06 Gamma Spectrometry

Gamma Spectrometry
Nuclear Energy Division Marcoule center
Fuel Cycle Technology Department
Fuel Technology Development Unit
Characterization and Vizualization

Technologies in DD&R
Gamma Spectrometry
Charly MAHE
charly.mahe@cea.fr
DEN/DTEC/SDTC/LSTD IAEA Practical training workshop Characterization and Vizualization Technologies in DD&R
2011, December 1
Gamma Spectrometry Introduction
Outline
Introduction
CdZnTe : Compact gamma spectrometry probes

Concrete measurements with HpGe detector
Feedback experience
2011, December 2
Objective: identify the g emitting radioelements in a contamination

& compare their relative importance
Result: spectra: interaction distribution in the detector depending on the

energy
x axis: energy (deposited in the detector).
y axis: number of pulses received at a given energy.
600
500
137Cs
400
Counts
60Co
300
40K
200
100
2026
1577
1352
1801
2251
229
454
678
903
1128
0
Energy (keV)
DEN/DTEC/SDTC/LSTD
DEN/VRH/DTEC/SDTC IAEA Practical training workshop Characterization and Vizualization Technologies in DD&R
2011, December 3
Constitution of a spectrometry chain
Detection
Detector - Pre-amplifier
Scintillator + Photomultiplier Production of a pulse whose amplitude
is proportional to the energy deposited
Semiconductor
in the detector
Amplifier Signal shaping
Analog-digital converter Conversion of the analog signal into a

digital value
Multichannel analyzer Recording of the events received in a memory.
Spectrometry software Piloting of the spectrum acquisition, visualization and processing
DEN/DTEC/SDTC/LSTD
2011, December 4
600
500
400
300
200
100
1352
1577
1801
2026
2251
1128
229
454
678
903
0
0
Calibration by modeling
Counts per second at E Fluence rate for a given activity

(1 Bq.g-1)
Fluence rate (E) - ph.cm-2.s-1 u(E)
Activity
(E) / u(E)
DEN/DTEC/SDTC/LSTD
2011, December 5
Characteristics of a detector:
spectrum resolution: measurement accuracy
The width half-way up a peak at a given energy is measured.
600
C o u n ts
500 1000
800
400
600
Counts
300 400
200 200
Energy (keV)
100 0
0
0
0
9
7
5
3
2
50
08
66
24
20
35
51
67
83
99
1352
1577
1801
2026
2251
229
454
678
903
0
1128
11
13
14
16
Energy (keV)
Ge NaI
As a general rule, semi-conductors (Ge) enable better spectrum resolution (factor of 10)
than scintillators (NaI).
DEN/DTEC/SDTC/LSTD
2011, December 6
Characteristics of a detector :
Sensitivity
Depends on the detecting material (density, luminescence yield for scintillators)
- on its volume (the bigger the detector, the higher the probability of a strong interaction,
and the higher the sensitivity)
Implementation constraints ( particularly important in decommissioning)

- footprint/bulk
- cooling (indispensible for the operation of Germanium detectors: liquid N2)
- generally, a dense collimator is used (W, Pb) to limit the field observed
Increase in the total mass of the detector
DEN/DTEC/SDTC/LSTD
2011, December 7
Choice of the detector depends on

The range of energy of the photons:
Low E (E<400 keV)
High E (400 keV<E<1500 keV)
The measurement time: sensitivity - estimation of counting time
saturation risk
The resolution required
Other operating conditions:
freedom of movement
risks of contamination, deterioration etc.
DEN/DTEC/SDTC/LSTD
2011, December 8
Gamma Spectrometry Compact gamma spectrometry probes
Detector requirements:
Compact
Good resolution (FP)
Not cooled
Inexpensive (consumables)
CdTe detectors
10 Gy.h-1 a few 100 mGy.h-1.
DEN/DTEC/SDTC/LSTD
2011, December 9
Gamma spectrometry
Compact gamma spectrometry at air temperature
428 keV - 125Sb
60001 512 keV - 106 Ru/Rh
601 keV- 125Sb 1173 keV - 60Co

50001 1332 keV
1274keV - 60Co
- 154Eu
662 keV - 137Cs
40001 10000
1000
30001
100
20001 10
1
720 820 920 1020 1120 1220 1320
10001
1
400 500 600 700 800 900 1000 1100 1200 1300 1400 1500
Application in endoscopy - Building 214 (Marcoule)

Dose rate: 200 mGy.h-1.
Radionuclides identified : 137Cs (65%) - 125Sb (17%) - 106Ru (15 %)
+ traces of 60Co and 154Eu (1 %)
DEN/DTEC/SDTC/LSTD
2011, December 10
Gamma spectrometry
Compact gamma spectrometry at air temperature
The collimator enables the detector to be shielded from part of the surrounding irradiation.
But it may, more specifically, enable the detector to be focused on a small portion of the
space.
Dense material (Lead or Tungsten)
DEN/DTEC/SDTC/LSTD
2011, December 11
Qualification of compact detectors: CdZnTe
Comparison of Ge / CZT by in-situ measurements
Ge 2 CZT 60 2 CZT 500 2

Spectre BLA319ENRA
(%) (%) (%) (%) (%) (%)
58Co 65,6 1,1 74,2 6.6 76,5 6.8
1,E+06
60Co 11 0,5 9,4 3.3 10,7 4,4

1,E+05
124Sb 5,8 0,4 7,5 3 7,5 3,4
1,E+04
122Sb 1,8 0,2
N (impulsions)
1,E+03 110mAg 8,7 0,4 8,9 3.2 5,3 2,8
1,E+02 95Zr
1,E+01 54Mn 1,7 0,2
1,E+00 59Fe
0 200 400 600 800 1000 1200 1400 1600 1800 2000 1 0,3
Energie (keV)
51Cr 4,6 0,7
DEN/DTEC/SDTC/LSTD
2011, December 12
Gamma Spectrometry CdZnTe / sIGAle
What kind of equipement ?
Gamma spectrometry :
CdZnTe probes (Ritec)
Operating range :
5 Gy.h-1 (500mm3) to 10 Gy.h-1 (0.5 mm3)
Very compact
Acceptable energy resolution (2 keV @ 662 keV)
Not waterproof !
automatic spectrum analysis not advisable (peaks
are skewed)
2011, December 13
Action for EDF/DRD in 2003

- Qualification of EDF detectors
- Creation of a gamma spectrometry measurement interpretation software assistant
- Training of operators in the use of a model system
Objective: Determine the main radioelements on a hot spot
Progress:
- System delivered in 2003 and assessed on sites
- Manual peak framing recommended
- EDF wishes to have an industrial product developed
DEN/DTEC/SDTC/LSTD
2011, December 14
Action for EDF/DRD in 2003
DEN/DTEC/SDTC/LSTD
2011, December 15
sIGAle : System of Identification of Gamma Activities at Low rEsolution
CdZnTe detectors
Compact gamma spectrometry detectors
Usable at air temperature
Resolution between Ge and NaI (2% at 662keV)
10 Gy.h-1 (detector 500 mm3) 8 Gy.h-1 (detector
0.5 mm3)
Implementation on dismantling worksite
(single spectra, high irradiation level, accessibility
problem)
Spectra with di-symetric peaks

Problem of analysis representativity
DEN/DTEC/SDTC/LSTD
2011, December 16
Easy-to-use specific software to analyse photoelectric peak in

CdZnTe Spectrum : SIGALE
Automatic peak analysis and

Gamma spectrum - 900 s - 20 mm3 probe
symetry corrections
45000
2500
40000
2000
35000
30000 1500
counts
25000 1000
co u n ts
20000
500
15000
0
0 20 40 60 80 100 120 140 160
10000
5000
0
0 200 400 600 800 1000
channels
Example of Gamma spectrum with a compact CZT probe : 60Co and 51Cr detected
900s
2011, December 17
Application range
CZT detectors volume from 0.5 mm3 to 500mm3
Important peak dissymmetry and presence of shape peak
Resolution/energy calibration different from HpGe

detectors
Poor statistical signal and high level of noise (important

Compton contribution to the spectrum)
2011, December 18
Peak detection
Calibration (K(E), activity)
Photon flux
Schedule :
2008 : final tests and in situ Reproductible analysis

qualification Specfic algorithm
2009 : industrialization User-friendly html interface
2011, December 19
Gamma Spectrometry Concrete measurement
Decommissioning process is based on waste zoning, method asked

by the Safety Authority
Implies an a priori knowledge of contamination levels and thickness
Measurements are used to support this a priori knowledge
At the moment Tomorrow???

coring Measurement of the contamination depth of nuclides
in concrete using spectrometric methods
Destructive Non destructive
Heavy Easy implementation
implementation Fast analysis
Long analysis
BUT
Reliability???
Costly process Benefit/coring???
2011, December 20
Gamma activity
Objective
Contamination depth
assessment from surface
A? d?
spectrometric measurement
Depth
Stakes
Decommissioning mastery
Optimisation of waste
management
Compliance with the

safety authorities
request
2011, December 21
Gamma activity
Objective
Contamination depth
assessment from surface A? d?
spectrometric measurement Depth
Stakes
Decommissioning mastery 0 .7
m a in s p e c tr a ( m )
d iffe r e nc e s p e c tra ( m -d )
0 .6 E1
E2
0 .5 a d d itio n a l s p e c tr a ( d )
N(E), r. u.
0 .4
0 .3
0 .2
Optimisation of waste 0 .1
0 .0
0 .0 0 .2 0 .4
, M e V
0.6 0.8 1.0
management
Compliance with the

safety authorities
request
2011, December 22
Context : Measurement technique based on

radiometric instruments to estimate 137Cs et 60Co
penetration depth in concrete
2005 Specific agreement aspects
Principle and method from Kurchatov Institute
First trials and evaluation (with KI software)
Common development of a full system (with Hpge detector)
Technical visit in France, system calibration
First in situ qualification : Grenoble and EDF (Brennilis)

2008
2011, December 23
Objective :
Adapt a method to give the best estimate of concrete
contamination using an HpGe detector
Detector
Table
Collimator
Concrete
2011, December 24
Summary of the method principles [1]

0.7
main spectra (m)
0.6
difference spectra (m-d)
E1
E1, N1 : Definition of a compton area
E2
0.5 additional spectra (d)
E2, N2 : Photoelectric peak

N(E), r. u.
0.4
0.3
Study of the variations of N1,N2 = f(Z,A), Z :
0.2
penetration depth A : total activity
0.1
0.0 Only 137Cs and 60Co depth estimation

0.0 0.2 0.4 0.6 0.8 1.0
, MeV
1.4 Various distribution profiles (exponential,

1.2 power-functions )
1.0
N1/N01, N2/N02
N2/N02
N1/N01 Results : both depth estimation and surface
0.8
activity of the area containing 80% of the total
0.6
activity
0.4
0.2 [1] Method and device to measure Cs137 soil contamination in-situ,
0 1 2 3 4 A.V. Chesnokov, A.P. Govorun, V.N. Fedin, O.P. Ivanov, V.I.
Z0, mfp Liksonov, V.N. Potapov, S.B. Shcherbak, S.V. Smirnov, L.I.
Urutskoev, Kurtchatov Institute, may 1998.
2011, December 25
Background influence analysis for

each measurement point Objectives :
Adapt this technique to low-level contamined
Discrimination of scattered and concrete
unscattered radiation from the
contamined layer Focus the framework on the mathematical
simulations (calculation parameters)
Different profiles of radionuclides Test the method for different kind of detectors
depth activity distribution
[1] Method and device to measure Cs137 soil contamination in-situ, A.V. Chesnokov, A.P. Govorun, V.N. Fedin, O.P.
Ivanov, V.I. Liksonov, V.N. Potapov, S.B. Shcherbak, S.V. Smirnov, L.I. Urutskoev, Kurtchatov Institute, may 1998.
2011, December 26
1st step : devices definition and modelling

MCNP model of the HpGe detector
MCNP modelling spectrum compared with experience
100
Spectre exprimental avec bruit de fond Validation (laboratory/modeling
Spectre du bruit de fond
Spectre exprimental sans bruit de fond

tests)
10 Spectre modlis avec MCNP
Integrated to KI software
Nb coups/s
1
0,05 0,15 0,25 0,35 0,45 0,55 0,65 40% HpGe detector
0,1
Both MCNP and specific
0,01
software modeling (Monte-Carlo)
0,001
Energie (MeV)
2011, December 27
MCNP - calculation code to calibrate the system for 3

profiles :
- exponential
- linear
- Dirac (ideal surfacic contamination)
2 kinds of concrete
Response from a 1 to 15 cm contaminated
layer
Need initial laboratory calibration of the
detector
2011, December 28
MATLAB development of 2 software modules
Calculation module Analysis module
2011, December 29
MATLAB Calculation module
Build the simulation function

Z0 = f(G/A) based on MCNP
models
Parameters :
profile
number of simulation files
(depending on the
contaminated layer)
E1min : lower bound of the
Compton part of the
spectrum
2011, December 30
MATLAB Analysis module
Gives the best estimation of Z0

from the experimental spectrum
Parameters :
Gnie 2K parameters
E1min : lower bound of the
Compton part of the
spectrum
Simulation files
2011, December 31
2nd step : Mechanical development and laboratory calibration
HpGe Collimator
Detector parameters and performances

evaluation
Full system measuring
Developement of a specific collimator
System calibration on large surfacic
reconstructed sources (137Cs & 60Co)
(Marcoule June 2007)
Parameters added to KI analysis software
2011, December 32
3rd step : First in situ trials : CEA GRENOBLE
1st in situ qualification in Grenoble

Poor statistical signal
Noise influence
Good implementation and on-line analysis
A 137Cs
N Mesure (KBq/m2) Z (cm)
5 44.3 14.5
6 22.6 5.5
7 38.8 14
First results from KI software associated 8 26.1 6.55

with the HpGe MCNP model 11 61.3 17.7
2011, December 33
3rd step : First in situ trials : EDF BRENNILIS

19 measurement points
Intercomparison with concrete samples
(realized by 2 destructive methods)
Uncertainty due to the surface of the
ground
Dose rate distribution of the sample points

Measurement points localization
2011, December 34
Good implementation of the system (acquisition time ~ 30

min/sample)
Good SNR for a majority of spectrum
Majority of 137Cs contamination, slight traces of 60Co
2011, December 35

N sample L0 (cm) L1 (cm)
3 0 8,635
4 0,55 16,5
5 1,87 16,5
6 0 11,22
8 0 6,93
9 0 2,31
11 0 10,34
To be compared with
12 0 7,15
classical sampling
13 0 10,34
technics
14 0 4,29
15 0 5,115
To be compared with
17 0 11,66
advanced sampling
18 0 2,365
technics
19 0 9,24
2011, December 36
EDF BRENNILIS / Results

In situ measurements from EDF Brenilis plant
Poor influence of the profile

(linear vs exponential)
Comparison with concrete
corring results from EDF
Measurements points 06 08 09 11 12 14 15 17 18 19
Z0 Exp. profile 9.7 8.1 3.2 9.6 9.9 5 4.6 10.6 4.3 9.7
CEA soft
(cm) Linear 9.4 8 3.5 9.3 9.6 5.2 4.9 10.2 4.5 10
profile
2011, December 37
2011 : in situ trials on UP1 plant (MAR200 dissolution of fission

products : contamined room)
Dose Rate mapping : location of interest points

2011, December 38
2011 : in situ trials on UP1 plant (MAR200 dissolution of fission

products : contamined room)
Point of interest DED at 45cm from the Detector

ground (mSv/h)
A 0,2 NaI et CZT500
B 1,3 CZT500
C 1,9 CZT500
D 2,7 CZT500
E 0,5 NaI et CZT500
F 0,4 NaI et CZT500
G 0,5 NaI et CZT500
H 1,5 CZT500
2011, December 39
Gamma spectrometry :
2 detectors :
NaI scintillator 1p*1p
CdZnTe 500mm3
2 measurement positions :
Low position : 200mm from the ground
Position haute : 500mm from the ground
Collimator configurations :
Backgound substraction
Teleoperated collimator system
OPEN CLOSING CLOSED

2011, December 40
NaI Detector :
Monte-Carlo model of the detector
Model validation on point-like sources (in laboratory)
Comparaison between simulated spectra and measured spectra
Comparaison spectre solution finale et spectre rel

1600 NaI
1400
Spectre modlis
Spectre rel
1200
Lead shieldind
1000
Coups
800
600
400
200
Source
0
25 75 125 175 225 275 325 375 425 475 Concrete
Canaux
=> Difference < 5%
2011, December 41
NaI Detector :
Calibration Z0 = f(G/A) and G*/G = Kcor (G/A) :
Exponential profile
Standard concrete (d = 2,35 g/cm3 without iron)
Z0 = f(G/A) G*/G = Kcor (G/A)
2011, December 42
Gamma Spectrometry Feedback experience
Characterization of the crosse GV de PHEBUS (CEA Cadarache)
Objective: identification of the radioelements, modeling by gamma

scanning, calculations of activity + uncertainties.
2011, December 43
Principle of gamma scanning
N sections - N measurement points
Acquisition of N Modeling of NN
spectra transfer functions
Vector D (j) Matrix M (i,j)
A = Ai =
i i
[M
j
1
(i, j ) D j ]
Calculation of total
activity
Sum of the activities per
tranche slice/cut?
2011, December 44
1st step: choice of the detectors + collimator
3 CdZnTe probes on board

(5 20 - 60 mm3)
= a wide measurement dynamic
Collimator dimensioned to obtain a 1 to 2 cm

resolution (90% contrast)
2011, December 45
2nd step: Efficiency calibration
2011, December 46
3rd step: Calculation of the transfer function matrix under MERCURE
Geometry
Matrix 35 35 A = M-1F
Source term
2011, December 47
3rd step: Calculation of the transfer function matrix under MERCURE

in .s-1.Bq-1
2011, December 48
4th step: Measurements (65 spectra)
Entry vector for the

calculation of activity
2011, December 49
5th step: Activity calculations
Section n1: 0.85 TBq
Section n2: 2.90 TBq
Activity profile by Total 137Cs activity: 3.75 TBq

section
2011, December 50
Inspection of the PETRUS line - CEA Fontenay-Aux-Roses
Objective: identification of the radioelements, characterization by

surface gamma spectrometry, gamma imaging
2011, December 51
-Dimensioning of the collimator

-Choice of the probe + Efficiency
calibration
- Digital calibration: transfer function
under MERCURE calculation code (CEA)
- vessel mapping in Bq.cm-2
2011, December 52
Complete system: (CEA

patent)
CdZnTe
Color camera
DR
-Inspection by gamma imaging coupled

with a system of laser pointer and
Laser pointer
collimated CdZnTe probe, Gamma
camera
-Modeling under MERCURE
2011, December 53
Characterization of the AVM FP vessels
Step 1: Identification of the hot spots by imaging
2011, December 54
Step 2: Collimated fluence rate profile or of collimated dose rate
2011, December 55
Step 3 : Calculation of the hot spot activity Ak and of the

homogeneous background activity Ai (modeling of a transfer matrix
under MERCURE)
Act. (MBq)
0,00E+00
1,00E+08
2,00E+08
3,00E+08
4,00E+08
5,00E+08
6,00E+08
7,00E+08
8,00E+08
9,00E+08
1
2
3
4
5
6
Activits par tranche

7
8
9
N tranche
10 1112
13
14
15
16
17
Fond homogne
Point n6
Pulseur
18
19
20
Calculation of the activity section by section and of the total activity:
Atotal = kAk + iAi
2011, December 56
Step 4 : Check the calculation by an inversed model and

comparison with the ambient dose rate
If standard deviation < criteria (e.g.10%) validation of the modeling
2011, December 57
EDF : Caracterization of mud by gamma-scanning

(CdZnTe Spectro, Dose rate measurement, collimated / uncollimated measurements, radiological
moedl)
Comparaisons 3 puits
1,00E+12
9,00E+11
8,00E+11
7,00E+11
6,00E+11
Activit (Bq) 5,00E+11

4,00E+11
3,00E+11
2,00E+11
1,00E+11
0,00E+00
1 Puits C1
2 3 Puits C3
4 5 6 7 Puits C2
Ntranche 8 9
Puits C2
10 Puits C3
Puits C1
EDF ( Saint-Laurent powerplant )
2011, December 58
Final control of wall and ground with HpGe
200
180
160
140
120
100
80
60
40
20
0
0 200 400 600 800 1000 1200 1400
E ner gi e
Ge 40 % detector
Acquisition time : 3 min
+ collimator
Observed surface : 4 9m
DL 137Cs 60 Co : 0.1 Bq.g-1
2011, December 59
Concrete measurements with LaBr3 and HpGe
LaBr3
Ge
Ex. Gutter measurements with

LaBr3
Ex. Gutter measurements with

HpGe
Application of high resolution gamma
spectrometry (Ge) and low rsolution (LaBr3)
2011, December 60

06 Gamma Spectrometry

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06 Gamma Spectrometry

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Gamma Spectrometry

Nuclear Energy Division Marcoule center

Fuel Cycle Technology Department

Fuel Technology Development Unit

Characterization and Vizualization

CdZnTe : Compact gamma spectrometry probes

Objective: identify the g emitting radioelements in a contamination

Result: spectra: interaction distribution in the detector depending on the

Constitution of a spectrometry chain

Amplifier Signal shaping

Analog-digital converter Conversion of the analog signal into a

Multichannel analyzer Recording of the events received in a memory.

Spectrometry software Piloting of the spectrum acquisition, visualization and processing

Counts per second at E Fluence rate for a given activity

Implementation constraints ( particularly important in decommissioning)

Increase in the total mass of the detector

Choice of the detector depends on

60001 512 keV - 106 Ru/Rh

601 keV- 125Sb 1173 keV - 60Co

Application in endoscopy - Building 214 (Marcoule)

Dense material (Lead or Tungsten)

Qualification of compact detectors: CdZnTe

Comparison of Ge / CZT by in-situ measurements

Ge 2 CZT 60 2 CZT 500 2

60Co 11 0,5 9,4 3.3 10,7 4,4

1,E+03 110mAg 8,7 0,4 8,9 3.2 5,3 2,8

1,E+01 54Mn 1,7 0,2

51Cr 4,6 0,7

What kind of equipement ?

Qualification of compact detectors: CdZnTe

Action for EDF/DRD in 2003

Objective: Determine the main radioelements on a hot spot

Qualification of compact detectors: CdZnTe

Action for EDF/DRD in 2003

sIGAle : System of Identification of Gamma Activities at Low rEsolution

Spectra with di-symetric peaks

Easy-to-use specific software to analyse photoelectric peak in

Automatic peak analysis and

sIGAle : System of Identification of Gamma Activities at Low rEsolution

CZT detectors volume from 0.5 mm3 to 500mm3

Important peak dissymmetry and presence of shape peak

Resolution/energy calibration different from HpGe

Poor statistical signal and high level of noise (important

sIGAle : System of Identification of Gamma Activities at Low rEsolution

2008 : final tests and in situ Reproductible analysis

Decommissioning process is based on waste zoning, method asked

Measurements are used to support this a priori knowledge

At the moment Tomorrow???

Compliance with the

Compliance with the

Context : Measurement technique based on

2005 Specific agreement aspects

Principle and method from Kurchatov Institute

First trials and evaluation (with KI software)

Common development of a full system (with Hpge detector)

Technical visit in France, system calibration

First in situ qualification : Grenoble and EDF (Brennilis)

Summary of the method principles [1]

E2, N2 : Photoelectric peak

0.0 Only 137Cs and 60Co depth estimation

1.4 Various distribution profiles (exponential,

Background influence analysis for

1st step : devices definition and modelling

MCNP modelling spectrum compared with experience