 13.12. Comparison of the
glow curves for iJF:Mg,Ti used
alternately in the annealed and
quenched states.
Glow-curve analysis 267
trapping centres exist in greater numbers than when the material has been subjected to a
rigorous annealing procedure. Figure 13.12 shows a comparison of the glow curves for
the two states of the material.
The LiF: Mg,Ti glow curve has been studied in rigour by a number of authors. It is
generally found to consist of a combination of six discrete trapping centres, some of
which interact with each other. Grant et al [2] have been able to reconstruct the glow
curve analytically by considering each trapping centre to act mathematically:
y = /
0
p e x p ( - f p d r i (13.15)
where
p
=
Se
-E/kT (13.16)
p is the probability that charge will be untrapped, S is a constant characteristic (s
_1
) of
the trapping centre, E is another constant characteristic (eV) of the centre, k is
Boltzmann's constant, 1.38 x 10~
16
erg K
_1
, and Tis the absolute temperature (K).
In that work, the trapping centres were found to be described by constants having the
values in table 13.1. Numerical evaluation of the probability of untrapping for reasonable
ambient temperatures shows that traps 1, 2 and 3 are most affected.
Table 13.1.
Trap S(s"' ) E (eV)
1
2
3
4
5
5. 00X10"
2. 00X10"
5. 00X10'
2
1.20X10'
2
2.20X10
13
0.82
1.08
1.13
1.15
1.36
In practice, it is usually best to take advantage of experimental fading data to form a
set of corrections. One can show that, if the logarithm of the thermoluminescence from
one peak is plotted as a function of the logarithm of the thermoluminescence from
another peak, a straight line will result. It seems reasonable, then, to adopt that way of
plotting as a standard method to achieve independence of temperature in applying the
data. One such example is illustrated below.
Figure 13.13 shows a sketch of the LiF glow curve with peak 2 shaded. In this
example, peak 2 is used as an indicator of fading and the integral under the curve (the
shaded portion) is accumulated separately and in addition to the integral over the whole
glow curve. In order to produce the fading effect for this example, dosemeters were
held at temperatures ranging from 50 to 100 C for 10 min. Figure 13.14 shows the value
of the complete integral plotted as a function of the integral over peak 2. The data form
a relation which can be used to correct other experimental data where the fading is
unknown.
268 A C Lucas
T,C
Figure 13.13. Glow-curve analysis used
in fading correction example.
1.0
0.8
0.6
0.4
0.2
o
P/S
Figure 13.14. Value of the glow-curve integral
plotted as a function of the integral over peak 2
(the shaded peak) of figure 13.13.
13.6. D etermination of time from exposure
Occasionally, where personnel dosemeter data are not clearly the result of known occupa-
tional exposures, it becomes useful to determine the time between exposure and readout
of the dosemeter. Algebraically, the time (in seconds) is
In (///)
-Se-
E
l
kT
(13.17)
where J is the measured luminescence for a given low-temperature peak, e.g. peak 2 or 3
for LiF, J
0
is the value of J if no time had elapsed, S, E and k are as defined above and T
is the absolute temperature (K).
The principal uncertainty in this method derives from uncertainty in estimating T.
A single degree error in its estimate results in error of the order of 10% in time estima-
tion. Where high precision is required in the estimate, the temperature may be deter-
mined by measuring the fading for a dosemeter which has been exposed and held under
controlled conditions for periods comparable to the subject exposure. This method has
been successfully applied in several investigations with good results.
Glow-curve analysis 269
13.7. Verification of data
Any given TL measuring system has, in principle, its own set of most probable failure
modes. Experience with systems having continuously operated strip chart recorders has
shown that operators may be trained to recognise faults in th shape of the glow curve
which may then be used to invalidate incorrect data. One such system which has been
operated in such a way is the Harshaw Model 4000 TL analyser.
In principle, it is further possible to effect automatic recognition of faults where glow
curves are accumulated in computer memory. Some specific faults which are detectable
are:
(1) lack of a glow peak,
(2) failure to heat,
(3) electrical interference,
(4) glow peak at wrong temperature,
(5) saturation of readout, and
(6) high dark current.
References
1 Laskey J B and Moran PR 1977 TLD-100 diffused with boron: a new 'surface sensitive' TL
phosphor Proc. 5th Int. Conf. on Luminescence Dosimetry, Sao Paulo, February 14-17 (Giessen:
I Physikalisches Institut of the Justus-Liebig Universitat)
2 Grant R M Jr, Stowe W S and CorellJ 1968 Computer assisted theoretical and experimental
analysis of the thermoluminescence of LiF:Mg Proc. 2nd Int. Conf. on Luminescence Dosimetry,
Gatlinburg, Tenn., September 1968. USAECRep. CONF 680920
Applied Thermoluminescence Dosimetry. Eds M Oberhofer and A Scharmann
1981 ECSC, EEC, EAEC, Brussels and Luxembourg
14
Application of TLD in medicine
A F McKINLAY
There are two important areas of absorbed dose measurement in medicine:
(i) absorbed dose measurement in radiotherapy, and
(ii) absorbed dose measurement in diagnostic radiology.
14.1. Radiotherapy measurements
The difficulties of accurately predicting absorbed doses in radiotherapy by calculation
have in the past led to the development of in vivo measurement techniques. While
entrance and exit absorbed doses could be measured using films and conventional ionisa-
tion chambers, intracavitary measurements were limited by the minimum size of available
ionisation chambers [1] (typically 20 mm x 5 mm diam.).
When Daniels first developed thermoluminescence as a practical method of assessing
ionising radiation exposure, it was realised that the technique could be applied in the field
of clinical measurement. Brucer used some of Daniels' single crystals of Harshaw LiF to
make internal in vivo measurements in cancer patients injected with radioactive
material [2].
The arrangement of radiotherapy treatment fields is conventionally carried out using a
combination of calculations involving standardised geometries together with depth dose
and transverse dose measurements in phantoms. The final check on the absorbed dose
delivered to the patient can be carried out by in vivo dosimetry. Similarly, absorbed doses
to organs not involved in the treatment, which should be kept to the minimum, can
be measured.
Thermoluminescence dosimetry has proved a useful technique for a variety of
purposes in radiotherapy, including measurements of therapy machine output, beam
uniformity checks and the measurement of absorbed dose in phantoms and in vivo for
both internally and externally applied fields. Thermoluminescent dosemeters have a high
precision, provide rapid retrieval of information (using on-site readers), have good
environmental stability, have good water or tissue equivalence and have a wide range of
sensitivities. The last characteristic is particularly important for in vivo measurements of
absorbed dose. Because of their small size, thermoluminescent dosemeters also give good
spatial resolution. This is of particular value in many radiotherapy techniques where the
absorbed dose has a rapid spatial variation. Thermoluminescent dosemeters may also be
used to measure the absorbed dose to experimental animals.
14.2 Diagnostic radiology measurements
The collective dose from medical exposure has been estimated to represent the largest
single man-made contribution to both the somatic and the genetically significant dose
272 A FMcKinlay
equivalent to the population of the United Kingdom as illustrated in figure 14.1
representing some 31% of the total somatic dose and 9% of the total genetic dose, and
95% and 85% respectively of the man-made contributions [3]. In other developed
countries, the estimated figures are similar. By far the largest contribution is from
diagnostic radiology, estimated as 10 times the sum of the contributions from nuclear
medicine and radiotherapy.
rQk\
FAL L -OUT, 0. 6%
/U^IISCEL L ANEOUS SOURCES, 0. 4%
^^OCCUPATIONAL EXPOSURE,0.4%
RADIOACTIVE WASTE D ISPOSAL ,0.2%
Figure 14.1. Annual genetically significant dose equivalent to the UK population. (Taylor
and Webb [3], reprinted with the permission of the National Radiological Protection Board,
Chilton.)
New radiodiagnostic techniques have been introduced, some involving the use of
complex machines such as the head and body scanners (computerised axial tomography,
CAT). Thermoluminescence dosimetry has proved to be a useful method in the
comparison of patient absorbed dose from these new techniques as well as from the more
traditional ones [4-6].
Diagnostic absorbed dose measurements are important for:
(i) improving the design of equipment to reduce patient absorbed dose, and
(ii) improving radiographers' techniques in the use of equipment to reduce patient
absorbed dose, and for providing a measurement database for epidemiological
analysis of population radiation absorbed dose from diagnostic radiology.
Thermoluminescent phosphors such as LiF:Mg,Ti and particularly the more tissue-
equivalent Li
2
B407:Mn have been used for such measurements. Thermoluminescent
dosemeters have three main advantages over ionisation chambers for this type of
measurement:
(a) they are small and unobtrusive,
(b) they are radio-transparent to most x-radiation, and
(c) they do not require connecting leads and are easily attached to the patient.
Application of TLD in medicine 273
14.3. Factors in the choice of dosemeters for clinical use
A number of factors have to be considered in the choice of the material and form of the
dosemeters for clinical dosimetry. The most important factors are:
(i) estimated absorbed dose range of the intended measurements,
(ii) estimated equivalent photon energy or linear energy transfer (LET) of the radiation,
(iii) immediate environmental conditions around the dosemeter, and spatial resolution.
14.3.1. Absorbed dose range
The sensitivity of any thermoluminescent dosemeter is proportional to the mass of active
phosphor present, within limits imposed by geometrical and thermal considerations
relevant to the readout system. Dosemeters which contain only thermoluminescent
material, e.g. powder, extruded ribbons and rods, have a much higher sensitivity than
dosemeters consisting of a phosphor held in a matrix of binder material, e.g. PTFE-based
discs, tape and micro-rods.
The range of absorbed doses encountered in clinical and biological irradiations is very
large. In diagnostic radiology, absorbed doses may range from less than 10/zGy to
lOOmGy to the gonads and from approximately lOOjuGy to about 100mGy to the skin.
Hence, at the lower end of the diagnostic radiology range, there is a need for a sensitive
form of dosemeter, e.g. powder or extruded forms. However, in therapy dosimetry, a
single treatment fraction of absorbed dose may be several grays, and, in many animal
or cell irradiations, tens of grays may be required. Less-sensitive forms of dosemeter can
be used, especially those incorporating the phosphor powder in PTFE as discs, tape and
micro-rods. The measurement of high absorbed doses will often necessitate using the
dosemeter above the linear thermoluminescence absorbed dose response region. Under
these conditions, the'degree of supralinearity needs to be determined. Often, in radio-
therapy, simultaneous measurements of absorbed dose in the treatment region and the
much smaller absorbed dose in the shadow of shielding may be required. In such cases,
two types of dosemeter, such as extruded rods and PTFE-based rods, may be used in
parallel. This particular combination of dosemeters, if appropriately oriented with respect
to the absorbed dose gradient, should provide good spatial resolution.
14.3.2. Photon energy range and LET of radiation
Modern routine radiotherapy and radiodiagnostic techniques use a wide range of photon
energies from conventional x-ray machines of approximately 10 keV to 200 keV, from
137
Cs (0.67 MeV) and
60
Co (1.25 MeV) teletherapy units and from accelerators producing
high-energy electrons and megavoltage photons.
The total light emitted by an irradiated phosphor is proportional to the total radiation
energy absorbed by it. In tissue, the absorption of Compton-scattered electrons is the
most important absorption process in the photon energy range from approximately
20keV to 10 MeV. For elements such as lithium, boron, oxygen, fluorine, etc, of low
atomic number, and for photon energies up to about 15 keV, the photoelectric effect
is dominant. Thereafter, up to 10 MeV, Compton scattering is most important. For
elements of high atomic number, such as those used as dopants (e.g. Ii, Mg, Mn, etc),
the photoelectric effect is dominant up to several hundred kiloelectronvolts.
274 A FMcKinlay
The advantage of using materials consisting mainly of atoms of low atomic number
with only a few dopant atoms of higher atomic number is obvious because of their good
approximation to tissue and air. This is particularly true of phosphors based on lithium
borate (figure 14.2).
0.0
1.0
-
-
I ' ' '
A
""
B
~^X
c \ \
D \ / \ S .
-N~C*^-
E
I i ' '
1 ' _
-
-
-
^^^
-
10 10" 10' 10
3
PHOTON ENERGY ( keV)
Figure 14.2. Photon energy responses of a number of phosphors relative to that of air.
Curve
A
B
C
D
E
Phosphor
CaF
2
CaSO
A1
2
0
3
LiF
Li
2
B
4
0,
Photon effective
atomic number
16.3
15.3
10.2
8.2
7.4
In order to evaluate the absorbed dose to a phantom or patient using thermolumi-
nescent dosemeters, it is essential to know the relative energy responses of the dosemeters
throughout the range of energies used. The primary response calibration of dosemeters
is usually carried out using a
60
Co source (1.25 MeV) and the responses at all other
energies and for all other radiations are expressed as multiples or fractions of this. For
clinical applications, the response is most usefully expressed as the light emitted per unit
absorbed dose in tissue or water. This will be a function of radiation energy and of the
physical form of the dosemeter.
The beam quality has to be known. Photon-beam quality determination, although in
principle relatively straightforward to determine in free air, is difficult to determine
uniquely in water or solid phantoms because of two effects:
(1) the contribution from lower-energy scattered radiation from the phantom and
external shielding material, e.g. the applicator cone at short focus-to-skin distances
(also at low photon energies the effects of dosemeter orientation and self-shielding
become increasingly important (figure 14.3)), and
Appl
110
100
90
an
> BO
<.
i
Q= 70
60
cation of TLD in medicine
i i _ _ i '
^^PERPEND ICUL AR
_
' ^~~ ^
/PARALLEL
; / :
1 1 1 1
275
0 1 2 3 4 5
HALF-VALUE THICKNESS (mm AD
Figure 14.3. The measured responses of LiF
extruded ribbon dosemeters, exposed with
their square faces parallel and perpendicular
to the axis of the incident radiation.
(Morgan and Bateman [7], reprinted with
the permission of Pergamon Press Ltd.)
(2) the effective 'hardening' of the beam with increasing depth in the water or solid
phantom.
The thermoluminescence absorbed dose (water and polystyrene) response of
LiF:Mg,Ti to high-energy radiations, of which those of principal interest in clinical
applications are megavoltage photons and high-energy electrons, has been widely investi-
gated and reported in the literature. The results have often been inconsistent. Some
investigators have measured approximately 10% reduction in response to high-energy
radiations compared with that to ^Co gamma radiation, and others have not found any
reduction. Much discussion has revolved around the application of various generalised
cavity theories to attempt to explain the observed effects and to reconcile the differences.
For useful reviews and entry into the literature of this subject the reader is recommended
to read the papers of Paliwal and Almond [8] and Ruden and Bengtsson [9]. The relative
energy responses of a number of different physical forms of LiF:Mg,Ti, powdered
Li
2
B
4
0
7
:Mn and CaF
2
:Mn dosemeters for a range of photon and electron energies of
particular relevance to clinical use are presented in table 14.1.
14.3.3. Environmental factors
Absorbed dose range and radiation energy considerations apart, environmental factors
such as temperature, humidity, contact with body fluids, insertion into catheters,
sterilisation, etc, influence the choice of dosemeter form and packaging. If dosemeters
are not protected from their environment, the result is often low precision and sometimes
gross error in absorbed dose measurement.
14.3.4. Temperature and humidity
During exposure under clinical conditions, dosemeters may come into contact with heat
(human body core temperature is 37 C) and/or high-humidity environments. If
implanted or introduced into body cavities, they can come into contact with body fluids.
Some phosphors (especially in powder form) have been shown [14] to be affected by
humidity (figure 14.4) as well as by storage at elevated temperatures which induces fading.
S'
Table 14.1.
^ \ ^ ^ Dosemeter
^ ^ ^
Radiation ^ \ ^
Photons 10 keV
17keV
23keV
37keV
51 keV
81 keV
97keV
6
Co 1.25 MeV
6 MV
18.5 MV
22 MV
35 MV
42 MV
50 MV
65 MV
Measured thermolu:
0.1 mm
LiF-PTFE
discs
3
1.2
1.4
1.45
1.43
1.36
1.15
1.12
1.00
0.96
-
-
-
0.96
_
_
minescence per gray in water for thermoluminescent dosemeters relative to '
0.4-0.5 mm
LiF-PTFE
discs
3
0.95
1.31
1.38
1.42
1.35
1.15
1.12
1.00
0.94
-
-
-
0.93
_
_
LiF extruded
ribbons
3
0.78
1.36
1.43
1.45
1.38
1.17
1.13
1.00
0.97
-
-
-
0.96
_
_
LiF-PTFE
rods
3
_
-
_
-
-
-
-
1.00
0.97
-
-
-
0.97
_
_
LiF
rods
3
_
-
-
-
-
-
-
1.00
0.97
-
-
0.90
b
_
0. 91
b
0. 91
b
LiF
powd
_
-
-
-
-
-
-
1.00
-
0.94
0.93
-
_
_
_
'"Co.
er
c
CaF
2
powder
c
_
-
-

-
-
-
1.00
-
0.96
0.96
-
-
_
_
Li
2
B0
7
:Mn
powder
c
_
-
-
_
-
-
-
1.00
-
-
0.98
-
-
_
_
Electrons 4.3 McV
5 MeV
6 MeV
7.4 MeV
9 MeV
9.8 MeV
10.0 MeV
11.6 MeV
12 MeV
14.3 MeV
15 MeV
18 MeV
19.4 MeV
20 MeV
28.2 MeV
30 MeV
35 MeV
39.2 MeV
40 MeV
0.93
-
-
0.93
-
0.93
-
0.93
-
0.94
-
-
0.96
-
0.96
_
_
0.98
_
0.90 0.90 0.92 0.92 - - -
0. 95
d
_ _ _ _ _
- 0.94
0.91 0.91 0.94 0.94 - _ ^
- - - - - 0.94 0.97
0.91 0.91 0.94 0.94 - - r
0.90
d
- - - - -
0.91 0.91 0.94 0.94 - - - '
- - - - 0.93 0.98 0.96 o
0.91 0.92 0.95 0.95 - - - "^
- - - - 0.92 0.97 0.96
- - - - 0.89 0.97 0.97
s
-
0.92 0.93 0.96 0.96 - - - a
0.92
d
- - - - _ |
0.92 0.94 0.96 0.96 - - - S'
0.94
d
_ _ _ - S'
0. 95
d
_ _ _ _ _
0.93 0.95 0.97 0.97 -
-,d
0.92"
a
Ruden [10].
Turner and Anderson [11].
c
Almond and McCray [12].
Bistrovic et al [13], lucite phantom.
- J
278 A FMcKinlay
80
LU
z
o
ft 60
LU
> 40
t
<
i
LU
20
-
"
"
"
^\ ^

-
i i i
20 40 60 80
RELATIVE HUMIDITY (%)
100
Figure 14.4. Effects of humidity on
the response of L i
2
B
4
0
7
:Mn 38 days
preirradiation storage at 40 C.
(Mason et al [14].)
14.3.5. Other agents
If dosemeters in solid form are attached directly on to the skin using adhesive tape, care
should be taken to remove all traces of adhesive from the dosemeters before readout.
Adhesives often exhibit thermoluminescence following exposure to visible light and/or
ultraviolet radiation. The simplest way of avoiding these effects is to seal the dosemeters
inside protective envelopes (e.g. polythene).
14.3.6. Sterilising of dosemeters
Occasionally, a clinician or biologist will require dosemeters to be sterilised. The three
common methods of sterilising, i.e. autoclaving, chemical sterilising and irradiation with
254 nm ultraviolet radiation, can all have a gross effect on the inherent sensitivity of the
dosemeter or may induce spurious luminescence. In general, provided the phosphor is
effectively sealed in a protective envelope or catheter which is opaque to the sterilising
ultraviolet radiation, either chemical or ultraviolet sterilising at normal ambient tempera
ture is recommended. Normal ambient temperature is emphasised, as the effects of
elevated temperatures on the normal sensitivity of phosphors, especially LiF:Mg,Ti, can
be significant. The effects of autoclaving can be particularly severe.
14.3.7. Spatial resolution
Good spatial resolution of absorbed dose measurement is generally useful, and is essential
in the determination of high absorbed dose gradients. Thermoluminescent dosemeters
are available in many shapes. Powder acts like a fluid and will adopt the shape of its
container. The microrod and extruded ribbon (and hot pressed) dosemeters are so small,
1 x 1 x 6 mm
3
and 3.2 x 3.2 x 0.9 mm
3
, respectively, that the effective size of the dose
meter is often limited in practice by the requirement to have adequate buildup to ensure
electronic equilibrium.
Application OF TLDin medicine 279
14.4. Radiotherapy absorbed dose measurements
14.4.1. Simple geometry phantoms
In radiotherapy, the specification of the complete absorbed dose distribution within the
radiation beam in a phantom is a prerequisite to ensuring that the prescribed absorbed
dose is delivered to the target volume in the patient. A common method is to employ
published depth dose data and an isodose chart. An example of such a chart is illustrated
in figure 14.5. This chart refers to a section containing the beam axis parallel to one side
5
_
i _
x
o
i
| 10
Q_
2
X
1
15
20
|
'-11^:
t \ \
J'
K)4
20%
1100%
- _ _ 90% - -
^ - _ _ e o% _ _ _ _ - ^ '
~- 70% - ^
~-___60%___ ^
~^_ 50% - '
- 40% - -
30% ^
. -
l
y
l \\ \ :
/ 1
y
'\
20%/
1 1

1 1

10%

_
-

-
Figure 14.5. Radiotherapy isodose chart for a
60
Co teletherapy unit. Field size l OXl Ocm
2
sourcetoskin distance 80 cm.
of a
60
Co 10x10 cm
2
therapy beam for a fixed sourcetoskin distance (SSD) of 80 cm.
The lines mapped on the chart link points of equal absorbed dose expressed as a
percentage of the peak absorbed dose. In the case of
60
Co radiation, the peak absorbed
dose occurs at the optimum 'buildup depth' in water, 5 mm. For xray beams produced
with generating potentials of less than 400 kV, the depth doses are conventionally
expressed as a percentage of the surface absorbed dose. Similar charts are used for fixed
sourceaxis distance (SAD) beams. However, in these, the isodose values are expressed
as a percentage of the absorbed dose at the target deep within the phantom, SAD isodose
charts are used when the target volume is located on the axis of rotation of the tele
therapy machine. The selection of an appropriate isodose chart can be difficult, as the
absorbed dose distribution in the phantom depends on the beam dimensions, SSD or
SAD, the radiation quality, the source size, the geometry of the beam and the positioning
of the beam collimators. The International Commission on Radiological Units (ICRU)
[15] therefore recommends the use of isodose charts which are exactly specified for the
280 A FMcKinlay
particular equipment being used. This criterion can be established, as 1CRU recommend,
by a series of single measurements using an ion chamber or thermoluminescent
dosemeters.
In their simplest form, the measurements consist of:
(1) measuring the depth dose distribution along the central axis of the beam in a water
or water-equivalent phantom, and
(2) choosing one particular phantom depth (which in the case of 150 keV to 10 MeV
and
l37
Cs and
60
Co teletherapy beams, ICRU recommends as 5 cm) and measuring
the radiation absorbed dose profile across the beam at this depth.
After normalisation of the depth dose measurements at 5 cm depth, the published
dose data which one intends to use can be compared with them and corrected
accordingly. Similarly, the measured beam profile can be compared with that obtained
from the published isodose chart.
Since 1968, the International Atomic Energy Agency (IAEA) and the World Health
Organisation (WHO) have been running a programme of intercomparison of ^Co tele-
therapy units in the various radiotherapy centres throughout the world. This resulted from
investigations carried out in 1965 which revealed that there was no suitably calibrated
radiation measuring instrument in use in about 30% of the radiotherapy centres
investigated [16]. A simple test procedure based on thermoluminescence dosimetry is
used to assess the accuracy of delivered absorbed doses in the centres.
LiF:Mg,Ti powder dosemeters contained in PTFE capsules are sent to radiotherapy
centres. The measurement technique used in this study illustrates:
(i) the practical use of thermoluminescent dosemeters for radiotherapy depth dose
measurements in a simple phantom, and
(ii) methods to eliminate effects of fading and other variable environmental factors.
The procedure used is illustrated in figure 14.6.
LiF
POWDER
STANCARD
ANNEAL
IRRADIATE
CONTROL
IRRADIATE
REFERENCE
A
B
C
D
R
-^
TEST
2Gy'
TEST
2 mm
^
READOUT
Figure 14.6. Method employed by IAEA and WHO for the intercomparison of delivered
absorbed doses from
60
Co teletherapy units in various radiotherapy centres throughout the
world. A and B are test measurement dosemeters. C and D are irradiated and unirradiated
control dosemeters. R are calibration reference dosemeters. (Eisenlohr and Jayaraman [16].)
Application O/TLD in medicine 281
Participant centres are sent four sets of dosemeters. They are requested to irradiate
one test set (A) with an absorbed dose of 2 Gy in water at 5 cm depth on the central axis
of a ^Co 10x10 cm
2
therapy beam with an 80 cm SSD. Another test set (B) is to be
irradiated under similar conditions for 2 min. A control set (C) which has been given a
known absorbed dose by IAEA and a control set (D) which is unexposed accompany
sets A and B at all times except during irradiation. Sets C and D provide information
about any environmental or spurious effects, such as thermal fading, unintentional
irradiation, etc, which might adversely affect the test dosemeters. In addition, reference
sets (R) are irradiated by IAEA in a standardised 10x10 cm
2 60
Co beam (SSD 80 cm)
at a depth of 5 cm in water. The absorbed dose rate expressed in grays per minute in
water is obtained from a measurement of the exposure rate in free air using a calibrated
ionisation chamber. All dosemeters are then read out together, eliminating possible
calibration errors due to fading and effectively standardising the readout procedure for
all dosemeters.
14.4.2. In vivo measurements
While the measurement of complete absorbed dose distribution in a phantom is essential
in planning the treatment of a patient, the ultimate check on the absorbed dose delivered
to the patient can only be made by in vivo absorbed dose measurements. Thermo-
luminescent dosemeters have proved to be particularly useful for this purpose.
The relevance of in vivo dosimetry is illustrated by the flowchart shown in figure 14.7.
This flowchart is a simplified form of that used by ICRU [15] to illustrate a systems
approach to radiotherapy. In vivo measurements verify that the absorbed dose prescribed
by the clinician, and calculated and set up by the physicist and the radiographer, has been
delivered. Further, it may be used to monitor any change in field uniformity caused by
changes in the many treatment parameters.
In vivo measurements can be divided into four classes.
Admini -
stration
Examine
and
diagnose
Decide
on
treatment
Measure
patient
Set up
patient
Start
trea ment
-
Make
casts etc.
for patient
Verify
dose
in vivo
Verify
and
accept
Monitor
further
treatment
in vivo
Com j ut e
dose
Assess
res j i t s
Figure 14.7. Flowchart illustrating the relevance of in vivo dosimetry in radiotherapy
planning and treatment.
282 A FMcKinlay
14.4.2.1. Class 1 -entrance absorbed dose measurements. These are used mainly to
check the machine output, the absorbed dose distribution profile across the patient,
particularly in the penumbra of shielding, and the positioning of shielding in relation
to the patient. If the measured values are at variance with those prescribed and calculated,
the cause can be investigated and appropriate corrective action taken. The spatial
resolution afforded by thermoluminescent dosemeters is particularly useful in these
measurements.
14.4.2.2. Class 2 - exit absorbed dose measurements. These are used mainly to check
the absorbed dose delivered to points deep within the body. The measurements should
agree with calculations for exit absorbed doses. For such measurements, the dosemeters
should be provided with sufficient backscatter material. Again, good spatial resolution
may be important.
14.4.2.3. Class 3 - intracavitary absorbed dose measurements. The absorbed dose within
a body cavity, e.g. the mouth, nasopharynx, oesophagus, vagina, rectum, etc, can be
measured using dosemeters sealed inside a catheter as shown in figure 14.8. The position
of the dosemeters may be checked using radio-opaque markers and exposing an x-ray
film. The increase in scattered radiation resulting from the presence of radio-opaque
markers of high atomic number can cause uncertainties of a few per cent in the absorbed
dose to the dosemeter. This can be measured and allowed for.
Figure 14.8. Solid forms of thermoluminescent phosphor. Left, TLD 700 extruded ribbon
dosemeters; right, LiF-PTFE micro-rod dosemeters; centre, micro-rod dosemeters in
catheter tubing. (Photograph courtesy of the National Radiological Protection Board,
Chilton.)
14.4.2.4. Class 4 - individual spared organ absorbed dose measurements. The absorbed
dose to spared (shielded) organs can be measured, but often no build-up can be used as
this would in itself result in an increased absorbed dose to the organ.
Application of TLD in medicine 283
14.5. Examples of the use of TL dosemeters in radiotherapy
Thermoluminescent dosemeters are routinely used for a number of different types of
in vivo radiotherapy measurements in centres throughout the world. The following
examples illustrate some of the principles of their use.
14.5.1. Measurement of absorbed dose during 'mantle therapy' for Hodgkin's disease
The radiotherapy treatment of Hodgkin's disease involves the irradiation of a large area of
the body. The treatment field is designed to deliver a therapeutic or prophylactic
absorbed dose to the axillary, cervical and mediastinal lymph nodes. Many different
treatment fields have been used, but one commonly used configuration consists of
anterior and posterior parallel and opposed fields as illustrated in figure 14.9. There is
Figure 14.9. Mantle therapy treatment for Hodgkin's disease. Shielding is shown as a
projection on to body surface.
also the need to shield presumed healthy organs, e.g. lips, eyes, lungs, kidneys, bone
joints, etc, and for posterior irradiation the spinal cord needs to be shielded. To avoid
excessive exposure of the skin (skin sparing), the treatment is carried out using either
^Co or megavoltage x-ray photons and the shielding is positioned some distance
(typically 20 to 50 cm) above the entrance surface of the body. This is achieved using
'individually tailored' moulds of polystyrene, one anterior and one posterior, with
appropriately cut out channels containing lead-shot shielding. Alternatively,
appropriately shaped lead absorbers, placed on a Perspex plate and positioned above the
body, have been used. The technique is termed the 'Gothic arch' or 'mantle' technique.
A typical four-week course of treatment involves a total prescribed absorbed dose of
between 30 and 40 Gy delivered in 20 fractions.
Thermoluminescent dosemeters, usually LiF extruded ribbons or rods or PTFE-based
discs or micro-rods sealed in thin protective polythene sachets, are attached to the body
under moulded blocks of wax or in small Perspex containers. The dimensions of the wax
or Perspex are chosen to provide build-up appropriate to the photon energy of the beam
and to ensure electronic equilibrium. With the use of high-energy photon radiation, e.g.
42 MV x-rays, Ruden [10] recommends the use of a maximum build-up of 15 mm
Perspex and an experimentally derived factor to correct the apparent absorbed dose.
14.5.2. Intracavitary absorbed dose measurement
The small size and shape of the extruded and PTFE-based micro-rod dosemeters have
enabled in vivo measurements of absorbed dose inside body cavities which hitherto were
284 A FMcKinlay
often difficult and sometimes impossible. As illustrated in figure 14.8, these dosemeter!,
can easily be inserted and sealed in catheters.
A very good example of such applications is the in vivo measurement of absorbed dose
distribution in the pelvis during intracavitary
226
Ra and external beam therapy for
carcinoma of the uterine cervix [17-19].
The dosemeters are introduced into the pelvis via the external femoral veins. In one
technique [17], sterile PTFE catheters are first inserted in the veins. This process can be
monitored using x-ray fluoroscopy and television. Inner tubes containing gold radio-
opaque markers are then introduced into the catheter to assess accurately the intended
positions of the TL dosemeters. The radium is then applied and its position in relation to
the dosemeter markers can be assessed. The marker catheter tubes are then removed and
replaced by two others, each containing 15 micro-rod dosemeters spaced some 16 mm
apart. Using this technique of outer and inner catheters, there is no need to sterilise the
inner dosemeter catheters.
14.6. Diagnostic radiology absorbed dose measurements
In the diagnostic range of photon energies, LiF phosphor can over-respond by as much as
40% compared with tissue. However, Li
2
B
4
0
7
:Mn is an extremely good match for tissue
over this range of photon energies and, by adjustment of the fractional amount of
manganese present, the response can be 'trimmed' to match more closely that of air,
water or tissue; e.g. Jayachandran [20] suggested 0.34%w/w for air equivalence and
Christensen [21] 0.45% w/w. Langmead and Wall [22] found that, using Li
2
B
4
0
7
:Mn
powder containing 0.15% w/w of manganese, they could measure absorbed dose in tissue,
from x-rays of unknown quality, with a predicted error associated with photon energy
of not greater than 5% and an overall uncertainty of not more than 15%. This is an'
important characteristic of Li
2
B
4
07:Mn phosphor because, while the effective energy of
the primary beam can be assessed, at least in air, by half-value layer measurements, the
quality of the lower-energy scattered radiation and the magnitude of its contribution to
absorbed dose are difficult to assess. li
2
B40
7
:Mn is therefore particularly suited for such
measurements. While sensitive solid forms of li
2
B
4
0
7
:Mn, such as extruded ribbons, are
commercially available, they are relatively expensive and this tends to exclude them
from large-scale measurement programmes. Loose powder is probably most suitable for
this application at present.
14.6.1. Human phantom measurements
In contrast with simple homogeneous phantoms, a most useful phantom for absorbed
dose measurements in radiotherapy and diagnostic radiology is one which is designed, as
far as is practicable, to simulate the structure of the human body. The torso and head and
neck of such a phantom are shown in figure 14.10. In proportion, it is equivalent to an
'average man' 1.75 m tall and weighing 73.5 kg. It is made from tissue-equivalent
synthetic rubber and contains a complete human skeleton, lung-equivalent material and
airways corresponding to the maxillary sinuses, nasopharynx, trachea, etc. It is
composed of a number of 25 mm thick transverse sections each containing a matrix of
5 mm diameter holes spaced 3 cm apart. Each hole can accommodate a dosemeter holder/
Application of TLD in medicine 285
Figure 14.10. Human-like phantom made
from tissue-equivalent synthetic rubber.
(Photograph courtesy of the National
Radiological Protection Board, Chilton.)
Figure 14.11. Dosemeter capsules, each containing 30 mg of phosphor, being inserted into
a transverse section of phantom. (Photograph courtesy of the National Radiological
Protection Board, Chilton.)
capsule or a solid plug of tissue-equivalent material. The complete phantom contains over
3000 holes and additional ones can be drilled if required. Suitable Perspex or polythene
capsules can each contain approximately 35 mg of powdered phosphor.
Human-like phantoms are extremely useful for absorbed dose measurements in
diagnostic radiology where their human form allows not only precise and realistic
positioning of 'the patient' in the beam but also positioning of dosemeters to measure the
absorbed dose to specific organs, including the gonads. Combined with the use of thermo-
luminescent dosemeters, they have proved especially useful in the assessment of'patient'
absorbed dose imparted by computerised axial tomography (CAT) (e.g. [4, 5]). The recent
measurements by Wall were performed using Li
2
B
4
0
7
:Mn powder dosemeters contained
in plastic containers and inserted in the phantom slices as illustrated in figure 14.11. In
286 A FMcKinlay
these examinations, regions of dosimetric interest included not only the section of the
patient (phantom) undergoing radiological examination at a particular instant in time but
also the adjacent sections which are irradiated as a result of the divergence and scatter
of the primary beam. Wall et al [5] also included measurements of absorbed dose to the
lens of the eye, thyroid, gonads and skin. For these they used Li
2
B
4
0
7
:Mn powder in
polythene sachets.
14.6.2. In vivo measurements
While measurements using human-like phantoms are extremely useful in the assessment of
absorbed dose in diagnostic radiology, the measurements are not performed under
entirely realistic conditions. The information gained from these measurements takes no
account of the skill and experience of the radiographer, the quality and suitability of
equipment and differences in shape and size of patients. In vivo measurements on patients
undergoing routine radiological examinations in hospitals provide a much more realistic
assessment under everyday practical conditions. Li
2
B
4
0
7
:Mn dosemeters are especially
useful for these measurements. They are tissue-equivalent and radio-transparent except
on high quality mammograms. In general they do not interfere with the diagnostic
quality of the image and cause little inconvenience to patient, radiographer and
radiologist.
Langmead et al [23] used Li
2
B
4
0
7
:Mn powder dosemeters, which were the same as
those shown in figure 14.12, for the measurement of absorbed doses to patients under-
going various forms of radiological examinations including cardiac catheterisation, barium
enemas, intravenous pyelography and mammography. Maximum skin and gonad absorbed
doses were measured. The measurement positions of the l x l cm
2
dosemeters for
mammography are shown in figure 14.13.
This series of measurements constituted a pilot survey of absorbed doses to patients,
and recently this work has been extended to include other radiological techniques.
Figure 14.12. Black polythene sachets containing Li
2
B
4
0
7
:Mn powder being attached to
the skin of a patient. (Photograph courtesy of the National Radiological Protection Board,
Chilton.)
Application of TLD in medicine 287
4 cm
Figure 14.13. Arrangement of Li
2
B
4
0,:Mn dosemeters (shown in figure 14.12) for
mammography measurements. (Langmead et a! [23])
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19 Joelsson I and Backstrom A 1970 Acta Radiol. Ther. Phys. Biol. 9 233
20 Jayachandran C A 1970 Phys. Med. Biol. 15 325
21 Christensen P 1967 Manganese-activated lithium borate as a thermoluminescent dosimetry
material, Riso Rep. 161 (Riso: Danish Atomic Energy Commission Research Establishment)
22 Langmead W A and Wall B F 1976 Phys. Med. Biol. 21 39
23 Langmead W A, Wall B F and Palmer K E 1976 Br. J. Radiol. 49 956
Applied Thermoluminescence Dosimetry. Eds M Oberhofer and A Scharmann
1981 ECSC, EEC, EAEC, Brussels and Luxembourg
15
Application ofTLD in biology and related fields
MOBERHOFER
15.1. Introduction
A number of scientists working in the field of biology and related topics have found
TLD techniques a very useful and satisfying way of solving some of their problems. The
diversity of applications allows room to present here only a few representative examples
of the whole spectrum. Short reviews of applications in the following fields are given:
(a) animal experiments,
(b) bone dosimetry,
(c) photon radiation quality measurements,
(d) toxicity determinations,
(e) general biology and biochemistry,
(/) ecology, and
(g) animal habit studies.
15.2. Animal experiments
15.2.1. Example one
As early as 1963, H N Kriegel and coworkers [1] applied TLD for internal body dosimetry
after ^Srj^Y incorporation in an animal experiment. Investigations were made into the
biological behaviour of radio-strontium in pregnant animals. Whereas the deposition of
radio-strontium in the foetus by placental transfer was known for a variety of experi-
mental conditions, there were doubts about the dose occupancy of the embryo during the
total gestation period arising from the radio-strontium deposited within the female
skeleton. CaF
2
:Mn dosemeters, prepared by pouring CaF
2
:Mn powder into plastic tubes
10 cm long and 1.5 mm in diameter and soldering the tubes at the ends, were implanted
close to the left uterus horns below the ovaries of a number of rats. After the animals had
recovered from the implantation operation, they received injections of practically carrier-
free solutions of '"'Sr/^Y with different activities (25 to 100/iCi) into their tail veins.
Seven days post-injection the animals were killed, the dosemeters were recovered and the
amount of ^Sr/^Y as a percentage of the initially administered activity was determined
by ashing of the killed animals at 800 C.
Dosemeters which had been implanted into animals which did not receive radio-
active injections and non-implanted dosemeters were used as controls. The distribution
and retention in the animal organism of '"Sr/^Y within the range of applied activities is
assumed to be independent of the initially deposited amount of radionuclide mixture.
290 M Oberhofer
If this is true, the TL of the phosphor used should be proportional to the injected activity
and/or proportional to the activity measured in the animal after seven days.
This was indeed the case, as could be shown. The dose was determined by putting
TL dosemeters identical to the ones used in the animal experiment into ^Sr/^Y solutions
of different activity concentrations in 250 ml bottles for seven days. The dosemeters were
exposed in the middle of the bottles so that the dose in rads could be calculated from
D
&
= 51.2 x 10
3
x W
0
xCxt (15.1)
where Wp is the mean beta-ray energy in megaelectronvolts, t is the exposure time, and
C is the concentration of the '"Sr/
90
Y solution in millicuries per millilitre. For 1 mCi ml"
1
the expression yields 405 rad.
Now correlating the TL output measured with the TLD system available to the
absorbed dose received by the dosemeters, a calibration factor of 2.2 x 10"
2
rad/relative
unit of TL output was calculated. With this factor, the external dose to the foetus of the
145 g rat, which had received 75 /iCi
90
Sr/
90
Y and retained 85% of that activity after
seven days, was determined as 32 rad within this period.
Experience shows that this dose, and consequently an incorporated '"Sr/^'Y activity
of 75 /iCi is sufficient to cause osteosarcomata with a high probability.
15.2.2. Example two
In another experiment, LiF TLD were applied to measure gamma-ray doses in vivo in
male sheep ingesting
137
Cs to demonstrate that designation of the whole body as a critical
organ will adequately reflect the dose to the gonads in the case of a relatively uniformly
distributed gamma-ray emitting radionuclide. The dosemeters, encapsulated in 4 mm
thick Teflon capsules for beta shielding, were surgically implanted and exposed in vivo
for 15 days to measure gamma dose rates of 20 to 60mradd~
1
in sheep with body
burdens of approximately 300 /dCi of
137
Cs. In a second group of sheep, dosemeters were
implanted prior to feeding with 50 /nCi of
137
Cs per day. These animals were killed at
intervals so that the accumulation of gamma-ray doses in various organs during a month
of
137
Cs feeding could be studied. The study resulted in the finding that the gamma dose
to the gonads is less than that to the midpoint of the whole body and that the use of the
whole body as the critical organ for relatively uniform distribution of gamma-emitting
radionuclides will adequately reflect the gamma-ray dose to the gonads.
15.3. Bone dosimetry
TLD has been used to measure the mean bone marrow dose in specimens of human
vertebrae irradiated with x-rays and gamma rays [2] following a proposal of F W Spiers.
For this purpose, 3 mm thick transverse sections of lumbar vertebrae with different
trabecular structures were cut and washed clean of marrow. The marrow spaces and the
trabecular thickness were measured and the specimens were filled with finely (< 10/mi)
ground TLD-grade LiF before they were covered with cortical bone slices and exposed.
After irradiation, the LiF was recovered and the mean marrow dose determined by means
of the TL of the LiF powder.
Application of TLD in biology and related fields
291
Higher mean marrow doses were obtained for specimens with smaller cavities and the
results agree reasonably well with calculations by Spiers based on the concept of a
distribution of pathlengths in trabecular bone.
Similarly, the mean marrow doses for trabecular bone containing ^Sr/^Y were
deduced by applying tire TLD method to sections of femur of a beagle dog and/or a
miniature swine which had been raised on a diet containing ^Sr/^Y [3]. In this case,
the concentration of ^Sr/^Y in the sections also had to be determined.
The experiments were repeated with specimens of human vertebrae artificially loaded
with (3-particle emitting radio-isotopes (e.g.
131
I).
The works described show that TLD can be applied successfully to problems of inter-
face dosimetry. This was also demonstrated by R J Schulz [4] who used ultra-thin
(5-10 /im) LiF-Teflon discs to study the changes in absorbed dose near tissue-bone
interfaces.
Later, dose and photon-energy measurements for bone marrow were performed in
human (wax) phantoms utilising TL phosphors to obtain rad/R curves for bone marrow
(figure 15.1) to be used in the design of a personal dosemeter following the variations of
absorbed dose in bone marrow with photon energy [5].
" 0 8
V * 100 Kvp X-RAYS
2 4
' Am GAMMAS
20 30 50 70 100 200 300 500 1,000
PHOTON ENERGY (KEV EFFECTIVE)
Figure 15.1. Mean dose to bone
marrow (rad/R) for a human
phantom with rotational irradia-
tion obtained with LiF dose-
meters. (After R A Facey [5].)
15.4 Photon radiation quality measurements
In a number of radiobiological experiments, variations of the x-ray spectra with depth in
tissue or bone, for example, may considerably influence the results. This is a reason for
checking the spectral composition of the radiation field at various points. For determina-
tion of the effective x-ray energy, two TL dosemeters with differing energy responses can
be used [6]: LiF, with a rather flat energy dependence of its sensitivity, and CaF
2
:Mn
or CaS0
4
:Dy(Sm, Tm), with a steep slope of the sensitivity curves in the energy region
from 45 to 150 keV, to mention two possible phosphors (see figure 5.4 in chapter 5).
If a sample of each phosphor is exposed simultaneously to the same radiation, the
quality of which is unknown, then the ratio of their TL responses uniquely determines
this quality. This occurs in locations normally not accessible by other techniques (for
example, ionisation chambers in vivo) or where the presence of another detector or some
detectors would influence the radiation field.
'Tandem' dosemeters have been built [7] which make it possible to distinguish
different radiation qualities in one reading. If a small hot-pressed CaF
2
:Mn dosemeter is
292 M Oberhofer
bonded to the top surface of an extruded LiF dosemeter, for example, and the system
heated out after exposure to an unknown 7-radiation field, a glow curve results with the
glow peaks from LiF and CaF
2
:Mn, the main peak height of which immediately indicates
the effective energy of the photon radiation. This is shown in figure 15.2. The peak-
height ratio curve derived from it is given in figure 15.3.
100
80
S 60
<
40 -
x
o
20 -
-
-
-
L iF
TL D-700 ,
\ 38 keV /
\L 70 /
f\ /&. i v
1 1 8
/
/ ifw jr'
169
/ /
/ ' 1250 \ \ ^ /
1 ^
===
r
CaF
2
:Mn
J~^ 38 keV
70 \
118 \
1250 ] - = = = .
15 30 45 60
HEATING TIME ( SEC)
Figure 15.2. Glow curves obtained with a LiF-CaF
2
: Mn ' tandem' dosemeter for different
quality photon radiation. (From Gorbics and Attix [7].)
o
fee
3.0
20
1.0
0.6
03
0.2
0.1
-
-

-
0 \
1 , , 1,
V - CALCULATED
\ CURVE
\ NORMALIZED
V_ 1
30 60 100
300 600 1000 2000
EFFECTIVE ENERGY ( keV)
Figure 15.3. Peak-height ratio of the glow curves obtained with the LiF-CaF
2
:Mn ' tandem'
dosemeter as a function of effective photon energy, derived from figure 15.3. (From
Gorbics and Attix [7].)
15.5. Toxicity determinations
Recently, W Kriegseis and A Scharmann described a novel potential application of TL for
the determination of the fibrogenic properties of quartz and coalmine dust, which cause
pneumoconiosis and/or silicosis if inhaled for a long time [8].
Irradiated dust samples of natural quartz exhibit characteristic TL maxima at 165 K
and 250 K. This TL is considered to be surface-specific and can be used to estimate
Application of TLD in biology and related fields 293
the amount of uncovered quartz surface, which was shown to take part in pathogenic
interactions. The TL emission is attributed to defects at the boundary between the
quartz surface and absorbed species containing OH groups, for instance water (methanol
in the case of carbon).
For toxicity determinations, the absolute TL intensity of the 165 K peak of the dust
samples, the relative increase of this intensity after water interaction and the TL curve
shape are taken as criteria.
Cytotoxicity results of biological in vitro cell tests confirmed the findings.
15.6. General biology and biochemistry
K S V Nambi in a summary on TLD [9] reports on various applications of TL techniques
in the study of biological and biochemical systems, mostly performed in India. Hydroxy-
benzoic and aminobenzoic acids, urea, nucleic acids, proteins, plant leaves, algae and
bacteria were investigated under different conditions for their TL characteristics [10]. The
inter- and intramolecular transfer of radiation damage in nucleic acids, proteins and their
constituents could be correlated with their TL behaviour [11]. The photosynthetic
electron transport routes in the Z-diagram were correlated with TL and additional routes
determined [12], and the interaction between salts and proteins could be understood
from the TL patterns [13].
15.7. Ecology
15.7.1. Plant nutrition studies
TLD has also been applied in some ecological studies, with good results.
A group of US research workers [14] used LiF powder micro-dosemeters to study
the dose to tree trunks in relation to the dose measured in the soil around the tree roots.
For this purpose, micro-rods were placed about 2 to 3 cm beyond the bark into the
trunks of some white oak trees around Argonne National Laboratory, others were buried
into the soil 5 ft away from the trees and others were located above the soil around the
trees to monitor the soil surface and ground for gamma and beta radiation.
The dosemeters within the tree trunks were removed in successive intervals of two
weeks. The experiment permitted a comparison of inter- and intraspecies variability
insofar as the selected trees were representative.
From the TL plots, seasonal changes in vegetation, marked first by the growth of grass
and secondly by the coming into leaf of the trees, could be seen, arising from alterations
in the localisation of soluble nutrients including '"'K, and other ions such as
137
Cs in the
micro-environment of the trees. The accumulated dose curve for the trees (figure 15.4)
was characterised by a sharp rise that coincided with bud break and early leafing. The
positioning of the micro-dosemeters just at the outer surface of the woody cylinder of
the tree trunk provided maximum exposure to the radionuclides being carried in the sap
stream. Movement of mineral elements in the trunk is greatly increased during the phases
of bud break and leaf and twig growth.
Further results from the experiment are as follows. The environmental radioactivity
in the trees at the time of the experiment could be related to cycling of natural
40
K
radionuclide and possibly of
137
Cs remaining from earlier fall-out. The concentration of
294 M Oberhofer
radon and of its accompanying daughters has also been shown to be related to
meteorological variables. The location of the micro-dosemeters just under the bark
greatly accentuates a response to differential movement of radionuclides in the sap.
Development of foliage by the grass and trees raises the level of K and Cs in the
above-ground environment.
UJ
i n
z
o
a.
10
UJ
or
I
_ i
i
Ul

C
-
-
)
T , -
"I
1 1 1
MARCH
5.5 mR/ week
, _
T /
/
/ T
\ \
]/
0.9 mR/ week V
i A
'
-"
^
[ l /
T \J
FUL L
-
U4-""
T
LEAF
I 1
BUD BREAK
, , i T i , , i '1
U APRIL 8 MAY 12
TIME ( WEEKS)
or
E
^
Ul
(/)
o
o
Q
UJ
\
<
_ l
Z>
Z>
o
<
Figure 15.4. Accumulated doses of the dosemeters placed in the tree trunks. Broken lines:
approximate seasonal dose rates. (After W C Ashby and others [14].)
15.7.2. Sedimentation studies
In the Joint Research Centre, Ispra, micro-TLD have also been used for the measurement
of phosphate diffusion in sediments [15], which is of interest with regard to the
eutrophication of lakes, for example. The study required knowledge of the concentration
gradient produced by the diffusion of phosphates from the lake water into the sediment.
Tliis concentration was determined with the help of a small P0
4
diffusion test facility
using a sediment core from the bottom of the lake of interest and sea water which
received a mixture of natural and radioactive phosphor (in the form of disodium
phosphate) in an amount corresponding to the actual phosphate content of the lake
water. After a certain sedimentation period, the
32
P concentration along the sediment
core was determined with micro-TLD (CaS0
4
:Dy) in a stringer which was inserted into
the core.
It turned out that phosphates concentrate near the surface of the sediment and that
there is little diffusion into the sediment. This also explains why phosphates are released
so easily from the sediment into the sea water under anoxic conditions during the hot
summer months.
Application of TLD in biology and related fields 295
15.8. Animal habit studies
Other scientists have reported applications of miniature TLD for measuring the dose to
small rodents moving around above the soil in a radioactive ecological site. Glass tubes
filled with powdered CaF
2
:Mn and LiF and placed in polyethylene tubing were fastened
around the necks of the rodents used in the experiment. From the dose measured, two
groups of animals could be distinguished: one group representing animals mostly dormant
underground and the other representing animals normally active, tire exposure to animal
per surface area being smaller in the former case.
This example shows nicely how TLD may be used to examine the habits of animals
and to assist in predicting precisely the exposures to an entire population, for example
insects.
References
1 Kriegel H, Hiring N and Neumann G 1963 Strahlentherapie 122 41
2 Zanelli G D 1968 Proc. Symp. on Microdosimetry, Ispra, Italy, 1967. Rep. EAEC-EUR 3747 d-e-f,
p527
3 Zanelli G D and Spiers F W 1969 Proc. 2nd Int. Conf. on Luminescence Dosimetry, Gatlinburg,
Tenn., September 1968. USAECPubl. Conf. 680920
4 Schulz R J 1966 Phys. Med. Biol. 11 623 (abstract)
5 Facey R A 1968 Health Phys. 14 557-568
6 Cameron J R and Kenney G N 1963 Radiat. Res. 19 199 (abstract)
7 Gorbics S G and Attix F H 1968 Int. J. Appl. Radiat. hot. 19 81
8 Kriegseis W and Scharmann A 1980 Proc. 6th Int. Conf. on Solid State Dosimetry, Toulouse,
France, 1-4 April 1980. Nucl. Instrum. Meth. 175 No 1 239^10
9 Nambi K S V 1977 TL: its understanding and applications Rep. INF. IEA 54, CPRD-AMD 1,
MAIO (Sao Paulo, Brazil: Instituto de Energie Atomica)
10 Aramu F, Maxia V, Serra M and Spano G 1972 J. Lumin. 5 439-448
11 Tatake V G 1975 Proc. Nat. Symp. on TL and its Applications... Kalpakkam, Madras, India,
12-15 February 1975. Bhabha Atomic Research Centre Rep. CONF-750294
12 Sane P V 1975 Proc. Nat. Symp. on TL and its Applications... Kalpakkam, Madras, India,
12-15 February 1975. Bhabha Atomic Research Centre Rep. CONF-750294
13 AltekarW, Tatake V G and Sane P V 1975 Proc. Nat. Symp. on TL and its Applications...
Kalpakkam, Madras, India, 12-15 February 1975. Bhabha Atomic Research Centre Rep. CONF
750294
14 Ashby W C, James N B, Kastner J, Oltmann B G and Moses H 1966 Thermoluminescent dosimetry
and environmental radiation studies ANL Rep. ANL-7220, pp 115-19
15 Oberhofer M 1977 Atomkernenergie 30 164
Applied Thermoluminescence Dosimetry. Eds M Oberhofer and A Scharmann
1981 ECSC, EEC, EAEC, Brussels and Luxembourg
16
High-level photon dosimetry with TLD materials
M OBERHOFER
16.1. Introduction
For very high dose levels in the 10
4
to 10
8
rad range, for example in radiation chemistry
and technology (polymerisation, vulcanisation of rubber, cracking of hydrocarbons),
food processing, radiation sterilisation, material testing, etc, chemical dose measuring
techniques such as the Fricke (Fe
2+
, Fe
3+
) system, the ceric-sulphate system, the ferric-
cupric system, the oxalic system or organic dyes in liquid solution are being used
successfully together with calorimetric methods.
The former techniques have been reviewed by Fricke and Hart [1], by Holm and Berry
[2] and by Stolz [3] and also in a publication by the IAEA [4]. Most of the methods
require much effort or, at least, careful attention in order to obtain good results and are
too expensive for routine measurements, where hundreds or even thousands of single
measurements have to be performed. A less expensive method may be found in the
application of the thermally stimulated emission of luminescence light (thermolumi-
nescence, TL) of certain materials following exposure to radiation (radiothermo-
luminescence, RTL) or in TL-related phenomena.
Some years ago, Gorbics et al [5] compared several such thermoluminescence dosi-
metry (TLD) systems for the 10
3
-10
6
R gamma exposure range. This investigation was
performed with the aim of finding the system with the most convenient handling
characteristics, for a special application, and also low cost for single throw-away use,
relatively small divergence from linearity, lack of dose-rate dependence, good reproduci-
bility of response from one dosemeter to another without the necessity for annealing,
weighing or individual calibration and similarity of atomic number between the TL
material (phosphor) and the dose reference material, here silicon. Additional desirable
features would be no signal loss with time, possibly no sensitivity to light, small size and
also the possibility of detecting exposure inhomogeneities within the irradiation volume.
The phosphors investigated by Gorbics and coworkers were calcium fluoride activated
with manganese (CaF
2
:Mn), lithium fluoride activated with manganese and titanium
(LiF:Mg,Ti) and lithium borate activated with manganese (Li
2
B
4
0
7
:Mn). All of these
phosphors have dynamic ranges extending to at least 10
5
R and do not exhibit excessive
TL signal fading during storage at room temperature. This is of importance if the exposure
has to be performed at a rather low exposure rate over an extended period of time or
if the phosphor can only be evaluated (read) at a later date.
In some cases, high dose level measurements have to be performed at elevated process
temperatures, requiring phosphors which do not lose their information during exposure
at these temperatures. From their comparative studies, Gorbics and coworkers concluded
that, for their purpose, a 0.4 mm thick, 5% loaded CaF
2
: Mn-Teflon disc was the choice
298 M Oberhofer
for routine measurements of absorbed dose (the TL reading could be performed with
a 3% standard deviation at 10
3
R, not corrected for phosphor mass variations) in
transistor (silicon) material, which at the time of the investigation (1973) was
commercially available at a price of $0.30 each.
For other purposes, the other two TL phosphors may be more suitable, depending on
the materials to be exposed to high doses. So LiF:Mg,Ti with an effective atomic
number Z of 7.4 may be the better phosphor for reference materials with similar Z.
Some of the results of Gorbics and coworkers will be presented below and will be
supplemented by further relevant data obtained by other authors. Besides LiF:Mg,Ti,
Li
2
B
4
0
7
:Mn and CaF
2
:Mn, some other phosphors (currently used mainly for personal
dose assessment and environmental dose control) will be considered for their suitability
for high dose level measurements. The review will conclude with a table of useful data on
phosphors applicable in dosimetry at high exposures.
16.2. Lithium fluoride
The TL phosphor LiF:Mg,Ti is available commercially in several forms, as a powder, as
hot-pressed chips and also incorporated in Teflon as rods, ribbons and discs.
Its glow curve, that is the TL light output plotted versus the heating temperature,
shows several peaks with the normally used 'dosimetry' peak at about 200 C. Either the
peak height or the light sum under the peak may be used for dosimetry. As the peak
height depends upon the heating rate (Randall-Wilkins shift) and its use for quantitative
exposure or dose measurements requires reproducible heating rates, the light sum is
normally used for most applications.
If the light sum response is plotted as a function of exposure, one observes that,
beginning with a certain exposure, the TL output increases more than proportionally
with exposure. This phenomenon is called 'supralinearity' and is observed in most TL
phosphors. The extent to which supralinearity exists is best seen if the relative TL
response of the phosphor per exposure unit, here per roentgen, is plotted over the
exposure. To be independent of the type of reader, the TL output per roentgen may be
normalised to an exposure, for example of 10
3
R.
This has been done in figure 16.1 for the 200 C peak of various LiF:Mg,Ti dosemeter
types manufactured by The Harshaw Chemical Co. (powder and chips) and/or Teledyne
Isotopes Inc. (the Teflon disc dosemeters). The curves were obtained with a Harshaw
Model 2000 TLD reader with the maximum heater temperature set to maintain the light
sum under the 200 C peak. The horizontal part of the curve indicates exposure pro-
portionality or linearity with exposure up to 1000R. Above 1000R, LiF:Mg,Ti is
supralinear with a maximum response per roentgen just below 10
S
R. From here on,
towards still higher doses, the response per roentgen decreases again. This is in good
agreement with the findings of other authors [6, 7], some of whom [8, 9] also find that
the supralinearity depends on the grain size of the phosphor.
In a very recent publication, Piesch et al [10] found a response that was higher by a
factor of 3.4 to 4.1 (
137
Cs irradiation), instead of 2.3 to 2.6 (
60
Co irradiation) according
to Gorbics et al, at the maximum compared with the response at 10 R. The authors also
found that supralinearity starts at 100 R and has a different form for LiF TLD 600 and
TLD 700 a reason to be careful in assuming that the characteristics of LiF:Mg,Ti
High-level photon dosimetry with TLD materials 299
3 r
LLl
o
a.
a.
LU
0 -
o
a.
in
UJ
tr
UJ
>
< 0
LU
CE
10'
-THICK TEFL ON
D ISCS
( 0 4 mm
- CHI PS
- POWD ER (10 mg)
- THI N TEFL ON
D ISCS (0.13 mm)
,, ,,l
10
3
10* 10
5
10
6
60
Co y-RAY EXPOSURE( R)
Figure 16.1. 200"C TL peak light sum response per roentgen for LiF (TLD 700) exposed to
60
Co gamma radiation, normalised to 1.00 at 10
3
R. (After Gorbics et al [5].)
dosemeters are the same even if material is used with identical activator composition and
preliminary treatment. Changes do occur from batch to batch and the dose response
curves need to be checked!
The upper dose limit is governed by saturation effects in the phosphor crystals and is
normally set 20% below the saturation value. The useful dosimetry range was found to
extend to about 10
S
R for all types of dosemeters which were checked. Supralinearity is a
drawback insofar as the response curve has to be known for dosemeter evaluation.
In the case of complete linearity, only the TL response per roentgen needs to be known
in order to arrive at the actual exposure in roentgens or dose in rads. According to La
Riviere [11], less supralinearity at high exposure levels up to 10
4
R occurs if the LiF
phosphor has been pre-exposed to a high dose and if the deep traps in the phosphor have
not been annealed. Practically no supralinearity up to 5xl 0
5
R is observed if the
LiF:Mg,Ti has been modified by diffusion of hydroxide ions into the lattice. The
chemical treatment is described by De Werd and Stoebe [12]. So far the method has not
found any practical application.
Concerning the reproducibility with which exposures may be determined at high doses
utilising commercial LiF:Mg,Ti dosemeters, the following standard deviations for
sample-to-sample reproducibility determined by Gorbics et al will be mentioned here.
At 10
3
R they obtained:
2.6% for 10 mg powder samples (home-dispensed),
0.9% for hot-pressed chips,
(a)
(b)
(c) 5.1% for 0.4 mm thick Teflon discs, and
(d) 4.5% for 0.13 mm thick Teflon discs.
The values were determined with the virgin dosemeters as received from the manufacturer,
without any heat treatment (annealing) before or after irradiation. No correction for mass
variations was applied.
300 M Oberhofer
As can be seen, the best results were for chips, with a standard deviation of about
1%. For exposures above 10
3
R, no similar data for sample-to-sample reproducibility
could be found in the literature.
In studying the reproducibility of different dosemeters of the same type, one should
always recall that there may be considerable changes from batch to batch, as was shown
by Regulla [13]. Not only is it apparently very difficult, if not impossible, for the manu-
facturer of the TL material to reproduce the average detector sensitivity from one batch
to another, but it also seems to be difficult to obtain the same sensitivity distribution
within a single batch. This can be seen from figure 16.2, where the distribution of the
sensitivity of two batches of LiF:Mg,Ti TLD 100 detectors delivered together is given.
For micro-rods exposed to 10R, Regulla finds sensitivity variations within one batch as
high as a factor of 3 and typical relative standard deviation values of around 15%. Within
four years the TL sensitivity of one dosemeter type from the same producer decreased
by a factor of 5! From this, it may be concluded that, also with regard to dosemeter
reproducibility, one should be very careful in assuming that the dosemeter-to-dosemeter
reproducibility stays the same from batch to batch, particularly over extended periods of
time. Like the dose characteristic, the reproducibility needs to be checked repeatedly.
Earlier it was mentioned that a good phosphor should have no excessive signal fading.
At ambient temperature (25 C), this fading may be rather low for LiF:Mg,Ti, about
5% in one year if thermally stabilised (for example, by a heat treatment at 100C over
lOmin after exposure just before reading). One should take care when considering the
fading characteristic, as large variations from the value given above can be found
depending on the environmental temperature and humidity. Thus, instead of 5% per year,
a signal loss of 10% is found in six weeks if the phosphor is kept at 32 C instead of
25 C [14].
LiF:Mg,Ti can also be used for exposure measurements beyond 10
5
R if, instead of
the 'dosimetry peak' at 200 C, some other glow peaks which appear at high doses are
used.
at
uJ
BATCH
X-504-S ( 3-4)
755 DETECTORS
i DETECTOR SENSITIVITY (ARBITRARY UNITS)
Figure 16.2. Distribution of the sensitivity of LiF:Mg,Ti TLD 100 micro-rods from the
same source, exposed to 10 R. (From Regulla [13].)
High-level photon dosimetry with TLD materials 301
Starting with 4 x 10
4
to 6 x 10
4
R, a peak appears which centres at a temperature of
around 280 C and saturates at about 2 xl 0
6
R [15]. The evaluation of the peak is some-
what difficult owing to the presence of the 200 C peak, which in spite of increasing
exposure is decreasing. As the total light output does not change too much with dose in
the temperature range of the peak, use is made of the ratio of the peak heights which
varies strongly with exposure. This method can be used for exposure measurements up
to 10
7
R, independent of sample weight. In figure 16.3 a
60
Co calibration curve for
LiF:Mg,Ti TLD700 (Harshaw) is reproduced [15], which is based on the ratio of the
200 C peak height to that at 280 C. According to Kitahara et al, undoped LiF may also
be used with success for high dose measurements [16]. The authors had prepared LiF
powder from purified Li
2
C0
3
, reagent grade HN0
3
and NH
4
F, which contained only
some natural impurities. The glow curves were characterised by two glow maxima, one
at 150 C and one at 335 C. The response curves of the material exposed to
60
Co gamma
radiation are reproduced in figure 16.4. This figure indicates that the response to ^Co
radiation is linear from 10
2
R up to about 5xl 0
4
R utilising the light sum under the
150 C peak. No linearity is obtained for the light sum under the 335 C peak. The
10 t-
5 1
i i i i i 11 I
0.01 10 0.1 1.0
DOSE, Mrad
Figure 16.3. LiF TLD 700 calibration curve, (peak height at 200 C) -e- (peak height at
280C) plotted against dose. (After Jones and Martin [15].)
6 0
Co GAMMA RAY IRRADIATION
O 150 C PEAK
a 335 C PEAK
EXPOSURE, R
Figure 16.4. TL response for the two LiF glow peaks of undoped LiF powder for
60
Co
radiation. (After Kitahara et al [16].)
302 M Oberhofer
latter peak may be used up to an exposure of 10
8
R with proper calibration of the
material.
Goldstein et al [17] find yet another glow peak between 425 and 475 C, not for
TL-grade but for optical-grade LiF manufactured by Isomet Corp. (Palisades, New Jersey,
USA). This material, Isomet 1, was chosen because of the lack of dominant glow peaks
below 350 C. All the crystals (ground and sieved to a size between 100 and 200 mesh)
which were checked showed a measurable TL for megarad exposure. The high reading
temperature (450 C) made it necessary to modify the heating and timing circuits in a
commercial reader, which was a Controls of Radiation Inc. TLD reader. As the infrared
light emission from the sample holder and the sample itself at 457 C is rather disturbing,
an infrared-light-absorbing filter and a blue filter were needed to minimize interference
by blackbody radiation. Figure 16.5 shows the relative light output of the 450C glow
peak for the Isomet material for exposures up to 10
9
R starting from 10
s
R. Values could
be read from glow curves for exposures as low as 10
4
R. As can be seen, the response is
nearly linear up to 5 x 10
7
R where the material starts to become saturated. If, instead of
Isomet 1, another LiF material from the same manufacturer, called Isomet 2, is exposed,
even higher values (2 x 10
8
R) for the beginning of saturation are noted.
10' 10
EXPOSURE ( R)
Figure 16.5. Relative TL output of the 450 C peak for two optical-grade LiF powder
materials from Isomet Corp. as a function of exposure. (From Goldstein et al [17].)
The curves are still useful beyond the saturation starting point if one takes advantage
of the changes in the shape of the glow curves above and below the saturation regions,
together with a progressive shift of the glow peaks towards higher temperatures with
higher exposures. Figure 16.6 shows what was obtained with 16 mg samples of Isomet 1
LiF powder exposed to ^Co radiation of indicated exposures. In the case of Isomet 1,
exposures higher than 10
8
R and, in the case of Isomet 2, from 5 x 10
8
to 10
9
R, may be
measured in this way.
Where a commercial TLD reader cannot be modified for enabling high-temperature
peaks also to be evaluated or where a high-temperature TLD reader cannot be built, yet
High-level photon dosimetry with TLD materials 303
APPROXIMATE TEMPERATURE ( C)
50 100 150 200 250 300 350 400 450 500
>-
m
3 5
Q.
3
O 4
g
3
2
UJ 1
1 1 1 1 1
- f\
- /
, 1/ - T ^ 1
1 1 1
f
, u-r-n , 1
1 1
\
/
XD
\ J
, 1 , I V
12 14 16 18 2 4 6 8 10
TIME (s)
Figure 16.6. Glow curves for Isomet 1 LiF powder sample exposed to (A) 8X10
S
R, (B)
10
7
R and (C) 2 X 10" R
6
Co radiation. (From Goldstein et al [17].)
another possibility exists to measure elevated exposures up to 2x 10
8
Rand even higher,
beginning at about 10
6
R, by performing optical density measurements of absorption
bands. Such absorption bands are induced in optical-grade l i F (Isomet 1, for example,
or similar material from E Leitz, Wetzlar, Germany) by radiation, if the exposure is-
sufficiently high. This method, of course, no longer has anything to do with TL, but it is
an interesting alternative and will be outlined here in some detail.
In figure 16.7 the optical absorption spectrum of optical- (standard uv) grade window
chemical LiF from Isomet Corp. is reproduced [18], which was obtained 24 h (to allow
for peak growth) after exposure to 2xl 0
7
R. For evaluation, the band at 450 nm
(M band) is preferably used, which according to Claffy and coworkers [19] is thermally
more stable than others (R and N
2
band).
Figure 16.8 gives the increase of optical density at the absorption peak as a function of
exposure for the three peaks. In these measurements, cleaved crystal plates were used.
The optical density was obtained before and after irradiation with a Cary Model II
spectrophotometer. Prior to exposure, the crystals were annealed at 550 C for 20 min.
Exposures beyond 2 x 10
8
R could still be measured, probably up to 10
9
R, by making use
of the N
2
absorption band. The method has the advantage that the crystals can be
thermally bleached and re-used. The re-use produces the same optical density versus
exposure curve and reproducibility remains unchanged. The variations in optical density
measurements at a given exposure for different crystals was found to be less than 5%.
The drawback of the method described is the relatively high cost of the single crystals,
causing Claffy et al [19] to check whether the LiF optical absorption method could be
performed with LiF samples in powder form. Leitz uv-grade LiF was ground, thoroughly
mixed and then sieved through 100-200 mesh. The 'apparent' optical density (AOD) of
304 M Oberhofer
20
15
10
05
-
-
-
\
l
1 M
N
2
-*l l
400 500 600
WAVELENGTH ( nm )
Figure 16.7. Absorption peaks of Isomet optical-grade LiF, 24 h after exposure to
2 X10
7
R. (From Vaugham and Miller [18].)
o
I0
6

9
Figure 16
grade LiF
io
5
io
6

7
EXPOSURE (R)
.8. Optical density of the three different absorption bands of Isomet optical-
versus exposure. (From Vaugham and Miller [18].)
30 mg samples was determined with a diffuse reflectance apparatus described in detail
there [19].
Two typical absorption spectra are shown in figure 16.9, which compare with the
spectra obtained by Vaugham and Miller (see figure 16.7). With increasing dose and the
subsequent changes in optical absorption (AOD) of the M band (X = 450nm) and the
R
2
band (X = 377 nm) in Leitz LiF, it follows that the method may be used for the
measurement of doses between IO
6
and IO
7
rad or between IO
6
and 10
s
rad, respectively.
Contrary to Vaugham and Miller's results for cleaved crystals, there is no linear response
of the M band utilising the powder material. The AOD exposure curves of the M and
R
2
bands are not linear, and therefore calibration curves are necessary.
Claffy and coworkers also showed that there was no detectable difference in TL output
of the LiF material in the 400-475 C region with or without a prior 60 min exposure to
light in the diffuse reflectance apparatus. This means that dose determination by AOD
High-level photon dosimetry with TLD materials
305
^ 0 . 9
Q
0 8
**
> 07
1-
to
Z 0.6 111
Q
_, 0 5
<
y
0
. 4
i
Q.
0.3
I
Z
W 0.2
cr
#
8: o.i
<
0
3
-
1~
1
50
/
/
\ /
\j
1
400
/">
/ \
/ \
/ \ .6.7x10' rod
' Y
\
\
A \
l\ \
/ \ \
/ \ *
s
-
/ \ ^
\ \
\ > N
\-6.Ax10
6
rQd s.
N^
>
^
~~
I I I I I
450 500 550 600 650
WAVELENGTH A, nm
Figure 16.9. Absorption spectra of Leitz
LiF powder exposed to "Co gamma radia
tion. (After daffy et al [19].)
measurement can therefore safely precede standard TL readout procedures, as described
by Goldstein et al [17], and thus replication of dose information be achieved. This may
be useful where repetition of exposure would not be feasible.
At room temperature, the stability of both the M and R
2
bands, as functions of time,
after exposure is adequate for most practical applications.
Also, the radiophotoluminescence (RPL ) of TLgrade LiF [20] as well as opticalgrade
LiF [19] may be utilised for high dose level measurements, which between 10 and 10
6
R
is nearly a linear function of exposure. This is shown in figure 16.10. Excitation should
be performed with 450455 nm light.
The maximum RPL occurs at an exposure of more than 10 times the saturation value
of TL measurements (see figure 16.10). The RPL also turns out to be very stable at normal
10
6
h
io
2
w
3
K)
4
10
5
10
6
10
7
10
8
w
9
DOSE [R]
Figure 16.10. Radiophotoluminescence (full curve, excitation with 450 nm light) and
thermoluminescence (broken curve, total light sum) of TLDgrade LiF:Mn,Ti (TLD 100)
as a function of exposure. (From Regulla [20].)
306 M Oberhofer
ambient temperatures and in the dark (uv light causes fading) after thermal stabilisation
at 100 C for 5 min. No fading could be observed within one month after the end of
irradiation. Instead of TLD-grade LiF (LiF 100, for example), non-TLD-grade LiF in
powder form can also be used for RPL measurements. For Leitz uv-grade LiF, Claffy
and coworkers [19] obtained optimum excitation with light at 455 nm. If the RPL is
plotted over the exposure of the material, one obtains the curves shown in figure 16.11.
There is apparently linearity only from 2 x 10
s
to 2 x 10
6
rad for the 520 nm band.
io
J
^
>-
DC
<
m
Q:
<
LU
or
O
2
o_
10 -
B
670 nm-BAND A * '
3mm No 2424 / /
A \ / /
(670+520 nm) / /
BANDS f /
3mm No 3384 /
/ /
/
-M- A
" " ^ B
10'
/
10
1
W' 10'
^_ 10
7
10
B
ABSORBED DOSE IN LiF, RADS
Figure 16.11. RPL of Leitz LiF as a function of exposure (
6
Co). Excitation with 455 nm
light, Corning filters indicated. (From Claffy et al [19].)
From what has been mentioned so far, it is evident that there are a number of ways to
apply TL-grade and also optical-grade LiF in high-level dosimetry, by taking advantage not
only of its TL emission but also of the emission of radiophotoluminescence light and by
performing absorption measurements. In any case, exposure to high doses causes changes
within the dosemeter materials, which remain even after a high-temperature annealing
and in most cases excludes re-use of the material.
Heating LiF:Mg,Ti at 400-700 C for several hours brings the material back to zero
signal, but at the same time reduces its sensitivity to, for example, 33% of its original
value after exposure to 2 x 10
s
rad. In this case, the material is thrown away, which may
be expensive considering that the cost of TL-grade LiF is rather high. The high cost of the
dosemeter material thus often excludes its application in high-level dosimetry.
16.3. Lithium borate
The next TL phosphor to be considered for the measurement of high doses is li^O^.Ma.,
which like LiF: Mg,Ti is commercially available in several forms. It can be purchased as a
powder (Harshaw), as hot-pressed chips (Harshaw) and incorporated in Teflon (0.13 mm
and 0.4 mm thick discs, Teledyne Isotopes).
The light sum response per roentgen as a function of ^Co gamma-ray exposure is shown
in figure 16.12 for virgin dosemeters of various forms. The curves in the figures were
High-level photon dosimetry with TLD materials
307
60
Co
Y
-RAY EXPOSURE (R)
Figure 16.12. 200-250C TL peak light sum response per roenten for Li
2
B
4
0
7
:Mn as a
function of exposure (
60
Co gamma radiation), normalised to 1.00 at 10
3
R. (After Gorbics
etal [5].)
obtained with the same instrument under the same conditions as the corresponding curves
for LiF: Mg,Ti in figure 16.1.
Compared with those curves, one also notes that here supralinearity starts around
10
3
R but extends up to higher doses. The hot-pressed chips are nearly linear up to
5 x 10
4
R and then demonstrate relatively little supralinearity up to 10
6
R. Linearity may
be significantly improved (up to 10
s
rad) by pre-exposure of the phosphor as was shown
in chapter 6 (6.3.1.3). All forms of Li
2
B
4
0
7
:Mn dosemeters can be applied for exposure
measurements up to 10
6
R.
Unfortunately, the reproducibility of Li
2
B
4
0
7
:Mn is rather poor in the dose range
from 10
s
to 10
6
R, which might exclude the use of the material in this dose range for
routine application. For the powder and hot-pressed chips, the standard deviation of the
TL readings at 10
3
R was determined to be about 5%, for the discs of 0.4 mm thickness
the standard deviation was 6.3% and for the 0.12 mm thick ones 12.7% was obtained
at the same dose.
The advantage of Li
2
B40
7
:Mn compared with LiF:Mg,Ti is its simple glow curve
with one main peak, the temperature position of which depends to some extent on the
exposure level. Another advantage is that the material does not exhibit complicated trap
dynamics and thus does not require complicated annealing procedures to obtain good
reproducibility. Zeroing of the phosphor only requires heating at 300 C for 15 min;
this may not be of interest to the user if the phosphor is used in powder form and thrown
away after use. This is to be recommended, as the material can be produced cheaply and
simply in large quantities in any laboratory.
From the point of view of tissue equivalence, Li2B
4
0
7
:Mn is an ideal phosphor, but it
also has some important drawbacks, namely that it is highly soluble in water and very
hygroscopic. This latter disadvantage can be improved by adding 0.25% Si0
2
to the basic
material. The phosphor may also show undesirably high fading from 0% within three
months at 25 C up to 37% per year at the same temperature, depending on its
production and composition.
308 M Oberhofer
16.4. Calcium fluoride
A high-Z TL phosphor with a much higher energy dependence compared with LiF:Mg,Ti
and Li
2
B
4
0
7
:Mn is CaF
2
:Mn, which also offers possibilities for high dose level measure-
ments with a reported linearity at response levels up to about 10
s
R, which is also about
the maximum measurable dose. According to measurements by Gorbics and coworkers
[5], this is not quite the case, as shown by the curves in figure 16.13, which were
obtained in the same way as the curves in figures 16.1 and 16.12. Apparently, supra-
linearity increases with decreasing phosphor thickness, as can be seen.
m u .
TEFLON y'^s
Figure 16.13. TL light sum response
per roentgen as a function of ' t o ex-
posure for CaF
2
:Mn-Teflon discs
(Teledyne Isotopes), 10 mg powder
(Harshaw) and 0.9 mm thick chips
(Haishaw), normalised to 1.00 at
10
3
R. (After Gorbics era/ [5].)
6 0
Coy -RAY EXPOSURE ( R)
Looking at the standard deviations of the TL light sum readings at 10
3
R without
correction for mass variations, CaF
2
:Mn is the next best to LiF:Mg,Ti with 2% for the
10 mg powder samples, 5.4% for the hot-pressed chips and 3.1% and/or 4.8% for the
Teflon discs of 0.4 mm and 0.13 mm thickness, respectively. Fading, which for many
applications is the limiting factor, is not negligible with CaF
2
:Mn, and was found to be
4% after 1 h, 8% after 10 h and 12% after 100 h. The same holds for calcium fluoride
activated with dysprosium (CaF
2
: Dy) (Harshaw TLD 200). Calcium fluoride activated with
thulium (CaF
2
:Tm) (Harshaw TLD 300) has a slightly better fading characteristic.
16.5. Other TLD phosphors
16.5.1. Metaphosphateglass
There are some more phosphors which are potentially suitable for high dose level
measurements, such as, for example, manganese-activated low-Z metaphosphate glass,
which is utilised as a photoluminescence reference light source in phosphate glass (radio-
photoluminescence, RPL) dosimetry. This material exhibits strong TL upon exposure and
is of interest because of the absence of any 'trap dynamics', that is the absence of shifting
of the trap distribution, which in other TLD phosphors such as LiF:Mg,Ti often
considerably impairs the precision of dose measurement.
Besides the possibility of obtaining higher precision with phosphate glasses, they are
easy to use, fast to re-use owing to the absence of complicated annealing programmes and
exhibit nearly no thermal fading.
High-level photon dosimetry with TLD materials 309
If, according to Regulla [13], manganese-doped (1.0%Mn) phosphate glass (identical
with the so-called radiation-resistant reference glass in RPL dosimetry) is exposed to
radiation and heated up to about 350 C, a TL glow curve is obtained, the light sum of
which is proportional to exposure from about lOmR to some kiloroentgens and then
slightly supralinear up to 10
6
R, where saturation is noted, as shown in figure 16.14. The
curve was obtained with 6x6x1. 5 mm
3
plane plates and a Harshaw Model 2000 TL
analyser. As can be seen from the figure, the upper limit of exposure detection is about
10
6
R, which may be extended to 10
7
R by measuring the decrease of photoluminescence
and to even higher exposures by using absorption measurements.
if)
10
8 h-
3 10'
g 10
6
<
o
z
Q
<
UJ
Q:
I
10-
10<
10
J
10'
_l_
D 1.07. Mn
O 0.37. Mn
A 0.17. Mn
_|_
10
J
10' 10
H
10
J
10
EXPOSURE ( R)
Figure 16.14. TL as a function of exposure for Mn-activated phosphate glass. (After Regulla
[13].)
The precision obtained with the material is particularly high, characterised by a
relative standard deviation better than 2% when individual detectors are re-used. There
is no observable thermal fading after proper post-irradiation annealing. The detectors
are mechanically and also chemically very stable, being neither toxic nor soluble in water.
The glass can also be made in the form of small rods and thus would be ideally suited for
a number of high dose level measuring problems, where small dosemeters are desirable.
16.5.2. Beryllium oxide
Beryllium oxide, BeO, is suitable for some high dose level measurements, because it is
rather energy-independent, has an effective atomic number Z of 7.5, which is comparable
with that of LiF:Mg,Ti and Li2B
4
0
7
:Mn, and in particular is known to be a material
of high chemical, mechanical and thermal inertness if used in its non-toxic ceramic form
(Thermalox 995 from Brush Beryllium Co., for example). As a TL phosphor, it may be
used up to exposures of 10
s
R and, with care, up to 10
6
R.
310 MOberhofer
Again BeO shows supralinearity, this time starting at 10-50 R, dose values which are
rather low and requiring calibration curves for high exposures. Reproducibility does not
seem to be too good. Crase and Gammage [21] report an intergroup standard deviation
from the mean response above a few milliroentgens in the range 8-11%. This may be
better at still higher exposures. Fading is accelerated by visible light, against which the
material has to be protected. Thermal fading is about 10% in three months at 30 C and
90% relative humidity. The material is not cheap, which does not favour its wide applica-
tion in routine high-level dosimetry.
16.5.3. Calcium sulphate
There are two calcium sulphate TL-grade types which are activated with different rare
earths, CaS0
4
:Dy and CaS0
4
:Tm. Those phosphors are of interest because, like
Li2B
4
0
7
:Mn, they may easily be produced in large quantities in any laboratory and, as a
consequence, are very economic TL materials.
According to Yamashita and coworkers [22], the dose response curve of CaS0
4
:Dy
is linear up to an exposure of 3xl 0
3
R, supralinear between 3 x l 0
3
and 10
4
R and
reaches the saturation level at around 10
s
R. This is also demonstrated in figure 16.15
(curve (A)), which is taken from reference [22]. With CaS0
4
:Tm (curve (B)), supra-
linearity already starts at 300 R, as can be seen from the same figure. There is only a little
fading for both materials (1-2% in one month, 24 h after exposure).
S K
s.
i n
(B) CaSOi, Tm^
( A) CaSOi Dy
,0-3 ,o-2 ,0-1
10 ' K)
2
EXPOSURE, R
K)
3
K)
4
K)
5
K)
6
Figure 16.15. CaS0
4
TL dosemeter response versus
Yamashita et al [22].)
l7
Cs gamma-ray exposure. (After
16.5.4. Aluminium oxide
Another TL emitter with a fairly linear response up to 10
5
rad [23] is A1
2
0
3
(ruby), which
is cheap and has a better energy dependence than CaF
2
:Mn and the phosphors CaS0
4
:Dy
and/or CaS0
4
:Tm. There is still a strong uv fading which necessitates keeping the
phosphor in the dark during application and evaluation.
16.6. Final remarks
Performing a review like the one presented here reveals that many of the TL phosphors
used today for low-level dose assessment in radiation dosimetry (mostly in personal
Table 16.1. Some data on TL phosphors which have potential for use in high-level dosimetry (doses given in rad)
TL material
LiF:Mg,Ti
LiF, powder, undoped
LiF, optical-
grade crystal
LiF, optical-grade powder
Li
2
B
4
0
7
:Mn
chips
CaF
2
:Mn
z
ef f
8.3
Isomet 1
Isomet 2
7.3
16.3
Type of
measurement
TL
TL
RPL
TL
TL
optical density
TL
optical density
RPL
TL
TL
For
60
Co radiation
linear range
10"
2
-10
3
-
10-10
6
2X10
2
- 5X10"
-
-
10"-5X10
7
10--2X10"
2X10
!
- 2X10
6
10' MO
3
10"
2
-5X10
4
10- - 10
3
( 10
5
)
Minimum
dose
10"
2
5X10"
10
2X10
2
2X10
5
10"
10'
10
4
10
6
2X10
S
10"
2
lO"
2
1 0 -
Maximum dose
10
s
(200 C peak)
10
7
(280 C peak)
10
6
10
5
(150Cpeak)
10
8
(335C peak)
10' (450 C peak)
2 X1 0 M0
9
2 X 10" (450 C peak)
10
7
-10'
2X10"
10
6
10
6
10
s
Fading at 25 C
5%/yr
0%/month
variable from 0%/3
up to 37%/yr
4%/l h
month
?

a
*-. "a
o
a.
o
Co
is-
to
S
*-*
3.
5.
Glass: Mn
BeO
CaSO:Dy
CaS0
4
: Tm
12.0
7.1
16.3
14.4
TL
TL
TL
TL
10~
2
-10~
3
10"
2
-10
1 0 - - 3 X1 0
3
10- - 3X10
2
10"
2
10"
2
i o -
i o -
10
6
10 MO
6
10
4
-10
5
10M0
5
8%/10h
12%/100h
0%/month
10%/3 months, 30C,
90% rel. hum.
1-2%/month
10.2
TL io-'-io
2
10" 10
5
312 MOberhofer
dosimetry) can to some extent also be utilised for high-level dosimetry depending on
quite a number of factors such as dose level, irradiation and storage temperature, atomic
number of reference material, ease of handling, sample-to-sample reproducibility and,
last but not least, phosphor price, if large numbers of dosemeters must be used. If price
be the governing factor, it seems that in many applications Li
2
B
4
0
7
:Mn is the best
phosphor, which, if home-produced, can be used as a throw-away material.
Table 16.1 concludes the review, summarising some relevant high-level dosimetry data
on the phosphors discussed here.
References
1 Fricke H and Hart E J 1966 Radiation Dosimetry vol. 2 Chemical Dosimetry (New York:
Academic Press) p 167
2 Holm N W and Berry J, eds 1970 Manual on Radiation Dosimetry (New York: Marcel Dekker)
3 Stolz W 1972 Strahlensterilisation, Grundlagen und Anwendungen in Medizin und Pharmazie
(Leipzig: J A Barth)
4 IAEA 1972 Dosimetry Techniques Applied to Agriculture, Industry, Biology and Medicine
(Vienna: IAEA)
5 Gorbics S C, Attix F H and Kerris K 1973 Thermoluminescent dosimeters for high dose application
Health Phys. 25 499-506
6 Sunta C M, Bapat V N and Kathuria S P 1971 Effect of deep traps on supralinearity, sensitisation
and optical TL in Lif TLD Proc. 3rd Int. Conf. on Luminescence Dosimetry, Danish AEC, Riso,
Roskilde. Riso Rep. 249, vol. 1. p 146
7 Eggermont G, Jacobs R, Janssens A, Segaert O and Thielens G 1971 Dose relationship, energy
response and rate dependence of LiF-100, LiF-7 and CaS0
4
:Mn from 8 keV to 30 MeV Proc.
3rd Int. Conf. on Luminescence Dosimetry, Danish AEC, Riso, Roskilde. Riso Rep. 249, part II,
p444
8 Shiragai A 1970 Effect of gTain size and initial trap density on supralinearity of LiF-TLD Health
Phys. 18 728
9 Zanelli G D 1972 Particle size and supralinearity in LiF Phys. Med. Biol. 17 99
10 Piesch E, Burgkhardt B and Kabadjova S 1975 Supralinearity and re-evaluation of different LiF
dosimeter types Nucl. Instrum. Meth. 126 563-572
11 La Riviere P D 1969 A unique throwaway LiF dosimeter Proc. 2nd Int. Symp. on Luminescence
Dosimetry, Gatlinburg, Tenn., September 1968. USAECRep. CONF 680920, p 78
12 De Werd L A and Stoebe T G 1971 The influence of hydroxide impurities on TL in LiF Proc.
3rd Int. Symp. on Luminescence Dosimetry, Danish AEC, Riso, Roskilde. Riso Rep. 249,
part I, p 78
13 Regulla D F 1972 Radiothermoluminescence of Mn-activated metaphosphate glass: its application
to low and high-level photon dosimetry Proc. on Dosimetry in Agriculture, Industry, Biology and
Medicine (Vienna: IAEA) paper SM/160/8, pp 215-227
14 Becker K 1974 Stability of film and thermoluminescence dosimeters in warm and humid climates
Atomkernenergie 23 267
15 Jones R J L and Martin J A 1968 Use of LiF (TLD-700) for doses greater than 0.1 Mrad Health
Phys. 14 521-522
16 Kitahara A, Saitoh M and Harasawa S 1976 Analysis of the TL-response of LiF-powder to thermal
neutron and gamma ray exposures Health Phys. 31 4-46
17 Goldstein N, Tochilin E and Miller W G 1968 Millirad and megarad dosimetry with LiF Health
Phys. 14 159-162
18 Vaugham W J and Miller L O 1970 Dosimetry using optical density changes in LiF Health Phys. 18
578
High-level photon dosimetry with TLD materials 313
19 Claffy E W, Gorbics S G and Attix F H 1971 Radiation induced optical absorption and photo-
luminescence of LiF powder for high level dosimetry Proc. 3rd Int. Conf. on Luminescence Dosi-
metry, Danish AEC, Riso, Roskilde. Riso Rep. 249, part II, p 756
20 Regulla D F 1972 Lithium fluoride dosimetry based on radiophotoluminescence Health Phys. 22
491-496
21 Crase K W and Gammage R B 1975 Improvements in the use of ceramic BeO for TLD Health
Phys. 29 739-746
22 YamashitaT, Nada N, Onishi H and Kitamura S 1971 CaS0
4
activated by Tm or Dy for TLD
Health Phys. 21 295-300
23 PhilbrickCR, BuckmanWG and Underwood N 1967 Ruby as TL irradiation dosimeter Health
Phys. 13 798
Applied Thermoluminescence Dosimetry. Eds M Oberhofer and A Scharmann
1981 ECSC. EEC. EAEC. Brussels and Luxembourg
17
Application ofTLD in reactor engineering
J R A LAKEY
17.1. Introduction
The reactor engineer must resort to in-pile measurements and shield radiation surveys to
check and monitor his design predictions and to monitor reactor plant performance. His
design codes usually give the flux of primary radiation, and it is possible to evaluate the
secondary radiation and to compute reliable values of kerma, absorbed dose and, where
appropriate, effective dose equivalent. Many assumptions must be made to reduce the
task to economically acceptable proportions, and benchmark experiments are used to
provide experimental data, so that a reliable dosemeter is essential.
The thermoluminescent dosemeter (TLD) has many advantages for the reactor
engineer, although it can rarely be used without calibration corrections using cavity
ionisation theory and subtraction of neutron'reactions. The TLD can be designed to yield
the desired response for gamma radiation and can be an effective 'gamma dose equivalent'
meter. The neutron response is more complex, and it is most useful for thermal-neutron
flux measurement provided that a self-absorption correction is applied. The reactor
engineer can take advantage of the passive response and linearity of the TLD, its possi-
bility of mass readout and its reasonable freedom from fading. The use of the same TLD
in occupational radiation surveys provides a link in the dosimetric study which eases
problems of interpretation.
The detector geometry is important in deriving its response function, although thin
TLD are exempt from some factors. In this chapter, reference is made to computer
codes used for evaluation of spectral and geometrical factors both for radiation sources
and detectors. Less sophisticated methods may be satisfactory, and the chapter
summarises in appendix 17.1 the useful point kernel/build-up factor equations which can
be applied to TLD.
Practical examples are described and include assessment of reactor coolant activity,
accumulated activity transfer and measurement of half-life.
Reactor shields have to be tested and the test data have an important influence on
future design, so that accuracy and precision requirements are important. Frequently,
the detector must occupy a hostile environment temperature cycling, time elapsed
from exposure to readout, location restricted due to shield layout, limited locations
inside shield, spectral and angular variation in air and the influence of mixed radiation
fields are considered. The use of spectrometry and computer code predictions and bench-
mark tests are essential features. Solution to these problems involves the application of
'cavity theory', which is described in appendix 17.2.
The use of TLD in hostile environments demands the use of a suitable protective
container, correction for fading, precautions due to activation (i.e. build-up of tritium)
and contamination.
316 JRALakey
The control of external radiation exposure of radiation workers requires reliable
knowledge of the radiation environment, and TL D can be used both to survey the en
vironment and to measure the exposure subsequently received. The advantage of TL D is
that the same detector can be installed in an anatomical phantom so that calibration
factors are common throughout the investigation. For example, this can be applied in
connection with the dosimetry of gamma photons from
16
N.
17.2. A survey of the applications of TL in reactor environments
Gay ton et al [1] review general applications of TL and stress the value of the device in
reactor environments because the dosemeter is passive and not subject to serious fading.
This is important when the experiments must fit within a commissioning programme.
Gammaray measurements within the pressure vessel of a shutdown reactor yield evidence
on which the radiation damage to closedcircuit TV equipment can be anticipated. It is
particularly useful for finestructure measurements at the shield surface but is of course
influenced by beta contamination. Gayton illustrated fuel structure measurements
(figure 17.1) and showed an application of TL D to spectrometry (figure 17.2).
17.2.1. The application of TLD to gamma dosimetry
The measurement of gamma dose in reactor shields is a valuable application of TL D and
the simple methods of calculation using buildup factor methods, summarised in appendix
17.1, are effective and reasonably accurate provided that the dosemeter has the same
radiation properties as the shield and that corrections are made to the buildup factors
to allow for multilayer shield effects. When measurements are made close to the core, in
particular for gamma heating, evaluation corrections must be made for the neutron
9 13 17 21 25 29 33 37 41 45
- - ' - - - 1261 3 2 / 3 6 / 4 0 / 4 4 / 4 B
IRON SHIELD
Figure 17.1. Section through end shield and cooling fins of a CEGB fuel flask with
associated surface exposure rate. (From Gayton et al [1].)
Application of TLD in reactor engineering 317
SJ E
E;
H'.r :r :r :c ~ j ~
V/////A
HZ&
7^7^r,^n
EZ
0 0
POLYTHENE : LOW DENSITY
BORON CARBIDE IN ARALDITE
ALUMINIUM TIE RODS
ALUMINIUM FRONT AND BACK PLATES
| N7N7N7N7N7N II
1 ^iruinnjui/uuuuinnnjuuinjijuirinmnjinnf
~ f ruuuiAfuuuuuuuui/uinnjwniuuuuuuuui
1
7N7N7N7N7N7
I . 1 l ?cm
I 30 cm
SCHEMATIC SECTION THROUGH DELTA SPECTR. SCHEMATIC SECTION THROUGH CENTRE CORE
Figure 17.2. Construction of the D elta spectrometer. (From Gayton et al [1].)
response, and the influence of the gamma/neutron response, the gamma spectrum and the
detector environment must be evaluated. Table 17.1 summarises the work in this field
and appendix 17.2 discusses the use of 'cavity' theory for this correction. In this chapter,
several attempts to measure gamma heating are described including a method of
evaluating gamma heating without knowledge of the gamma spectrum. The most
sophisticated methods apply Monte Carlo codes to correct the detector response to yield
a reliable measurement of energy deposition. Future developments using very thin
dosemeters promise to improve the methods since the correction factors can be reduced.
17.2.2. Measurement of gamma build-up factors
De Franceschi et al [15] took advantage of the TL of concrete itself to measure build-up
factors for concrete shields with a ^Co source. Concrete has low sensitivity, about 30 rad
being the minimum, and is linear to 2xl 0
4
rad. The authors did not apply a cavity
correction factor although the decision was intuitive. Results agreed well with
calculations using the empirical Taylor fit to dose build-up factors.
Burke and Becks [16] measured dose build-up factors from 0.662 MeV gamma rays on
multilayered aluminium and lead shields and compared the results with the DP-1 code and
with the build-up factor from the semi-empirical Kalos method. Excellent agreement was
obtained with the slightly modified Kalos formula.
The original formulation by Kalos is [17, 18]
B(X,Y) = B
b
(Y)+[B
b
(X+Y)-B
b
(X)]k(X)C(Y) (17.1)
where B(X, Y) represents the dose build-up factor in air for normally incident gamma
rays penetrating X mean free paths (MFP) of material 'a' followed by 7 MFP of material
V, B
b
(Y) is the single-slab build-up factor for Y MFP of material ' b' , and B
b
(X + Y) is
the single-slab build-up factor for (X + Y) MFP of material ' b' . Also
k(X) =
B
3
(X) - 1
B
b
(X) - 1
(17.2)
is recognised as the ratio of the scattered dose component transmitted through X MFP
of material 'a' relative to that transmitted through X MFP of material ' b' , and C is a
oo
Table 17.1. Previous use of TLD in reactor dosimetry.
<5
Author Source of radiation Dosemeter type Comparison of results Comments
Beyer [2]
Leonard and
Bransford [3]
Simons et al [4]
Reilly et al [5]
Gayton et al [ 1 ]
Tappendorf [6]
Water-moderated critical
assembly
TLD 600, 700
powder and PTFE rods
Water-moderated AFFRI- TLD 700 rods
TRIGA reactor
Reflector and core of fast TLD 100, 700 rods
reactor assembly in steel tubes
In-pile environments TLD 700 rods and PTFE
associated with lead shields discs
and adjacent voids
Various CEGB power
reactors
ATR critical facility
Simons and Yule [7] Zero-power fast reactor
TLD rods and powder
CaF
2
:Mn rods
1 X 1 X 6 mm
3
TLD 700, CaF
2
rods and
PTFE discs
23SJJ
"
7
Au (Cd covered)
activation foils
Paired tissue-equivalent and
graphite ionisation chambers
Two-dimensional discrete
ordinate transport code
ANISN computer code
Variation of
6
Li content in different batches
of TLD 700 allowed for
Gamma heating measurement. Errors of
10-20% due to neglect of fast and thermal
neutron response of TLD 700
The need to make cavity corrections before
comparing expt and calc. is emphasised -
no results given
Gamma heating measurements. Bragg-Gray
cavity correction factors successfully used
for PTFE discs. Mentions 65 M PTFE discs
but no results presented
Review article referencing gamma heat
measurement and thermal neutron flux
monitoring experiments
Gamma heating measurements. Uses CaF
7
in
preference to LiF because of its negligible
response to thermal neutrons. Simple cavity
correction applied
Gamma heating measurements. Mainly con-
cerned with influence on response of
dosemeter size and surrounding material
Muir and La Bauve [8] Core reflector and shield of TLD 700 chips in stainless
a fast reactor assembly steel
Knipe [9]
Gomaae/ a/ [12]
Boulette et al [13]
Lowe [14]
Zero-power fast reactor
assembly
Tanaka et al [10]
60
Co source
Maerker et al [11] Tower shielding facility
at ORNL
Vertical channel of 2 MW
research reactor, water-
moderated, reflected 10%
enriched uranium fuel
Fast reactor mock-up
assembly
Zero energy reactor
TLD 700 rods
TLD 700 rods
TLD 700
TLD 700 chips and PTFE
discs, LijB
4
0, tablets
TLD 700 rods in stainless-
steel capsules
TLD 700 in PES
Computer code
Computer code and
ionisation chamber
Point kernel calculation
Ionisation chamber and
computer code
Intercomparison of results
from glass, sand, LiF and
Li
2
B
4
0, dosemeters
Discrete ordinate transport
theory
"
5
U foil
Absolute dose measurements. Quite good
agreement with code. Differences attributed
to code approximations. Cavity correction
factors applied
Gamma heating measurements. Assumed TL
response of TLD 700 to thermal neutrons is
negligible. Cavity correction factors applied.
Agrees within 10% with ion chamber
measurements
Gamma ray heating. General approximation
derived for TLD is calibrated in iron.
Suggests that neutron contribution to
TLD 700 response is negligible
Radiation heating in stainless steel and
sodium systems. Results compare well with
ion chamber. Deviations from calculated
results are due to neutron effects
Recommends TLD 700, sand and glass for
gamma heating measurements, and Li
2
B
4
0,
for thermal neutron measurements.
However, agreement only to within a factor
of 2
Absolute dose measurement. Agreement to
within 30%. Discrepancies attributed to
calculational errors
Agreement within 5.0% of calculated
gamma flux in the reflector region
5
El
<-+
o
a'
I'
320 JRALakey
correction factor from the fit to the Monte Carlo calculations. Kalos postulated that
C(Y) = 1 for lead followed by water
(17 3)
C( r ) = exp(-1. 7F) + ( a/ f c) [ l - exp( - r ) ] for water followed by lead
where
a
~ (P Compton/MtotaOa ^ (^Compton/A'totaOb
i.e. the ratio of Compton attenuation coefficients to the total attenuation coefficients in
the respective media. Shimizu discusses the rationale for this form of equation, in
particular the fact that k{X) C(Y)-+a for large values of Y.
The authors compared the resulting inferred build-up factors with calculated and
experimental data for aluminium-lead slabs and with limited comparisons made for other
slab combinations and source energies, and decided to modify only the C{Y) term in the
Kalos formula. Let
C(y) = e x p ( -
7
r ) +/ 3 [ l - e x p ( - y ) ] (17.4)
where /3 = 1.5 for any high-atomic-number (Z) material followed by any low-atomic-
number material, @ = a/k(X) for any low-Z material followed by any high-Z material,
where a is the same as above, and
McomptonOower-Z material)
7 = .
Mcom
P
ton(higher-Z material)
Furthermore, when applying the formula to a multilayered slab of n layers, they
treat the first (n 1) layers as a single slab of the (n l)th material for the purpose of
calculating a and 7. The build-up factor for this (n l)th slab, however, is computed by
applying the formula to a double-layered slab of (n - 2) layers followed by the (n - l)th
layer. For example, the build-up factor for a slab consisting of X MFP of lead, followed
by Y MFP of aluminium, followed by Z MFP of lead is calculated first by applying the
above formula to X MFP of lead followed by Y MFP of aluminium. Using this build-up
factor and a for aluminium followed by lead the build-up factor for the triple-layered
slab is computed.
17.2.3. High-energy gamma rays
Bishop et al [19] utilise reactor coolant water on the LIDO reactor to create a uniform
disc source mainly of
16
N and shielded spectra calculated using the MCNID Monte Carlo
code. A similar rig is installed at the URR Risley giving 6-7 R h"
1
at the source surface.
The energy of photons is 6.13 MeV and a convenient calibration source can be achieved
using
19
F(p, a7)
16
0 with a proton energy of 340 keV.
Nitrogen-16 has a half-life of 7.4 s and emits gamma rays of 7.1 MeV and 6.1 MeV
in 6% and 76% of its disintegrations. Dose rate measurements in a simple geometry have
been used to evaluate the intensity of this source in the coolant of water-moderated
reactors. Avery et al [20] made calculations of steam pipe dose rates using the MORSE
code. The presence of
1S
C activity (ratio 12.0 2,
16
N to
15
C) and uncertainties in the
delay time from leaving the core (~4 s) and the partition coefficient of
16
N between
Application of TLD in reactor engineering 321
steam and combined steam and water (~0.69) had to be considered to gain a value for
16
N flux which produces 0.9 2% of the dose rate (between 100 and 500 mR h"
1
at full
power at distances up to 100 cm from 14.45 cm radius steam pipe).
D Faddy and G Thompson (private communication) have used TLD LiF powder
calibrated at 0.66 MeV gamma-ray energy to evaluate coolant activity of a pressurised
water reactor (PWR) by measurements on coolant pipes. Locations were selected in
contact with lagging at the centre of long pipes and in locations well shielded from
sources other than the adjacent pipe. Gamma exposure rates were calculated with a point
kernel build-up factor code.
17.2.4. Fast reactor core measurements
Simons et al [4] used TLD for dose mappings, single-cell heterogeneity, blanket-reflector
and reflector-core interface studies in the EBR-11 series of ZPR-3 critical assemblies.
TLD rods loaded in 0.125 inch diameter and 0.035 inch wall thickness 304 stainless-steel
tubes were irradiated for approximately 100 W h. Analysis utilised the two-dimensional
discrete ordinate transport code DOT in R-Z geometry, and the gamma calculations were
S ^ approximations. Some problems were experienced in correlating the gamma-ray
energy deposition with TLD responses.
Simons and Yule [7] reviewed earlier gamma heating measurements in which cavity
theory has been applied to TLD. With large cavities, the electron spectrum is important,
and these authors averaged over the three components of the primary electron spectrum
produced by the more energetic gamma ray. Tabulated values of mass stopping power
were used but, although the method works, it has not been tested over a range of gamma
energies.
Figure 17.3 illustrates how the correction for the energy absorbed per unit mass of the
dosemeter material varies with the energy absorbed per unit mass of the wall when the
three levels of cavity are considered the escape of scattered radiation is not taken into
account. The dosemeters were applied to heating measurements in a range of gamma-ray
spectra typical of the fast reactor.
17.2.5. Reactor gamma heating measurements
Haack and Majborn [21] compared the use of TLD against calorimeters in an experimental
tube of the Danish Research Reactor DR3. Bismuth shielding was used to vary the ratio of
thermal neutrons to gamma rays (around 10
12
neutrons/cm
2
s and 10
6
rad gamma/h).
Li
2
B
4
0
7
:Mn was used because it had high sensitivity to thermal neutrons compared with
LiF TLD 700 which i s
7
Li-enriched and therefore relatively insensitive to thermal neutrons
-responses were reported at 320R and 1.4R respectively for the ^Co equivalence to
10
10
neutrons/cm
2
. Dosemeters were mounted in 6 mm diameter holes in aluminium rods
and the dose due to
28
A1 decay was corrected, but this was only possible for LiF TLD 700
and corresponded to about 5% of the measured 7-ray dose. Fast-neutron flux was about
4 x 10
10
neutrons/cm
2
s, and its contribution was negligible in this experiment. Figure
17.4 gives the relationship between calorimeter and TL measurements and shows excellent
agreement, and it was concluded that TLD have the advantage of small probe size,
322
J R A Lakey
50
0.5 1.0 5
GAMMA-RAY ENERGY ( MeV )
Figure 17.3. Variation of \/f(Ty) as a function of energy for a 3 X 3 X 0.8 mm'' (g =
0.243 g cm
- 2
)
7
LiF dosemeter surrounded by iron, based on large-cavity, general-cavity and
small-cavity ionisation theories.
TJ
a
3 -
UJ
O
a
o
a- o
i -
x CALORIMETER MEASUREMENTS
o THERMOLUMINESCENCE
MEASUREMENTS
WITHOUT Bi
.WITH Bi
0 20 40 60 80 100
HEIGHT ABOVE CORE CENTRAL PLANE ( cm)
Figure 17.4. 7-ray dose rate versus height above core central plane as measured with the
calorimeter and with thermoluminescence dosemeters (referring to a reactor power of
0.97 MW).
measurements can be made simultaneously in many positions and thermal flux can be
deduced.
Experiments were performed by Reilly et al [5] to simulate in-pile environments
associated with lead shields and adjacent voids. No correction was made for self-shielding
Application of TLD in reactor engineering 323
or the cavity effect but a simple application of the mass stopping power ratio in water
regions close to lead gave the correct response as predicted by ANISN (Engle [22]).
Gomaa et al [12] used TLD and other devices to measure gamma heating of the EY-R R -1
reactor. The TL materials were
7
LiF-Teflon 0.5 mm x 8 mm diameter and 0.4 mm x
10 mm diameter and a
7
LiF crystal 3 x 3 x 1 mm
3
. These were calibrated with ^Co
gamma rays. Radiation effects were observable at 10
s
rad in
7
LiF-Teflon which became
coloured but these were usable up to 10
s
rad.
17.2.6. Fast test reactor mock-up shield tests
Radiation heating studies in a stainless-steel and sodium shield were reported by Boulette
et al [13]. Lithium fluoride rods were enclosed in stainless steel and irradiated for
lOOOWh. Uncertainties in the TLD dose interpretation include sample non-uniformity,
calibration, spectrum variations and fast-neutron effects. Experimental biases were
estimated to be +30% out of core and 10% in the core.
Analysis was performed using discrete ordinates transport theory (S
8
P
3
) for gamma
flux and three-dimensional diffusion theory for the source calculations (3 DB code). The
illustrated distribution, which does not include the biases (figure 17.5), extends along the
centreline of the EMC, traversing the axial shields and reflectors as well as the core region.
This distribution records the heating in steel. Estimated one standard deviation limits are
shown but the experimental bias would increase the discrepancy between theory and
experiment.
Muir and La Bauve [8] reported gamma measurements in this facility compared with
calculated data using a flux-dose conversion factor without correction for cavity ionisa-
tion theory. Correction for cavity theory used the method of Simons and Yule [7] and
fast-neutron effects were calculated using the work of Wingate et al [23].
Benchmark measurements were established by Maerker et al [11] in a stainless-steel
and sodium system using TLD and ion chambers. Calculations applied cross-section data
from ENDF/B-IV in the two-dimensional discrete ordinates code DOT starting with an
absolute disc source produced at the Tower Shielding Facility at ORNL. The gamma-ray
spectral effect of replacing TLD material with iron and the neutron response of the TLD
were estimated. All dosemeters were in excellent agreement but showed increasing
underprediction of the gamma-ray heating with penetration.
50 100 150
DISTANCE ( c m)
Figure 17.5. Analytical/experimental com-
parison of gamma heating in stainless steel
in FTR /EM C along axial centreline.
324 JRALakey
17.2.7. Gamma heating measurements in an unknown spectrum
Tanaka et al [10] derived a method for estimating gamma heating from TLD measure-
ments in the absence of knowledge of the gamma spectrum. The absorbed dose D
M
(E
y
)
at a point in a material 'M' for gamma rays of energy E
y
is given as
D
M
(E
y
) = CE
y
^(E
y
) mMenC^M (17.5)
where E
y
is the gamma-ray energy (MeV), C is the conversion constant from mega-
electronvolts to ergs (erg/MeV), *p(E
y
) is the gamma-ray fluence of the energy E
y
(cm
-2
),
and
m
l^en(^y)M is the mass energy absorption coefficient of the material 'M' (cm
2
g
-1
).
Assuming the gamma-ray spectrum is not influenced by the existence of a TLD, the
absorbed dose B
TLD
(E
y
)
M
m
TLD at the same position in the material 'M' is represented
as follows
^TLDC^TOM
=
^ TLD( V) K^TOTLD-M
= CE
y
^(E
y
)
mt
i
en
(E
y
)
TLD
(
7
)TLD-M (17.6)
where K
TLD
(E
y
) is the kerma of TLD for gamma rays of energy E
y
(erg g"
1
), K ^ T L D M
is the absorbed dose correction factor to obtain the absorbed dose of TLD placed in the
material 'M' from the kerma, and mMen^^LD is the mass energy absorption coefficient
of TLD (cm
2
g
_1
).
The observed value by TLD is the thermoluminescence induced by energy absorption
of gamma rays. Therefore, the relation between the thermoluminescence and the
absorbed dose of the TLD must be defined. Furuta and Tanaka [24] have obtained a
general relation of the thermoluminescence and the adsorbed dose for any TLD and
radiations, and showed that the integral thermoluminescence of TLD is given using a
conversion efficiency by
^TLDt ^M
=
V(Ey)TLD ^ T L D ^ J M (17.7)
where Gj
h
o(E
y
)
M
is the integral thermoluminescence of TLD exposed in material 'M'
(light unit), and v(E
y
)
TLD
is the mean (conversion) efficiency to obtain the integral
thermoluminescence from the absorbed dose (light unit/erg g
_1
).
From equations (17.5)-(17.7) the relationship of the absorbed dose of material 'M'
and the integral thermoluminescence of TLD which is exposed by gamma rays at the
relevant point in material 'M' becomes
r, (
F
\ -
l
1 m/ * en( g
T
)M , .
u
U\p-i)-T7^r\ rTTTT 77TT ^ TLD( ^
7
) M
?V

7-lTLD-M VifiyJTLD mMenl/^/TLD


= /
7
('
7
)
TLD
.
M
Gj
LD
(E
y
)
M
. (17.8)
Consequently, the conversion factor /
7
("
7
)TLD-M
mu s
t be defined for estimating the
absorbed dose of gamma rays in the material by TLD.
17.2.7.1. Absorbed dose correction factor. The absorbed dose correction factor is
dependent upon the size and the kind of TLD, the surrounding material and gamma-ray
energy. This factor [7, 25] is close to unity in the energy region below 2 MeV in any
combinations of TLD and material. In contrast, this factor has values differing from unity
Application of TLD in reactor engineering 325
in the energy region higher than 2 MeV. It has been suggested that the conversion factor
becomes nearly constant in the region higher than
60
Co gamma-ray energy.
17.2.7.2. Mean (conversion) efficiency. It has been considered that the mean efficiency
for gamma rays is independent in the gamma-ray energy range from 0.1 keV to 10 MeV,
where the integral thermoluminescence is proportional to the amount of irradiation.
Thus, the mean efficiency can be given by a constant, say I?TLD- If the absorbed dose of
T LD is known for a gamma-ray field, the mean efficiency can be calculated from equation
(17.7). It is difficult, however, to know accurately the absorbed dose of T LD , since it is
not always easy to evaluate the electronic equilibrium or to know the absorbed dose
correction factor. Fortunately, the absorbed dose correction factor is close to unity for
60
Co gamma rays. Then, when the T LD is calibrated by a known field of
60
Co gamma rays
in air, the mean efficiency may be represented as
J?TLD = rK^CohLD = I / ^ T L D C
6 0
^ ) * . (17.9)
In practice, when the T LD is exposed by
60
Co gamma rays of 1 R and the roentgen (R)
^Co equivalence unit is used as a light unit of the integral thermoluminescence, the value
of the mean efficiency may be defined as
7?TLD = - ^
m / i e
" L
C

) a i r
(R "Co equivalence/erg g"
1
). (17.10)
86.9
m
/ien(
6
Co)
T LD
From these considerations, the conversion factor is approximated using the mean
efficiency and the mass energy absorption coefficient, as follows:
/
7
(
7
) T LD - M =
mMe
"f f
M
(17.11)
7?TLD m^en( ^7) T LD
17.2.7.3. The interpolation method. The most important factor in the conversion factor
is the ratio of the mass energy absorption coefficients of the material and T LD . AS an
example, figure 17.6 shows the ratio of the mass energy absorption coefficient of iron
to those of various TLD normalised at
60
Co gamma-ray energy, and the effective atomic
number of these TLD is shown. Though the deviation of the ratio from unity is fairly
large in the region below 1 MeV, it is noticed that the deviation decreases when the
atomic number of T LD is close to that of iron, which varies smoothly with the effective
atomic number of the T LD . Thus, the ratio becomes smaller than unity for the TLD with an
effective atomic number larger than that of iron, but it becomes larger than unity for the
T LD with an effective atomic number smaller than that of iron. The same characteristics
of the mass energy absorption coefficient may be considered to be held between any
TLD and materials. This is a fundamental and important fact to be used for this method.
By exposing several kinds of T LD whose atomic number is different from that of the
material considered and using the value of the conversion factor for ^Co gamma rays to
estimate the absorbed dose of the material, it is found that
/
7
r C o
W M
^ ^f
c
C

)M
(17, 2)
VTL.D mMenl ^hhD
The results will be underestimated for a T LD having a smaller atomic number than that of
the material, or overestimated for the opposite case.
326 JRALakey
Q _
_l >
~
2
UJ i n
CM
C i-
1
*-t;
E <
^ S
^ N
UJ - I
v - <
c 2
a- o
E z
I U U
10
1.0
0.1
: Fe/
7
UF (Mg)
="'N Fe/Na
2
SCUDy)
~ \ Fe/CaSCMTm)
^
%
\ Fe/SrS04(Dy)
"- N \ Fe/BaSCM Dy)
:
n
" \ \
\ \
\
?^^^^ ^^^ *
-\ " ^ '
A /'
: v.^ ^/
i > i<"i i ' i i
2
8.2
11.6
15.2
29.2
45.5
^ ^
11 I I
0.03
10
0.1 1.0
PHOTON ENERGY ( MeV)
Figure 17.6. T he ratio of the mass energy absorption coefficient of iron to those of various
T LD normalised at "Co gamma-ray energy (1.25 MeV).
If the conversion factor defined by equation (17.12) is used over the whole energy
range, the absorbed dose estimated by various TLD increases with the effective atomic
number of the T LD . Thus, the absorbed dose in the material can be estimated by
interpolating the values expressed as a function of the atomic number, which are
measured by using several kinds of T LD .
This useful method is limited in accuracy by the unknown shape of the relationship
between response and Z and by the need to place the two detectors precisely in the same
position.
The experiments in the Zebra Reactor carried out by Knipe [9] used a zirconium-
walled solid-state cavity dosemeter (SSCD ) incorporating
7
LiF thermoluminescent
dosemeters (T LD ). The TLD used
7
LiF (0.007%
6
Li and 99.993%
7
Li) manufactured by
Harshaw in rods 1 x 1 x 6 mm
J
. Post-irradiation annealing used was for 1 h at 400 C,
16 h at 80 C and readout by Conrad Model 7100. ^Co was used for calibration using an
equilibrium wall of T LD during exposure and supralinearity appeared at 200 rad to the
LiF. Irradiations were held within this limit at a core temperature of 50 C and readout
took place seven days after irradiation to allow for fading.
Neutron effects were corrected using the method of Wingate et al [23] and were less
than 0.1% in the core due to
6
Li(n, CL)T reactions. The major contribution was due to
7
Li
and F recoils.
The T LD 'cavity' was corrected for energy deposition relative to the 'wall' using the
Monte Carlo tracking program PROCEED [26] and the measurements were compared to
Monte Carlo calculations using the MCNID program [27] in one-dimensional plane
Application of TLD in reactor engineering
327
geometry. The dose at points in the core was dominated by the gamma rays which
originated in the immediate vicinity and so splitting for variance reduction was limited
to regions close to the source and standard deviations of 4% were obtained. Doserate
conversion factors [28] for zirconium were obtained by interpolation and were used to
obtain energy deposition rates. Corrections were applied for neutron interactions (15%)
and the cavity correction for the zirconium wall was approximately 13%; figure 17.7
1500r
1000 f .

w 500h
2
z
o
u
cc
UI
i -
<
cc
o
a
a
UJ
m
cc
o
in
m
<
100
50
10
:
t .
+ +! r,
i
-
-
'.
.
-
j QJ
^ on
r^
U
, I . I . 1

ft.
K
UJ UJ
1- cc
Z 5 0
O U
i
MONTE CARLO CALCULATION
( STANDARD DEVIATION U'U)
+ TLD MEASUREMENTS

*
#
.+
+
cc
L
E
T
E
D

B
R
E
E
D
E


Q_ f ^
UJ O
Q 3
1 , 1 .
*

(_)
_) UJ
UJ 1
UJ u.
1- ui
I/) cc
1
P
H
I
T
E
/

+

L
E
C
T
O
R

< l i -
CC UI
o cc
. 1
UI
1-
9;
< <
^ ^
o in
, i .
0 200 400 600 800 1000 1200 K00 1600 1800
DISTANCE FROM CORE CENTRE ( mm)
Figure 17.7. Comparison of Monte Carlo calculations of absorbed dose rate and TL D
measurements in Zebra Assembly 12.
gives the comparison with the calculations. The TL D measurements were clearly
responding to the fine structure in the core and were systematically lower by an average
10%. The TL D measurements were also lower in the steelaluminium reflector but were in
good agreement within the axial breeder. These discrepancies were thought to be due to
shortcomings in the calculations, probably source data, rather than to errors of experi
mental technique.
17.3. Application to neutron dosimetry
The use of TL D for thermalneutron dosimetry gives the possibility of an absolute
response due to the use of known capture cross sections and reactions. Surprisingly the
literature, summarised in table 17.2, shows considerable variation and it is now evident
that selfabsorption corrections are of great importance (the method developed by
Horowitz et al [53] is indicated in appendix 17.3). However, the response also depends
on the readout cycle used, the isotopic composition of the TL material and the neutron
Table 17.2. Summary of TL response of LiF to thermal-neutron experiments.
oo
LiF responsej
Author TLD 100 TLD 600 TLD 700 Dosemeter type Readout cycle Comments
Cameron et al [29]
Wingateef al [30]
Simpson [31]
Distenfeld et al [32]
370
200
220
200 Woodley and
Johnson [33]
Ayyangarera/ [34, 35] 95
Wallace and Ziemer [ 3 6 ] 310
Reddyeffl / [37] 535
Tochilin et al [38, 39] 160-250
0.7
880
550 0.9
2190
1200-1700
Scarpa [40] 65
0.87-0.96
1.1-1.6
1.0
Powder in polythene
cylinders 0.108 cm X
0.5 cm
Powder
Powder in stainless-
steel capsules
Powder in polythene
capsules
Powder in gelatin
capsules
Powder
Powder in gelatin
capsules
400 C integrated Gives cadmium ratio showing variation of
counts response with neutron temperature.
Recommends small dosemeter to minimise
self-shielding. Elementary self-shielding
factor calculation
- Contains consideration of the variation in
response of TLD 700 to thermal neutrons.
Fission foil and tissue-equivalent chamber
calibration
Peak height response Plutonium-beryllium used as neutron source
Thermal column of graphite research
reactor used
400 C integrated
readout
Achieved proportionality between thermal
neutron flux and TL response for TLD 600
up to 10
12
n/cm
J
. Emphasises need to allow
for response of TLD 700 to thermal neutrons
Integrated TL response Primarily a LijB
4
0
7
study
Integrated TL Emphasises need for small dosemeter to
response up to 380 C minimise self-shielding
- Pu-Be source + graphite moderator, cali-
brated with Au foil. Gamma dose
determined by shielding TLD 100 from
thermal neutrons
- Values quoted in a study of BeO TLD
Jahnert [41, 42]
Dua e t al [43]
Majborn [44]
Haack and
Majborn [45]
Ayyangar et al [46]
McKlveen and
Schwenk [47]
Tanaka and
Furuta [48]
Rossitei el al [49]
Horowitz et al [50]
Schumacher and
Krauss [51]
Bartlett and
Edwards [52]
490
360
2650
330
0.35
2.5
1.3
1.4
TLD 700 powder
TLD rodsj
TLD chips
TLD chips
Integrated response
up to 350C
300 C
1520
1350
893
-
2400
2180
-
1.1
-
-
1.62
0.19
1.26
0.23
Powder in nylon
capsules
Chips
Powder in PTFE
capsules and chips
Powder in PTFE
capsules and chips
Chips
PTFE-LiFi discs
6 mm diameter,
4 mm thick
Chips
140C preheat
followed by 270C
readout
Integrated response

-
-
Integrated count
a particle response survey, a particle
response to energy 2 MeV. Response to
10
, o
n/ cm
2
Linearity to 10
, 2
n/ cm
2
for TLD 600.
Variation of
6
Li in different batches of
TLD 700 noticed
Thin TLD are used to show effect of self-
shielding though response of chips only is
given
Feasibility study of Danish Research Reactor.
Study compares favourably with calori-
metry measurements
Found thermal neutron response to
decrease with sample thickness because of
self-shielding
Linearity of TL response up to 10'
2
n/ cm
2
with those from BF
3
detector
Parallel field, self-shielding correction
applied
Measurements made to calibrate medical
therapy dosimetry system
Response to thermal neutrons calculated
from TL response 2.5 MeV a particles
ix
=
Q
a
3.
t 10
1 0
n/ cm
2
= 1 R '"Co gamma radiation.
TLD chips - sintered blocks of LiF, 0.3 X 0.3 X 0.089 mm
3
t TLD rods - sintered blocks of LiF, 1 X1 X6 mm
3
.
" PTFE discs - discs containing 30% LiF, diameter 4 mm, thickness 0.4 mm.
to
330 JRALakey
temperature in which the device is exposed. Some attempts have been made to use
activation of the phosphor to yield a measurement free of gamma effects.
The application to fast-neutron dosimetry is more difficult and does not readily permit
correction for the gamma field. However, various spectrometer systems have been
attempted using TLD in neutron moderators. The use of TL for neutron spectrometry
has been attempted using the Delta spectrometer (figure 17.2) in which TLD are installed
in a 31 cm long x 9 cm radius polythene cylinder. A removable polythene core 10 cm in
diameter is separated by 1.5 cm boron-loaded Araldite and the TLD capsules containing
natural LiF and
7
LiF are placed at 1 cm intervals along the face. The threshold sensitivity
is 10
6
n/cm
2
and the theoretical resolution is 10%. An equivalent gamma spectrometer
contains lead- and aluminium-shielded TLD in nine separate units from which nine energy
groups can be resolved.
A simpler device using a polythene cylinder containing pairs of TLD 600 and TLD 700
along the axis supplemented by a 10 inch polythene sphere containing one pair of
detectors is reported by Singh [54]. The author concludes that this is a useful device for
monitoring in shielded areas and can yield an indication of neutron energy by comparison
of the reading at 10 cm depth and at the maximum provided that the gamma radiation
field is negligible.
17.3.1. TLD 700 response to reactor neutrons
Leonard and Bransford [55] reported measurements in six fields in the exposure room of
the AFRRI-TRIGA reactor:
(1) in free air from the bare TRIGA core,
(2) behind 2, 4 and 6 inches of lead, and
(3) through 3.54 and 7.08 inches of water.
The authors reported errors as large as 10-20% using TLD 700 to determine the gamma
dose in tissue-equivalent material at a depth of 18 cm if the response of the dosemeter
to fast and thermal neutrons was ignored. This response was determined by calibration
against tissue-equivalent and graphite ionisation chambers. However, the 'quench effect'
reported by Oltman [56] due to fast neutrons was avoided by pre-irradiation of the
TLD 700 using "'Co to gain a 50-100 rad dose.
Reactor flux measurement using TLD in a research reactor (McKlveen and Schwenk
[47]) gave erratic results at thermal-neutron fluxes less than 10
4
n/cm
2
s but these
problems were mainly due to fission-product-decay gamma rays from a previous high-
power operation, and at fluxes above lO^n/cm
2
s supralinearity was apparent and reports
were made of extra sensitivity. At fluxes exceeding 10
12
to 10
13
TLD ribbons were badly
discoloured and at 10
12
significant activation products were present. The fluence used was
around 10
13
n/cm
2
for low flux measurements, although the authors do not clearly
specify irradiation times.
Mayhugh et al [57] use CaS0
4
:Dy, CaF
2
:Dy and natural CaF
2
for thermal-neutron
dosimetry. After neutron irradiation, the phosphor is stored and the decay of
165
Dy
(2.3 h) gives the lowest detectable limit of 5 x 10
7
n/cm
2
;
4s
Ca (165 d) with a limit of
6xl 0
10
n/ cm
2
could also be used. The procedure involves annealing immediately after
irradiation to remove the TL induced during irradiation.
Application of TLD in reactor engineering
331
Similar results were reported by Wang et al [58], but the authors' lower detection limit
for dysprosium activation was 2 x 10
8
n/cm
2
.
17.3.2. Response of
6
LiF and
n
LiF TLD to fast neutrons
Furuta and Tanaka [59] examined the response using monoenergetic fast neutrons from
a 2 MV Van de Graaff accelerator. The devices were calibrated experimentally and
changes in glow curve were recorded and expressed by Gaussian analysis. The authors
conclude that neutron kerma efficiencies were
T?(X)
6
LiF(n) = 4. 17xl O
- 3
i7(X)
7
LiF(n) = 4. 34xl 0"
3
compared to y efficiencies
i?(X)
6
LiF(
6O
Co) = 0.0112
T?(X)
7
LiF(
60
Co) = 0.0117
R ^Co equivalences/erg g *
R ^Co equivalences/erg g
_1
R/erg g"
1
R/erg g
_1
.
The energy response of integral thermoluminescence is given for
6
l i F in figure 17.8 and
for
7
l i F in figure 17.9.
o
a.
3
ij
icr
8
O LU
S n! io-"
-. 10-6 pi
-CALCULATION (WITHOUT RECOILED FLUORINE)
(WITH RECOILED FLUORINE)
EXPERIMENT
ul_
' !
C
- 10" o
a.
10
0.01
5 ^
or
U T-
8 - oi
<
5 O
^ > _
100 0.1 1.0 10
NEUTRON ENERGY ( MeV )
Figure 17.8. Energy response of integral thermoluminescence of
6
LiF TLD to neutrons.
17.4. Environmental monitoring
The use of TLD measurements to evaluate population exposure due to the noble-gas
fission product releases from Three Mile Island emphasised the advantage of a passive
system for emergency use. Although the natural radiation background varies, it can be
adequately predicted and with suitable sensitivity exposures as low as about 0.1 mR
can be estimated.
332 JRALakey
o
z
z E
10"
10'
10
<_>
_ l
o ^
s it io-'
2
Mxl / 10)
_i i
0.01
CALCULATION (WITHOUT REC. FLUORINE J
CALCULAT. (WITH RECOILED FLUORINE)
EXPERIMENT (THIS WORK )
(C.L. WINGATE ET AL )
D .. ( N. GOLDSTEIN ET AL )'
Z
10'
10
10"
-8 z o
a.
3
Z
or "~
UJ Y
<
100 0.1 1.0 10
NEUTRON ENERGY ( MeV)
Figure 17.9. Energy response of integral thermoluminescence of
7
IiF TLD to neutrons.
Burke and Marcus [60] reported the problem of interpreting environmental radiation
levels in terms of the gaseous release from a boiling water reactor (BWR) power station.
Fluctuations caused by cosmic radiation and terrestial radiation have to be identified
the latter appears to be most important and is dependent on soil moisture changes and
surplus ground water which dilute and shield the sources. This variation has been
modelled and compared with monthly TL D measurements. After correction for reactor
source and meteorological variations (assumed constant across the site), an improved
correlation was obtained.
Brinck et al [61] describe the Environmental Protection Agency field study to assess
TL D and other dosemeters for the detection of external radiation exposure due to dis
charged radioactive gases from a BWR. The TL D system used a hotpressed CaF
2
:Mn
cylinder bonded to a heater element and installed with an aluminiumleadtin shield to
eliminate overresponse to gamma radiation below 100 keV. Calibration used a radium
source and fading was found to occur mainly in the first 5 h after exposure with no
measurable fade after 24 h. Thus monthly readings are not affected by fade if all readings
are delayed until 5 h after the end of the exposure period.
Internal background due to dosemeter activity was around 1.980.09/jRh
1
. This
yields a minimum detectable exposure over 1 month of 3 x 720 x 0.09 /JR or 0.19 mR
provided that natural environmental background variation can be eliminated. Surveys of
natural radiation background have been made by Powers et al [62] and showed back
ground variation by 30% over 4 week periods. The lower level of annual dose due to
normal reactor operation which could be measured with these dosemeters was 5 mR.
TL D were used by Weng et al [63] to record fallout during the period 19711975
produced by nuclear tests at Lop Nor, China. The detectors were CaS0
4
:Dy and
CaS0
4
:Tm manufactured by the authors and three samples were installed in each
measuring location at 1 m above ground. These detectors appeared to be affected by
exposure rate and read low for rates of 0.1 to 2 mR min
1
.
Application of TLD in reactor engineering 333
17.5. Miscellaneous applications
The use of TLD for activity assessment is an excellent supplement to more complicated
procedures and TLD can frequently be used in hostile situations where other radiation
monitors would be useless.
Activated corrosion products (crud) are a major source of occupational radiation
exposure during maintenance operations of water-moderated power reactors [64, 65] and
typically contribute up to 88% of the total dose rate. Reliable spectral analysis is useful
to evaluate the activity distribution [66] although the spectrometer can be calibrated on
sections of the reactor coolant pipework, TLD measurements can be used to obtain the
absolute level of dose rate.
17.5.1. Accumulated activity transfer
TLD can be used to evaluate integrated activity transfer or mean flow rate by analogy
with methods developed using other radiation detectors as shown by Lakey [66]. When
activity is transferred along a pipe or conveyor belt, the dose (in rad) received by a
collimated detector viewing a section of the pipe is
cna
D =
v
where C is the total activity transferred (Ci), n is the dose rate per unit activity (rad s
- 1
Ci
_1
), a is the aperture width (cm), and v is the source velocity (cms
- 1
), n can be
obtained by calibration with a point source of the appropriate nuclide. A known quantity
of activity held in the flow as a tracer can be used to assess the mean flow rate.
17.5.2. Measurement of half-life of
131
I in thyroid
Malone and Cullen [67] applied four I JF- PTFE disc dosemeters, set in a dressing, to the
surface of the patient's neck. Dosemeters were removed and returned to the hospital for
readout, thus reducing the number of visits required to be made to the hospital. A simple
neck phantom constructed from lucite (water-filled) was used for measurements with
131
I. It was necessary to use a more effective tissue-equivalent fluid for
12S
I measurements
and the composition of this fluid is given in the paper.
Appendix 17.1. Calculation of gamma photon absorbed dose
The most important quantity characterising the penetration and diffusion of gamma
radiation in extended media is the linear attenuation coefficient n, whose magnitude
depends on the photon energy E and the atomic number Z of the medium, /u may be
defined as the probability per unit path length that a photon will interact with the
medium.
In 'good' geometry (or narrow-beam) conditions, it can be assumed that every
scattering and absorption event leads to permanent removal of photons from the beam.
The reduction in intensity of an incident beam I
0
(photons/cm
2
s) to I
x
(photons/cm
2
s)
having passed through a thickness x cm of material with linear attenuation coefficient /i
334 JRALakey
is given by
4=/
0
exp( - Mx) .
For situations more complex than a collimated beam, the attenuation is still
exponential but is modified by two additional factors:
(1) a geometry factor, depending essentially on source geometry, and
(2) a 'build-up' factor which takes into account secondary photons produced in the
absorber (mainly as the result of Compton scattered photons which reach the
detector).
The dose (or flux) at the detector will be the sum of the uncollided flux 7
0
exp( jux)
plus the radiation which undergoes scattering to reach the detector. Allowance for this
scattered radiation is made by the introduction of a 'build-up' factor B whose magnitude
is a function of energy, n and x. Thus for a broad beam of x-rays
I = I
0
exp ( - fix) B (E, jix).
Selection of build-up factor depends upon certain 'rules of thumb' based upon qualitative
application of theory. For heterogeneous shields comprising alternate layers of a heavy
and light element, approximate methods for the determination of build-up factor have to
be used.
(a) High-Z material followed by low-Z material. An approximate procedure is to take B
as the product of the separate build-up factors for the two materials. In high-Z materials,
scattered photons are only slightly degraded in energy and only scattered through small
angles, and therefore the uncolhded source term incident at the second absorber is simply
multiplied by the build-up in the high-Z material.
(b) Low-Z material followed by high-Z material. The build-up factor for this system
corresponds roughly to that of the heavy element whose thickness (in mean free paths)
corresponds to that of the composite system.
A17.1.1. Empirical relationships for build-up factors
(a) Linear build-up factor:
B{E,
i
xx)= 1 +a(E)nx.
(b) Taylor form:
B(E,nx)=A(E)exp[-a
l
(E)nx] + (1 -A)exp[-a
2
(E)
l
ix]
where A, ai and a
2
are 'fitting' parameters. This expression may be approximated to
B(E, fix) = apx.
This will lead to an underestimation at low values of/JJC.
(c) Capo's form: a four-term polynomial which covers a wide range of energies (0.5-
10 MeV) and is accurate over 10-20 mean free paths:
B(E, nx) = fa(E) + 0i()M* + fo{EWxf + P
3
(.E)(Mxf-
Application of TLD in reactor engineering 335
A17.1.2. Calculation of flux from extended sources
Calculation of flux enables the exposure rate to be estimated by the expression:
X= 1.7x10~
6
(pE Rh"
1
.
Use Q for source strength:
Qo point source (photons/s),
Qx line source (photons/cm s),
Q
2
plane source (photons/cm
2
s),
Q
3
volume source (photons/cm
3
s).
Extended sources may be treated as arrays of point sources and by application of the
expressions in A17.1.2.1 the flux due to extended sources may be derived.
A17.1.2.1. Flux from point source. For a point source located a distance r from the
point of measurement:
Qo
4717
2
With attenuation:
Qo
4irr
With buildup:
Qo
4nr
4> = -exp(-/jtx).
<p = -^
2
exp(-nx)B(E, fix).
A17.1.2.2. Flux from a line source. For a line source, distance Z, without any shielding,
halfangle i//:
< P = .
2TTZ
For an infinitely long source, i// = -njl:
- * .
4Z
A17.1.2.3. Flux from a shielded line source, distance Z, neglecting build-up
A
Q l
< ^
4> = sec i(jit, \p).
2TTZ
336 JRALakey
A17.1.2.4. Flux from a shielded line source, distance Z, with linear build-up
Q\ Q^ixt rii
4> = sec Hjit, \jj) + [exp( /ir sec0)] sec 6 dd.
2TTZ 2ITZ J
0
A17.1.2.5. Flux from a plane source of radius A, unshielded at a perpendicular distance
Z from its centre
0 =
7
l o 8 e
(
1 +
^ l
A17.1.2.6. Flux from a plane source of radius A, shielded, neglecting build-up
A17.1.2.7. Volume source. Flux in a cloud of radioactive or airborne contamination
(where /i is small). At the centre, flux due to volume element is
4irr
2
dr
4-nr
2,
and therefore
, = 2
3
f dr =
Jo
Q
3
A.
A17.1.2.8. Flux in an absorbing medium. For example, a solid or liquid where n is
significant:
4irr
2
dr
47T7-
2
and therefore integrating gives
d<p = Qi exp(-/zr)
4> = Q
3
\ exp(-/ i r)dr = [1 - exp( - j u4) ] .
Jo M
A17.1.2.9. Flux in an infinite absorbing medium. A large compared to l//i, / i / >3.
Therefore
exp(-/L4)->-0
and hence
0 = Q
3
ln-
Application of TLD in reactor engineering
A17.1.3. Absorbed dose in infinite absorbing radioactive medium
This can be calculated on the basis of:
Energy absorbed/cm
3
= Energy released/cm
3
337
Energy released
Absorbed dose rate
Q
3
E MeVcnTV
Q
3
E 1.602x10"
100
3600 rad h"
A17.1.4. Calculation of coolant activity
If the residence time of the coolant in the reactor core is T (s) and the external circuit
time is t (s), the activity N
0
at the exit from the core in dis g
_1
s"
1
is
N
0
=
20 [1 -exp(Xr)]
1 - exp[ - X( r + r ) ]
where is the cross section per gram, <j> is the average core flux, and X is the decay
constant for activity.
Appendix 17.2. Cavity ionisation theory
Measurement of the absorbed dose in a medium exposed to ionising radiation necessitates
the introduction of a radiation-sensitive device into that medium. Usually, this device
will differ from the medium in both atomic number and density and will constitute a
discontinuity which was considered to be a cavity in the original Bragg-Gray theory [68].
To derive a more general treatment, it is necessary to consider the boundary or
interface between the medium and the detector.
Figure 17.10 depicts the dose distribution commonly encountered at an interface
between two dissimilar materials when placed in a photon field. The photons passing
through the wall medium Z\ generate an electron spectrum characteristic of that medium
and the incident photon. In medium Z
2
, representing the detector, the photons generate
an electron spectrum characteristic of medium Z
2
.
Now, take the case of the 'cavity' in the dissimilar medium. The absorbed dose
required is the dose in the wall medium but the dose measured is actually the dose in the
WALL
Figure 17.10. Typical dose distribution at
gamma-iiradiated interface.
338 JR A Lakey
'cavity' in the wall medium. A cavity correction factor has to be applied to convert the
latter to the former. The size of the cavity with respect to the range of maximum energy
electrons in the wall determines the cavity theory to be applied.
If the cavity is small (figure 17.11(a)), then it can be assumed that no electrons are
generated by photons in the cavity and the electron spectrum characteristic of the wall
remains undisturbed. In this case, the ratio of energy deposited in wall medium to that
deposited in the cavity is just the ratio of mass stopping powers averaged over the
electron spectrum as assumed in the Bragg-Gray theory. If the cavity is large (figure
17.11(c)), then inside the cavity the electron characteristic of the cavity material is
[a) (>) (c)
Figure 17.11. Absorbed dose distribution through cavities of varying size: (a) very small
cavity; (b) intermediate sized cavity; (c) very large cavity.
established and the ratio of absorbed dose in the wall to that in the cavity is equal to the
ratio of mass energy absorption coefficients of the two media, i.e. the interface effects are
negligible when averaged over the whole cavity. It is the intermediate case (figure
17.11(b)) that is most difficult because the electron spectrum in the cavity is a mixture
of the wall and cavity electron spectra. This is usually just the situation when TLD are
placed in radiation fields. Burlin [69] has formulated a theory to predict the ratio of
absorbed dose in cavity to surrounding medium and table 17.3 presents values of these
correction factors calculated for Harshaw type LiF TLD chips in different energy photon
fields in different wall media.
The Burlin theory states that:
cavity correction factor = / =
absorbed dose in cavity medium
absorbed dose in wall medium
= d
m
S^+(l-d)
(P-en/p),
cavity
(Pen/P>
Wall
Application of TLD in reactor engineering 339
Table 17.3. Ratio of absorbed dose in TLD chip to
absorbed dose in wall medium for different photon
energies.
Initial photon energy (MeV)
Wall media
Al
Air
Cu
Pb
0.1
0.586
0.973
0.082
0.019
0.5
0.936
0.935
0.951
0.387
1.0
0.988
0.939
1.049
0.969
where
m
5wa!i
ty
is th
e
ratio of mass stopping powers for cavity and wall, p
en
/p is the mass
energy absorption coefficient,
_ l _ e xp( - l s )
Bx
B is the effective mass attenuation coefficient of the electrons, and x is the mean electron
path in the cavity.
Table 17.3 reveals the importance of the correction factor whenever measurements
are made using TLD in media of different radiation attenuation properties. The effects
are most noticeable when cavity and wall medium differ in effective Z by more than a
factor 2.
Apparent changes in response of TLD can be produced by backscattering from objects
to which the dosemeter is attached. Johns [70] has recently made the point that the
reported differences in 'response' of a LiF TLD on a phantom compared with that in free
air can be shown to correspond roughly to the changed intensity which one would
expect due to backscattering. Thus, if response is defined properly, there is little
difference between the response on the phantom and in free air.
The energy-dependent response of lithium fluoride was studied by Van Prooyen and
Johnson [71] using Burlin cavity theory. The ratio of cavity dose to medium dose was
evaluated experimentally with the dosemeter embedded in various thicknesses of the
media of interest. Results were given for lucite and copper and were shown to fit Burlin's
theory.
The advantage of thin TLD is illustrated in table 17.4 which gives Lowe's [72] calcula-
tions of the cavity correction factor for a polyether sulphone (PES) LiF dosemeter with
thickness 5 mg cm
-2
exposed in aluminium to a wide range of gamma energies.
Table 17.5 presents experimental results of TLD chip response in different media when
exposed to the same source at the same distance for the same length of time the results
have been normalised to the response in lead to facilitate comparison.
Using the Burlin cavity theory, these measured doses can be converted to the dose in
air at the same point these values are of course equal for each photon source assuming
negligible attenuation of photons by the wall medium.
If we assume that the 1 MeV cavity correction factor is valid for
60
Co gamma photons
(~ 1.25 MeV), we can interpret the experimental data in table 17.5 using the data from
340 JRALakey
Table 17.4.
Cavity correction factor Initial electron
Gamma source (3 mg cm"
2
PES LiF in AI) energy (MeV)
Co
1.13,1.33 MeV 1.070 1.038
, J 7
Cs
0.66 MeV 1.077 0.477
X-ray
100 keV 1.082 0.100
Table 17.5. Absorbed dose in TLD chip in different
surrounding media for three photon energies.
131
Cs
6
Co
"N
table 17.3:
For lead
dose in air
Wall medium
Al Fe
0.662 0.672
0.761 0.762
0.592 0.680
_-chip (^en/P)chip
/ G-Ien/P)pb
1.00 0.027
= x
Pb
1.000
1.000
1.000
0.969 0,038
= 0.73
which is very close to measurements in aluminium which gives the correct dose.
For aluminium
0.761 0.027
dose in air = x = 0.77.
0.988 0.027
Appendix 17.3. The intrinsic TL response per absorbed neutron
Horowitz et al [53] used the Kandi-II diffractometer to derive the TL response in TLD 600
taking great care to correct for neutron self-shielding and derived a response which
showed that the neutron-induced kerma is 0.135 0.01 times as effective as the ^Co-
induced kerma in producing TL in TLD 600. Table 17.6 gives the absorption parameters
Application of TLD in reactor engineering 341
Table 17.6. Absorption parameters of TLD 100, TLD 600 and TLD 700 the thermal
neutrons (n
t
h).
njh cross section TLD 100, TLD 600, TLD 700,
Reaction (10""cm
2
) E(cnT') S(cnT' ) E(cm
M
)
6
Li ( n, a)
r
6
Li(n, 7)
7
Li ( n,
7
)
" F( n ,
7
)
942.4f
40 X 1CT
3
36 X 10'
3
9X 10"
3
4.33
1.8 X lO""
2.1 X10"
3
5.5 X10- *
57.14
2.43 X 1(T
3
1.01 X10"
4
5.72 X l O"
4
4.03 X 10"
3
1.71 X10"
7
2.2 X 10"
3
5.5 X10"
4
f Vlasov et al [73] quote a confidence level of 0.5%. Below 10 keV, follows the 1/v law to
within 1%.
of TLD materials TLD 100 and TLD 600 are dominated by the large cross section and
large positive Q value of
6
Ii(n, a)r reaction which yields a 2.06 MeV a particle and
2.72 MeV triton for every absorbed neutron. In TLD 700 the
7
Li(n, 7)
8
Li and
19
F(n,7)
20
F
reactions are of comparable cross section. Becker [74] has tabulated the expected values
of the impurity content of Harshaw LiF as follows:
Al(20ppm), Ca(6ppm), Mg (300 ppm), Si(40ppm), Ti(5ppm);
Dy(1. 5xl0"
3
ppm), Eu (7x 10
_s
ppm), Mn (1.5 xl0
_2
ppm).
These imply a negligible contribution to thermal-neutron absorption of TLD 700 but the
response to thermal neutron kerma is still very complex due to the two reactions. In
TLD 600 and TLD 100 the only thermal-neutron reaction of importance is
6
Li(n, a)r.
In view of the large discrepancies reported in the literature, the authors carried out
neutron sensitivity measurements in an experimental configuration where flux depression
effects are negligible and self-shielding can easily be determined. A
6
LiF shield 1 cm thick
was used to screen out thermal neutrons and the attenuation of ^Co photons used for the
gamma calibration was 2.5%. The results of TLD 600 and TLD 700 irradiation are given in
Table 17.7. Doses did not exceed 100 R, thus avoiding a supralinear response and no
significant fading was observed.
Table 17.7. Thermal neutron sensitivity of TLD 600 and TLD 700f.
TLD 600 sensitivity in R (
6
Co).
E
n
= 13.8 MeV
0 = 81.0 MeV
S"
370 45
327 20
S' S n
4020 480 2630 315 0.14, 0. 018
1470 90 2330 145 0.13
2
0.008
h
0.13
5
0.011
TLD 700 sensitivity in R (
60
Co).
= 81.0 MeV
S" = S'
0.12 0.007
S
0.19 0. 011
h
0.149
f S" is the experimentally measured sensitivity, S' is the sensitivity corrected for neutron
self-shielding, and S is the response translated to a Maxwellian distribution of thermal
neutrons at T= 293.6 K.
342 JRALakey
The authors obtained a value of (TLD600) = 0.13
5
0.011 and stress that the
response of TLD 600 is very strongly dependent on geometry. (TLD 700) = 0.149, but this
neglects the kerma produced by decay of
6
Li and
20
F which contributes 50% of the TL
sensitivity (see table 17.8). Attix calculated (TLD 100) = 0.37 using a track interaction
model but this should be regarded as speculative. The authors conclude that the TL
sensitivity of high LET kerma is lower than currently predicted. The Horowitz method
[75, 76] applied by Furuta and Tanaka [77] gave excellent agreement with the value of
= 0. 91xl0
7
n/cm
2
R.
Table 17.8. Induced kerma in TLD 700.
Reaction
6
Li ( n, a) r
"Li - ^ "Be
"Be>-2a
3
F -^*
J
Ne
Charged particle
species
a
T
e"
a
e"
Kerma
(MeV/absorbed
2.02
2.76
~0. 6
~3
- 0. 7
nth)
(Kerma)
(MeV cm"' )
8.14 X 10"
3
11.12 X 10"
3
- 1. 3 X 10"
3
- 7 X 10"
3
- 0. 4 X 10
3
A17.3.1. The calculation of intrinsic TL response per absorbed neutron: Correction for
self-shielding
Horowitz et al [53] calculate the self-shielding factor provided that sufficient details of
the experimental configuration have been reported (e.g. isotropic fluence, cylindrical
samples with given radius and height). For powdered samples an average density of
1.25 g cm
-3
is assumed. The absorption probability x has been calculated via the Monte
Carlo technique and is sampled over a Maxwellian spectrum at T= 293.6 K. They have
presented these results in a separate publication for a large variety of cylindrical
geometries. The self-shielding factor can be deduced from the relation
X<M/4 = 20F
or
0/ 0=^x/ 42F (A17.1)
where A is the surface area of the TL sample exposed to the thermal neutrons, V is its
volume, 0 is the unperturbed impinging neutron fluence (neutrons/cm
2
), 0 is the average
neutron fluence within the TL sample and 0/0 is the self-shielding factor.f Equation
(A17.1) is to be applied only for the case of an isotropic fluence. The ratio n
:
can thus be
calculated from the experimentally measured sensitivity 5,- to thermal neutrons in the
following manner:
n
{
= kerma in TL sample due to 5,- R(
60
Co)/o: and triton kerma in TL sample
due to an impinging neutron fluence of 10
10
n/cm
2
= S
ip
KcyS0>(4.78)(l .6 x 10
-6
)
= ^,-5
I
-C
I
/a7v'ocj,-0(0/0)(4.78)(1.6 x 10
- 6
). (A17.2)
f The macroscopic cross section E is calculated from the formula o(2200)N
0
pu>j/A. For a Maxwellian
energy distribution the cross section at 293.6 K is 12.9% smaller. The density p equals 2.64 g cm"
3
.
When powder is used the density is 1.25 g cm"
3
and the cross sections in Table 17.6 should be reduced
accordingly.
Application of TLD in reactor engineering 343
Table 17.9. Data for LiF phosphorsf.
A
C
t Attix [78].
TL D 100
25.94
80.7
0.074
TL D 600
25.06
83.5
0.956
TL D 700
26.02
80.5
0.000 07
It is important to note that the geometry of the flux-dosemeter sample enters only
through the self-shielding factor. In equation (A17.2), i = 1, 6, 7 representing TLD 100,
600 and 700, respectively, 5,- is the experimentally measured TL sensitivity in (
60
Co)
roentgens required to produce the same integral TL signal as an impinging neutron fluence
of 10
10
n/cm
2
, Ai is the atomic number, Q is the conversion factor from
60
Co roentgens
to ergs/g, 4.78(1.6 x 10"
6
) is the energy in ergs liberated per absorbed thermal neutron,
a is the
6
Ii(n, a)r microscopic cross section at E
n
= 25.3 meV expressed in cm
2
, N
0
is
Avogadro's number, and CJ,- is the
6
Li isotopic content. Table 17.9 shows the accepted
numerical values for A
h
C
t
and co,-. Equation (A17.2) for TLD 700 (neglecting, for the
moment, the kerma contributions from the
7
Li(n, y) and
19
F(n, 7) reactions) reduces to
6.9xlO
9
(S/0)
n
7
= = (A17.3)
(0/0)
In the case of TLD 700, (0/0) is almost exactly one. It is thus immediately obvious that the
values of S ranging from 0.7 to 2.5 result in values of n
n
ranging from 0.48 to 1.7.
Equation (Al 7.2) for TLD 100 and TLD 600 reduces to
5.04 xlO
5
(5/0) 6.43xlO
6
(S/0)
n
6
= = and n, = . (A17.4)
(0/0) (0/0)
A table of Monte Carlo calculated self-shielding factors for most standard sized LiF
TLD is given by Horowitz et a! [79].
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18
Application ofTLDfor dating: a review
G A WAGNER
18.1. Introduction
In nature, many materials occur which are TL phosphors. These materials may be of
geological, archaeological, biological and even extraterrestrial origin and comprise
different objects such as rocks, ceramics, slags, bones and meteorites. They are exposed
to natural radiation and, therefore, may acquire significant levels of natural TL. By
measuring this, one can determine the radiation dose that these objects have received
during the past. In other words, these materials can be used as natural TL dosemeters for
their natural radiation environment.
Apart from direct dosimetry applications, such as recording the radiation dose in space
by studying meteorites, the natural dose is especially useful for determining age. Since
the natural dose steadily accumulates with time, the total dose is directly related to the
radiation exposure, that is the 'age' of an object. Another, however less important,
application of natural TL is its use for thermometry. In this approach, one determines
from the degree of natural TL fading the thermal history of an object. A further TL
application which is due to the TL characteristics rather than natural TL is the source
identification of objects.
The purpose of this chapter is to summarise the present state of the methodical
development and applications of TL dating. The other aspects which are connected with
TL in natural objects are covered by the literature and references given in the bibliography.
18.2. D ating method
18.2.1. Basic principle
TL dating of geological and archaeological samples essentially consists of two basic steps,
the determination of the natural dose D
n
which a sample has absorbed during its past and
the determination of the corresponding natural dose rate D
n
. From these two values, the
TL age t can be calculated according to
t=D
n
/D
n
.
For the determination of the natural dose from the naturally occurring TL, one needs to
know the TL sensitivity which varies from sample to sample. The sensitivity has to be
measured for each sample and is derived from the artificial TL which is induced by
laboratory irradiation with known doses. This necessitates calibrated radiation sources.
The natural dose rate mainly originates from the radioactive elements, uranium, thorium,
potassium and rubidium. To a lesser degree, cosmic radiation is also a contributing factor.
348 GA Wagner
Various methods exist for the evaluation of the natural dose rate. They will be discussed
in more detail later.
Assuming no partial fading of natural TL over the sample's history, the age determined
in this way dates either the formation of the sample or the time of previous heating
which was sufficiently high for complete erasure of any previous TL.
18.2.2. Complications
Unfortunately, in practice, TL dating is more complex than this simple principle might
suggest. Several difficulties have to be taken into account. These difficulties can be
divided into those which are caused by the TL phenomenon itself, those which are caused
by the artificial irradiation and those which are introduced when evaluating the natural
dose rate.
The major problems caused by the TL phenomenon are lower TL efficiency for
a-radiation than for /3- or 7-radiation, non-linear growth of TL with increasing dose
(supralinearity, saturation), change of TL sensitivity by heating (especially the pre-dose
effect), spurious (i.e. non-radiation-induced) TL, and thermal and anomalous fading
of TL.
The lower TL efficiency of a-radiation with respect to either 0- or 7-radiation is the
consequence of the high ionisation density along the a-particle tracks with the associated
saturation of the available electron traps. The ratio of a-radiation TL efficiency to that of
0- or 7-radiation is usually expressed as the fc-value (Tite [78], D W Zimmerman [27]), or
the a-value (Aitken and Bowman [31]). The different TL efficiencies are manifested in
a modification to the general age equation
kD
a
+Dp+D
y
+D
c
where Dp is the artificial 0 dose ('equivalent dose') which produces a TL signal equivalent
to the naturally occurring TL. D
a
, Dp, D
y
and D
c
are the fractional natural a-, /3-, 7- and
cosmic-ray dose rates, respectively.
Supralinearity is the increase of TL sensitivity during the first few hundred rad of a
radiation dose (Tite [78], Aitken [1]). In the case of supralinearity, a correction
('intercept correction', Fleming [12]) has to be applied for dating. At higher doses, around
10
s
rad, the TL growth curve becomes sublinear due to saturation of the electron traps.
Saturation generally restricts TL dating to the last million years.
One often observes a change in TL sensitivity after a sample has been heated in order
to drain its TL. This difference in sensitivity between first and second glow may be due in
part to the changed transparency of the sample and in part to the pre-dose effect. The
pre-dose effect is the increase of sensitivity from first to second glow, which depends on
the magnitude of the radiation dose that the sample has absorbed before heating
(J. Zimmerman [29]). Regardless of its causes, the consequence of the sensitivity change
for dating is that natural TL and the equivalent dose cannot be measured on the same
sample material. Instead, one needs in principle at least two aliquots. From the first
aliquot one derives the natural TL. The second aliquot receives a known artificial dose in
addition to the natural ones before one measures its TL. In this way, one constructs a TL
Application of TLD for dating: a review 349
growth on unheated sample material. In practice, more than two aliquots are needed in
order to check the identity of the aliquots and the linearity of the TL growth curve.
Spurious TL may have several causes such as pressure, friction, light exposure and
chemical reactions. Since a spurious TL component would increase the apparent age, one
suppresses it by measuring the TL glow under an extremely pure nitrogen or argon
atmosphere (Aitken et al [5]). On the other hand, fading of the natural TL would lower
the apparent age. Thermal fading, as well as spurious TL, can be recognised by the plateau
test (Aitken et al [5a], McKeever [17]). Another, not yet well understood, kind of fading
is the so-called 'anomalous fading' which is commonly observed in feldspars and zircons
(Wintle [24]). It may be detected by storing artificially irradiated sample aliquots for
several weeks and comparing their TL signal with freshly irradiated aliquots (Wintle [26]).
In order to determine the ^-factor (or a-factor) and the equivalent dose, one needs well
calibrated radioactive sources. Usually
241
Am or
242
Cm are used as a sources and ^Sr/ ^Y
as 0 sources. The energy dosimetry of such sources is an extremely difficult task since it
depends on many parameters such as type, size and activity of the source, the radiation
geometry, the type and thickness of the target and others. Large systematic errors in
dating may and do result from inadequately known sources. Lately, major efforts on an
interlaboratory basis have been in the more accurate calibration of sources. Literature
pertinent to this aspect is given in the references.
When evaluating the dose rate, major problems are caused by the heterogeneous,
spatial distribution of radioactivity, by possible disequilibrium in the radioactive decay
chains and by the absorption of radiation by the water content in the sample.
When the radioactivity is heterogeneously distributed on a scale which is comparable
with or larger than the range of the radiogenic particles, detailed microdosimetry con-
siderations have to be taken into account for the dose rate evaluation. This is best
explained by using, as an example, pottery which contains quartz grains of lOOjum
diameter in a fine-grained matrix of less than 10 /im grain size. All the radioactivity is
contained in the matrix. The 0- and 7-particles from the matrix with their average ranges
of a few millimetres and 30 cm, respectively, would penetrate the quartz grains and the
matrix equally. However, the a-particles with their average range of 25 fim would only
reach the outer shell of the quartz grain leaving an a-sheltered core. Therefore the a dose
received by the quartz grains would be less than that received by the matrix. This
illustrates that dose rates can be evaluated only for defined grain sizes. This necessitates
grain size fractionations for the dating of samples with heterogeneously distributed
radioactivity (Fleming [11]).
Radioactive disequilibrium within the decay chains is a serious setback for TL dating.
For correct evaluation, it would be necessary to know at which member within the chain
disequilibrium occurs (Meakins et al [51]). One of the members most susceptible to dis-
equilibrium is
222
Rn in the
238
U chain. As a rare gas with a half-life of 3.8 days, radon-222
may easily diffuse from a sample (Desai and Aitken [49]). There are several approaches to
discover radon loss (Aitken [43], Carriveau and Harbottle [47]). Other candidates for
disequilibrium are
230
Th and
226
Ra (Pernicka [57]).
Finally, any water content in the sample and the surrounding soil may absorb
radiation. In order to make appropriate corrections, the natural water content has to be
determined (J. Zimmerman [27]). Apart from the present moisture content, its seasonal
and long-term climatic changes must also be considered.
350 G A Wagner
18.2.3. Dating techniques
Because of the complications outlined in the previous section, several dating techniques
have been developed.
18.2.3.1. Quartz inclusion technique. The quartz inclusion technique was developed for
the large (compared to a range) quartz grains in pottery (Fleming [12]). The quartz grains
free of radioactivity are separated from the crushed pottery and their a dose shell is
etched away with hydrofluoric acid. The remaining cores of the quartz grains which are
used for TL measurement have only received the /3 and y contribution of dose from the
matrix. Since the |3 dose is also to some degree attenuated in coarse quartz grains, a
correction must be applied (Mejdahl [53], Bell [45]). However, new investigations have
somewhat modified this simple picture. The quartz grains themselves may be radioactive
(Sutton and Zimmerman [59]) and their etching rate can vary considerably among the
grains (Bell and Zimmerman [8]). The main advantages of this dating technique are the
elimination of the difficult a dosimetry and the resistance of quartz against anomalous
fading.
18.2.3.2. Fine-grain technique. On the other hand, the fine-grain technique uses only
the matrix of the pottery below 10 jLim grain size (D W Zimmerman [27]). This fraction
received the full a, 0 and 7 contributions of the natural dose rate. For artificial irradiation,
one needs both a and /3 sources. Because the fine-grain matrix from archaeological
ceramics commonly contains feldspar (Singhvi and Zimmerman [19]), the TL of fine-grain
fractions is susceptible to anomalous fading.
Both the quartz inclusion and the fine-grain techniques are the standard TL dating
techniques for archaeological ceramics.
18.2.3.3. Subtraction dating technique. Both techniques are combined to the subtraction
dating technique (Fleming and Stoneham [15]). In this case, only the a dose of the fine-
grain matrix is used by subtraction of the 0 and 7 dose recorded in the coarse quartz
grains from the total dose recorded by the matrix. The advantage of this technique is the
elimination of the environmental 7 dose. This technique, therefore, is suitable for the
dating of objects which have been removed from their natural environment, such as
museum objects. Its dating accuracy, however, is lower than for the two standard
techniques.
18.2.3.4. Zircon inclusion technique. The zircon inclusion technique (Sutton and
Zimmerman [20], D W Zimmerman [28]) uses the highly radioactive, coarse zircon grains.
The lOOjum large grains are separated from the pottery and their TL is measured. It is
possible to use single grains for dating. Because the zircon grains are large compared to
the a range, but small compared to the j3 and 7 ranges, they absorb practically only their
own a. dose. Therefore, zircon inclusion ages of ceramics are independent of the moisture
content and the environmental radioactivity. Serious obstacles, however, are the zoned
uranium inhomogeneity within most grains and the anomalous fading of TL in zircon.
This technique is of current interest mainly for authenticity testing.
Application of TLD for dating: a review 351
18.2.3.5. Pre-dose dating technique. Glow curves of quartz show a large peak in the
110 C region. The peak-height for a given test dose depends strongly on the pre-dose that
the quartzes have received before heating to about 500 C. This sensitisation behaviour
is the basis for the pre-dose dating technique for quartz (Fleming [13,14a], Aitken [3]).
The sensitisation from the natural pre-dose is compared to that induced by a known
laboratory dose. This technique is especially suited for young, quartz-bearing ceramics.
Owing to saturation it is restricted to roughly the last thousand years.
18.2.3.6. Photo transferred TL technique. Recently, efforts have been made to use photo-
transferred thermoluminescence (PTTL) for dating, PTTL describes the phenomenon of the
re-excited TL by uv illumination after annealing. It is explained by the uv-induced trans-
fer of electrons from deeper traps into shallower traps. Feasibility studies for PTTL dating
of zircon, apatite (Bailiff [6]) and of quartz (Bowman [9], Sasidharan et al [18]) have
been carried out. The PTTL technique looks promising, since many of the difficulties
caused by the TL phenomenon can be circumvented.
18.2.4. Natural dose rate
The natural dose rate, which an archaeological or geological sample receives, originates in
part internally, i.e. inside the sample, and in part externally, i.e. in its environment.
Therefore, dose rate evaluation has to take into account both the sample and its
surroundings. The degree to which the dose rate is internal and the degree to which it is
external depends on the size of the sample in comparison to the range of the various
radiations. For instance, a brick from inside a thick, homogeneous wall would receive
virtually all its dose internally with the exception of a small external cosmic-ray contribu-
tion. On the other hand, a brick fragment lying in soil would receive essentially only its
a and (3 doses internally and its y dose externally. These examples illustrate that sampling
for TL dating must be done thoughtfully with radiation dosimetry in mind.
There are several techniques by which the natural dose rate can be determined: the
direct analysis of the radioactive elements, a counting (or uranium and thorium) and
TLD techniques. Since all these techniques have advantages and disadvantages a combina-
ticn of different techniques is best (Aitken [42]).
For direct analysis, the radioactive elements, uranium, thorium, potassium and
rubidium, are determined in the sample and surroundings. For U, Th and Rb, neutron
activation may be used, and for K and Rb, atomic absorption or flame photometry may
be used. Fission track analysis of U and Th (Wagner [60]) has the advantage of revealing
the distribution of these elements on the microscopic scale. The dose rates are calculated
from the elemental contents (Bell [44, 46], Carriveau and Troka [48]). For the evaluation
of dose rate from U and Th decay chains, one needs to know about the degree of radio-
active equilibrium.
Direct a counting of the sample has the advantage of taking into account the dis-
equilibrium. This technique is well suited for the determination of the a dose rate. The
powdered sample is put on a ZnS screen and the scintillations are counted (Tite and
Waine [21]). In order to evaluate the contribution from U and Th to the (3 and 7 dose
rate, however, one needs to know the Th/U ratio and the degree of radioactive
equilibrium.
TLD can also be used for measuring external dose rate (Aitken [41], Mejdahl [54]) as
well as the internal dose rate of pottery (Mejdahl [53, 73]). CaF
2
and CaS0
4
are used as
352 G A Wagner
phosphors. The external dose rate is recorded by putting capsules in the position from
which the samples have been removed for dating. The capsules are left for one year in
order to make allowance for seasonal variations of the dose rate. The use of TLD for dose
rate evaluation has the advantage of eliminating the calibration of radioactive sources
(Aitken [40]). TLD also takes into account radioactive disequilibrium and radiation
attenuation by the moisture content. Some problems still exist with the energy depend-
ence, the TL stability and the radiation geometry of the phosphors.
18.3. Dating applications
18.3.1. Archaeological
18.3.1.1. Ceramics. Already, 20 years ago, in the early stage of TL dating, ceramic
materials had attracted the interest of those working with this method. Ceramics are in
the category of the most common and most important archaeological objects. They are
produced by firing clay. The temperatures of firing are sufficiently high to reset the TL
clock of the clay. It has been shown that firing at 400 C for 30 min eliminates the
previous TL (Carriveau [64]). Therefore, the TL age determines a well defined event.
Actually, the essential methodical progress in TL dating was achieved during the 1960s
when studying ceramics. As a consequence, most dating techniques were developed
first for ceramics and later applied also to other materials. The research papers listed in
the references reflect this development.
There are numerous applications of TL dating to ceramic materials, mostly to pot-
sherds, but also to bricks, fired clay and soil and to furnaces. The measured TL ages range
from the earliest fired clay artifacts, such as the palaeolithic figurines from Dolni
Vestonice (Zimmerman and Huxtable [82]) to recent samples. The appended literature
gives a cross section through these widespread activities.
As an example, in figure 18.1, glow curves of the fine-grain and the coarse quartz
fractions from a fired clay are shown. The fired clay was found on the inner wall of a
mediaeval potter's furnace at Liibeck. TL dating established that this furnace was
abandoned in 1240 AD + 60 years (1 a) (Wagner [79]).
A byproduct of ceramic dating is authenticity testing of ceramic works of art (Fleming
[66]). Although in this application there is much less necessity for age accuracy, one has
to restrict the amount of material because of great value of many art pieces. TL authen-
ticity testing can be carried out on less than 50 mg drilling powder. Also, bronze objects
which still contain sand or clay in their core are suitable for TL authenticity testing as was
demonstrated on the famous bronze horse from the Metropolitan Museum, New York
(Zimmerman et al [83]). The techniques of zircon grain, quartz inclusion and fine-grain
dating proved the authenticity of this much debated art object.
18.3.1.2. Heated rocks. In archaeological excavations, rocks are occasionally found
which appear to have been heated by prehistoric man. During the heating process,
temperatures may have been reached which were sufficiently high to erase the previous
geological TL in these rocks. The TL age of such rocks dates the heating. Because
geological ages are generally some orders of magnitude larger than archaeological ages,
one must ensure that no residual TL survived the heating. Such residual TL may be
recognized from the shape of glow curves and through the plateau test.
Application of TLDfor dating: a review
FINE GRAIN
353
170 rod
eau
~[ 1
-
200 300 400
TEMPERATURE C O
Figure 18.1. Glow curves for particles from a fired clay.
As an example, the quartz inclusion and fine-grain techniques have been applied to
burnt sandstones which probably served as cooking stones. Reasonable TL ages of the first
millenium BC have been found (Huxtable et al [88]).
Another heated stone material is flint. Its heating probably served the purpose of
improving its properties for tool making. The flint samples must not be crushed due to
triboluminescence. Instead TL is measured on polished slices of flint (Goksu and Fremlin
[86]). The complicated dosimetry problems when irradiating thick slices of flint have
been overcome by Aitken and Wintle [84]. TL dates up to 50 000 years have been
reported by Goksu et al [87]. The work on the Terra Amata site has shown that flint
dating might be applicable at least up to 250 000 years (Wintle and Aitken [93]).
18.3.1.3. Slags. Metallurgical slags are produced, analogous to ceramics, by an event
which involves heat. It should therefore be possible to date ancient smelting activities
with TL. Such data would be highly welcomed by metallurgists. Unfortunately, very
little work has been done on slags. Carriveau [99], using slag material which was ground
to a fine powder, reported few ages on silver slags and iron slags which seem to be in
reasonable agreement with independently known ages. In the case of copper and bronze
slags, which did not have nearly as many silicate inclusions, Carriveau found TL ages
consistently much higher than they should be. However, in order to date ancient metal-
lurgical activities, one may also apply TL dating to heated soil adjacent to slags, crucibles,
tuyeres and smelting furnaces.
18.3.1.4. Bones and shells. Bones and shells have also been considered for TL dating. Pre-
liminary experiments have revealed high levels of spurious TL, namely triboluminescence
354 G A Wagner
and chemiluminescence (Jasinska and Niedwiadomsky [98], Christodoulides and Fremlin
[96]). In order to lower this spurious component, Driver [97] used thin slices instead of
powdered material and extracted the organic matter. Before judging if these biological
materials are suitable for TL dating, further studies on their TL characteristics are
necessary.
18.3.2. Geological
18.3.2.1. Volcanic events. Volcanic rocks form at high temperatures and cool down
rapidly to low temperatures. From this point of view, they seem to be well suited for TL
dating. Volcanic rocks from the Quaternary Period are difficult to date by other existing
methods. Therefore the potential of TL dating for young volcanic rocks has been realised
for some time. However, the TL characteristics of volcanic rocks are not known well
enough yet. Also difficulties with sample preparation and natural dose rate evaluation still
exist. However, some direct applications of TL dating to volcanic rocks have been
reported. May [113] dated plagioclases from Hawaiian alkalic basalts. The method seems
to work for ages up to 250 000 years. Another example is the dating of tuff layers with
human footprints in Anatolia, for which ages between 26 000 and 65 000 years were
reported (Goksu [109]). In order to circumvent anomalous fading, commonly observed
in plagioclase, Valladas [92] used high temperature TL between 500 and 700 C.
Apart from direct applications to volcanic rocks, it is also possible to use adjacent
rocks which were sufficiently heated. This approach was applied to the inversely
magnetised lava flows of Laschamp and Olby in the Chaines de Puys (Gillot et al [108]).
Quartz separated from a granitic inclusion within the Laschamp flow gave 35 000
3000 years and quartz pebbles from baked palaeo-soil undernearth the Olby flow gave
38 000 6000 years.
18.3.2.2. Calcareous deposits. In the early stages of TL dating, most activities were
concentrated on limestone age determination. However, many difficulties had been
encountered (see e.g. Zeller and Ronca [119]). Recently, interest has been revived in TL
dating of calcareous deposits, essentially of stalagmites. Such age data would be of great
interest to Quaternary geology and Palaeolithic prehistory.
In a systematic study Win tie [118] investigated the TL characteristics of stalagmites.
In that study some problems such as spurious TL, changing natural dose rate due to
initial disequilibrium in the uranium decay chain and others have been overcome. A major
problem still seems to be the heterogeneous distribution of uranium.
18.3.2.3. Loess, till and ocean deposits. In the past few years, many TL ages in
Quaternary sediments such as loess and glacial till have been reported by Soviet and
Chinese workers (see e.g. Hiitt etal [120]). Obviously there must be some process connected
with sedimentation which erases the previous TL, resetting the clock. The bleaching of
TL is most probably caused by exposure to light. This was recently shown experimentally
by Wintle and Huntley [122] who exposed ocean sediment to simulated sunlight. By
using the fine-grain technique, these authors obtained, for an ocean sediment core, TL
ages between 9000 and 140 000 years which are in agreement with independently known
ages.
Application of TLD for dating: a review 355
18.4. Conclusion
Methodically, TL dating is by no means easy. Owing to its complex nature it is still a
long way from becoming a routine dating method. Even when dating pottery, methodical
difficulties still arise. Therefore, most laboratories engaged in TL dating combine its
practical application with methodical studies.
Reliable dating techniques now mainly exist for archaeological ceramics. However,
quite commonly even such material must be rejected due to unsatisfactory TL character-
istics. For archaeological ceramics which have been thoughtfully collected (Aitken [61])
and which have satisfactory TL characteristics, age accuracies of 5% to 10% can be
obtained.
At the moment, interest is increasing in the application of TL dating to Palaeolithic
and Quaternary samples such as heated soils and stones, stalagmites, volcanic rocks and
young sediments.
References and selected reading
Dating techniques
1 Aitken M J 1968 TL-dating in archaeology, in Thermoluminescence of Geological Materials ed D J
McDougall (New York: Academic Press) p 369
2 Aitken M J 1976 TL age evaluation and assessment of error limits: revised system Archaeometry
18 233
3 Aitken M J 1978 Pre-dose dating: prediction from the model PA CT J. 2/3 319
4 Aitken M J and Fleming S J 1972 TL dosimetry in archaeological dating, in Topics in Radiation
Dosimetry Supplement I, ed F H Attix (New York: Academic Press) p 1
5 Aitken M J, Fleming S J, Reid J and Tite M S 1968 Elimination of spurious TL, in Thermo-
luminescence of Geological Materials ed D J McDougall (New York: Academic Press) p 133
5a Aitken M J, Tite M S and Reid J 1963 Thermoluminescence dating: progress report Archaeometry
6 65
6 Bailiff I K 1976 Use of phototransfer for the anomalous fading ofTL Nature 264 531
7 Bailiff I K, Bowman S G E, Mobbs F S and Aitken M J 1977 The phototransfer technique and its
use in TL-dating J. Electrostatics 3 269
8 Bell W T and Zimmerman D W 1978 The effect of HF acid etching on the morphology of quartz
inclusions for TL-dating Archaeometry 20 63
9 Bowman S G E 1978 Phototransferred TL in quartz and its potential use in dating PACT J. 2/3
381
10 Charalambous S and Michael C 1976 A new method of dating pottery by TL Nucl. Instrum. Meth.
137 565
11 Fleming S J 1966 Study of TL of crystalline extracts from pottery Archaeometry 9 170
12 Fleming S J 1970 TL-dating: refinement of the quartz inclusion method Archaeometry 12 133
13 Fleming S J 1973 The pre-dose technique: a new TL dating method Archaeometry 15 13
14 Fleming S J 1975 Supralinearity corrections in fine-grain TL-dating: a re-appraisal Archaeometry
17 122
14a Fleming S J 1978 The pre-dose method: basic elements PA CT J. 2/3 315
15 Fleming S J and Stoneham D 1973 The subtraction technique of TL-dating Archaeometry 15 229
16 Huxtable J 1978 Fine-grain dating, PACT J. 2/3 7
17 McKeever S W S 1979 A note on the plateau-test in TL-dating Ancient TL 6 13
18 Sasidharan R, Sunta C M and Nambi K S V 1978 Phototransfer method of determining archaeo-
logical dose of pottery sherds PACT J. 2/3 401
19 Singhvi A K and Zimmerman D W 1978 The luminescent minerals in fine-grain samples from
archaeological ceramics PA CTJ. 2[3 12
356 GA Wagner
20 Sutton S R and Zimmerman D W 1976 TL-dating using zircon grains from archaeological ceramics
Archaeometry 18 125
21 Tite M S and Waine J 1962 TL-dating: a re-appraisal Archaeometry 5 53
22 Valladas G, Gillot P V and Guerin G 1978 Dating plagioklase? PACT J. 2/3 251
23 Valladas G and Valladas H 1978 High temperature TLArchaeo-Physica 10 506
24 Wintle AG 1973 Anomalous fading of TL in mineral samples Nature 245 143
25 Wintle A G 1975 Effects of sample preparation of the TL characteristics of calcite Mod. Geol. 5
165
26 Wintle A G 1978 Anomalous fading PACT J. 2/3 240
27 Zimmerman D W 1971 TL-dating using fine grains from pottery Archaeometry 13 29
28 Zimmerman D W 1978 TL-dating using zircon grains PACTJ. 2/3 458
29 Zimmerman J 1971 The radiation-induced increase of the 100"C thermoluminescence sensitivity
of fired quartz / . Phys. C: Solid St. Phys. 4 3265
Artificial irradiation, radiation sources
30 Aitken M J 1978 Interlaboratory calibration of alpha and beta sources PA CT J. 2/3 443
31 Aitken M J and Bowman S G E 1975 TL-dating: assessment of alpha particle contribution
Archaeometry 17 132
32 Aitken M J and Wintle AG 1977 TL-dating of calcite and burnt flint: the age relation for slices
Archaeometry 19 100
33 Murray A S and Wintle A G 1978 Beta source calibration PACT J. 2/3 419
34 Pernicka E and Wagner G A 1979 Primary and interlaboratory calibration of beta sources using
quartz as thermoluminescent phosphor Ancient TL 6 2
35 Stadler A and Wagner G A 1978 TL-dating of ceramics: laboratory simulation of the natural radia-
tion dose PACT J. 2/3 448
36 Varma M N and Carriveau G W 1978 A precise alpha source calibration for TL-dating PACT J. 2/3
414
37 Wintle A G and Aitken M J 1977 Absorbed dose from a beta source as shown by TL dosimetry Int.
J. Appl. Radiat. hot. 28 625
38 Wintle A G and Murray A S 1977 TL-dating: reassessment of the fine-grain dose rate Archaeometry
19 97
39 Zimmerman D W 1972 Relative TL effects of alpha- and beta-radiation Radiat. Effects 14 81
Radiation dose rate
40 Aitken M J 1968 Evaluation of effective radioactive content by TL dosimetry, in Thermo-
luminescence of Geological Materials ed D J McDougall (New York: Academic Press) p 463
41 Aitken M J 1969 Thermoluminescent dosimetry of environmental radiation on archaeological sites
Archaeometry 11 109
42 Aitken M J 1978 Dose-rate evaluation PACT J. 2/3 18
43 Aitken M J 1978 Radon loss evaluation by alpha counting PACT J. 2/3 104
44 Bell W T 1976 The assessment of the radiation dose-rate for thermoluminescence dating Archaeo-
metry 18 107
45 Bell WT 1979 Attenuation factors for the observed radiation dose in quartz inclusions for TL-
dating Ancient TL 8 2
46 Bell W T 1979 Thermoluminescence dating: radiation dose-rate data Archaeometry 21 243
47 Carriveau G W and Harbottle G 1978 Direct measurement of the fraction of radon loss in ceramics
by gamma-ray-spectroscopy Archaeo-Physika 10 423
48 Carriveau G W and Troka W 1978 Annual dose rate calculations for TL-dating Archaeo-Physika 10
406
49 Desai V S and Aitken M J 1974 Radon escape from pottery: effects of wetness Archaeometry 16
95
50 Malik S R, Durrani S A and Fremlin J H 1973 A comparative study of the spatial distribution of
uranium and of TL-producing minerals in archaeological materials Archaeometry 15 249
Application of TLD for dating: a review 357
51 Meakins R L, Dickson B L and Kelly J 1978 The effect on TL-dating of disequilibrium in the
uranium decay chain PACT J. 2/3 97
52 Meakins R L, Dickson B L and Kelly J 1979 Gamma-ray analysis of K, U and Th for dose-rate
estimation in TL-dating Archaeometry 21 79
53 Mejdahl V 1978 TL-dating: a TL technique for beta-ray dosimetry PACT J. 2/3 35
54 Mejdahl V 1978 Measurement of environmental radiation at archaeological sites by means of TL
dosimeters PA CTJ. 2/3 70
55 Mejdahl V 1979 TL-dating: beta-dose attenuation in quartz grains Archaeometry 21 61
56 Murray A S, Bowman S G E and Aitken M J 1978 Evaluation of the gamma dose-rate contribu-
tion PACT J. 2/3 84
57 Pernicka E 1979 Radiometric detection of deviations from secular equilibrium in the uranium
decay chain 19th Int. Symp. on Archaeometry, London
58 Sasidharan R, Sunta C M and Nambi K S V 1979 Error implications in case of underdetermined
U-Th concentration ratio in pottery samples Ancient TL 2 8
59 Sutton S R and Zimmerman D W 1978 TL-dating: radioactivity in quartz Archaeometry 20 67
60 Wagner G A 1976 Dose rate evaluation for TL-dating by fission track counting Proc. Symp. on
Archaeometry and Archaeological Prospection, Edinburgh
Archaeological applications
(a) Ceramics
61 Aitken M J 1977 TL-dating and the archaeologist Antiquity 51 11
62 Aitken M J, Zimmerman D W and Fleming S J 1968 Thermoluminescence dating of ancient pottery
Nature 219 442
63 Becker K and Moreno A 1974 Some applications of thermoluminescence measurements in ancient
ceramics Proc. 4th Int. Conf. on Luminescence Dosimetry, Krakow (Krakow: Institute of Nuclear
Physics) p 1023
64 Carriveau G W 1974 Annealing threshold and TL-dating of ceramic material MASCA Newsletter
10 3
65 Fleming S J 1968 Thermoluminescence age studies on mineral inclusions separated from ancient
pottery, in Thermoluminescence of Geological Materials ed D J McDougall (New York: Academic
Press) p 431
66 Fleming S J 1970 Authenticity testing of art ceramics by the thermoluminescence-method - some
important examples, in Application of Science in Examination of Works of Art ed W J Young
(Boston: Museum of Fine Arts) p 206
67 Fleming S J 1972 Thermoluminescence authenticity testing of ancient ceramics using radiation-
sensitivity changes in quartz Naturwissenschaften 59 145
68 Gorier J 1965 Die Thermolumineszenz und ihre Anwendung zur Alterbestimmung von Keramik-
scherben Archaeo-Physika (Koln: Bohlau Verlag) p. 109
69 Grogler N, Houtermans F G and Stauffer H 1960 Uber die Datierung von Keramik und Ziegel
durch Thermolumineszenz C. R. Reunion Soc. Suisse Phys. 33 595
70 Huxtable J, Aitken M J and Weber J C 1972 Thermoluminescence dating of baked clay balls of the
poverty point culture Archaeometry 14 269
71 Ichikawa Y, Nagatomo T and Hagihara N 1978 Thermoluminescent dating of Jomon pattern
pottery from Taishaku Valley Archaeometry 20 171
72 Mazess B and Zimmerman D W 1966 Pottery dating from thermoluminescence Science 152 347
73 Mejdahl V 1969 Thermoluminescence dating of ancient Danish ceramics Archaeometry 11 99
74 Mejdahl V 1972 Progress in TL-dating at Riso Archaeometry 14 245
75 Mejdahl V and Winther-Nielsen M 1978 Dating of Danish ceramics by means of the quartz inclusion
technique PA CTJ. 2/3 131
76 Pernicka E 1979 Beitrage zur Thermolumineszenz-Datierung urzeitlicher und fruhgeschichtlicher
Keramikfunde Anz. Osterr. Akad. Wiss. Math.-Naturwiss. Kl. 1979 1
77 Ralph E K and Han M C 1966 Dating of pottery by thermoluminescence Nature 210 245
78 Tite M S 1966 TL-dating of ancient ceramics: a reassessment Archaeometry 9 155
358 G A Wagner
79 Wagner G A 1979 TL-Datierung am Topferofen Koberg 15 in Liibeck Liibecker Schriften Archaol.
Vorgeschichte 3 83
80 Wagner G A and Bischof H 1977 Echtheitstests mittels Thermolumineszenz an altchinesischen
Keramikplastiken Archaol. Naturwiss. 1 20
81 Whittle E H and Arnand J M 1975 Thermoluminescent dating of neolithic and chalcolithic pottery
from sites in Central Portugal Archaeometry 17 5
82 Zimmerman D W and Huxtable J 1971 Thermoluminescent dating of Upper Palaeolithic fired clay
from Dolni Vestonice Archaeometry 13 53
83 Zimmerman D W, Yuhas M P and Meyers P (1974) TL authenticity measurements on core material
from the bronze horse of the New York Metropolitan Museum of Art Archaeometry 16 19
(b) Heated rocks
84 Aitken M J and Wintle A G 1977 TL-dating of calcite and burnt flint: the age relation for slices
Archaeometry 19 100
85 Bowman S G E and Seely M A 1978 The British Museum flint dating project PACT J. 2/ 3 151
86 Goksu H Y and Fremlin J H 1972 TL from unirradiated flints: regeneration JL Archaeometry 14
127
87 Goksu H Y, Fremlin J H, Irwin H T and Fryxell R 1974 Age determination of burnt flint by
thermoluminescent method Science 183 651
88 Huxtable J, Aitken M J, Hedges JW and Renfrew AC 1976 Dating a settlement pattern by
thermoluminescence: the burnt mounds of Orkney Archaeometry 18 5
89 Ichikawa Y and Nagatomo T 1978 Thermoluminescence dating of burnt sandstones from Senpkuji
CwePACTJ. 2/ 3 174
90 Melcher C J and Zimmerman D W 1977 Thermoluminescent determination of prehistoric heat
treatment of chert artifacts Science 197 1359
91 Rowlett R M, Mandeville M D and Zeller E J 1974 The interpretation and dating of humanly
worked silicous materials by thermoluminescent analysis Proc. Prehist. Soc. 40 37
92 Valladas G 1978 Thermoluminescence dating of burnt stones from a prehistoric site PACT J. 2/i
180
93 Wintle A G and Aitken M J 1976 Thermoluminescence dating of burnt flint: application to a Lower
Palaeolithic site, Terra Amata Archaeometry 19 111
94 Wintle A G and Oakley K P 1972 Thermoluminescent dating of fired rock-crystal from Bellan
Bandi Palassa, Ceylon Archaeometry 14 277
95 Wright D A 1979 A Swedish vitrified fort: dating by conventional TL Ancient TL 8 13
(c) Biological materials (bones, shells)
96 Christodoulides C and Fremlin J H 1971 Thermoluminescence of biological materials Nature 232
257
97 Driver H ST 1978 The preparation of thin slices of bone and shell for TL PACT J. 2/3 290
98 Jasinska M and Niewiadomski T 1970 Thermoluminescence of biological materials Nature 227
1159
(d) Metallurgical slags
99 Carriveau G W 1974 Dating of 'Phoenician' slag from Iberia using thermoluminescence tech-
niques MASCA Newsletter 10
100 Carriveau G W 1974 Application of thermoluminescent dating to prehistoric metallurgy Preprint
(e) Identification
101 Afordakos G, Alexopoulos K and Miliotis D 1974 Using artificial thermoluminescence to
reassemble statues from fragments Nature 250 47
Application of TLD for dating: a review 359
102 Carriveau GW and Nievens M 1978 Guatamalan Obsidian source characterization by thermo-
l umi nescence/ Vl Cr/ 2/3 506
103 Goksu H Y and Tiiretken N 1978 Source identification of Obsidian tools by thermoluminescence
PACT J. 2/3 356
104 Huntley D J and Bailey D C 1978 Obsidian source identification by thermoluminescence
Archaeometry 20 159
105 Leach B F and Fankhauser B 1978 The characterization of New Zealand Obsidian sources using
thermoluminescence Preprint
Geological applications
(a) Volcanic events
106 Aitken M J, Fleming S J, Doell R R and Tanguy J C 1968 Thermoluminescent study of lavas
from Mt Etna and other historic flows: preliminary results, in Thermoluminescence of Geological
Materials ed D J McDougall (New York: Academic Press) p 359
107 Bechtel F, Schvoerer M, Rouanet J F and Gallois B 1978 Extension a la prehistoire, a l'ocean-
ographie et a la volcanologie de la methode de datation par thermoluminescence PACT J. 2/3
481
108 Gillot P Y, Labeyrie J, Laj C, Valladas G, Guerin G, Poupeau G and Delibrias 1979 Age of the
Laschamp Paleomagnetic excursion revisited Earth Planet. Sci. Lett. 42 444
109 Goksu H Y 1978 The TL age determination of fossil human footprints Archaeo-Physika 10 455
110 Huxtable J and Aitken M J 1977 Thermoluminescent dating of Lake Mungo geomagnetic polarity
excursion Nature 265 40
111 Huxtable J, Aitken M J and Bonhommet N 1978 Thermoluminescence dating of sediment baked
lava flows of the Chaine de Puys Nature 275 207
112 Hwang F S W 1970 Thermoluminescence dating applied to volcanic lava Nature 227 940
113 May R M 1977 Thermoluminescence dating of Hawaiian alkalic basal t s/ Geophys. Res. 82 3023
(b) Calcareous materials
114 Bangert J and Hennig G J 1978 Effects of sample preparation and the influence of clay impurities
on the TL-dating of calcitic cave deposits PACT J. 2/3 281
115 Gallois B, Nguyen P H, Bechtel F and Schvoerer M 1978 Datation par thermoluminescence de
coraux fossiles des Caraibes PACT J. 2/3 493
116 Johnson N M and Blanchard R L 1967 Radiation dosimetry from the natural thermoluminescence
of fossil shells Am. Mineral. 52 1297
117 Nambi K S V and Mitra S 1978 Thermoluminescence investigations of old carbonate sedimentary
rocks Neues Jahrb. Mineral. Abh. 133 210
118 Wintle AG 1978 A thermoluminescence dating study of some quaternary calcite: potential and
problems Can. J. Earth Sci. 15 1977
119 Zeller E J and Ronca L B 1963 Reversible and irreversible thermal effects on TL in limestone
Earth Science and Meteorites compiled by J Geiss and E D Goldberg (Amsterdam: North-
Holland) p 281
(c) Loess, glacial till, ocean sediments
120 Hiitt G, Smirnov A and Tale I 1978 The application of thermoluminescence of natural quartz to
the study of geochronology of sedimentary deposits PACT J. 2/3 363
121 Wintle A G and Huntley D J 1978 TL dating of sediments PACT J. 2/3 374
122 Wintle A G and Huntley D J 1979 Thermoluminescence dating of deep-sea sediment core Nature
279 710
360 GA Wagner
Extraterrestrial applications
123 Brito U, Lalou C, Valladas G, Ceva T and Visocekas R 1973 Thermoluminescence of lunar fines
(Apollo 12, 14 and 15) and lunar rock Geochim. Cosmochim. Acta 3 (Suppl. 4) 2453
124 Crozaz G, Walker R and Zimmerman D 1973 Fossil track and thermoluminescent studies of Luna
20 material Geochim. Cosmochim. Acta 37 825
125 Durrani S A 1971 Thermoluminescence in meteorites and tektites Mod. Geol. 2 247
126 Durrani S A 1977 Temperature and duration of the shadow of a recently-arrived lunar boulder
Nature 266 411
127 Houtermans F G and Liener A 1966 Thermoluminescence of meteorites J. Geophys. Res. 71
3387
128 Liener A and Geiss J 1968 Thermoluminescence measurements on chondritic meteorites, in
Thermoluminescence of Geological Materials ed D J McDougall (New York: Academic Press)
p559
129 McKeever S W S and Sears D W 1978 Thermoluminescence and terrestrial age of the Estacado
Meteorite Nature 275 629
130 McKeever S W S and Sears D W 1979 Meteorites and thermoluminescence Metecritics 14 29
131 Melcher C L and Sears D W 1979 Thermal stability of thermoluminescence in chondrites
Meteoritics 14 249
132 Sears D W 1978 The dating of meteorites PACT J. 2/3 231
133 Vaz J E and Sears D W 1977 Artificially-induced thermoluminescence gradients in stony
meteorites Meteoritics 12 47
Applied Thermoluminescence Dosimetry. Eds M Oberhofer and A Scharmann
1981 ECSC, EEC, EAEC. Brussels and Luxembourg
19
TL dating: techniques and problems
M J AITKEN
19.1. Introduction
The basic notion of TL dating is that the firing of pottery by ancient man resets the
'TL clock' to zero and that, during the subsequent centuries, the trapped electron popula-
tion builds up at a uniform rate due to the weak flux of ionising radiation provided by
radioactive impurities (a few parts per million of uranium, thorium and potassium-40)
in the clay itself and in soil in which the pottery was buried after the archaeological site
fell into disuse. Suitable apparatus for detecting the consequent 'natural' TL is shown in
figure 19.1. Because the minerals in pottery have a rather low TL sensitivity, and because
the accumulated exposure during antiquity is only of the order of a thousand roentgen,
the natural TL is usually rather dim. Not only is a fast heating rate required, together with
a high-sensitivity low-noise photomultiplier (e.g. EMI Type 9635) and a solid angle of
light collection approaching 7r steradians, but also it is important to have severe
discrimination against thermal radiation by means of carefully selected colour filters
and to suppress any non-radiation-induced TL. This latter, usually referred to as 'spurious'
TL, is a surface effect induced during sample preparation; for most samples it is
adequately suppressed by making the measurement in an atmosphere of dry oxygen-free
nitrogen or argon.
Sample
Heater curreni of = 100A to give
healing rale of 20 C per second
Figure 19.1. Apparatus for TL dating measurement.
362 M J Aitken
The 'glow curve' for natural TL a typical one is shown in the top right-hand corner
of figure 19.1 - has no TL below about 250C. This is because the traps which are
emptied below that temperature are too shallow to retain their electrons without serious
loss during the centuries of burial. For dating purposes, we are concerned with the TL
emitted above 350 C; in practice, the useful range does not usually extend beyond
450 C because above that temperature thermal radiation becomes excessive despite
colour discrimination, and in any case the TL intensity usually falls off due to increased
thermal quenching (de-excitation of the luminescent centre by emission of a phonon
instead of a photon). For a single trapping level, the glow curve would be a single peak
about 50 C wide; that of figure 19.2 is evidently composed of a number of overlapping
peaks and it is to be inferred that there are several types of trap present, either within the
same mineral or in several different minerals. The presence of several types of trap has the
advantage that it permits the 'plateau test' (see figure 19.2) to be used to check whether
the traps associated with a given temperature range are deep enough for stable retention
of electrons during antiquity. Further reading about the technique will be found in the
references and in particular chapter 3 of reference [1].
50
c 30-
10
500
- 1000
- 500-
200 300 400 500
Temperature (C)
Figure 19.2. The plateau test. The upper part shows the glow curves corresponding to the
natural TL and to the artificial TL following 1000 rad of beta irradiation. The lower part
shows the equivalent dose, which here is taken to be equal to
natural TL
artificial TL
X 1000 rad
as function of temperature. The onset of the plateau is indicative that a sufficiently high
glow curve temperature has been reached for the TL to be associated with traps that are
deep enough to retain their electrons with negligible leakage during archaeological times.
The onset of the plateau is usually around 350C.
TL dating: techniques and problems 363
19.1.1. The age relation
In its simplest form, this is
natural TL
age = . (19.1)
(TL per unit dose) x (dose per year)
TL per unit dose is the sensitivity of the sample for acquiring TL; it is measured by
exposing the sample to a known dose of nuclear radiation from an artificial radio-isotope
source. The resulting glow curve is referred to as 'artificial TL' . Dose per year (D) is
evaluated from radioactive and chemical analysis of the sample and its surrounding soil.
The natural dosage received by the pottery (see table 19.1) is a mixture of alpha, beta
and gamma radiation plus a contribution of a few per cent from cosmic rays. On account
of the high ionisation density, they produce alpha particles substantially less efficient
than beta particles and gamma rays. Hence it is necessary to rewrite (19.1) in the form
C M
t = : ^. (19.2)
Xafla + XpCD/J + Ay+A: )
where t is the age in years, G
N
is the natural TL, Xa
an
d Xp
a r e TL
P
er r a
d fo
r
alpha and
beta particles respectively, and D
a
, Dp, D
y
and D
c
are the respective annual dose rates
for alpha, beta, gamma and cosmic radiation.
Experimentally, it is convenient to define
* = Xalxp
and denoting the equivalent dose by
Dp = GN/X/3
Table 19.1. Component dose ratef for typical pottery and soil.
Effective
a p 7 Total total*
191
190
177
558
f Dose rates are given in milliiads per year and correspond to pottery and soil having 2.8 ppm of
uranium, 10 ppm of thorium and 2% potassium (measured as K, 0). The corresponding alpha count
rate would be 10 per kilosecond for a thick sample of area 13.8 cm
2
and a counting efficiency of 85%;
the uranium and thorium contributions to the count rate would be approximately equal.
% Assuming = 0.15.
Thorium-232 series:
Radio-isotopes before thoron
Thoron and later products
Uranium-238 series:
Radio-isotopes before radon
Radon and later products
Potassium-40
Totals
Effective dose rates
X}
Sj
-
1517
227
(41%)
i EH SJ)
sH 4
s
"
136.4 41
206 124
206 124
(37%) ' (22%)
818
852
177
1848
-
364 M J Aitken
we have
t= ^-
E
. - . (19.3)
kD
a
+D
B
+D
y
+D
c
So far it has been assumed that the acquisition of TL is linear with dose and that, as is
implicit in the caption to figure 19.2, there is no change of TL sensitivity when the sample
is heated to 500 C in the course of measuring the natural TL. For most samples these
assumptions are upset by two effects, supralinearity and sensitisation, which will be
discussed in 19.3.
19.1.2. Sample preparation
For accurate dating, the technique of sample preparation is intrinsic to the principles on
which the age is calculated. This is because of the heterogeneous nature of pottery fabric
it is a baked clay matrix in which there are mineral inclusions, sometimes ranging up
to a millimetre in diameter. These inclusions, usually of quartz or feldspar, were either
present in the raw clay or were added by the potter in order to improve refractory
qualities. The TL sensitivity of these inclusions is much higher than that of the clay
matrix but in general (potassium feldspars and zircons are notable exceptions) the
radioactive impurities are carried in the matrix. The average range of the alpha particles
from uranium and thorium, which provide a substantial part of the natural radiation
dosage, is only about 25 fun and as a consequence the average dose received by an
inclusion decreases with size once its diameter exceeds a few microns. Since the grain-
size distribution varies between fragments, for accurate results it is necessary to separate
out grains of a given size range and to use these for measurement of both natural and
artificial TL.
19.1.2.1. Fine-grain technique. There are two basic approaches. In the fine-grain
technique developed by Zimmerman [2], the material extracted consists of grains that are
small enough for the attenuation of the alpha dosage to be negligible. The pottery frag-
ment is crushed by slowly squeezing in a vice; grains in the size range 1-8 /im are
separated in acetone and utilising the fact that the settling time is determined by the
diameter. After separation, the selected grains are resuspended in acetone and deposited
on aluminium discs (usually 10 mm in diameter and 0.5 mm thick) in a thin layer of a
few microns. About a dozen such discs are prepared from each sample and if all goes well
the TL reproducibility is about 5%.
19.1.2.2. Quartz inclusion technique. In the quartz inclusion technique developed by
Fleming [3], the grains selected are large enough for there to be severe attenuation of the
alpha dosage, but not so large that there is serious attenuation of the beta dosage. By
etching these grains in hydrofluoric acid, the outer skin that has received alpha dosage
is removed and in evaluating the age is put equal to zero. The size range of the grains is
usually 90-150 /nm, a small correction being made for the attenuation of the beta dosage.
Weighed portions of these grains (typically 5 to 10 mg) form the samples on which the
TL measurements are made.
TL dating: techniques and problems 365
As just indicated, the quartz technique is based on the assumption that the grains are
devoid of radioactivity. However, recent measurements by Sutton and Zimmerman [4]
indicate that in some grains there is a small but just significant content of uranium.
Another recent quartz investigation, by Bell and Zimmerman [5] using an electron micro-
scope, categorises grains into 'shiny' and 'frosty'. With the latter, the etching by
hydrofluoric acid proceeds in an irregular way that does not correspond to the orderly
removal of the outer skin assumed above. In passing, one may note two other recent
publications connected with quartz. In dating the sandy clay of the burnt floor and walls
of a kiln, Valladas [6] found it possible to eliminate intrusive unheated grains by virtue
of their lower magnetic susceptibility the heated grains were presumed to have acquired
iron impurity from the clay matrix during firing. Courtois et al [7] in dating Amazonian
pottery noted a parasitic TL component that they ascribed to the deliberate addition of
siliceous wood by the potter.
19.2. Application
19.2.1. Archaeological dating
Had radiocarbon dating not been well established, thermoluminescence would have had
the task of establishing the chronological framework of prehistoric archaeology. Leaving
until later the question of TL potentiality prior to the 50 000 year limit of radiocarbon's
range, let us consider what TL has to offer in a complementary role [5]. First and fore-
most, it gives a direct date for an object of archaeological significance. The changing
technique and style of pottery often form the basis of archaeological chronology, whereas
the association of a radiocarbon sample with an archaeological phase may be open to
question. Also, the event dated by TL is the actual firing of the pottery whereas in the
case of radiocarbon dating of wood or charcoal the event may be several centuries earlier
than the archaeological association. Secondly, there are some sites prolific in pottery on
which suitable radiocarbon samples do not occur.
The accuracy obtainable with TL in good circumstances is at present somewhat better
than 10% of the age. It is unlikely that it will ever be improved beyond 5% because
the stored information in the pottery is not recorded to any better accuracy for
instance, owing to uncertainty about the average water content during burial (which
affects the dose rate). This is somewhat poorer than is usually quoted for radiocarbon
though for some periods it is no worse than indicated by a realistic assessment of
accuracy having regard to the short-term fluctuations discussed in 19.4.
The 'good circumstances' required for high TL accuracy refer on the one hand to
pottery having satisfactory TL characteristics and on the other to whether or not the actual
burial situation permits a reliable estimate of the gamma dose rate. The latter is
determined by the soil or rock within 0.3 m of the sample and unless the surround is
homogeneous it is difficult to make a reliable estimate. These considerations mean that
samples should be collected specifically with TL dating in mind and preferably by the
TL specialist who in any case should visit the site either to bury TLD capsules or to
make measurements with a scintillation spectrometer. Table 19.2 lists typical collection
requirements. Pottery may display unsatisfactory TL characteristics in a variety of ways.
366 MJAitken
Table 19.2. Notes on collection of potsherds for TL dating.
The sherds
1 Number: For each level we need a set of between 6 and 12 sherds.
2 Size: At least 6 mm thick, at least 30 mm across. Bigger sherds are preferred.
3 Type: We like a variety of fabric types, if available. Surface decoration or glaze does not
matter.
4 Context:
(i) Only sherds that have been buried to a depth of 30 cm (1 ft) or more for at least
two-thirds of their burial time are acceptable. This means that pits and ditches
that have been filled up fairly quickly (either by silting or by ancient man) are
ideal sources.
(ii) The sherds should be at least 30 cm from any boundary (e.g. edge of pit, change
of soil type, wall, floor rock surface),
(iii) The best situation is one of sparsely occurring sherds in a uniform soil which is
relatively free of other materials (e.g. rock, building debris, shell or bone). A small
scatter of stone does not matter as long as none of the sherds selected were close
against a large one; the bigger the stone the more serious will be the effect.
Treatment
5 Avoid prolonged exposure to direct sunlight. (With flint samples try and avoid any
exposure to sunlight at all, and put them in an opaque bag.)
6 Avoid excessive heating of the sherds. Their temperature should not exceed the boiling
point of water (100C, 212F).
7 Avoid exposure to ultraviolet, infrared, x-rays, beta-rays or gamma-rays.
8 (a) The sherds should not be washed but put directly in a plastic bag plus any lumps
of earth attached, within a few minutes of removal from the soil and tied up
tightly. This bag should be put inside a second outer plastic bag, which should also
be tied tightly. This will allow us to measure the water content of the sherds as
found in the ground. (The procedure is not necessary for flint samples.)
(b) If washing is necessary to confirm the identity of the sherds, then this consideration
should take priority. However, if the sherds have to be washed, then detergents or
other additives must not be used for washing. Do not bother to dry the sherds.
Please tell use whether or not washing has been done.
9 We require a small handful of soil that is typical of that in which the sherds are buried.
The soil should be tightly double-bagged as for the sherds.
10 Exposure of the soil to sunlight, ultraviolet, etc, does NOT matter.
11 We require also a sample of each type of material occurring in large proportions within
30 cm of the sherd. In the case of a scatter of small stones in the soil, these should be
included in the soil sample in correct proportion.
General
12 Please, above all, avoid sherds whose inclusion in a set is in any way doubtful. The
method gives the date at which the pot was made; consequently we do not want residual
pottery from earlier periods. A sherd which has been burnt at some later period is of no
use because the date obtained may be intermediate between the firing and the burning.
13 Information about burial conditions is essential; this should include a sketch section of
the context (and, if possible, photographs) showing very roughly the points from which
the sherds were taken and the deposits for at least 30 cm around.
TL dating: techniques and problems 367
Table 19.2-Continued
14 Please try and give a rough estimate of how the average water content of the soil relates
to that of the sample supplied. It is also useful to know how the water content of the
soil varies between contexts and with respect to surface conditions (e.g. 'though bone
dry at the surface in these hot climatic conditions, by a depth of 2 m the soil was pretty
well saturated'). Obviously it is also important to know if the water table is (or has
been) anywhere near to the contexts concerned. If there is any seasonal or long-term
information about variations in rainfall, we would like to know it.
15 The sherds are destroyed in the course of measurement.
Acceptance of samples (by Oxford Research Laboratory for Archaeology)
16 The present policy is to undertake a limited number of specific projects rather than to
accept samples on a piecemeal basis. Primary considerations are:
(i) whether the present accuracy (between 5% and 10% of the age) is good enough
for the problem concerned,
(ii) suitability of site and material, for the technique,
(iii) archaeological importance, and
(iv) lack of, or ambiguity in, other dating evidence.
17 Since some types of clay do not have suitable TL characteristics, it is a good idea to send
a variety of samples for preliminary testing before going to the trouble of proper
collection. These test samples do not need burial soil, nor do they need to fulfil the
collection requirements; they are needed solely as examples of the types of fabric
available on the site.
The TL may be too dim, the growth with dose may be unmanageably non-linear, it may
exhibit anomalous fading (see 19.3) despite passing the plateau test, or it may be largely
composed of spurious TL. For one reason or another, a substantial proportion of
archaeological sites cannot be dated by TL.
What are possible materials for TL dating prior to the 50 000 year limit of radio-
carbon? Baked clay in the form of pottery does not extend beyond about 10 000 years
ago, though occasionally earlier in the form of figurines: in Czechoslovakia, for instance,
there are baked clay fragments which have been TL dated by Zimmerman and Huxtable
[8]. However, fire was used by ancient man as a means of cracking flint for use in tools
and weapons, and some such flints are sufficiently heated for use in dating [9-11].
Heated stones associated with fireplaces are another possibility [12].
All discussion so far has been concerned with samples that have been heated. There is
also the possibility that deposited carbonate (e.g. stalagmites and travertine associated
with cave dwelling) can be dated by TL. The vital question is whether or not the crystals
start off with a trapped electron population of zero on formation. Besides this, with semi-
transparent materials such as flint and calcite there is the possibility that ambient light
has induced a significant TL signal in the sample; exposure to light can be controlled
during excavation and in the laboratory but not during antiquity. Promising TL measure-
ments have been made on Foraminifera from ocean cores and extension to shells
associated with human habitation, although beset with problems, would be a very
worthwhile development.
368 MJAitken
19.2.2. Recent geology
The carbonate materials just mentioned are more directly relevant to Quaternary geology
than to archaeology. In this context, the obvious material for TL dating would seem to be
volcanic lava and, in particular, lava carrying reversed magnetisation such as the Laschamp
flow in the French Chaine-des-Puys [13]. Unfortunately, it seems to be a fairly general
rule that the feldspar minerals carried in volcanic lava suffer from anomalous fading.
This phenomenon does not appear to afflict quartz (or calcite), but unfortunately the
amount of quartz in lava flows of interest is rather meagre. However, when clay or rock
having satisfactory TL characteristics has been heated by the lava flow, there is a
possibility of obtaining a date indirectly.
19.2.3. Authenticity testing
It is here that TL has had as revolutionary an impact as that of radiocarbon in
archaeology. For testing authenticity it is usually a question of deciding between an age
of less than a century and one of upwards of a thousand. Uncertainty about gamma
dose rate is then unimportant and it does not matter that the 'burial circumstances' are
unknown. The result of a TL test may alter the value of an object from an astronomical
figure to a negligible amount. Consequently, although the answer does not need to be
accurate, it does need to be reliable and so tests need to be conducted with meticulous
care. Reputable art dealers have doubtful pieces tested as a matter of routine, the usual
fee for such a service being 50-100. A sample of about 50 mg is sufficient in most
cases and this is obtained by drilling a small hole in an unobtrusive location.
There are some styles of ceramic ware for which art historians have had doubts as a
whole, and application of TL in some such cases has led to agonising reappraisals. It has
had academic impact in the sense that previously the art historian may have been
studying the forger's view of man's cultural and artistic development rather than
actuality. An example [14] of this is the so-called Hacilar ware anthropomorphic vessels
and figurines said to be 7000 years old and to have come from the renowned site of that
name in south-west Turkey. Because their supposed origin was from a cultural phase
following soon after the first appearance of pottery in that part of the world, the fineness
of technique and beauty of form attracted particular interest. Of the seven most
important pieces tested the magnificent double-spouted vessels, each spout being in the
form of a head with obsidian eyes only one was found to be genuine. Out of a total of
66 pieces tested there were 48 modern forgeries. In another application to Chinese
Hui Hsien ware there were no genuine examples among the pieces available for testing.
Can a modern forgery be irradiated so that it will exhibit TL appropriate to a genuine
object? An inexperienced operator could well be misled by even a clumsy attempt.
To do the job properly, the forger would need to employ a physicist having some training
in TL and with appropriate experimental facilities available. Even then it is difficult to see
how artificial irradiation could fool a technique such as zircon dating (see 19.3). On
account of their high uranium content, zircons carry a very much higher equivalent dose
than other constituent minerals in pottery and it is not possible to achieve this situation
by external irradiation. Another possibility is by reconstitution, i.e. the fake object is
made from ground-up ancient brick by means of some chemical cementing agent. If no
heat is used in the process, then the TL age will be that corresponding to the ancient
TL dating: techniques and problems 369
brick. Of course, there is much more to it than this; it is likely that the chemical agent will
reveal itself by excessive spurious TL and in any case there are other techniques that can
be applied, e.g. thermogravimetric analysis and archaeomagnetism.
19.3. Recent research and outstanding problems
19.3.1. Supralinearity and sensitisation
Evaluation of TL sensitivity as indicated in figure 19.2 by measurements made on a
sample from which the natural TL has been drained in the course of the first glow curve
is not, in general, a valid procedure. A substantial change in sensitivity may occur when a
sample is heated; part may be due to changed transparency and reflectivity and part may
be due to the radiation dose that the sample has received previous to heating, the latter
being referred to as the pre-dose effect. Whatever the details of the mechanisms involved,
this sensitisation between 'first glow' and 'second glow' presents a very serious complica-
tion in TL dating. The effect itself can be circumvented by using the additive method of
equivalent dose evaluation (see figure 19.3). This has the procedural disadvantage of
500 1000
Addilive dose (rads)
1500
Figure 19.3. Additive method of evaluating equivalent dose (ED). Of three equal samples,
the first is used to measure N, the natural TL, the second to measure (N + 10), the natural
plus artificial TL after a dose of p rad, and the third (N + 2/3); in the above, 0 = 700. The
supralinearity correction A is determined by means of a growth curve such as figure 19.4
using samples from which N has been removed. The sum of ED and A equals AD, the
archaeological dose.
requiring precise interrelation of the TL from different portions and the more serious
objection that, although the additive method checks for linearity in the acquisition of
TL in the dose region above the level of the natural dose, it can say nothing about
linearity at lower levels of dose. In fact, a common characteristic of many TL minerals
(and of some artificial phosphors, lithium fluoride for example) is a lower sensitivity
during the first few hundred rads of dosage than subsequently; this supralinearity is
illustrated in figure 19.4.
An empirical way of correcting for supralinearity is to use already glowed portions
to determine the second-glow growth characteristic, and to assume that despite a change
370
600
700
300 400 500
Radiation dose (rad)
Figure 19.4. Typical supralineai dependence of TL on radiation dose for pottery samples
irradiated with beta or gamma radiation. The degree of supralinearity is measured by the
intercept A.
in sensitivity on heating there is no change in the intercept A. The justification for this
procedure is that it gives improved agreement in tests with known age samples. It must be
admitted that it is a rather bland assumption and indeed with some samples a pre-dose
effect shows itself in the supralinearity [15, 16]. Studies of the supralinearity character-
istics of individual minerals are only of help as a general guide because the quantitative
behaviour depends on the annealing conditions that the particular sample has
experienced. Also, in the fine-grain technique, one is dealing with a mixture of minerals
of unknown identity. An advantage of the quartz inclusion technique is that if attention
is restricted to the 'benign' peak at 375 C, the sensitivity change on heating is often less
than 5%, giving grounds for belief that the supralinearity intercept will be free from pre-
dose effects too. Unfortunately, the 'malign' 325 C peak commonly dominates the
TL from quartz.
It is not difficult to suggest mechanisms that might give rise to supralinearity and pre-
dose effects though far from easy to establish which is operative in any particular
mineral. The simplest explanation is that additional traps are being created in the early
stages of the irradiation, thereby increasing the sensitivity. An alternative is the
'competition model' in which it is assumed that there is a second set of traps (which do
not give rise to TL) competing for electrons. These are assumed to saturate earlier than
the TL traps and so, as the competing traps gradually approach saturation, the
competition is suppressed and more electrons are available for the TL traps. Another
explanation is in terms of an enhancement in the probability that an electron freed from
a trap will produce luminescence such enhancement could arise because of an increase
with dose of the number of activated luminescent centres, for instance.
With increasing application to Palaeolithic samples, low-dose non-linearity becomes
unimportant but allowance for the effect of approaching saturation becomes critical.
Failure to make sufficient allowance can lead to substantial overestimate of age. There is
not much work to hand on the question of whether in this dose region any reliance can
TL dating: techniques and problems 371
be placed on the second-glow growth characteristic, and non-linearity in the additive
first-glow growth characteristic is an insensitive indicator of approaching saturation. The
situation is further complicated by the likelihood that, at these high dose levels, trap
creation becomes important so that the TL growth characteristic continues to rise beyond
the level corresponding to saturation of existing traps.
19.3.2. Pre-dose dating
In the case of the 110 C peak in quartz the pre-dose effect is so strong that it is the basis
of an accurate dating technique particularly applicable to samples of the last thousand
years [17, 18]. There is no sensitisation until the sample has been heated to 400-500 C
and detailed investigation by Zimmerman [19] has established a model (see figure 19.5)
in which the essential mechanism is thermal transfer of holes from 'reservoir' traps to
luminescent centres (which are thereby activated). This is the only well established model
that we have in TL dating at present.
This 110 C peak is not present in the natural TL, its half-life being only about 2 h.
It is, however, a highly sensitive peak, and exposure to a dose (the test dose) of around
1-10 rad is usually sufficient to induce an accurately measurable TL. The increase in
sensitivity (as indicated by the response to the test dose) consequent on briefly heating
the sample to 400 or 500 C is proportional to the total radiation dose (the pre-dose)
that the sample has received subsequent to its firing in antiquity. Thus although the traps
responsible for the 110C peak carry an insignificant number of electrons, there is
nevertheless a memory of the radiation dose that has been received, a memory that is
unlocked by the brief heating to 400 or 500 C (such as the sample experiences in the
course of a normal glow curve).
The sequence of measurements is essentially as follows:
(i) Give test dose and measure response, S
0
.
(ii) Heat to 500 C (the activating temperature),
(hi) Give test dose and measure response, S^.
(iv) Give laboratory calibrating dose, LD (usually several hundred rads).
(iv)(a) Give test dose and measure S^.
(v) Heat to 500 C.
(vi) Give test dose and measure response, 5
N+( 3
.
Since (5
N
S
0
) is proportional to the dose received during antiquity, AD, and
( 5N
+J 3
5N) is proportional to LD, we have
Jw Sn
AD =
7
xLD. (19.4)
It is of course necessary to check, for each sample, that the proportionality of the
sensitivity increase to dose is valid for the range of dose concerned. The effect usually
saturates in the region of 500 rad.
The pre-dose phenomenon can usually be observed in any fine-grain or whole-grain
sample containing quartz, but for accurate results it is best to extract the quartz as in the
inclusion technique though it is important to omit the etching with hydrofluoric acid
372 MJAitken
since for some reason this upsets the pre-dose behaviour. For a 10 mg sample of separated
quartz, a typical sensitivity change is in the range 2-20% per rad of pre-dose and so an
equivalent dose of as little as 10 rad can be measured accurately. Not all pottery contains
quartz with satisfactory pre-dose characteristics, but when the technique is applicable
it is a very powerful method, particularly for authenticity testing. It can often give an
answer in cases when the conventional method is inapplicable because of too low TL
intensity in the high-temperature region of the glow curve or because it is upset by
spurious TL or held in doubt because of the possibility that abnormal fading or reheating
has occurred.
From studies of the associated radioluminescence, exoelectron emission and the effect
of ultraviolet irradiation, Zimmerman [19] has established that the sensitivity enhance-
ment is due to an increased availability of charged luminescence centres and has proposed
the model shown in figure 19.5. In this T
t
and T
2
are electron traps and L and K are hole
traps. Ti is the shallow trap which, with the luminescent centre L, is responsible for the
110C TL peak. Trap T
2
is presumed to be deep enough not to be emptied by heating
to 500 C and it is introduced into the model so that charge balance can be maintained.
The TL process consists of the thermal release of electrons from the traps T
t
and the
capture of some of these into the luminescent centres L. Such capture only occurs for
centres which are charged with a hole and so the TL sensitivity is proportional to the
number of centres which are so charged.
Conduction band
- O-
-o-
R
Figure 19.5. Energy-level model for the pre-dose
effect. (After Zimmerman [19].)
' Valence band
Firing of the pottery in antiquity is hypothesised to empty nearly all traps and
consequently the sensitivity S
0
after firing is low. Subsequently, the natural radiation
dose rate produces electrons in the conduction band and holes in the valence band; the
electrons are trapped in T
2
(because T
x
is too shallow to retain them) and the holes are
captured at K (rather than L because of the former's presumed higher capture cross
section). Thus during antiquity the hole population in K gradually builds up.
In step (i) of the pre-dose procedure, the test dose charges the traps T
t
with a small
number of electrons and puts a small number of holes into A". On heating through 100C
the electrons are released and those that find a charged luminescent centre give rise to
TL. Because there has been no change in the number of holes trapped at the centres of
TL dating: techniques and problems 373
type L, the observed sensitivity S
0
is the same as if the measurement had been made
immediately after firing.
The heating to 500 C in step (ii) causes thermal release of holes from K and these are
then captured at L (because any recaptured at K are immediately re-ejected). Hence, the
sensitivity S^ measured in step (iii) is proportional to the number of holes that had been
accumulated in K during antiquity.
19.3.3. Transfer dating
In the context of thermoluminescent dosimetry, it is well known that, with natural
calcium fluoride, electrons can be transferred from deep to shallow traps by illumination
with ultraviolet light. By observing the TL from the shallow traps only, a measure of the
deep-trap population can be obtained without heating the sample to the high temperature
that would be necessary for direct observation of its deep trap TL. Currently, the effect
in this and other phosphors is under development for ultraviolet dosimetry.
The effect has been studied in quartz by Schlesinger [20]; for instance, by means of
250-350 nm light, electrons can be transferred from a peak at about 500 K to peaks in
the range 150-300 K, the sample being held at liquid-nitrogen temperature. At that
author's suggestion, preliminary studies have been made by Bowman and Bailiff [21-24]
with a view to utilisation in dating. With the above discussion of non-linearity and pre-
dose difficulties in mind, there is obvious advantage in being able both to measure the
deep-trap population (by transfer) and to empty the deep traps (by prolonged bleaching)
without having to heat to 400 or 500 C, for heating is certainly responsible for some of
the sensitivity changes that occur between first glow and second glow. Of course, the
bleaching with ultraviolet may give rise to sensitivity changes for other reasons, but the
work of Bowman [22] suggests that with careful selection of wavelength this is not
necessarily so.
There are also advantages simply because the TL is observed at a lower temperature.
Interference by thermal radiation and spurious TL is avoided; this is particularly relevant
when the TL is green or of longer wavelength, as in the case of calcite, and it is difficult
to discriminate by means of colour filters. Also, thermal quenching of the luminescent
centres is less.
In principle, the technique gives greater selectivity of the traps from which electrons
are released and thus it may be possible to avoid traps having malign properties such as
anomalous fading.
19.3.4. Anomalous fading
The expected lifetime of an electron in a trap of depth E and frequency factor s is
given by
T
- -i
s'
1
exp(E/kT) (19.5)
where k is Boltzmann's constant and T is the storage temperature.
Determinations of E and x by means of kinetic studies lead to lifetimes that are of the
order of a million years or more for peaks occurring at glow-curve temperatures of 350 C
or higher. However, grossly anomalous behaviour has been observed by Wintle [25] in
374 MJAitken
the behaviour of feldspar minerals. For volcanic lavas of known age, the observed TL
was significantly too low sometimes by an order of magnitude, although the expected
ages were no greater than 50 000 years and the TL utilised was in the 400-500 C region
of the glow curve.
The results of short-term stability tests were more anomalous still: losses of 10-40%
of the 350-500 C TL in periods varying between a few hours and a few
days were observed for some samples of sanidine, fluorapatite, labradorite, andesine,
zircon and bytownite. Not all samples of these minerals showed the effect, and for quartz
and calcite the fading was insignificant over months of storage. The phenomenon has also
been observed in lunar samples and it has been suggested by Garlick and Robinson [26]
that it is due to the subsidiary escape of electrons from traps due to overlap of
wavefunctions a wave-mechanical 'tunnelling' process.
Apart from their discouraging implications for geological lava dating, these
observations call into question the basic validity of pottery dating using fine-grain samples
or other forms of sample in which there is a substantial contribution from feldspar
minerals (unfortunately the TL from feldspars is in general much brighter than that from
quartz). However, the satisfactory results obtained with samples of known age indicate
that this behaviour is not common among the mineral constituents of pottery. Also, the
short-term stability tests that are now made routinely on fine-grain samples show that
for most sites it is only the occasional sample which exhibits measurable loss (5-10%)
for a storage period of up to a month. However, there are some sites for which the
majority of samples are afflicted [27, 28].
The rate of percentage loss is initially rapid [29], getting progressively slower as the
time elapsed since irradiation increases. To account for the initial rapid loss in terms of
equation (19.5) (and to explain the observation that there is substantial fading even for
storage at 77 K) requires "~0. 5eV and x~10
3
s
_ 1
, and it is difficult to accept the
thermal release model on which (19.5) is based as valid for such values. The tunnelling
explanation [29] is more credible, and in terms of this the progressive slowing down of
the fading is seen as the using up of nearby centres, tunnelling to these being much more
probable than to distant ones. From the dating point of view, the crucial questions are,
first, whether for a sample which shows no anomalous fading over a period of months
it can be reliably assumed that there has been none over thousands of years and,
secondly, whether study of short-term fading can be used to make a quantitative estimate
of long-term fading. Comparison with radiocarbon can give some degree of answer to the
first question. But beyond the limit of radiocarbon, in the middle and lower Palaeolithic
ages where there is most need for TL, the only empirical approach is through
intercomparison of TL dates obtained on different materials if there is fading, the
amount is likely to be different. However, until satisfactory calcite dating is achieved, the
only generally available material is burnt flint (and that is rather sparse). Although short-
term tests and comparisons with radiocarbon may give no indication of fading in flint,
the utilisation [10] of this material in dating sites that are approaching an order of
magnitude older than the limit of radiocarbon raises the question as to whether the
tunnelling probability can indeed be sufficiently low, and gives emphasis to the need for
a quantitative understanding of the process.
An experimental study by Zimmerman [30], following the work of Wintle [29]
suggests that there is a correlation between anomalous fading and the short-term delayed
TL dating: techniques and problems 375
luminescence that follows irradiation; this may provide a much needed tool for
investigating the affliction.
Although the tunnelling process is only weakly dependent on temperature, the deeper
the trap the lower should be the probability. Hence there should be advantage in utilising
traps beyond the usual 500 C limit of the TL glow curve. Access to these is possible by
means of the ultraviolet transfer technique and Bailiff [23] has obtained encouraging
indications that anomalous fading can thereby be reduced and perhaps eliminated.
19.3.5. Trap depth determination
One of the most widely used methods for determination of trap depths is by study of the
temperature dependence of the TL during the initial rise of the glow curve peak. The
portion of glow curve used needs to be sufficiently below the peak temperature for there
to have been no significant emptying of the traps. The TL intensity is then proportional
to exp{E/kT}, and a plot of the logarithm of the intensity versus {kT)
_1
yields a
straight line of slope E. Using this method the mean lifetime for the 325 C peak in
quartz has been reported as 3000 years for geological alpha quartz [31] and as 200 years
for quartz extracted from Romano-British pottery [32]. Both of these values conflict
strongly with the observation that for this pottery sample the TL age based on the 325 C
peak is within a few per cent of the TL age based on the 375 C peak (for which the
predicted lifetime is 40 million years). There is even greater conflict with the observation
that for burnt sand having a radiocarbon age of 30 000 years the TL age based on the
lower peak is within 10% of that based on the upper one [32].
Investigation by Win tie [32] indicates that the reason for this discordance is that as the
glow-curve temperature increases, efficiency of the luminescent centres decreases because
of increasing de-excitation by emission of phonons rather than photons (i.e. thermal
quenching). Thus the TL intensity rises less rapidly than in the absence of the effect and
an erroneously low value of E is obtained. Study of the prompt luminescence confirmed
that the luminescence efficiency was in fact strongly temperature-dependent. Use of
alternative methods for determining trap depth (by isothermal decay and by peak shift
with heating rate) predicted a lifetime of about 30 million years, a value that is consistent
with the TL ages mentioned earlier.
For the 230 C peak in the archaeological quartz, the peak shift method predicted
40000 years instead of 2 years according to the initial rise method. For the 110C peak
in quartz and for the 275 C peak in calcite, thermal quenching effects are not significant;
the lifetime of the latter is calculated to be 100 million years from trap depth
measurements [33].
19.3.6. Influence of temperature of irradiation
For some phosphors, the TL peak-height response is slightly dependent on the tempera-
ture of irradiation [34]. For natural calcium fluorite and for CaS0
4
:Tm, the response is
lower by 5-10% if the irradiation is carried out at 100 C instead of 20 C; for LiF
(TLD 100) the response is about 10% higher and for CaF
2
: Mn it is the same to within 0.5%.
For fluorapatite and burnt limestone, the response was the same to within 5%, but for
the 325 C peak of an archaeological sample of quartz, the response was lower by 17%.
376 MJAitken
The possibility that the decreases were due to thermal untrapping of electrons was
excluded. In the case of the quartz sample, the effect was still present when the dose rate
was reduced by a factor of 3000 but it was absent for a saturating dose of 40 krad. A
possible explanation is that the effect is due to temperature dependence of the trapping
cross section. However, on the basis that alpha-particle tracks are microscopic regions of
TL saturation, this explanation is not consistent with the observation that the effect
occurs as strongly for alpha irradiation as for beta.
On the basis of the above results, the effect is not significant for dating. Additionally,
in one sample of archaeological quartz the effect was present in the 325 C peak but not
in the 365 C peak and it is the latter on which reliance is usually placed for dating. On
the other hand, Khazal et al [35] have reported a strong temperature dependence for the
375 C peak in a sample of natural quartz, though using a heavy dose of gamma radiation.
Relative to irradiation at room temperature, they found a response of x 0.65 at 0C,
of x 0.018 at - 25 C, of x 0.0054 at - 78 C and of x 0.0017 at - 95.4 C.
Strong temperature dependence has also been reported for the efficiency of ultraviolet
transfer in natural calcium fluorite [23, 36]. The efficiency is of the order of 50% greater
at 10 C than at room temperature, the effect getting stronger as the wavelength of
illuminating light is increased. It has been suggested that the effect is associated with one
or two excited levels of the donor trap, these levels lying a few tenths of an electronvolt
below the conduction band.
19.3.7. Assessment of dose rate
The established system for fine-grain dating is to use thick-source alpha counting for
evaluation of the uranium and thorium contributions and some form of chemical analysis
(e.g. flame photometry, x-ray fluorescence, atomic absorption) for the potassium. The
use of a disposable zinc sulphide screen remains supreme over other more sophisticated
techniques on account both of cheapness and of low background. Using the a-value
system [37], the conversion of the alpha count rate into effective alpha dose rate can be
made without knowledge of the stopping power of the sample or indeed of the decay
chain details. However, both of these are needed for evaluation of beta and gamma dose
rates and a reassessment of the energy release per parent nuclide disintegration has
recently been made by Bell [38, 39]. This reassessment is based on published nuclear data
tables and, owing to the complexity of the decay schemes, it is no mean task. The revised
values [39] for the alpha, beta and gamma contributions (in mrad per year per ppm by
weight of parent) are 73.8, 2.86 and 5.14 respectively for the thorium series, and 278,
14.6 and 11.5 for the uranium series. The beta and gamma dose rates from 1% of natural
K
2
0 are 68.2 and 20.5.
For quartz inclusion dating the preferred method of dose rate evaluation is by TLD
and, incidental to developing such a system for beta dose rate evaluation, Bailiff [23] has
made an experimental check of the value derived by Bell from the nuclear data tables;
there is agreement to within the 5% limit of experimental error. Other systems for dose
rate evaluation by TLD have been reported by Mejdahl [40-42] and by Aitken [43].
For some pottery and soils, the degree of escape of the radioactive gases
220
Rn and
2
"Rn is sufficient to affect the dose rates substantially. The earlier assumption that
such escape does not occur on wet sites has been shown [44] to be invalid. It has also
TL dating: techniques and problems
'O'ring seal
377
Highly polished
inner surface
Black wax seal
Sample tray
36 mm
Figure 19.6. Gas cell for evaluation of radon emanation.
been shown [45] that the established method of alpha counting in which the sample is
sealed in a container can give rise to a gross overestimate of the activity if there is
substantial radon emanation in the sample. A more satisfactory technique is to measure
the alpha activity with the sample unsealed and to evaluate the gas escape in a separate
experiment in which the sample is sealed in a gas cell (see figure 19.6) such that the only
particles which can reach the scintillator screen are from emanated radon. Confirmatory
checks that laboratory assessment does give a reliable indication of the situation during
burial can be made by radiochemical measurement of polonium-210; this is supported
by 21-year lead-210 which is subsequent to radon in the uranium decay chain.
19.3.8. Environmental uncertainties
However accurate the laboratory techniques and however well behaved the TL minerals,
there remain several environmental causes of uncertainties. One of these is the change of
radioactivity in a sample due to leaching or deposition by groundwater; in geology,
uranium is well known for its mobility. Another is the attenuation of the dose rate by
the water content of sample and soil. Pottery commonly has a saturation water content
of around 10%, and soil 20%. The average water content during burial depends on the
climatic history of the site and perhaps on water table variations, but even if these latter
are known they are not easily translated into water contents except when the site is
known to have been excessively wet or excessively dry throughout. Even in the former
case there remains doubt as to the extent to which water content affects the alpha
dose rate the pore structure of pottery is not necessarily fine enough for water to be
interposed in the path of the majority of the alpha-particle tracks.
Specifically with regard to gamma dose rate, it has to be assumed that the sample has
spent the major part of its burial time with the same surroundings as found by the
excavator. Quite apart from later erosion or other disturbance, there is sometimes doubt
as to how rapidly the sample became buried. There is also the question of how strictly the
collector has kept to the requirement of a homogeneous surround of soil to a distance of
378 MJAitken
0.3 m, a requirement that is often restrictive and irksome particularly if none of the
samples on a site fulfil it.
Hence there is strong reason to develop subtraction methods by which the gamma
dose rate is eliminated and at the same time to attempt to use impervious materials to
avoid uncertainty due to water content. With any subtraction technique, there is an
inevitable increase in the size of the error limits, and with most samples, until evaluation
of equivalent dose is more precise, what is gained on the swings is lost on the roundabouts.
However, for pottery samples in which the alpha particles contribute at least a third of
the fine-grain TL, Fleming and Stoneham [46,47] have demonstrated that dates accurate
to 12% can be obtained by subtracting the equivalent dose obtained with quartz
inclusions from the equivalent dose obtained with fine grains. This removes dependence
on beta and gamma dose rates and, besides allowing dating of pottery from burial
contexts which do not meet the usual requirements, it makes it possible to date objects
from museum shelves, as demonstrated by application to four Renaissance terracottas
[47]. However, besides the need for a strong alpha contribution, there is also the
requirement for a large enough sample (at least several cubic centimetres) to provide
sufficient quartz.
Several other subtraction methods have been proposed. Poupeau et al [12] suggest
that for dating heated rocks from ancient fireplaces it is feasible to eliminate the gamma
dose rate by using two rocks of very different radioactivity, one high and one low; also,
rocks have the advantage of low water content and low radon emanation. In application
[48] to the Palaeolithic site of Pincevent in France, the archaeological dose in quartz
grains in a piece of granite was found to be 5600 rad whereas that in pieces of sandstone
was very low (<0.2 ppm U, <0. 6 ppm Th, <0. 1% K
2
0). Its quartz was effectively acting
as a monitor of the environmental dose (gamma plus cosmic) so that the net dose
obtained by subtraction (5600 1500) arose from only the internal radioactivity of the
granite. In the 'quartz attenuation' technique proposed [49], but not yet demonstrated,
by Mejdahl and McKerrell, the net quantity utilised is the difference in dose between
inner and outer parts of large quartz grains (about 0.5 mm across) due to attenuation of
beta radiation. The same authors also propose quartz-feldspar subtraction which utilises
the difference in dose between large grains of potassium feldspar and large grains of
quartz due to the beta contribution from internal potassium in the feldspar. Anomalous
fading in the latter is likely to be a difficulty here.
There is complete elimination of the need to make direct measurement of any radio-
activity in the method DATE (difference d'attenuation temporelle des emissions)
proposed by Langouet et al [50]. In this the dose rate is evaluated by determining the
equivalent dose indicated by a TL peak having too short a lifetime for linear accumula-
tion. The ratio of this to the true equivalent dose (as indicated by a peak having a
sufficiently long lifetime) can be used as a measure of the dose rate as long as the
too-short lifetime is known. Effectively it is determined by measuring the equivalent dose
ratio for a series of similar samples of known age. The basis of this method is most easily
appreciated by recalling a simple version of it that was used by Johnson [51] in dating
contact-baked limestone. In this, the lifetime of the lower peak was short compared to
the age so that the peak was in thermal equilibrium at a level determined by
X
l
D = G
1
lr
1
(19.6)
TL dating: techniques and problems 379
where Xi is the TL per rad for this peak, G] is the observed peak-height, 7i is its lifetime,
and D is the dose rate.
For a higher peak of long lifetime,
X2Dt = G
2
(19.7)
where t is the age. Hence if T\ is known and the ratio X1/X2 determined by artificial
irradiation, t can be found. According to the preliminary results obtained by Langouet
et al, the 325 C peak in quartz has a sufficiently short lifetime for their purpose. This
conflicts with the earlier discussion in 19.3.5; presumably different types of quartz
are involved.
19.3.9. Zircon dating
Zircon grains carry such a high concentration of uranium (typically several hundred parts
per million) that the TL contribution from radioactivity in the pottery matrix in which
they are embedded, and from external gamma rays, is barely significant. This powerful
form of radioactive inclusion dating was first proposed by Zimmerman [52] and is under
development at the Laboratory for Space Physics of Washington University, St Louis,
Missouri, USA. Its validity for archaeological dating has been tested by Sutton and
Zimmerman [53] with zircons extracted from half-a-dozen pottery fragments of known
age and its utility in authenticity testing has been demonstrated by application to the
ceramic core of the famous bronze horse of the New York Metropolitan Museum of
Art [54].
In its original form, this technique involved measurement of TL sensitivity and alpha
dose rate as in conventional TL dating. Single grains were dated individually, alpha
radiation being used for sensitivity measurements and induced fission tracks for the
uranium and thorium content. However, although for some grains the age obtained was
correct, for others it was substantially too low. On investigation this was found to be due
to anticorrelation between TL sensitivity and radioactivity, the spatial distribution of the
former being mapped by means of cathodoluminescence and of the latter by means of
induced fission tracks. The TL sensitivity measured by artificial irradiation is dominated
by the regions of high sensitivity and since these are remote from the uranium and
thorium the value obtained is not relevant to age calculation. For obvious reasons the
mapping cannot be done until all TL measurements on a grain are complete and hence the
occurrence of zoning in a substantial proportion of grains means that there is a great deal
of wasted effort. To circumvent this, the so-called 'natural method' is being developed:
after measurement of the archaeological TL, GN, for a grain, or a group of grains, the
sample is stored for a time t' of the order of six months after which the re-accumulated
TL, GR, is measured again; the age t is given by
GN .
t = -rf. (19.8)
In concept the method could not be simpler but the experimental difficulties are severe.
Apart from the need for high detection sensitivity in order to obtain a statistically
meaningful number of counts, say a thousand, in the measurement of G
R
, it is vital to
eliminate spurious TL which without extreme precaution is liable to mask GR. Quite apart
380 M J Aitken
from measurement problems, there is the ever-present difficulty that some grains exhibit
anomalous fading. Nevertheless, zircon dating is potentially of high importance just
because it avoids uncertainties arising from water content and environmental radiation.
Also, in the natural method it avoids the assumption that TL sensitivity is independent of
dose rate.
In an attempt to reduce the storage time required for measurement of G
R
, Mobbs
[55] investigated the possibility of storage at liquid-nitrogen temperature so that lower-
temperature peaks, which are an order of magnitude more sensitive, could be utilised.
The regrowth of the higher-temperature 'dating' TL would then be inferred by measuring
the ratio of high-temperature TL to low-temperature TL following artificial irradiation.
Unfortunately, this ratio was found to be different from grain to grain and consequently
it seems likely that it will be different between different sensitivity zones within a grain,
in which case the approach is invalid.
References and further reading
1 Aitken M J 1974 Physics and Archaeology 2nd edn (Oxford: Clarendon Press)
2 Zimmerman D W 1971 Archaeometry 13 29-52
3 Fleming S J 1970 Archaeometry 12 135-46
4 Sutton S and Zimmerman D W 1978 Archaeometry 20 67-9
5 Bell W T and Zimmerman D W 1978 Archaeometry 20 63-6
6 Valladas H 1977 Archaeometry 19 88-95
7 Courtois L et al Proc. 5th Int. Conf. on Luminescence Dosimetry, Sao Paulo (Giessen:
I Physikalisches Institut of the Justus-Liebig Universitat) p 459
8 Zimmerman D W and Huxtable J 1971 Archaeometry 13 53-7
9 Goksu H Y, Fremlin J H, Irwin H T and Frysell R 1974 Science 183 651-4
10 Wintle A G and Aitken M J 1977 Archaeometry 19 111
11 Aitken M J and Wintle A G 1977 Archaeometry 19 100
12 Poupeau G, Sutton S, Walker R and Zimmerman D 1977 Thermoluminescent dating of heated
rocks 1976 Symp. on Archaeometry and Archaeological Prospection, Edinburgh ed H McKerrell
(London: Her Majesty's Stationery Office)
13 Gillot P Y, Valladas J, Laj C, Valladas G, Guerin G, Poupeau G and Delibrias G 1979 Earth Planet.
Sci. Lett. 42 444-50
14 Aitken M J, Moorey P R S and Ucko P J 1971 Archaeometry 13 89-141
15 Fleming S J 1975 Archaeometry 17 122-9
16 Bowman S GE 1975 Archaeometry 17 129-32
17 Flemings J 1973 Archaeometry 15 13-30
18 Aitken M J and Murray A S 1976 The pre-dose technique: radiation quenching 7976 Symp. on
Archaeometry and Archaeological Prospection, Edinburgh ed H McKerrell (London: Her Majesty's
Stationery Office)
19 Zimmerman J 1971 / . Phys. C: Solid St. Phys. 4 3265-76
20 Schlesinger M 1965 J. Phys. Chem. Solids 26 1761
21 Bailiff I K 1976 MSc Thesis Oxford University (unpublished)
22 Bowman S G E 1975 DPMI Thesis Oxford University (unpublished)
23 Bailiff I K 1976 Nature 264 531-3
24 Aitken M J, Bailiff I K, Bowman S G E and Mobbs S F 1976 The phototransfer technique in TL
dating 1976 Symp. on Archaeometry and Archaeological Prospection, Edinburgh ed H McKerrell
(London: Her Majesty's Stationery Office)
25 Wintle A G 1973 Nature 244 143-4
26 Garlick G F C and Robinson I 1972 in The Moon eds S K Runcorn and H Urey: International
Astronomy Union pp 324-9
27 Whittle E H and Arnaud J M 1975 Archaeometry 17 5-24
TL dating: techniques and problems 381
28 Whittle E H \915 Archaeometry 17 119-22
29 Wintle A G 1977 / . Lumin. 15 385-93
30 Zimmerman D \V 1977 Radiative recombination and anomalous fading 1977 Symp. on Archaeo-
metry and Archaeological Prospection, Philadelphia Abstracts, p 42
31 Aitken M J and Fleming S J 1972 Topics in Radiation Dosimetry, Supplement I, ed F H Attix
(New York: Academic Press) pp 1-78
32 Wintle A G 1975 Geophys. J. R. Astron. Soc. 41 107
33 Wintle A G 1976 Basic problems in TL dating the formation of calcite 1976 Symp. on Archaeo-
metry and Archaeological Prospection, Edinburgh ed H McKerrell (London: Her Majesty's
Stationery Office)
34 Aitken M J, Huxtable J, Wintle A G and Bowman S G E 1974 Proc. 4th Int. Conf. on
Luminescence Dosimetry, Krakow (Krakow: Institute of Nuclear Physics) p 1005
35 Khazal K A R, Hwang F S W and Durrani S A 1975 The effect of the temperature of irradiation
on the TL sensitivity of quartz 1975 Symp. on Archaeometry and Archaeological Prospection,
Oxford Abstracts, p 8
36 Sunta C M and Watanabe S 1977 Proc. 4th Int. Conf. on Luminescence Dosimetry, Krakow
(Krakow: Institute of Nuclear Physics)
37 Aitken M J and Bowman S G E 1975 Archaeometry 17 132
38 Bell W T 1976 Archaeometry 18 107
39 Bell W T 1977 Archaeometry 19 99
40 Mejdahl V \91Q Archaeometry 12 147-71
41 Mejdahl V 1972 Archaeometry 14 245-56
42 Mejdahl V 1972 Dosimetry techniques in thermoluminescent dating Danish Atomic Energy
Commission, Riso Rep. 261
43 Aitken M J 1969 Archaeometry 11 109-14
44 Desai V and Aitken M J 1974 Archaeometry 16 95
45 Desai V 1974 MSc Thesis Oxford University (unpublished)
46 Fleming S J and Stoneham D 1973 Archaeometry 15 229
47 Fleming S J and Stoneham D 1973 Archaeometry 15 239
48 Poupeau G, Sutton S, Walker R M and Zimmerman D W 1976 Thermoluminescent dating of fired
rocks: application to site of Pincevent Ninth Congr. Union Int. Sci. Prehist. Protohist., Nice in
press
49 Mejdahl V and McKerrell H 1976 Progress and problems with automated TL dating 1976 Symp.
on Archaeometry and Archaeological Prospection, Edinburgh ed H McKerrell (London: Her
Majesty's Stationery Office)
50 Langouet L, Roman A and Gonzales R 1976 Datation de poteries anciennes par la me'thode DATE
1976 Symp. on Archaeometry and Archaeological Prospection, Edinburgh ed H McKerrell
(London: Her Majesty's Stationery Office)
51 Johnson N 1965 / . Geophys. Res. 70 4653
52 Zimmerman D W 1971 Science 174 818
53 Sutton S and Zimmerman D W 1976 Archaeometry 18 125
54 Zimmerman D W, Yuhas M P and Meyers P 197'4 Archaeometry 16 19
55 Mobbs S F and Aitken M J 1977 Thermoluminescence and phototransfer at low temperatures
1977 Symp. on Archaeometry and Archaeological Prospection, Philadelphia Abstracts, p 41
56 Aitken M J 1977 Antiquity LI 11
57 Sanders H P 1973 Archaeometry 15 159
58 Morariu, V V, Bogdan M and Ardelean I 1977 Archaeometry 19 185
59 Aitken M J, Zimmerman D W, Fleming S J and Huxtable J 1970 Thermoluminescent dating of
pottery Proc. 12th Nobel Symp., Uppsala, August 1969, in I Olsson (ed) Radiocarbon Variations
and Absolute Chronology (Stockholm: Almqvist and Wiksell) pp 129-40
60 Bronson B and Han M C 1972 Antiquity XLVI 322-6
61 Caton Thompson G and Whittle E H 1975 Antiquity XLIX 89-97
62 Fagg B E B and Fleming S J 1970 Archaeometry 12 53-5
63 FlemingSJ 1971 British School at Athens Supplementary Volume No. 7, pp 343-4.
64 Fleming S J and Fagg B E B 1977 Archaeometry 19 86-87
65 Huxtable J, Aitken M J and Weber J C \912 Archaeometry 14 269-75
Applied Tliermoluminescence Dosimetry. Eds M Oberhofer and A Scharmann
1981 ECSC, EEC, EAEC, Brussels and Luxembourg
20
Application ofTL dosemeters in dose standardisation and
inter comparison
G SCARPA
20.1. Introduction
As is universally accepted for all physical quantities and units, radiation quantities and
units, such as exposure, kerma and absorbed dose, should be standardised on an inter-
national basis, which means that the methods and criteria for their instrumental and
theoretical evaluation should be the same all over the world.
The International Commission on Radiation Units and Measurements (ICRU) is
the institution charged with the task of formulating the recommendations on methods
for the establishment of radiation quantities and units under any practical conditions.
The advantages of such standardisation are obvious in all the fields of application of
radiation. Investigations in radiation therapy and radiation biology have demonstrated
that differences of 10% in absorbed dose can produce clearly observable variations in
biological response [1]. On the other hand, scientists carrying out studies on dose-effect
relationships must be able to repeat their experiments and to compare their results with
those of other centres. In radiation protection, health physicists have to comply with
national and international regulations. In industrial radiation processing also there are
strict rules on minimum and, sometimes, maximum doses.
The methods of achieving such a standardisation (or uniformity of evaluation) of
absorbed doses can be grouped into two classes:
(1) the indirect classical methods of 'dissemination of standards', and
(2) the direct intercomparison methods.
20.2. Dissemination of standards
The dissemination of standards is a very well established technique, developed mainly in
the UK [2] and based on the instrumental hierarchy illustrated in figure 20.1. Every
country should have:
(a) one national 'primary' standards laboratory, with primary standard dosemeters,
such as free-air chambers and graphite chambers;
(b) a limited number of 'secondary' standards dosimetry centres, with secondary
standard dosemeters, i.e. very stable and very well maintained dosemeters, which
are periodically checked with the national primary standards; and
(c) an unlimited number of so-called 'field' dosemeters, which are simply the instru-
ments used to carry out routine dosimetry in every institute; the field instruments
are periodically sent to secondary standard dosimetry centres and checked with the
secondary standard dosemeters.
384 G Scarpa
Country A
Primary
standard
Secondary
standard
periodica] checks
Secondary
standard
Country B
Primary
standard
Secondary
standard
Secondary
standard
Figure 20. 1. Diagrammatic illustration of instrumental hierarchy used in dissemination of
standards. F = field instrument.
The primary instruments belonging to different countries are periodically intercompared
by using special 'transfer' standards. In this way, indirectly, all the field dosemeters of all
countries should be kept at the same response level and, therefore, should measure doses
in a uniform way.
20,3. D irect intercomparison methods
The main feature of these systems is the active participation of many (sometimes
hundreds of) institutes belonging to the same country (interregional or national inter-
comparisons) or, more often, to different countries (international intercomparisons).
All participating organisations are linked in that they are concerned with the same sort
of activity, e.g. radiobiological experiments on late effects,
60
Co radiation therapy,
neutron radiation therapy, environmental dosimetry, and so on.
As illustrated in figure 20.2, the peripheral institutes do not interact directly, but
through a central laboratory, which is seldom a primary standards laboratory. According
to the procedure used, a distinction can be made between (a) 'instrument inter-
comparisons' and (b) 'dose intercomparisons', the subject of the first being the dosimetric
devices by which the laboratories evaluate doses, while the second kind of inter-
comparison deals with the results of such evaluations.
In the intercomparisons of instruments (see figure 20.3) each participant takes (or
sends) his own instrument (the one used for routine measurements) to a central
institution where a very stable irradiation facility is available to give an unspecified, but
constant, dose. The instruments are then taken (or sent) back and read by participants,
and results are eventually compared.
In the intercomparisons of dose (see figure 20.4) a central institution takes (or sends)
dosimetric integrating devices (transfer devices) to each participant. The participant
irradiates them to an agreed dose using the same irradiation facility as for routine experi-
ments, calibrated by means of the local field instrument. The transfer devices are then
taken (or sent) back to the central laboratory, where they are read and results are
compared.
Application of TL dosemeters in dose standardisation and intercomparison 385
Country A I Country B
Institute
^ ^ ^
Institute
^ ^
1
1
Central
laboratory
1
1
^ ^
Institute
Institute
Country C | Country D
Figure 20.2. Diagrammatic illustration of direct intercomparison method.
Preparation of
dosemeters by
peripheral
institutes
Taking or
sending to
central lab.
Reading by
peripheral
institutes
Taking or
sending back
of dosemeters
Irradiation to an
unspecified but
constant dose
Figure 20.3. Diagrammatic illustration of a dosemeter intercomparison.
Preparation of
transfer devices
by central lab.
Reading of
transfer devices
by central lab.
Taking or
sending to
peripheral
institutes
Taking or
sending back
to central lab.

Irradiation to
a specified dose
Figure 20.4. Diagrammatic illustration of a dose intercomparison.
From the practical point of view of having uniform dose units in every institute
carrying out irradiations (for clinical, biological or industrial purposes), method (b) is
more direct and so more reliable [6], as it also takes into account the technique, right or
wrong, by which local instruments are actually used. In other words, two institutes may
have fully comparable dosimetric instruments but still irradiate animals or patients to
significantly different doses, just because the instruments are used in a different way. This
concept does not apply, of course, to radiation protection, both as personal and environ
mental dosimetry, where doses are not 'administered' but 'received' and people are only
interested in knowing whether or not the dosemeters they use give a correct reading. In
this case, instrument intercomparisons should be undertaken.
3 86 G Scarpa
Both field dosemeters used in method (a) and transfer devices used in method (b) can
be classified into two main categories:
(1) classical electronic dosemeters, such as ionisation chambers, scintillation dosemeters,
etc, and
(2) solid-state dosemeters (also referred to as 'passive' dosemeters), mainly represented
by TL detectors.
Instruments of the first category are large, delicate and expensive so that they usually
need to be carried personally to and from the irradiation site. Solid-state devices, in
contrast, are so small, rugged and inexpensive that they can be sent by mail without any
complications and at a far lower cost. This is the reason why the great majority of inter-
comparisons are now performed by means of mailed TL phosphors (so-called 'mailed
intercomparisons
,
).
20.4. Characteristics of TL dosemeters used for mailed intercomparisons
The most important features of such solid-state dosemeters are their long-term stability,
their reproducibility, their sensitivity and their energy response.
The need for a good long-term stability arises from the fact that in every inter-
comparison the time elapsing between initial preparation of dosemeters and final readout
is rarely shorter than a couple of weeks, and sometimes as long as three months (environ-
mental dosemeter intercomparisons). During this period, dosemeters undergo two
opposed phenomena: on the one hand an increase of the zero-dose signal (background) in
the form of non-radiation-induced (NRI) peaks, and on the other a decrease of the
radiation-induced signal (fading). Both phenomena are more or less influenced by
ambient temperature and humidity. From this point of view, excellent TL materials seem
to be LiF and BeO.
The reproducibility of measurements should be within 2 or 3% for a single detector,
falling to less than 1% if groups of 8-10 detectors are employed.
As to sensitivity, it should be adequate at the dose level of interest, e.g. the order of a
gray in the field of radiotherapy and radiobiology and the order of a fraction of a
milligray in intercomparisons of environmental detectors. CaF
2
and CaS0
4
seem to be the
best in the latter case.
A more or less pronounced energy dependence of the response is a property shared by
all known TL materials. Calcium-based TL detectors, such as CaF
2
and CaS0
4
, are the
worst from this viewpoint, even though the use of appropriate metal filters can overcome
this drawback, at least to some extent. LiF and BeO have, in contrast, the flattest energy
response curve, due to their tissue equivalence.
20.5. Practical examples of mailed intercomparisons
20.5.1. IAEA-WHO
60
Co dose intercomparison
The first large-scale postal intercomparison by means of TL detectors was that started in
1966 by the IAEA in connection, later, with the WHO, aiming to check the accuracy of
dosimetric evaluations performed in a number of radiotherapy institutes throughout the
Application of TL dosemeters in dose standardisation and intercomparison 387
world, using ^Co facilities. More than 400 experimental data have been collected in a
recently published survey of results [3].
Transfer dosemeters were LiF-filled capsules, in groups of three, which the participants
were asked to irradiate within a water phantom, at 5 cm depth, to a dose of 2 Gy, as
evaluated by each institute. Two control capsules, one exposed to a known dose and the
other not exposed, were sent together with the test capsules to detect possible
environmental influences during transport and storage.
About one-third of the participants obtained results which were outside the range
5% of the correct dose. Improvements were observed in subsequent intercomparisons of
the same kind.
20.5.2. EULEP dose intercomparison
Another very important intercomparison project was the one organised in 1971-1976 by
the European Late Effect Project Group (EULEP) among 18 European radiobiological
and biomedical laboratories working in the field of late effects of x-rays in mammals.
The project was divided into three successive sessions, each composed of two or three
experimental runs.
Excluding the first run of the first session, in every experiment the participants were
asked to expose a mouse-sized test phantom containing three LiF-filled capsules, one
central and two peripheral. Apart from the test phantom, additional mouse-phantoms
had to be placed around, in order to simulate the real irradiation of a group of mice. The
central dosemeter had to receive an absorbed dose of 2 or 3 Gy, in condition of
maximum backscatter and using a minimum focus-to-phantom distance of 60 cm. The
participants were invited to use an HVL between 1 and 3 mm Cu and to quote the actual
HVL employed.
The knowledge of HVL was necessary to evaluate, at least roughly, the average energy
of the x-ray beam actually used by each participant. Based on this energy, an appropriate
correction factor could be applied in order to allow for the energy response of LiF,
ranging between 1.26 and 1.15 in this HVL interval [1,4, 5].
The results of the three intercomparison sessions are summarised in table 20.1. A
considerable improvement can be seen in some cases: in the third session (1976) only
one institute was outside the limit of 5% of the standard dose.
The following recommendations were formulated [1].
(a) The accuracy of the dosimetry is considered to be satisfactory when the mean value
of the results from a laboratory differs by less than 5% from the standard value.
(b) When a difference between 5 and 10% exists, a small discrepancy in the dosimetry
in indicated.
(c) If the difference is more than 10%, a recalibration of the dosimetry system is
recommended.
20.5.3. International intercomparisons of environmental dosemeters
Three international intercomparison studies of environmental dosemeters have been
organised in 1974, 1976 and 1977 by Gesell and Burke, with 56, 128 and about 150
participants, respectively. A fourth session is now in progress. The aim of these
388 G Scarpa
Table 20. 1. Mean relative absorbed dose and corresponding standard deviation for 1971,
1973 and 1976 EULEP dosimetry intercompaiisons. (From Broerse et al [1].)
Participants
1
2
3
4
5
6
7
8
9
10
11
12
13
14
15
16
17
18
Mean
1.169
1.045
1.049
1.017
0.996
0.953
0.830
1.125
1.010
1.090
0.977
-
-
-
-
1.041
1.123
-
1971
Stand.
dev. (%)
1.5
0.7
1.9
1.5
2.1
2.0
13.3
5.9
0.4
2.5
0.6
-
-
-
-
0.3
11.2
-
Mean
0.929
1.027
1.078
0.985
1.019
0.959
0.850
0.992
1.011
1.028
0.968
1.070
0.979
1.013
-
-
-
-
1973
Stand.
dev. (%)
1.8
2.7
4.5
0.9
2.3
5.9
6.7
3.4
0.9
7.2
2.0
0.7
0.1
1.3
-
-
-
-
Mean
1.011
1.079
1.019
0.969
0.982
0.956
0.952
0.995
0.974
0.951
-
0.960
-
0.960
0.956
0.976
1.033
0.993
1976
Stand.
dev. (%)
1.6
3.5
1.6
1.7
2.7
0.7
4.5
6.0
0.7
3.5
-
4.1
-
2.1
1.9
5.0
5.0
1.6
procedures is to verify the accuracy and reliability of small and inexpensive passive
detectors (mainly TL phosphors) commonly used today to measure environmental doses,
instead of scintillation or gas ionisation devices.
Each participant was requested to send by airmail a set of six dosemeters of each type
that he wished to intercompare: two 'field' dosemeters, two 'laboratory'dosemeters and
two 'control' dosemeters. Upon receipt, the dosemeters were transferred to a low-
background shielded area, whose exposure rate had previously been measured. After a
few days the field dosemeters were separated from the others and deployed at the field
site, where a portable recording ion chamber was also located to estimate radiation
exposure during the experiment. The exposure of field detectors lasted 90 days; in the
mid-part of this period the laboratory dosemeters were irradiated to an unrevealed extent
by a
226
Ra source. At the end of the third month, the field dosemeters were recovered,
reunited with the laboratory and control detectors and returned by airmail to the
participants, together with a response form.
On this form, the participants were asked to estimate the actual field and laboratory
exposures (Xp and X]_) from the data measured with the three groups of dosemeters,
using the following formulae:
Xp = Xp - X
c
+ X
ATL = X^ - XQ
where X' are the exposures measured with field (F), laboratory (L) and control (C)
dosemeters and X
s
is the exposure received from control dosemeters in the storage site.
Application of TL dosemeters in dose standardisation and intercomparison 389
The participants were also requested to state their error estimates (two standard
deviations), including all the known errors, such as those arising from the detector
imprecision, calibration errors, etc. The results of the first two intercomparisons have
already been published by Gesell and Burke [7,8].
Referring to the second intercomparison study, figures 20.5 and 20.6 illustrate the
distribution of the results of the 'laboratory' and 'field' dosemeters exposed to 21.3 and
17 mR, respectively. If results exceeding 3a are eliminated as outliers, the resulting
averages are 18.8 and 16.4 mR and 71% and 65% of the data fall within 20% of these
15 -
<-) 10
z
UJ
o
I I I I I I I I I I I I I I II ' I I I I I I I I I I ' I I I ' I '
RJ
^ESTIMATED
LABORATORY
EXPOSURE
. . n. nl l nn. . . . n.
10 15 20 25 30 35 40
EXPOSURE ( mR)
Figure 20.5. Second international intercomparison of environmental dosemeters: results of
'laboratory' dosemeters. (From Burke and Gesell [8].)
15 -
6 io
a
UJ
i 11 i 11 i i i i 11 1 1 1 11 i i i 11 i i 1 1 1 1 1 1 1 1 1
IONIZATION
CHAMBER
MEASUREMENT
in
n/
n...n v.
J_ I _ 1 1 JL
- 5 0 5 10 15 20 25 30
EXPOSURE ( mR)
Figure 20.6. Second international intercomparison of environmental dosemeters: results of
'field' dosemeters. (From Burke and Gesell [8].)
390 G Scarpa
average values. As regards the types of TL detectors used in this study, 36% were
LiF:Mg,Ti, 18% CaF
2
:Dy, 17% CaS0
4
:Dy and 10% CaF
2
:Mn.
20.6. Conclusions
The direct intercomparison method, both for dosemeter intercomparison and dose inter-
comparison, is becoming more and more widely used for dose standardisation purposes.
In the last two decades a number of intercomparisons have been undertaken on a
national, as well as an international, scale. Most of them have been based upon the use of
small, inexpensive TL dosemeters, which may very easily be sent by ordinary mail. The
ever-increasing number of intercomparisons is justified by the valuable data that can be
easily collected by this method, at a very low cost.
It must be emphasised, however, that the intercomparison method is normally not a
substitute to the classical method of dissemination of standards, but merely a comple-
mentary technique, useful to spot possible failures of the latter. It must be added that
sometimes a direct intercomparison is the only system that can be used to standardise
doses, e.g. among countries in which neither primary nor secondary standards are yet
available.
References
1 Broerse J J. Zoetelief J and Puite K J 1978 Dosimetry intercomparisons for evaluation of late
effects of ionizing radiation A eta Radiol. Oncol. 17 225
2 Kemp L A W 1977 Dissemination of the roentgen unit for radiotherapy purposes, in Ionizing
Radiation Metrology (Bologna: Editrice Compositori) pp 227-249
3 Eisenlohr H H and Jayaraman S 1977 Phys. Med. Biol. 22 18
4 Puite K J and Crebolder D L J M 1974 Energy dependence of TL dosimeters for x-ray dose and
dose distribution measurements in a mouse phantom Phys. Med. Biol. 19 341
5 Puite K J 1976 Phys. Med. Biol. 21216
6 Broerse J J and Puite K J 1974 The usefulness of intercomparison studies for the improvements of
x-ray dosimetry Phys. Med. Biol. 19 732
7 Gesell T F, de Planque Burke G and Becker K 1975 An international intercomparison of environ-
mental dosemeters under field and laboratory conditions Rep. ORNL-TM-4887, April
8 de Planque Burke G and Gesell T F 1979 Second international intercomparison of environmental
dosemeters under field and laboratory conditions Health Phys. 36 (3) 221
Applied Thermoluminescence Dosimetry. Eds M Oberhofer and A Scharmann
1981 ECSC, EEC, EAEC, Brussels and Luxembourg
APPENDIX
The new radiological (SI) units and their conversion to the
units previously used
At the 15th and the 16th General Conferences of Weights and Measures, special names
were adopted for some units of the Systeme International d'Unites (si) used in the field
of ionising radiation dosimetry.
The gray, symbol Gy, has been adopted as the special name for the si unit of absorbed
dose and of other quantities in the field of ionising radiations, which can be expressed
in joules per kilogram (e.g. absorbed dose index, kerma and specific energy imparted).
One gray is equal to one joule per kilogram:
1 Gy = 1 J kg"
1
.
The sievert, symbol Sv, has been adopted as the special name for the si unit of dose
equivalent. One sievert is equal to one joule per kilogram:
1 Sv = 1 J kg
-1
.
The becquerel, symbol Bq, has been adopted as the special name for the si unit of
radioactivity. One becquerel is equal to one second to the power of minus one:
1 Bq= 1 s"
1
.
Unit multiples are expressed by adding the following symbols of prefixes to the unit
symbols:
Name Letter Multiple
tera
giga
mega
kilo
milli
micro
nano
T
G
M
k
m
M
n
10
12
10'
10'
10
3
10"
3
icr
6
10"'
To convert from one set of units to the other, the following relationships hold:
1 rad(rd) = 10"
2
Jkg"
1
=10"
2
Gy
1 Gy = 100 rad
l r em=10"
2
Jkg"
1
= 10~
2
Sv
1 Sv = 100rem
392 Appendix
1 Ci (curie) = 3.7 x 10
10
s
_1
= 3.7 x 10
10
Bq (exactly)
1 Bq = x 10"
10
Ci~ 2.703 xl O"
n
Ci .
3.7
No special name for the unit of exposure, up to now called the roentgen (R), was
adopted. The unit for exposure is 1 coulomb per kilogram:
1 R = 2. 58xKr
4
Ckg
_ 1
1 Ckg
_1
= xl 0
4
R.
2.58
Thus we can summarise this in the following:
Absorbed dose l r a d =1 0 "
2
Gy l Gy = 100rad
Kerma l r ad = l (T
3
Gy l Gy =1 0 0 r a d
Dose equivalent l r e m=10"
2
Sv l Sv =1 0 0 r e m
Activity 1 Ci =3. 7Xl 0' Bq 1 Bq = 2.703 X 1 0 ' " Crf
Exposure 1 R = 2.58 X 10""C kg"
1
1 C kg"' = 3.876 X 10
3
Rf
| These values are rounded
Index
Absorbed dose, 230, 231, 392
calculation of, 333, 337
correction factor, 324
index, 391
measurement in medicine, 271, 284-6
Absorption bands, 303
of ionising radiation, 153, 172
mechanisms of radiation absorption, 151
reader, 155
self-, 87, 182, 183, 184
Accessory instrumentation,
see Instrumentation
Accidental exposure, see Exposure
Accident dosimetry, see Dosimetry
Accumulated activity transfer, see Activity
transfer
Accuracy, 123, 149-50, 171, 193
definition, 143
improvement, 68
in supralinearity range, 84
in low dose measurements, 150
of TL-measurements, 149
Acetone, 69
Activation, 252-3
determination, 24-5
energy, 24, 29, 91
Activator, 239, 253
Activity, 392
transfer, accumulated, 333
Actual fading, see Fading
Additivity rule, 87
Adhesives, TL of, 278
Address list of instrument manufacturers, 64-5
Afterglow, 4
AgBr, see Silver bromide
Ag centres, 153
Ag* centres, 153
Age determination, see Dating
Age equation, 347-8, 363-4
Ageing effect, influence on PM gain, 49
Aggregates, 13
Air, 126
hot, 49
reference medium, 86
Air-crafts,
mean exposure levels in, 224
measurements in, 224
Albedo dosemeter, see Dosemeter
calibration, 190
choice and use, 249-50
effective response, 190
response, 249
schematic diagram of types, 248
single sphere, 189-90
Albedo dosimetry, 190
Albedo factor, 189
Alcohol, 69, 242, 243
Alkali halides, 12, 14, 155, 163
A1,0
3
, see Aluminium oxide
Alpha converter, 160
Alpha particles, 151, 235, 236
Alumina, 118
sensitivity to neutrons, 121
special emission, 119
Aluminium oxide , 118- 21, 311
dose characteristic, 120
dosimetric properties, 119-20
dose range, 170
effective atomic number, 170, 274
energy dependence, 87, 117
fading, 173
half-lives of peaks (trap levels), 119
high photon dose measurements, 310
glow-curve, 118
history, 118
main glow, 170
neutron dosimetry with, 244
peak temperature, 119
physical properties, 118, 170
effect of proton radiator, 244
regeneration, 119
sandwiches, 244
triboluminescence, 120
Al okaCo. Lt d, 64, 76
394 Index
Alpha-factor, 349
Alpha-particles, 236, 238
Ambient temperature profile, 210
American National Standards Institute Inc.
(ANSI), 168, 197, 198, 199
Amplifier, signal, 49-50
Analysis of TL and TSC data, 32-6
phenomenological, 18-21
Angle of incidence, 244, 250, 251
Angular response, 169, 177
Animal habit studies, TLD-application for, 295
Animal experiments, 289-90
Anneal, automatic, 56, 76-8, 93
Annealing, 169, 175, 193
fast, 136-7
furnaces, see Furnace
isothermally, 78
of Teflon dosemeters, 175
post-irradiation, 168, 208, 209, 210
pre-i rradi at i on, 40, 134, 174, 188
post-read (out), 40, 134- 8
pre-read(out), 40, 42, 94, 130-1
procedures, 93-4
repeated, 205
standard technique, 100, 134, 136
stands, 77-9
temperature, 135
treatment, 188
Anomalous fading, see Fading
ANS-standard for environmental TLD-systems,
198
ANSI, see American National Standards Institute
Inc.
Applications of TLD, 182-92
Archaeological dating, see Dating
Argon, 126, 213
flow-rate, 215
Argon-41, 225
Arrhenius equation, 16
ATLAS, 56, 58
Atomic number, effective, 88
Auger recombination, 17
Austrian Atomic Energy Research Organisation
Ltd, TL-dosemeter, 179
Authenticity testing, 368
Automatic anneal, see Anneal
control system, 51
instruments, 53, 178, 192
residual reading, 176
performance, 180
Automation, 52- 3, 59, 168, 171
Automated reader, see Reader
Automatic control system, 51
Automatic system, residual reading, 176
Average dose equivalent, 167
Average man, 284
Background
fluctuations, 221, 222
increase, 212, 214
component, elimination, 221
dose, local individual, 223
measurements, at Karlsruhe, 224
radiation, 197, 220, 223, 224, 225
energy spectrum, 224
reduction, 70
signal, 44, 50, 146
Backscatter, 172, 189, 245, 247, 251
Badge, 59, 169, 184, 189, 190
boron loaded plastic, 190
handling, 53
multi-detector, 167
shielding, 186
Band
band-band recombination, 18
gap, 18, 153
model, 18-21, 152
Bar-code, 179
Basal layer, 185
Basic dosemeter, see Dosemeter
Batch-to-batch variation of TL-response to
thermal neutrons, 233
Batch history, 219
sensitivity variation within, 172
uniformity, 173, 198, 199, 201, 202, 217,
219
BCD, see Binary code decimal
identification, 179
punched hole identification, 60
Barium tungstate, TL of, 33-6
BaWO, see Barium tungstate
Beam hardening, 275
uniformity checks, 271
Belt dosemeter, see Dosemeter
BeO, see Beryllium oxide
BeO : Na, see Beryllium oxide
Beryllium oxide
BeO, 8, 109-11, 152, 234, 241
annealing procedure, 93
ceramic, 158
see also Thermalox chips, 184
discs, beta-ray energy response, 89
dose range, 170
dose rate dependence, 95
dosimetric properties, 110, 311
effective atomic number, 110, 158, 170
emission temperature, 92
energy response, 87, 88, 172, 184
fading, 92, 110, 173
glow-curve, 110
high photon dose measurements with,
309-10
history, 110
Index
395
Beryllium oxide (continued)
LET response, 111
light emission, 110
light sensitivity, 110
linearity range, 84
main glow, 170
neutron sensitivity, 90-1, 111, 234
peak half-lives, 92
preparation, 110
properties, 170
physical, 110
relative response as a function of LET of
charged particles, 108
reproducibility, 94
response curve, 110
sensitivity to fast neutrons, 91
supralinearity , 110, 310
thermally stimulated exoelectron emission,
158
thermal neutron response, 234
tissue equivalence, 110
toxicity, 139
TSEE curve, 159
BeO:Na, 110
neutron response, 241
Becquerel, Henri, 3
unit (Bq), 391
Beta-radiation dosimetry, 88- 9, 182- 4, 186,
193, 265
Beta-rays, 167, 182, 184, 253
response t o, 88
Biochemistry, TL-application in, 293
Bimolecular kinetics, sec Second-order
kinetics
Binary code decimal (BCD), 179
identification, 179
Biological effects, 230
Biology, application of TL in, 289-95
Black-body radiation, 239
Block-heating, 61, 62
Body-dose, see Dose
Boltzmann factor (constant), 16, 91
Boron-loaded plastic badge, see Badge
Boron shield, 189
Boyle, Robert, 3
Bones, dating of, 353
Bone dosimetry, 290-1
Bq, see Becquerel, unit
Bracelet dosemeter, see Dosemeter
Bragg-Gray principle, 86, 337-8
Bragg reflections, 18
Built-in heater elements, sec Heater elements
Build-up, 175
factors, measurement of, 317, 320
Bulb dosemeter, see Dosemeter
Burlin theory, 338-9
Cadmium shield, 189, 236, 250
Calcareous deposits, dating of, 354
CaF,,CaF
2
:nat.,CaF
2
:Mn,CaF,:Dy,CaF
2
:Tm,
see Calcium fluoride
Calcium fluoride, CaF
2
, 4, 7, 70, 111- 5, 170,
254
dosemeters, shielded, 224
history, 6
effective atomic number, 117, 170
energy dependence, 274
(response), 87, 172
fading, optical, 129
systems reproducibility, 202
thermal neutron response, 234
Calcium fluoride, CaF, : Dy (TLD 200), 8, 188,
199, 252
annealing procedure, 93
characteristics, 199
directional dependence, 128
dosemeters, 186, 206
dose range, 170
dosimetric properties, 114-5
emission temperatures, 92
energy dependence, 207
fading, 92, 114, 128, 129, 173, 199, 208,
211, 266-7
fading reduction, 209, 210
glow-curve, 114
high-dose properties, 188
linearity range, 84
lower exposure limit, 199
main flow, 170
multi-element dosemeter, 178
neutron activation reactions, 252
neutron sensitivity, 115, 234
neutron separation, 253
peak half-lives, 92
over-sensitivity reduction, 205
physical properties, 114
precision, 123
reproducibility, 174
relative response at maximum, 188
response to 9 MeV photons, 187
self-irradiation, 199
supralinearity, 115, 188
Teflon, fading, 208
radiation damage, 188
residual dose, 188
response change, 188
TLD-200, 188, 199, 252
sensitising, 114
thermal neutron response, 234
thermal neutron dosimetry with, 252
uniformity, 123
wavelength of TL, 114
396 Index
Calcium fluoride, CaF, : Mn (TLD-400), 4,
113- 4, 243'
annealing procedure, 93
beta sensitivity, 182
characteristics, 199
dosemeter, 206
dose range, 170
dosimetric properties, 114, 311
emission temperature, 92
energy response, 172
fading, 92, 113, 173, 199
fast neutron response, 243
glow-curve, 112, 113
heat-rate influences, 134
high photon dosimetry with, 308
linearity, 84, 113, 114
lower exposure limit, 199
low temperature peaks, 131, 132
main glow, 170
neutron activation reactions, 252
neutron response, 114, 243
neutron separation, 253
peak half-life, 92
powder dispensing, 73
preparation, 113
properties, 170
physical, 113
relative energy response, 275, 276
relative response at maximum, 188
reproducibility, 308
residual dose, 188
saturation, 113
self-irradiation, 199
sensitivity, 113
supralinearity, 188, 308
Teflon dosemeters, 113, 244
high dose properties, 188
neutron dosimetry with, 244
Teflon sandwiches, 244
thermal neutron sensitivity, 20, 234
wavelength of TL, 113
Calcium fluoride, natural, CaF
2
: nat., 3, 4, 6,
111-3, 245
characteristics, 199
close range, 170
dosimetric characteristics, 112
emission temperatures, 112
fading, 199
frequency factors, 112
glow curves, 111-2
half-lives of trap levels, 111
history, 111
impurity activators, 111
light sensitivity, 112
linearity, 112
lower exposure limit, 112, 199
main glow, 170
neutron dosimetry, 244, 252
neutron sensitivity, 113, 234
peak stability, 111
properties, 170
sandwiches, 244
self-irradiation, 199
sensitivity, 112
thermal neutron response, 234
trap depths, 111-2
UV stimulation, 111
wavelength of TL, 112
Calcium fluoride, CaF,: Tm (TLD-300), 253
fast neutron response, 264
glow-curve, 203
traps, 261
Calcium sulphate, CaS0
4
, 6, 115-8, 239-40
colour of TL light, 70
effective atomic number, 117, 170, 274
energy dependence (response), 117, 172
fading, 211
optical, 129
history, 6, 115
main glow, 170
multi-element dosemeter, 178
neutron dosimetry with, 239-40
neutron sensitivity, 117
systems, reproducibility, 202
thermal neutron response, 234
Calcium sulphate, CaSO: Dy, 8, 115, 243
background, 214, 215
activation energies, 116
annealing, 77
beta-sensitivity, 182
characteristics, 199
dosimetric properties, 116-8, 311
embedded in p-sexiphenyl, fast neutron
response, 243
emission temperatures, 116
energy response, 87
fading, 116, 173, 174, 199, 207, 211, 239
fast neutron response, 243
frequency factor, 116
friction, 213
glow-curve, 116, 213, 240
half-lives of traps (peaks), 116
high photon dose measurements with, 310
intermediate and fast neutron dosimetry,
243
light influence, 213, 214
sensitivity, 116
linearity, 117
lower exposure limit, 199
neutron activation reactions, 252
neutron dosimetry with, 252
neutron separation, 253
Index 397
Calcium sulphate, CaS0
4
: Dy (continued)
preparation, 115
properties, 170
physical, 116
regeneration, 117
relative response at maximum, 188
residual dose, 188
self-irradiation, 199
sensitivity to 7-rays and charged particles,
239
supralinearity, 188, 310
Teflon dosemeters, 115
fading, 207
high dose properties, 188
thermal neutron response, 90, 234, 239
trap depths, 116
wavelength of TL, 116
Calcium sulphate, CaS0
4
: Mn, 6, 7, 115
basic work on, 6
fading, 92, 115, 173, 239
glow curve, 112, 115
mixtures with compounds of high thermal
neutron capture cross section,
239-40
powder dispensing, 73
properties, 115, 170
quantitative measurement of UV radiation, 6
sensitivity, 115
thermal neutron response, 233, 234, 239
Calcium sulphate, CaS0
4
: Sm
glow curve, 116
glow peak, 115
fading, 115
light sensitivity, 115
neutron spectrometer, 244, 245
sensitivity, 115
wavelength of TL, 115
Calcium sulphate, CaS0
4
: Tm, 115
dosimetric properties, 116-8, 311
energy response, 87
fading, 173, 174, 239
glow curve, 116
high dose properties, 188
high photon dose measurements with, 310
light sensitivity, 116
linearity, 117
neutron dosimetry with, 117, 243, 244
neutron energy dependence, 241
multi-element dosemeter, 178
physical properties, 115
preparation, 115
properties, 170
radiation damage, 188
regeneration, 117
relative response at maximum, 188
reproducibility, 174
residual dose, 188
response change, 188
sandwiches, 244
sensitivity to 7-rays and charged particles,
239
supralinearity, 188, 310
Teflon dosemeters, 115
thermal neutron response, 234, 239, 240
wavelength of TL, 116
Calibration, 39, 51, 58, 70, 79, 120, 149, 150,
169, 171, 180, 186, 190, 198, 201,
210, 213- 8, 214, 215
Calibration detector (dosemeter), 138, 220
Calibration, individual dosemeter, 217
factor, 56, 149, 171, 217
field, 190, 192
internal, 217
source, 58, 168
techniques, 198
Calibrators, 79-80
Capacity, thermal, 40
Capture, 230, 239, 252
Capture cross section, 235
Cascades, 15
Cathodoluminescence, 4
Cathode sensitivity, optimal, 49
Cavity theory, 86, 89, 275, 337-40
CEA, see Commissariat a l'Energie Atomique
CEC recommendations for personnel TLD
systems, 168
Cellulose nitrate, 159
detector, 160
Central Research Institute for Physics, 64
Ceramics, 152
dating of, 352
Charge, 48
carriers, lifetime, 27
digitiser, see Digitiser
neutrality, condition of, 20
Charge-to-pulse converter, 51
Chemical effects, 230
Chemi(o)luminescence, 4, 39, 42, 86, 126
reduction, 45, 126
Chips, 167, 171, 180, 200, 212
embedded in Teflon, 178
extruded, 67
handling, 74
hot pressed, 58, 171
Ci, see Curie
Cleaners, ultrasonic, 75-6
Cleaning, 212
procedures, 138-9
Clinical measurements, 271-87
Coalmine dust, determination of fibrogenic
properties, 292-3
C0
2
-cooling, 76
398 Index
Codabar, see Bar code
Coefficients of variation, 123
Collective dose, 271
Coloration, 152, 162
during anneal, 78
Colour centres, 155
Colouring, 155-6
Comitato Nazionale Energia Nucleare (CNEN),
185
Commissariat a l'Energie Atomique, 178
Commission of the European Communities,
168, 169, 198, 200
Compressed LiF TLDs, preparation, 98
Compton effect, 15, 273
Computer memory, 260
on-line, 168, 171, 190, 261
simulation, 30-2
Conduction band, 15, 16, 18, 152, 153, 157
Conductivity, thermal, 40
Contamination of phosphor surfaces with dirt,
125, 138
organic, 69
influence on TL read-out, 212
Control dosemeters, see Dosemeters
system, automatic, 51
Conversion factors, 131, 231
of SI units, 391
Converter output, 51
Cooling, 46
Cooling-down period, 69
Combustion phenomena, 69
Computer, 52-3, 180, 269
CON-RAD, 72
Converters, 50
Cooling-rate, 135
Corindon, 118, 119
Corrections, 172, 192, 199
Coulomb interaction, 151
Counter, 51
CNEN, see Comitato Nazionale Energia
Nucleare
Compensation shield, 206
CR-39,160
Critical organ, 167
Cross-contamination, 74
Cross section, 16
Crystal, 171
Curie, 392
Current, 48
Current leakage, influence on dark current of
photomultiplier, 50
Czochralski method, 98
Dai Nippon Tokyo Co. Ltd, 64
Damage, see Radiation damage
Damage, effect, 212
Dark current, 49, 50, 170, 200, 204
fluctuations, 175
long term variation, 178
standard deviation, 219
Data analysis, 32-6, 225, 261
processing, 180, 190
recording, 180
security, 192
verification, 269
Dating, 39, 347-81
accuracy, 365
apparatus, 361
applications, 352-4
archaeological, 352-4, 365-7
basic principle, 347
complications, 348-9, 361-81
environmental uncertainties, 379-9
geological, 354
geology, recent, 368
method, 347-52
of bones, 353
calcareous deposits, 354
ceramics, 352
loess, 354
ocean deposits, 354
pottery, 365
rocks, heated, 352-3
volcanic, 354
shells, 353-4
slags, 353
till, 354
volcanic events, 354
zircon, 379-80
radiocarbon, 365
recent geology, 368
techniques, 350-1
fine grain technique, 350, 364
phototransferred TL technique, 351
pre-dose technique, 351, 371-2
subtraction technique, 350, 378
quartz inclusion technique, 350, 364-5,
377
transfer technique, 373
zircon inclusion technique, 350-1, 379-80
D A Pitman Ltd, see Pitman
Defect creation, mechanism, 14-6
Defects
electronic, 11
ionic, 12
in crystals, 16
surface, 154
Density, optical, 152
Depth-dose, 182, 184
distribution, 187, 280
in tissue, 182
Desmarquest & CEC SA, 64, 97
Index
399
Detection limit, lower, 44, 175
threshold, 86
Detector material
specific requirements, 170
handling, 138-9
self-shielding, 233
tissue-equivalence, 187
Detectors, loose, systems for evaluation,
54-9
Diagnostic radiology, measurements, 271-2,
284-6
Diamond spars, 118
Dielectric measurements, 103
Digitiser, 51, 260, 261
Dimers, 103
Dipole, 103
coupling, see Dimers
Directional dependence, 199, 205
Direction of incidence
see Radiation incidence
Directly ionising radiation
see Radiation
Dirt, influence on TL-readings, 75, 212
Disc, handling, 74
memory, see Memory
Dispenser, 71-4
flat-plate, 72
handling, 73-4
malfunctioning, 74
Dissemination of standards, 383
Discharges, influence on background signal,
50
Directional dependence of TL-phosphors, 128
Donor-acceptor recombination, 19
Dose
body-, 167
calculation, 53
depth, 184
equivalent, 167, 177, 190, 231, 245, 246,
247, 392
extremity-, 167, 182-4
finger-, 184
hand-, 184
profile, measurements of, 225
range, 169
reassessment, 168
residual, 44, 191
skin-, 167, 177, 182
surface absorbed, 167
threshold, 86
whole body-, 167, 177, 182
zero-, 86
Dose equivalent, 167, 231, 391
Dose limit
lower, 86, 170
upper, 85-6
Dosemeter
albedo (neutron), see also Albedo dose-
meter, 189-91, 192, 193, 247, 251,
264
badges, commercial, 177-8
basic, 167, 177
belt, 190
bracelet, 184
bulb, 46, 47, 58, 186, 200, 206
calibration, see Calibration
card, 171, 180
control, 205, 207, 213, 215, 216, 220
curling, prevention of, 68
discriminating, basic, 168, 177
extremity, 167, 168, 185, 193
field, 215, 216, 383
identification, automatic, 180
intercomparison, see Intercomparison
film, 5, 157
finger, 183, 184, 185
hand,185
loss, 180
multi-element, 177-8, 182
non-discriminating, basic, 168
ring, 183, 184, 185
scintillation, 152, 163
solid state, 8, 162
systems, personnel, 177-81
practical, 177-81
re-assessment, 176
tandem, 291-2
three-element, 183
Dosemeters (TL-)
advantages over ionisation chambers, 272
choice for clinical use, 273
in medicine, 273
properties, 170
recommended performance, 169
types of, 168, 179
thin, 184
tissue equivalent, 124, 182
Dose rate, 170
assessment of for dating, 376-7
natural, 351-2
Dose-rate dependence, 95
Dosimetry
accident, 90, 191-2, 253
beta, 182, 193
see also Beta-radiation dosimetry
environmental, 177
extremity, 177, 182-4, 193
film,167, 168
integrating, 3
military, 39
patient, 39
peak of LiF, 99
400
Index
Dosimetry (continued)
personnel, 111, 167-95, 237, 247, 248,
249, 250, 251
application of TLD in, 167, 195
photon, 184
requirements, 123
solid state, 152
routine, 71, 95, 149
therapy, 58, 253
thermoluminescence, 5, 123
Drawer assembly (system), 42, 43
for glass-bulb TL-dosemeters, 47
mechanism, 53
Dust, 49
Eberline Instrument Corporation, 65, 72
Ecology, TL application in, 293-4
Edgerton, Germeshausen & Grier, Inc., 114
Effective atomic number, 88
Effective dose equivalent, 167
Effects used in solid state dosimetry, 152
EG&G, see Edgerton,
Elastic collisions, 14-5
Electrical conductivity, 20
Electroluminescence, 4
Electrometer amplifier, 259
Electron, 151
Electron-hole
pairs, 15, 152
holes, 102
traps, 102
equilibrium, 86-7, 278
Electron paramagnetic resonance (EPR), 33
Electronic processes, 14-5
Electronic circuitry, malfunction of, 52
Electronics, logarithmic, 260
Emission, infrared, 175
spectra, 236, 239
Emissivity of planchets, 69
Encapsulation, 198
Energy band
diagram, 152
model, see Band model
compensation (filter shields), 198, 205, 206
components in radiation field determina-
tion, 88
dependence, 87, 162, 171-2, 199, 205, 224
fluence, 230
gap, 18
level diagram, 19
levels, 18
range, 169, 170
response, see also Response, 86-7, 169
calculation, 86-7
examples of, 87
of TL materials to photons, 86
modification by filters, 88
spectrum, neutron, 230
states, 18
traps, see Traps
Entrance absorbed dose, 271
measurements, 282
Environmental TL dosemeters, 206
dosimetry, 39, 58
intercomparison, 387-8
effects on TLD signal, 212-3
factors (parameters), 169, 198, 275
measurements, interpretation, 222
monitoring, see also Monitoring, 197-227,
331-2
programmes, 221
Epoxy resin, 244
EPR, see Electron paramagnetic resonance
Epidermis, basal layer, 167
ERDA, see United States Energy Research and
Development Administration
Error, parameters, 198, 220
overall, measurement, 198, 199
sources, 124- 41, 145- 6, 218
Errors
avoiding of, 168
due to detector, 145-6
due to presence of neutrons, 90
due to reader and evaluation procedure, 146
due to thermal treatment, 146
Escape coefficient, 19
probability, 16
Etchants, 160
Etching rate, 160
EURATOM, 168, 171, 172, 177
European Community, see Commission of the
European Communities
Evaluation
second, 176
manual, 180
Exit absorbed dose, 271
measurement, 282
Excitation (thermal), 11, 16-8, 152
Excitons, 15
Exoelectrons, 157
emission, 152, 157
Expected lifetime, 373
Exposure, 392
accidental, 167
interpretation, 198
Extremity dose, dosimetry, see Dose, Dosi-
metry
Extruded TL materials, 171
ribbons, see Ribbons
Fachverband fur Strahlenschutz e.V., 169, 200
Index 401
Fading, 40, 44, 91-2, 128-30, 162, 168, 169,
170, 172-3, 174, 198, 199, 200,
205-11, 214, 349
actual, 207
anomalous, 349, 373
at 70C, 211
characteristics of some TL materials, 173
correction, 210-11, 266-8
factors, 129
due to humidity, 215
experiment, 207
film-, 156
improvement of fading characteristics, 210
light induced, see also Fading, optical,
128-9
optical, 93, 128-9
rate, 210, 211
real effect, 210
reduction, 209, 210
Fast annealing procedure, 136
Fast neutron detection, see Neutrons
Fast reactor core, measurements, 321
Fast test reactor mock-up, shield tests, 323
Fatigue effect, influence on PM sensitivity, 49
Fault recognition, 269
F-centre, 13, 103, 155
F'-centre, 13
Fy^-centre, 13
Field application, 198
calibration, see Calibration
cycle, 198
dosemeter, see Dosemeters
exposure, 211
calculation, 216
interpretation, 220-1
period, 198
location, 210
Filament, 46
Film, 152, 156
badge, 177
dosimetry, 167, 168
dosemeter, 5, 157
response to 7-rays, 156
Filters, 49, 88, 124, 177, 184, 186, 187, 205,
224
Fine grain dating technique, see Dating
Finger dose, see Dose
ring dosemeter, see Dosemeter
First-order kinetics, 21
Fission foil, 245
Fluence, 230, 241, 245, 247, 251, 252
rate, 230, 232
to dose equivalent conversion factor, 231
Fluorescence,4
Fluorescent foils, 5
light, 213, 214
effect on TL-phosphor, 213, 214
Fluorescent x-rays, 87
Fluorite, see Calcium fluoride, natural
Wblzendorfer, 7
Franck-Condon principle, 17
Frenkel defect, 14
Frequency factor, 17, 24, 29, 373
determination, 24-6
temperature dependence, 26
plot for TLD data analysis, 225
Friction, effect of on TL-response, 212, 213
Furnace, 40, 76-7, 137
Future trends
in personnel dosimetry, 192-3
in neutron dosimetry, 253-4
Gamma, build-up factors, see Build-up factors
radiation detection in presence of neutrons,
see also mixed fields, 90
dosimetry in reactor-shields, 316-7
heating, measurements in an unknown
spectrum, 324
equivalent dose reading, 192
photons, 151
Gamma-ray rejection, 261
Gas dryer bottle, 69
flow meter, 69
rate, 134
flushing, 42, 69-70, 126
influshing, influence on background, 215
heating, 45
inert, 42, 212
Geological dating, see Dating
Geology, recent, dating, see Dating
GesellschaftfurStrahlen-undUmweltforschung
mbH Munchen (GFS), 185, 206
Glass bulbs, 46
bulb dosemeter, see Dosemeter
dosemeter, dosimetric properties, see
Phosphate glass
Glow curve, 11, 17, 40, 50, 83, 213, 233, 236,
237
analyses, 41, 189, 191, 259-69
dependence on read-out atmosphere, 126
digitised, 52, 261
for natural TL, 362
interpretation, 260
linear, 259
logarithmic, 260
measurement, 7
plotting, 52, 51, 54
recording of, 259-60
shape, 168
storage, 260-1
TL and TSC, calculated, 29-30
402
Index
Glow, peak, 83
transient, 3
Glucose, 243
Gold foil, 236
Grain size, 243, 253
Gray, unit, 230, 391
S-shift, 33
Gy, sec Gray
Half-intensity, 26
Half-life, 252
of fading, 91
for different phosphors, 92
Half-width, 26, 32
Halide ions, 12
Hand dose, see Dose
dosemeter, sec Dosemeter
Handling of detectors, 138-40, 193, 212
Harshaw, 65, 72, 80, 97, 111, 114, 138, 171,
177, 178, 179, 199, 206, 217, 261
automated TL analyser system, 56, 60, 126,
180
performance, 180
automated personnel monitoring TLD
system, 60
microprocessor controlled TLD system,
60-1
digitised glow-curve displayer, 261
TL analyser, 54, 269
H-centre, 14, 27
Health Physics Society Standards Committee
(HPSSC), 168
Health risk, 140
Heat cycle, 41, 51, 55
testing, 51
Heater
built-in heater element, 47-8
block method, 44-5, 61
device, 39
element, 43, 49, 175
built-in, 47, 69
infrared emission, 86
hot gas, 45
optical, 46
planchct, see Planchet
RF-heating, 46
Heating,
fractional, 33
linear, 41, 238
medium, 40, 45
method, 42, 44
multiple plateau, 42
non-linear, 41
optica], 46-7, 64, 184
planchets, see Planchcts
plateau, 233, 238
power, 42
programmable, 42
ramp, 233
rate, 21, 134, 298
effect on TL output, 134
influence on peak position, 50-1
fluctuations, 134
hyperbolic, 22
RF-, 46
system, 40-8
technique, fractional, 33
Heist KG, 185
HFS, see Hyperfine structure
High dose properties of TL-phosphors, 188
High dose range, 187, 191
High-energy radiation, 275, 320-1
High-exposure, 176
High-level photon dosimetry with TLD-
materials, 297-313
High temperature anneal, 94
High-tension variations influence on PM
sensitivity, 50
History of TL, 3-9
Hodgkin's disease, 283
Hole centres, 33
Hopping process, 34
Host, 253
Hot finger, 44, 45, 60, 178
Hot gas TLD reader, 53, 56, 94
Hot gas heating, 45, 178
Hotplate, 178
Hot pressed TL-materials, 171
HPSSC, see Health Physics Society Standards
Committee
standard, 169
Human phantom measurements, 284-6
Humidity, 129
detector, 170
effect on TL read-out, 212, 275-6
Hyperfine structure, 13
Identification, automatic dosimeter, 180
1CRP, see International Commission on
Radiation Protection
ICRU, see International Commission on
Radiation Units and Measurements
Imperfections, 11
Implantation of TL dosemeters, 139, 275
Impurities, 11
Impurity ions, 16
Incandescent light, 69
Incidence of radiation, 167, 170, 205
Indirectly ionising radiation, 151
Individual spared organ absorbed dose measure-
ments, 282
Index 403
Induced activity, 252
Inert gas atmosphere, 42
flushing, 69, 95
Inflection temperature, 26
Influence quantities, 170
Infrared emission (radiation), 49, 175
emissivity of planchets, 69
heating, see Heating, optical
sensor, 44
Initial rise method, 26, 32
Institute of Radiation Protection and
Dosimetry, IRO, CNEN, Brasil, 206
Institute of Radiation Protection, Helsinki,
177
multi-element cards, 179
Instrumentation, 39-66
Instrumentation accessories, 67-81
Instrument AB Therados, 65
Instruments
automatic, 53
stability checking, 20
Integral method, 134
Integration interval, 42
of TL-signal, 41
Intercept correction, 348
Intercomparison, 383-91
direct methods, 384
experiments, 197
international, 389
mailed, 386
of
60
Co-teletherapy units, 280
Interlaboratory comparison, 197, 200
test programme, 169, 200
International Commission on Radiation
Protection (ICRP), 167
International Commission on Radiation Units
and Measurements (ICRU), 383
International Organisation for Standardisation,
169
Intermediate and fast neutron dosemeters,
241-53
Interpolation method, 325-7
Intracavitary absorbed dose measurements,
271, 282, 283- 4
Interstitials, 12, 14
Intrinsic response, 176
per absorbed neutron, 340-3
In-vivo dosimetry, 58, 271, 281-2, 286, 290
Ionic conductivity measurements, 103
Ion implantation, 253
Ionisation, 152, 153
chamber, 225
Ionising radiation,
directly and indirectly, 151
detection by TL, 4
IR-heating, see Heating, optical
Irradiation geometry,
effect of, 127
history, 176, 188
of phosphors, temperature effects, 127
Irradiator, 79-80
automatic, 80
reference dose-, 79
ISO, see International Organisation for
Standardisation
Isodose chart, 279
Isomet, optical grade LiF, 302-3
Jahn-Teller effect, 13
J-131 in thyroid, half-life measurement, 333
Kapton (tape), 44
trays, 80
Kerma, 230, 231, 391, 392
Kinetic balance, 20
KOH, see Potassium hydroxide
Ar-value (factor), 348-9
Landauer, R S Jr & Co., nuclear station film
badge, 179
Latent dose information, loss of, see also
Fading, 93, 212
Latent track, 160
Law of detailed balancing, 16
Lens systems, 44, 125
LET, see Linear energy transfer
influence on supralinearity, 84-5
Lethargy, 231-2
Liberation rate, 20
LijB
4
0
7
: Ag, see Lithium borate
Li;B
4
0
7
: Ag, Cu, see Lithium borate
LLB
4
0,: Cu, see Lithium borate
LL,B
4
0
7
: Mn, see Lithium borate
Li
2
B
4
0
7
: Mn, Si, see Lithium borate
LiF, see Lithium fluoride
LiF : Mg,Ti, see Lithium fluoride
LiF : Na,Mg, see Lithium fluoride
Lifetime, 21, 29
Light collecting system, 49
Light dependence, 198, 199, 212
detecting system, 39, 48-52
detector, 49
effects, 212
emission, non-radiation induced, 94
sensitivity, 170, 200
Light source, 49, 51-2, 55, 70-1, 124-5, 146,
217
check,219
emission spectrum, 124-5
errors due to, 125
external, 70-1
long term fluctuations, 218
404
Index
Light source (continued)
internal, 58, 217
and external, daily check with, 21 7
plastic scintillator, 70, 217
temperature dependence of light
intensity, 217
properties, 217
reading, relative standard deviation, 219
temperature effects, 218
Light stimulation, 175, 212
Light sum (integrated), 6, 51, 120, 298
Light yield, 87
Linear energy transfer (LET), 231, 233, 236,
241
Linearity, 83
ranges of, 84
Linearity curve,
example of, 84
Literature on TL and/or TLD, 80-1
Lithium borate, graphite mixed, 182
tissue-equivalence, 184, 205
systems, reproducibility, 202
Lithium borate, LLB.,0,: Ag,Cu, 170, 171,178,
184, 238, 239
Lithium borate, L i ^ O, : Ag, 107, 238-9
sandwiches, 244
Lithium borate, Li, B
4
0, : Cu, 108-9
dosimetric properties, 108-9
physical properties, 109
preparation, 109
Lithium borate, Li,B
4
0
7
: Mn, i'TLD-800), 8,
106-9, 1*70, 188, 238-9
annealing procedures, 93
characteristics, 199
chips, 184, 186
colour of TL-light, 49, 70
diagnostic measurements with, 284
disadvantages, 307
dosemeters, energy response, 107, 183, 206
dose range, 170
dose-rate dependence, 95
dosimetric properties, 107, 311
effective atomic number, 170
emission temperatures, 92
energy dependence, 87, 107, 183, 171-2
fading, 92, 106-7, 173, 174, 211, 212, 215,
238
reduction, 210
glass dosemeters, 171
glow curve, 106, 239, 307
high photon dose measurements with,
306-7
history, 106
humidity influences, 129-30
in-vivo measurements with, 286
isotropically enriched, 239
light sensitivity, 107
linear range, 84, 239
lower exposure limit, 107, 199
main glow, 170
minimal detectable dose, 107, 199
medical application, 272
phosphors
neutron dosimetry with, 238-9, 244
neutron sensitivity, 90, 107-8, 234-5
peak half-lives, 92
physical properties, 106, 170
powder dispensing, 73
preparation, 106
properties, 106, 170
regeneration, 107
relative response as a function of LET of
charged particles, 106, 108
relative response at maximum, 188
response to high LET radiation, 106
response change, 188
reproducibility, 174, 307
residual dose, 188
sandwiches, 244
self-irradiation, 199
silicon rubber dosemeters, 106
supralinearity, 107, 188, 307
Teflon dosemeters, fading, 212, 215
thermal neutron sensitivity, 90, 233, 234-5
tissue-equivalence, 184, 205, 238, 274, 307
TLD-800, high-dose properties, 188
TL-yield, 102
wavelength of emitted TL light, 107, 239
Lithium borate, LL, B
4
0, : Mn,Si
dosemeter system, energy dependence, 206
multi-element dosemeters, 178
properties, 170
radiation damage, 188
relative response at maximum, 188
residual dose, 188
response change, 188
supralinearity, 188
Lithium carbonate, LijC0
3
, 239, 240
Lithium fluoride, LiF : Cu,Ag,
properties, 170
Lithium fluoride, LiF : Mg,Ti (TLD-100), 8,
97, 97- 105, 171, 183, 186, 194,
212, 215, 235, 235- 8
annealing procedure, 93, 174
background, 214, 215
beta-dosimetry with, 265
beta-sensitivity, 89, 182, 224
capture cross section, 235
characteristic, 199
chips, 184, 186
colour of TL light, 49, 70
compressed, 98
Index 405
Lithium fluoride, LiF : Mg.Ti (TLD-100)
(continued)
cooling-rate influence, 136
damage by neutrons, 238
data analysis, 261
depth dose distribution, 187
directional dependence, 128
discovery, 6
dose characteristic, 103-4
dosemeters, energy dependence, 87, 183, 206
with moderators, 245
dose range, 170
dose-rate dependence, 95
dosimetric properties, 103-5, 311
effective atomic number, 103, 170, 199,274
emission characteristics, 102
temperatures, 92, 102
wavelengths, 49, 102, 236
energy response, 87, 105, 171-2, 173, 184,
186, 206
fading, 92, 171, 174, 199, 208, 209, 211,
266-7
optical, 129
reduction, 209, 210
fast neutron response, 243
first applications, 6, 97
friction, 213
glass dosemeters, 171
glow curve, 30, 99-101, 112, 136, 213,
238, 261, 262, 298
after irradiation at different
temperatures, 128
effect of low post-read-out annealing
time, 136
explanation, 27
graphite mixed, 182
heat-rate influences, 134
high-dose properties, 188
high-energy radiation, 275
high LET radiation exposure, 100
high photon dose measurements with,
298-306
history, 8, 97
light influence, 213, 214
linearity range, 84, 236
lower exposure limit, 199
low temperature peaks, 131, 132
main glow peak, 170
medical application, 272
microrods, 185
model, 102-3
multi-element dosemeter, 178
neutron activation reactions, 252
neutron dose dependence, 236
neutron energy dependence (response),
241, 242
neutron dosimetry with, 235-8
neutron sensitivity, 105-6, 189, 234
neutron spectrometer, 245
optical emission spectrum, 49, 236
optical-grade crystal, dosimetric properties,
311
optical-grade powder, dosimetric properties,
311
optical-grade, TL properties, 302
peak half-lives, 92, 102
peak height ratio, 189
peak temperatures, 92, 102
thermal neutron response, 234
physical properties, 99-103
powder, 97-8
dispensing, 73
non-TL-grade dosimetric properties, 311
preparation, 97-9
pre-read-out annealing, 131-2
properties, 99-105, 170
proton radiator effect, 244
PTL, 97
PTL-717, 171
PTL pellets, preparation, 98
PTL, sodium stabilised,
annealing, 100
preparation, 98
radiation damage, 188
reassessment of dose, 176
regeneration, 104
relative energy response, 275, 276
relative response as a function of LET and/
or particle energy, 105
relative response as a function of LET of
charged particles, 108
relative response at maximum, 188
relative response to beta rays, 89
reproducibility, 94, 137, 171, 174, 299-300
residual dose, 188
response change, 188
response to 9 MeV photons, 187
response to fast neutrons, 91
response to slow neutrons, 90, 105
RPL of, 305
reproducibility, 94, 137, 171, 174, 299-300
self-irradiation, 199
sensitivity, 103, 133, 135, 136, 137
sodium-stabilised LiF PTL, 98
supralinearity, 103-4, 188, 236-7, 298-9
systems
relative standard deviation, 203
reproducibility, 202
Teflon dosemeters, 99, 182, 188
discs, 183, 184, 185
fading, 208
preparation, 99
406
Index
Lithium fluoride, LiF : Mg,Ti (TLD-100)
(continued)
sensitivity to sunlight, 93
therapeutic use, 58
thermal neutron response, 234, 239, 240
tissue equivalence, 103, 205
TLD, 97
compressed, preparation, 98
powder, preparation, 97-8
TL yield, 102
toxicity, 139
trap characteristics, 101-2
trap formation, 103
trap level, half-lives, 102
trap mechanism, 135
trapping centres, 261, 267
triboluminescence, 95
UV influence, 130
sensitivity, 93
variation of response with neutron energy, 242
wavelength of TL, 49, 102, 236
Lithium fluoride, LiF : Na,Mg, 178
fading, 209
reduction, 210
high dose properties, 188
radiation damage, 188
relative response at maximum, 188
residual dose, 188
response change, 188
Lithium fluoride, LiF : Tl,Ti, 178
Lithium sulphate, LijS0
4
, 239, 240
Lithium tetraborate, see Lithium borate
Loess, dating of, see Dating
Log normal probability plot for TLD data
analysis, 225
Long term stability, 204-5
Low dose measurements, 51
accuracy, 150
with TL powders, 74
Low energy photons, see Photons
Lower detection limit, 170, 175, 178, 199,
180, 202, 204, 216, 220
Lowest detectable dose, 223
definition, 200
Low level measurements, 126
Low temperature peaks, elimination, 51
Luminescence
common features, 152
signal, 41
spurious, 69
Luminescent signal, 41
Magnesium, 102
Magnesium borate, MgB
4
0
7
, 109
Magnesium borate, MgB
4
0
7
: Dy(Ti) sintered,
171
Magnesium borate, MgB
4
0
7
: Dy/Tm, 109
annealing, 109
effective atomic number, 109
emission spectra, 109
fading, 109
sensitivity, 109
Magnesium borate, MgB
4
0
7
: Tm, 109
Magnesium orthosilicate, see Magnesium
silicate
Magnesium silicate, Mg
;
Si0
4
: Tb, 213, 234,
252, 253
background, 214, 215
friction, 213
light influence, 213, 214
thermal neutron response, 234
Magnetic recording devices, 260
Manipulator, 56
Mass energy absorption coefficient, 86
Magnetic fields, influence on PM sensitivity, 50
Mailed intercomparison, see Intercomparison
Malfunctions of read-out system, 180
Malfunction rate, 192
Mammography, measurements, 287
Manganese sulphate, MnS0
4
, first applications,
6
Mantle therapy, 283
Manual evaluation, 181
Manufacture Beige de Lamps et de Material
Electronique, SA (MBLE), 111, 206
Manufacturers of TLD-equipment, 64-5
Markers, radio-opaque, 282
Maximum permissible dose (MPD), 167, 184,
197
Maximum temperature, 24, 32
MBLE, see Manufacture Beige . . .
Measurements, repeated, 205
Measuring techniques, pitfalls, 39
Measuring time, 41
Medicine, dosimetric applications of TLDs in,
271-87
M-centre, 13
Mean (conversion) efficiency, 325
Mean lifetime, 18
Memory, 261
Metal block, 44
Metaphosphate glass, see Phosphate glass
Meteorites, TL from, 7
thermal history, 7
Methanol rinse, 76, 139
MgB
4
0
7
, see Magnesium borate
Mg
2
Si0
4
: Tb, see Magnesium (ortho) silicate
Microcomputer control, 180
Microprocessor, 52-3, 261
Micro-rod, 67, 78
cleaning, 76
Military dosimetry, see Dosimetry
Index
407
Minicomputer, 52-3, 180
Mirror systems, 49
Mixed beta-gamma radiation fields, dosimetry,
177, 183
Mixed gamma-neutron radiation fields, 189,
192
Mixtures of TL phosphors with hydrogenous
components, 242-3
MnSQ,, see Manganese sulphate
Mobility, 20
Models, kinetic, 21-4
Moderation, 249, 250
Moderator, 241, 245, 247, 249
Moisture dependence, see also Humidity, 198,
199
effect on TL signal, 212
Monitoring,
environmental, 150, 197-227, 205, 210,
214, 220, 223
performance criteria, and technique, 197
individual, objective, 167
long term, 200
neutron, 190
personnel, see also Dosimetry, personnel,
39, 53, 167, 168, 171, 177, 184,
191, 192
performance specifications, 198
periods, 207
routine, with TLDs, requirements, 171
service, role of, 167, 177, 180, 192
requirements, 171
automatic computerised, 180
systems, personnel, 44
Monomolecular kinetics, see First order kinetics
MPD, see Maximum permissible dose
Mu-metal screen, 50
Multidetector badge, see Badge
Multi-element dosemeter, see Dosemeter
Multi-element TLD card, 129
Multiple plateau heating, see Heating
Multiplier, see Photomultiplier
Multisphere technique, 190
NaCl, see Sodium chloride
National Panasonic Matsushita Electric Trading
Co. Ltd, 65, 177, 178, 180, 184
National Panasonic automatic TLD reader
system, 63-4
National Panasonic composite TL dosemeter,
179
National Radioprotection Board (NRPB) TLD
badge, 179
Natural calcium fluoride, see Calcium fluoride
Natural dose rate, see Dose rate
Natural radiation and TL, 7
N-centre, 13
Neptunium, 245
Neutron, 15, 151, 167, 189
albedo, see also Albedo, 245, 247, 248, 249,
250, 251
beams, 244, 245, 247
capture, cross sections, 235
detection, 190
detectors, characteristics, 161, 233
dose equivalent, 190
measurement of, 261
doses in mixed y-n fields, 159
dosimetry, 157, 159, 160, 161, 189-90,
327-331
application of TL materials in, 229-57
energy, 243, 244
energy groups, 232
fast, 229, 232, 241, 245, 248, 249, 253,
254
induced defects, 152
induced resistance change, 162
intermediate, 232, 241
monitoring, see Monitoring
reaction, 229-30
response of TL materials, 89-91
response, influencing factors, 91
fast neutron detection, 159
spectrum, 249, 252
interpretation, 192
stray radiation fields, 190
thermal (see also slow), 232, 235, 237, 239,
240, 241, 245, 248, 249, 250, 251, 252
Nitrogen, 42, 45, 56, 62, 69, 70, 95, 124, 126,
134, 213, 217, 218
effect on plastic scintillator light sources,
217
Noise, of PM tubes, see PM tubes
Non-radiation-induced (signal) light emission,
see Light emission and signal
Non-stationary processes, 18
Nuclear facilities, environment monitoring of,
224
Nuclear track detectors, 159
etching technique, 160
Ocean deposits, dating of, 354
OCR-A figure identification, 62
On-line computer, see Computer
Operational aspects, 123-141
Operation voltage, see Voltage
Operator, 140
Optical density, 152
measurement, 303
fading, see Fading
heating, see Heating
system, 49
Optimal systems, 221
408
Index
Organic crystals, 163
Orientation in radiation fields, 192
Output devices, 48
writing, 52
Oven, annealing, see Furnace
Oxygen effects, 69, 212
Pair production, 15
Panasonic, see National Panasonic . . .
Pathway, optical, 51
Patient dosimetry, see Dosimetry
Peak area measurement, 51
Peak height, 83
influence of temperature of irradiation,
375-6
Peak height ratio for photons and neutrons,
189
Peak height measurement, 50-1, 134
Peak position, 25
Peltier cooling, 49
Penetrating radiation, see Radiation
Penetration depth, 15
Per cent standard deviation, 147
Performance specifications (criteria), 168, 169,
171, 198, 199, 220
Performance testing pilot study, 169
Performance test, 200
of TLD systems, 181
Personnel dosimeter systems, 59-64, 177-81
Personnel dosimetry, see Dosimetry
monitoring, see Monitoring
Person, orientation, 192
Phantom, 190
human, 291
measurements, 271, 284-5
simple geometry, 279-81
Phenomenological analysis, see Analysis
Phosphate glass, 6, 153, 225, 308-9
depth dose distribution, 187
dosimetric properties, 311
energy response, 87
fading, 200
response to 9 MeV photons, 187
silver activated, 6
Phosphor characteristics, 199
dispenser, see Dispenser
high dose properties, 188
general properties, 170
Phosphorescence, 3
Photocathode, see also Cathode, 49
Photodetector, solid state, 49
Photoelectric effect, 15, 273
Photographic emulsion
properties, 5
plates, sensitivity to radiation, 4
process (effect), 152, 156-7, 162
Photoluminescence, 4
Photomultiplier (tube), 44, 49, 107, 110, 125,
202, 239, 260
aging effects, 49
background signal (dark current), 50
current, 50
dark current, 49, 50, 124, 200, 216, 219
fluctuation, 86, 175
discharges, 50
dynamic range, 49
fatigue effect, 49
gain, 50
gain drift, 49, 50
high tension variation influences, 50
magnetic field influences, 50
noise, 49
overall sensitivity, 49
response to I R, 49
sensitivity, 50
changes, 50
signal, 51
special response, 49, 50, 52
temperature effects, 49
Photon counting, 51, 253
beam quality determination, 274
dosimetry, see Dosimetry
high level, 297-313
energy spectrum (radiation quality),
determination, 92, 157, 169, 291
interactions, 18
Photons, 15
energy response of TL materials to, 86-8
high energy, 186-7
low energy, 184-6
Phototransferred TL technique, 351
Physicochemical changes, 94
Physikalische Technische Werkstatten Dr
Pychlau KG (PTW), 185
Physikalisch Technische Bundesanstalt (PTB),
168, 184
requirements, 168, 169, 170, 171, 175
Pitman automatic TLD reader, 61-2
Pitman, D A, Ltd, 65, 72, 73, 75, 79, 80, 99,
179, 217
Pitman TLD reader, 55, 56
Planchets, 42, 43, 49, 67-8, 125-6, 219
cleaning, 69
emissivity, 69
heating, 42-4
infrared (IR) emission, 44
method, 44
optical properties, influence on TL signal,
125
organic contamination, 69
problems with, 44
reflectivity, 44, 69
Index 409
Plant nutrition studies, 293-4
Plastic scintillator light source, see Light source
Plastics, 163
Plateau heating, see Heating
test, 349, 362
Plotter, 52
PM, see Photomultiplier (tube)
Polaions, motions of, 34
POLON,65
Polyethylene, 244, 245, 246, 247, 248
pouch, 184, 185
Polyimide film, see Kapton
Polytetrafluorefhylene, see Teflon
Polyvinylchlorine foils, 212
Positron, 151
Postal service, 168
Post-irradiation annealing, see Annealing
Post-irradiation heat treatment, see also
Annealing, 93
Post-read-(out) anneal(ing), see Annealing
Potassium hydroxide, 160
Potsherds, collection of for TL dating, 366-7
Pottery dating, see Dating
Powder aliquots, 71
dispensers, see Dispenser
grains, 88
embedded in Teflon, 171
manipulation, 71, 74
sieving, 75
Precision, 123, 143-50, 168, 169, 214
definition, 143
obtainable with several dosemeters of same
type, 147-9
obtainable with one single dosemeter, 146-7
influence of cleaning on, 139
influence of dose on, 149
parameters affecting, 124
Pre-dose, 154
effect, 348
luminescence, 154
dating technique, 351, 371-2
Pre-exposure, 176, 211
Pre-heating, 209, 210
Pre-irradiation anneal, see Annealing
Pre-read(out) anneal, see Annealing
Pre-read treatment, see Annealing
Pressure reduction valve, 69
Printer, 52
Printing calculators, 52
Primary standards, 383
Programmable heating, see Heating
Properties of commercial TLD systems, see
TLD systems, commercial
Proton, 151
radiator, see also Radiator, 241, 243, 244,
245
internal, 254
range, 245
recoil, 159
p-sexiphenyl, 243
PTEE, see Teflon, 40
PTB, see Physikalisch Technische Bundesanstalt
PTL 710, 716, 717, 97
PTL 717,
7
LiF : Na,Mg, high dose properties,
188
Publication, TL, approximate number, 8
Pulse height analyser, 52
P^'C, see Polyvinylchlorine
Quality factor, 231
Quartz, determination of fibrogenic properties,
292-3
glass discs, 44
inclusion dating, assessment of dose rate, 377
inclusion technique, see Dating
window, 110
Quenching of spurious luminescence, 212
thermal, 19
R, see Rontgen
Rad, 391
Radiation Detection Company, 65
Radiation absorption, 172
background, 197, 223
damage, 188, 192
directly ionising, 151
incidence, 127, 167, 170, 193
penetrating, 167, 177
non-penetrating, 167, 177, 182
quality, 167, 177, 193
Radiationless transition, see Transition
Radiative transition, see Transition
Radiator, see also Proton radiator, 159
liquids, 243
Radi-Guard, 61
Radioactivity, 391
Radiocarbon dating, see Dating
Radiological Service TNO, 65, 185
Radiological units, 391
Radiolysis, 14-5
Radiophotoluminescence (RPL), 6, 152, 153-5
dosemeters, 6
properties, 162
glass for environmental dosimetry, 200
of TL and optical grade LiF, 305-6
reader, block diagram, 155
principles, 154
Radiotherapy (absorbed dose) measurements,
271, 279-82
Radon measurements, 159
Ramp heating, see Heating
410 Index
Randall-Wilkins shift, 298
theory, 210
Random uncertainties, 143-4
Range changes, 260
changing method, 259
Ratemeter, 51, 152
R-centre, 13
Reactor engineering, TLD in, 315-6
Reactor gamma heating measurements, 321
Reader, 39
properties, 219
quality, 202
systems, 53-64
temperature, 170
Readers, 53-64
automatised, 53, 178
main properties, 171-2, 178
Reading, method, 39
residual, 175-6, 188, 191
second, 191
Read-out (technique), 171, 175, 178
automatic, 202
instrument, operation errors, 124-6, 169
reader instability, 124-6
procedure, optimal, 40, 44
process, 132-3
errors, 132-4
second, 176
systems, 174, 233
automatic, 175, 177
performance, 180
properties, 178
time, 51
Re-assessment of dose, see Dose
Recoil proton, see Proton range, 241, 243,
244
Recombination, 16, 17, 18, 91
centres, 19, 36, 152, 153
coefficient, 19, 21
rate, 20
Recommendations, technical, 168
Recorder, 52
magnetic, 260
strip-chart, 259
Recordings
interpretation, 260
strip-chart, 260
Reference dose irradiator, see Irradiator
Reference energies for photons, 169
Reference light source, see Light source
Reference medium, 86
Reflectivity, 44
changes in, 49
of planchets, 125
Reflector, 58
Regeneration, 168
Relative standard deviation, see Standard
deviation
Relaxation, thermal, 16
Rem, 391
meter, 190
Repeated annealing, see Annealing
measurements, see Measurements
Reporting, 198
Reproducibility, 44, 45, 48, 94, 173-5, 178,
181, 198, 199, 200, 201, 204, 204,
212, 218-20, 225
curves, 173, 174
evaluation, 94
frequency distribution, 181
improvement, 72
influence of cleaning, 139
of TLD systems, 197
Residual dose, see Dose
Residual dose reading, see Reading
Response, energy, 86-8
handling, 52
to beta-rays, 88-9
to neutrons, 89-90
to photons, 86-8
variations, 175
Retrapping
coefficient, 19, 21
rate, 20
Re-use of phosphors, 85, 94, 134, 138, 173-5,
168, 188
RF heating, see Heating
Ribbons, extruded, 40, 167
cleaning of, 138
Ring dosemeter, see Dosemeter
Rocks, dating of heated, see Dating
Rods, glass-encapsulated, 58
Rod handling, 74
Rontgen, WC, 4
Rontgen, unit, 392
Room temperature, influence on readings, 124
Routine dosimetry, see Dosimetry
measurements, 41
RPL, see Radiophotoluminescence
systems, reproducibility, 181
Ruby, 118
Sample changer, 53
preparation for dating, 364
thickness, 88
Sandwiches, of TL-phosphors and hydrogenous
plastic, 244-5
SAPHYMO-SRAT, 65
Sapphire, 118
Saturation, 83, 85-6
Scattering of ionising radiation, 151
Schottky effect, 13
Index 411
Scintillation dosemeter, see Dosemeter
Second (dose) evaluation, 176, 191
Second-order kinetics, 23
Secondary electronic equilibrium, 198
Secondary radiation, 229
Standards, 383
Sedimentation studies, 294
Selection rule, 17
Self absorption, see Absorption
Self-irradiation, 198, 199, 210
shielding (detector), 233
trapped holes, 12, 33
trapped hole model, 33
Semiconductors, 152
Sensitisation and dating, 369-70
Sensitivity,
detector, 49, 201
check, 51-2
factor, see also Calibration factor, 147, 149
loss, 78
reduction by dirt, 138
variations, reasons for, 147, 213
variation within batch, 172
to beta-radiation, 182
Sensors, infrared, 44
Service
centralised, 177
experience, 180
Shells, dating of, see Dating
Sherd
collection, 366
treatment, 366
Shrink foil, 185
Shielding, 198
Sievert, unit, 391
Sieves, 75
Silicon diodes, 161
Signal amplifier, see Amplifier
background, 44
conditioning system, 50
non-radiation induced, 42
spurious, 42, 44, 212
creation of, 93
Signal-to-noise ratio, 49, 51
Silicon diodes, 161
fading, 161
Silver phosphate glass, see Phosphate glass
bromide, AgBr, 156
Single-crystal method, 98
Single-sphere albedo dosemeter, see Albedo
dosemeter
SI units, 391
unit multiples, 391
symbols, 391
Skin dose, see Dose
Skyshine, 224, 225
Slags, dating of, see Dating
Sodium chloride, 12
Sodium-stabilised LiF PTL, 100
annealing, 100
preparation, 98
Sodium-stabilising effect, 100
Solidification method, 97-8
Solid state dosemeter, 8
properties of, 162
Solid state dosimetry, effects used in, 152
Solubility of TL detectors, 139
Source fluctuations, 222
Spark counter, 160
Spatial resolution, 271, 278
Specification for TLD systems, 198
Specific energy imparted, 391
Spectral transmission factor, 125
Spectrometer, 244, 247
Spurious TLD signals, see also Signal, 212,
349
Stability, 170
long term, 201, 204-5
of TL dosimetry, 39, 94
Stabiliser, 55
Standard annealing technique, see Annealing
Standard deviation, 144, 170, 173, 174, 175,
181, 200, 202, 203, 218, 219, 220
against exposure curve, 219, 220
for the dark current, 219
Standard error, 144
Standardisation, 383-91
Standard,
dissemination, 383
test programme, see Test programme
Sterilising of dosemeters, 278
Stimulated exoelectron emission, see also
thermally stimulated exoelectron
emission, 15 7-9
Stimulation,
UV light, 175
visible light, 175
Storage of phosphors, 128, 216
Stray radiation fields, 190, 205
Strip-chart recordings, 260
Studsvik automatic TLD reader, 62, 63
Studsvik Energiteknik AB, 65, 79, 178, 180
Studsvik TL dosemeter, 179
Supralinearity, 83-5, 187, 191, 233, 236, 298
and dating, 369-70
function of LET, 84
Subtraction dating technique, see Dating
Surface absorbed dose, see Dose
Sv, unit, 391
Swiss badge, 179
Swiss Public Health Department TL dosemeter,
179
412 Index
Tandem dosemeter, see Dosemeter
Teflon, 40, 44, 113, 167, 171, 178, 179, 183,
206, 213, 244
disc dosemeters, annealing of, 78
dosemeters
annealing, 175
cleaning, 75
Teledyne Isotopes Inc., 52, 65, 71-2, 77, 79,
99, 115, 178, 185
Teledyne Isotopes Automatic TLD reader, 61,
68
Teledyne TLD reader, 54-5, 67
Temperature build-up, 69
effects, 170
influence on PM overall sensitivity, 49
on TL, 275-6
influences on TL read-out instruments, 124,
201
maximum, 41
profile, 55
rise, linear, 41
shift, 27, 29
time profile, 40, 43
Test exposure, 199
methods, 197
procedures, 168, 199
programme, 169, 178, 180, 193, 197, 201,
204, 210, 220
results, 198
Thermal emission, 49
The Harshaw Chemical Company, see Harshaw
Theory of TL, 11-38
Therados, see Instrument AB Therados
Therados TLD system, 58-9
Therapy dosimetry, accuracy, 140
dosimetry, see Dosimetry
machine output, 271
Thermal activation energy, see Activation
energy
capacity, 42, 43, 69
conductivity, see Conductivity
contact, 40, 44, 45, 46, 48, 77-8, 134
energy, 16, 19
excitation, see Excitation
neutron detectors, 232-40
neutron response, 189
Thermally stimulated conductivity (TSC), 11,
17, 27, 32
Thermally stimulated exoelectron emission
(TSEE), 11, 17, 157
curve for BeO, 159
gas flow proportional counter, 158
sensitivity, 162
Thermally stimulated luminescence glow
curve, 12
Thermalox 995, 84, 309
energy response, 87
Thermal quenching, see Quenching
Thermal separation, 49
Thermocouple, 43, 44
Thermodynamic equilibrium, 16
model, 16
Thermoluminescence, TL, 3, 32, 39
dosimetry, see Dosimetry
glow curve, see Glow curve
Thermoplates, see also Furnaces, 76
Three and four element cards, 179
Three element dosemeter, see Dosemeter
Threshold dose, see Dose
Thresholds, 252
Till, dating of, see Dating
Time from exposure, determination of, 268
Tissue, 182
effective atomic number, 103
Tissue equivalence, 167, 171, 198
equivalent detectors, 171,177, 182, 192,193
directional dependence, 172
of BeO, see Beryllium oxide
of LiF, see Lithium fluoride
of LijB
4
0
7
, see Lithium borate
TLD, see Thermoluminescence dosimetry and/
or Dosimetry
TLD 100, see Lithium fluoride, LiF': Mg,Ti
chips, energy response, 186
sandwiches, 244
TLD 2 00, see Calcium fluoride, CaF,: Dy
TLD 300, see Calcium fluoride, CaF,: Tm
TLD 400, see Calcium fluoride, CaF
2
: Mn
TLD 600,
6
LiF : Mg,Ti, 97, 178, 181, 189,
235, 237, 240
glow curve, 238
TLD 700,
7
LiF : Mg,Ti, 97, 178, 181, 184,
186, 188, 189, 199, 235, 237, 252,
253
ribbons, response to 9 MeV neutrons, 187
TLD 800, see Lithium borate, LL,B
4
0
7
: Mn
TLD, applications, 182
for animal habit studies, 295
for dating, 347-81
for sedimentation studies, 294
in biochemistry, 293
in biology, 289-95
in ecology, 293-4
for environmental studies, 197-227
in medicine, 271
to personnel dosimetry, 167-95
in reactor engineering, 315-46
TLD badge
reading, 59
card, 60
equipment, manufacturers, 64-5
phosphors, see Phosphors
Index
413
TLD badge (continued)
method, applications, 39
systems, relative standard deviation against
exposure, 203
systems, commercial,
properties of, 180, 198-213
maximum permissible errors, 169-70
reproducibility, 178
TL dating, see Dating
dosemeters, see Dosemeters (TL)
efficiency, 102
intrinsic, 102
increase of, 84
intensity, 20, 29
materials, characteristics, 84-96, 199
properties of commercial TLD systems,
198-213
specific requirements, 170
thermal neutron response, 234
maximum shift, 32
measurements, accuracy, see also Accuracy,
149-50
precision, see also Precision, 146-9
natural, 7
output, effect of light on, 128-9
phosphors for high level dosimetry, 311
photon energy response, 274
properties, 170
sensitivity to fast neutrons, 91
sensitivity to slow neutrons, 90
products, preparation and properties,
97-122
powder, see also Powder, 67, 71
publications, 8
reader systems, see Reader systems
reader temperature, 170
yield, definition, 83, 102
non-radiation induced, 94
TNO, see Radiological Service TNO
TNO automatic TLD system, 62, 63
TNO badge, energy response, 186
TNO hot gas automatic TLD reader, 56, 57
TOLEDO, 55, 56, 217
Toxicity, biological of TL materials, 139
determination, 292-3
Track counting, 160
detection, 152, 159-60
sensitivity, 162
technique, 160
latent, 160
Transfer dating, see Dating
Transfer standard, 384
Transformer, 42
Transit exposure, 198, 216
Transition coefficient, 17
Transition probability, 19, 91
Transitions
radiationless, 17, 29
radiative, 18
Transparency, 145
Trap (centres), 11, 16, 19, 40, 152, 153, 156,
157, 261, 362
creation, 84
depth, 17, 24, 152-3, 373
determination, 375
mechanism, 135
parameters, determination, 24-6
Trapping model, 16
levels, 19
Traps, thermally disconnected, 31
Trap-to-trap migration, 111
Tray, 42, 44
infrared emission, 44
Tribo(thermo)luminescence, 4, 67, 86, 95, 116,
175, 212
elimination, 95
of AL0
3
. 120
ofCaS0
4
: Dy/ Tm, 116
Trichlorethylene, 69, 139
toxicity, 140
Trimers, 103
Tritium, neutron-induced, 192
Tritons, 235, 236
TSC, see Thermally stimulated conductivity
data analysis, 32-6
intensity, 29
shift of maxima, 28, 30, 32
TSEE, see Thermally stimulated exoelectron
emission
Tunnelling process, 374-5
Turntable, 56
Tweezers, mechanical, 74, 138, 212, 213
manipulation of phosphors with, 212
Tweezers, vacuum, 74-5, 138
Two element card, 179
Ultrasonic bath, 139
cleaners, see Cleaners
Ultra-thin bonded discs, 183
Ultraviolet (UV) light, 253
Uncertainty of measurement, 221, 223
of TLD systems for environmental
monitoring, 221
overall, 169, 218-20, 223
Uncertainties
random assessment, 143-4
systematic assessment, 144-5
United States Energy Research and
Development Administration
(USERDA), 197
Uranium, 245
UTB, see Ultra-thin bonded discs
414 Index
UV dosimetry, 8
light, effect of, 212
photo-transfer technique, 176
radiation, discovery, 4
re-estimation, 176
stimulation, 175, 212
Vacancies, 12, 13
Vacancy aggregates, 13
Vacuum
needle, 45, 53, 56
tweezers, see Tweezers
Valence band, 15, 18, 152
Variance, 144
V,-centre, 155
Vj." centre, 13
V^-centre, 27
in alkali halides,
model, 12, 27, 33
VEB RFT-Messelektronik, 65
Vibrator, 71
time-setting, 73
Victoreen Instrument Division, 65, 206
Victoreen TLD reader, 58, 59
Visible light stimulation, see Light stimulation
Volcanic events, dating of, sec Dating
V/O 'Licensintorg', 65
Voltage, 170
Wavelength, 49
Whole-body dose, see Dose
Window, 182, 183, 184, 193
Wblsendorf fluorite, 7
X-rays, 151, 177, 237, 253
discovery and TL, 4, 237
X, t (X, Y) recorder (plotter), 52
Yield, see TL yield
Z-centre, 103
Z
2
-centre, 103
Zero-dose, 86, 175
reading, 69, 146, 170, 173, 174, 175, 176,
178, 192, 198, 200, 201, 202, 204,
212, 216, 219, 220
reduction of, 213
Zinc oxide, ZnS, 252, 253
Zircon dating, see Dating
Zircon inclusion technique, 350
ZnO : Tm, see Zinc oxide
Of related interest
Thermoluminescence
Dosimetry
(Medical Physics Handbooks 5)
A F McKinlay (National Radiological
Protection Board, Chilton, UK)
A concise introduction to the increasing
use of thermoluminescence dosemeters
for the accurate measurement of the
exposure and dose of ionising radiations
used in the diagnosis and treatment of
disease. Covers basic theory, practical
applications of dosemeters, calibration
and operating problems, design and
operation of the associated read-out
equipment.
1981 x+170pp ISBN 0-85274-520-6
Fundamentals of Radiation
Dosimetry
(Medical Physics Handbooks 6)
J R Greening (Royal Infirmary,
University of Edinburgh)
An introductory textbook on the principles
and methods of radiation dosimetry
providing the pertinent information
required by a newcomer to the field.
Particular emphasis is placed on the
special quantities and units encountered
in radiation dosimetry, the relationships
between them, and the principles
underlying their measurement. For
workers in radiation therapy,
radiodiagnosis, radiation protection,
radiation physics and related fields.
1981 xii + 160pp ISBN 0-85274-519-2
Physics in Medicine and
Biology
A monthly journal (from 1982) published
by The Institute of Physics containing
original research papers and review
articles on many aspects of radiation
physics and other topics including TLD
September 1981 issue contains a review
article:
The theoretical and microdensimetric
basis of thermoluminescence and
applications to dosimetry,
by Y S Horowitz, Ben Gurion
University of the Negev, Israel
Subscription enquiries to The Institute of
Physics, Techno House, Redcliffe Way,
Bristol BS1 6NX, UK
^ l^ gg^ iniiiMiiMiiHMA
ISBN 0-85274-544-3

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