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J. Environ. Radioacrivity, Vol. 33, No. 3, pp.

195-212, 1996
Copyright 0 1996 Elsevier Science Limited
Printed in Ireland. All rights reserved
0265-931X(95)00098-4 0265-931X/96 $15.00 + 0.00
ELSEVIER

Estimating and Accounting for 13’Cs Source Burial through


In-Situ Gamma Spectrometry in Salt Marsh Environments

A. N. Tyler,” D. C. W. Sandersor? & E. M. ScotV


OThe Department of Environmental Science, University of Stirling, Stirling FK9 4LA, UK
‘The Scottish Universities Research & Reactor Centre, East Kilbride, Glasgow G75 OQU,
UK
“The Department of Statistics, University Avenue, University of Glasgow. Glasgow
G12 8QQ, UK

(Received 31 March 1995; accepted 8 December 1995)

ABSTRACT

The use of in-situ gamma ray spectrometry provides a means of rapidly


estimating environmental radioactivity inventories. However, one of the
principal limitations of this technique has been the injluence of variations in
vertical activity distribution on the observed photon jluence. This paper
demonstrates that the quantification of the forward scattered ratio of the
spectrum (Q) can be used to: (i) estimate the mean mass depth (p) of the
vertical activity distribution within sediment profiles, and (ii) provide a
calibration correction coefficient for in-situ gamma spectrometry in envir-
onments which exhibit variable and non-exponential activity distributions,
such as salt marshes around the Irish Sea. This paper presents a succes$il
application of a spectrally derived calibration correction coefficient to in-
situ spectra from a salt marsh at Caerlaverock, Dumfries, SW Scotland,
improving the correlation between soil core and in-situ derived activity
estimates from r2 = 0.097 (uncorrected) to Y’ = 0.801 (corrected). The
scope for extending this approach to a wider range of environments, to
airborne gamma spectrometry and to measurements of sedimentation rates
is considered. Copyright 0 1996 Elsevier Science Limited

INTRODUCTION

In-situ gamma ray spectrometry is a widely used tool for the rapid esti-
mation of natural and anthropogenic radioactivity (e.g. Beck et al., 1972;

195
196 A. N. Tyler et al.

Helfer & Miller, 1988; Miller et al., 1990; ICRU, 1994). However, a criti-
cal limitation of this approach relates to the need to know the extent of
self shielding, due to the vertical activity distribution, in order to deter-
mine the relationship between measured gamma ray fluence rates and
estimated activity concentrations.
In conventional treatments an idealised exponential activity distribution
with depth has frequently been adopted, described either in terms of the
reciprocal of relaxation length CX, cm-’ (Beck et al., 1972) or in terms of a
mass depth coefficient, p = p/a, g cm-2 (ICRU, 1994). In either case the
vertical activity distribution is represented by a single parameter whose
value is either assumed for a given application or determined by labora-
tory analysis of core samples. This approach may be considered proble-
matic from two perspectives: (i) the activity distribution in the
environment may not in fact generally follow an exponential form; and (ii)
the need for independent determination of calibration data limits the
status of in situ spectrometry as an absolute method.
Two solutions to this latter problem have been proposed: (i) based on
differential attenuation of linked gamma ray emission lines from certain
sources (e.g. Rybacek, 1992, Miller et al., 1994); and (ii) the use of infor-
mation derived from the scattered gamma ray spectrum (Zombori et al.,
1992a, b; Tyler, 1994). The second of these approaches has the advantage
of relying on a single full energy peak.
Zombori et al. (1992a, b) proposed the use of the relative intensities of
forward scattered radiation, observed in the valley between the Compton
edge and the full energy peak of an individual gamma ray line, and the full
energy peak of the same gamma ray as a means of quantifying the extent
of source burial. Narrow beam experimental results were presented based
on a 13’Cs point source under a variable depth water tank to support this
suggestion. Consideration was also given to the problem of a non-expo-
nential activity distribution described empirically as the sum of two expo-
nential terms.
This paper presents the results of laboratory investigations of the
forward scattering ratio (Q) in broad beam geometry which confirm the
existence of a systematic relationship between mean mass depth (b) of a
given source under conditions more closely related to field geometries than
Zombori’s original experiments. Results are then presented of a field
assessment of the method applied to a coastal salt marsh at Caerlaverock
in the inner Solway region of SW Scotland. The study site is an example of
an environment where progressive accumulation of anthropogenic activity
has occurred as a result of past BNFL Sellalield derived marine dischar-
ges. This has led to the development of strongly non-exponential activity
distributions exhibiting both pronounced subsurface maxima and
‘37Cs source burial in salt marshes 197

systematic spatial variations within the site. Investigations were conducted


to assess the potential of the forward scattering approach for estimating
mean mass depth and for improving the accuracy of in-situ determinations
of activity per unit area in these salt marsh environments.

PRINCIPLES AND DEFINITIONS

The full energy peak to forward scattered ratio

Zombori et al. (1992a, b) demonstrated the build-up of secondary scat-


tered y photons in the valley region (between the full energy peak and
Compton edge) relative to the full energy peak for a point 137Cs source
buried beneath a tank of water over a range of water depths. In principle,
the extent of forward scattering is systematically related to the interaction
probability associated with the photon trajectory between source and
detector and hence to the amount and type of material intervening. Thus
the amount of forward scattering relative to the size of the full energy
peak will provide a measure of the extent of source burial.
Figure la identifies the valley region between the ‘37Cs full-energy
peak and the Compton edge of a y ray spectrum, and indicates the
origins of its principal contributions. Examples of interactions corre-
sponding to these spectral contributions are also shown schematically in
Fig. l(b). Given constant detector characteristics, source configuration
and ground clearance, the spectral contributions from multiple Comp-
ton scattering within the detector crystal prior to photon escape (b,),
and from forward scattering interactions in the source and air path (bz)
are proportional to the source activity, and thus also to the full-energy
peak intensity (A). However, as source burial increases, the contribu-
tions to the valley region from forward scattering of primary gamma
photons within the soil (bz) will increase relative to the size of the full
energy peak. Thus the spectral step (Br) will increase relative to the area
under the full energy peak (A).
This approach to estimating source burial provides only a single para-
meter (Q) with which to describe the source depth, where Q is given by:

In general it may be expected that environmental source profiles are


better described by two or more parameters as protile shapes may vary
considerably in addition to the overall depth. However, at present Q
potentially provides a means of monitoring variations in mass depth for
198 A. N. Tyler et al.

b)

n- A
bl

SURFACE

so so 100 120 140 160 180


Channel Number

Fig. 1. The Contributions to a 13’Cs spectrun. Net spectrum collected from a 13’Cs planar
sheet buried by three perspex sheets. The full energy peak A is a result of full 13’Cs gamma
photon interactions through multiple Compton scatter and photoelectric absorption in the
detector. The valley step Br has contributions from multiple Compton scatter within the
detector prior to escape (61) and forward scatter through inelastic interactions with orbital
electrons of atoms in the soil followed by full interaction in the detector (bz). Maximum
energy transfer through a single Compton interaction results in the Compton edge C.

an activity distribution which retains its essential shape from place to


place. The purpose therefore of this paper is to examine the extent to
which measured forward scattering ratios can be related to a single
measure of activity distribution, i.e. the mean mass depth of the source.

Mean depth and mean mass depth for a generalised activity distribution

The approximation of the exponential decrease of activity with depth was


introduced by Beck et al. (1972) where the parameter a (cm-‘) was defined
as the reciprocal of the relaxation length of the exponential distribution,
such that:
A = A, . e-az (2)
where z is linear depth (cm) and A, is the activity measured at the surface
(Bq kg-‘). However, fluence rates in soil are a function of the soil density
in addition to source depth z. Thus, source burial may, by preference, be
quantified in terms of mass depth or mass per unit area (gem-*) which is
given by pz (ICRU, 1994; Rybacek et al., 1992). Given that the soil
density p varies with depth, and the depth intervals selected also tend to
vary, then the combined effect will lead to further variations in pz within
the soil column. The function mass per unit area, defined as r, is given by
eqn (3):
137Cs source burial in salt marshes 199

5= ‘p(z’)
dz’ (3)
s0
where r is the total mass depth or effective mass per unit area (gem-2).
If activities are expressed in Bq m-*, integration of activity for each
unequal depth division may lead to biasing in the observed activity profile.
Thus activities within each layer should be expressed in terms of activity
per unit mass (e.g. Bqg-‘).
The relaxation mass per unit area or mean mass depth is defined as fi,
which is equivalent to p/a. Then from eqn (2), and as defined by ICRU
(1994), the activity distribution with depth A(t) (Bq g-‘) is given by
eqn (4):

A(<) = Ao. e(9)

Such exponential distributions have mean values of a-’ (eqn (2)) and /I
(eqn (4)). However, the assumption of the exponential model is a gener-
alisation which is more often than not inaccurate, particularly for aged
deposits of longer lived radionuclides such as 137Cs, where post deposi-
tional processes or multiple deposition events can lead to the development
of subsurface activity maxima within the soil depth profile. In salt marsh
environments, as shown below in Fig. 2, the assumption of the exponen-
tial proIile breaks down completely. For such non-exponential cases, it is
suggested that the mean mass depth (p) may also be a useful measure of
source self shielding in a general case. In this case /I should be obtained by
evaluating the mean ratio from eqn (5):

where r is the mass depth (gem-2) and A(t) is the activity per unit mass
(Bq g-l).

METHODS

Laboratory simulations

Zombori et al. (1992a, b) modelled the spectral response of source burial


with a narrow beam geometry from a 137Cspoint source. In order to simu-
late the scattering contributions due to source burial for a general profile,
r
A. N. Tyler et al.

12 01 53 34

1
W/g
I.
0.0 0.4

wg
‘I
0.8 0.0 0.4

Ws
0.8
/

0.0
"

_---
0.4

W/g
0.8 0.0
7
0.2

wl
0.4

Fig. 2. Caerlaverock mass depth 13’Cs profiles: 14 (7.20gcmS2), 12 (10.78gcmm2), 01


(11.24 gcme2), 53 (13.23 cme2), 34 (20.7 gcmm2) and 44 (26.50 gcmm2). See Fig. 3 for
sample locations.

under broad beam conditions more appropriate to field geometries, a


laboratory experiment was conducted with an extended 1 m* ‘37Cs source.
For the laboratory based modelling, a ‘37Cs extended layer source was
constructed by painting 40.67 kBq f 4% of spiked emulsion paint onto a
1 x 1 x 0.01 m plywood sheet and sealing the activity with vinyl and
polyurethane paints (Tyler, 1994). Uniformity was checked using a colli-
mated gamma ray spectrometer and found to be within approximately 5%
of the mean activity over 1Ocm dimensions. Absorber materials were
chosen after calculating the relationships of pL, with energy (30-3000 keV)
for a variety of readily available materials, including plaster board, wood,
polythene, polystyrene and polymethylmethacrylate (perspex). Perspex
was chosen as the attenuating medium as it was chemically easier to define
than wood and most closely resembled pm of peat, soil, water and air for
energies above about 200 keV (Tyler, 1994).
A Bicron 3” x 3” NaI(T1) detector coupled to a Canberra Series 10p’us
MCA was used to collect spectra from 30 keV to 3000 keV into 512 chan-
nels. Twenty 1 m* perspex sheets were placed on a background calibration
pad and a background spectrum was collected at the centre with the 20
perspex sheets (total thickness 20cm) separating the detector from the
pad. The top sheet was then removed and replaced by the ‘37Cs sheet and
another spectrum collected from the same position. The 13’Cs sheet was
then moved down one sheet in the profile so that it was covered by one
perspex sheet and another spectrum was collected. This was repeated until
the 137Cssheet was buried by 19 perspex sheets.
137Cs source burial in salt marshes 201

TABLE 1
The Regions of Interest for the Series 10PiuSMCA and 3” x 3” NaI(TI) Detector (Tyler,
1994)

Radionuclide Channel numbers Peak position Energy range ke V

‘37CS 97-131 114 563.3760.7


‘34cs 126150 138 6464-769.6
40K 218-267 243 1332-1606
214Bi 267-3 13 290 162&1900
“*Tl 383-470 427 235&2884

After each spectrum was collected, the region of interest data (Table 1)
for a ‘37Cs window was noted to determine counting statistics. Counting
times were adjusted to keep counting precision better than 3%. Typical
count times varied from 300s for the surface sheet to 2000s for 19 sheets
of burial. Full spectra and region of interest data were transferred to
personal computer and analysed using software written in-house.
The background spectrum was subtracted from each spectral measure-
ment. From these net spectra, the valley height BT was calculated as the
difference between the mean counts across channels 88-100 (500-575 keV)
in the valley, and channels 126-130 (736760keV) to the right of the
photopeak (Fig. l(a)). The full energy peak area (A) was integrated over
the channels 97-131 (Table 1, Fig. l(a).

Field observations

Airborne y ray surveys have demonstrated the spatial extent of the accu-
mulation of Sellafield derived activity on estuarine sediments and salt
marshes in the Solway region of the Irish Sea (Sanderson et al., 1992,
1994). The study site discussed here is from a salt marsh from the inner
Solway at Caerlaverock National Nature Reserve (Fig. 3). A series of soil
samples and in-situ spectra was collected from this site in 1992 at the same
time as an airborne survey of the surrounding area. The sampling pattern
adopted (Tyler et al., 1996) was selected to enable both lateral and vertical
distributions to be investigated and includes a transect orthogonal to the
coastline along which detailed investigations were made of the vertical
activity profile.
In-situ measurements were made with the same 3” x 3” NaI(T1) detector
as described above. The detector was supported by a tripod at 1 m above
the ground and spectra were acquired over an 800s period.
In an attempt to eliminate the scattered contribution to the valley
region, full spectral stripping of spectra collected in the field was under-
202 A. N. Tyler et al.

Tidal Barrier

Solway c 0 (I s I
Position 01 at ceotreof hexagc

Fig. 3. Map showing the hexagonal sampling plan at the Caerlaverock salt marsh.

taken using reference spectra collected from 1 x 1 x 0.3 m concrete cali-


bration blocks (purchased from the Geological Survey of Canada). The
calibration pads were separately spiked with uranium, thorium and
potassium. An additional background pad (concrete pad without a spike)
was used to provide background spectra which were subtracted from the
spectra collected on the reference pads to provide reference spectra of I-J,
Th and K. These reference spectra were used to derive stripping coeffi-
cients for regions of interest data (Table 1) and for full spectral deconvo-
lution from the composite spectra collected in the field in proportions
dictated by the net full energy peaks using the standard method (e.g.
IAEA, 1991; Grasty, 1981).
Following background subtraction and full spectral stripping, the valley
step was estimated from the net spectra (e.g. Fig. 4) using a slightly
modified mean count rates within the valley region to avoid potential
from ‘34Cs over stripping. The size of the valley step BT was estimated
from the difference in the mean count rates across channels 88-95 (500-
540 keV) in the valley region and channels 126130 (736-760 keV) in the
region to the right of the full energy peak (Fig. 4). The area (A) was given
by the integrated area under the full energy peak, and Q was calculated
from eqn (1).
137Cs source burial in salt marshes 203

4.0 ,., ,,/,~ ,,, ,,I ,. ,,, ,,I,,, ,,I ,,,I,, ,,, ,I ,,I

- CAER01Speclrum
---Shipped6pect~m

0.0
60 60 100 120 140 160 160

Channel Number

Fig. 4. The ‘37Cs portion of a typical spectrum collected at the centre (position 01) of the
calibration site at Caerlaverock and also shows the same spectrum after stripping out the
Th, U, K and ‘34Cs contributions.

Sediment samples

Thirty-one sediment samples were collected at the Caerlaverock calibra-


tion site in Dumfries, Scotland from the hexagonal sampling plan shown
in Fig. 3. A 105mm diameter adapted golf hole corer was used for
sampling (Tyler, 1994; Tyler et al., 1996). Undisturbed samples were
collected to 30cm depth. It was estimated that under the prevailing sedi-
mentary characteristics, over 90% of the total ‘37Cs photon fluence origi-
nates from the top 30cm of sediment (Tyler, 1994). Six of these soil cores
(14, 12, 01, 53, 34 and 44, Fig. 3) were sectioned in the field into a
combination of 2- and 5 cm intervals. These samples represented a transect
across the salt marsh perpendicular to the coast line which was thought to
provide the greatest variation in ‘37Cs depth distribution characteristics.
In addition, one of these cores (53) was collected off-centre from this
transect to provide a check in the spatial extent of this trend. The
remaining 25 cores were sectioned into 15 cm intervals. The samples were
then weighed wet, dried at between 40 and 60°C and reweighed. The
samples were ground in a 1 kg capacity mixer mill and placed in counting
containers of standard geometry (150 cm3) and sealed with laboratory
sealing film. After a minimum of 3 week’s storage time, the samples were
counted on laboratory-based high resolution hyper-pure germanium
(HPGe) detectors for 40-80 ks and activities for a range of radionuclides
were quantified using Canberra Spectran AT software. The efficiency
calibration was determined using a range of deeply buried soils spiked
with an Amersham QCY 46 mixed gamma spike. Corrections for indivi-
204 A. N. Tyler et al.

dual density variations were made and the analytical performance verified
using IAEA Soil 6 and NBS SRM 4353 standard reference materials.
The 137Csdepth distribution profiles were estimated by plotting activity
concentration (Bq g-‘) against depth intervals (e.g. Fig. 2). The mean
mass depth /? was estimated by rebinning the mass depth profile into equal
intervals (1 gem-‘) and completing the numerical integration, from
eqn (6).

(6)

where A(t) is the activity (Bqg-‘) and A[ are equal mass depth intervals,
of the order of 1 g cm-*.

RESULTS

Laboratory simulations

The Poisson error on the estimates of Q was calculated from 1 Q standard


deviations within each region. The error on the area under the full energy
peak A, was calculated in terms of counting statistics and ranged from 0.6
to 2.5%. Statistical errors on Br for individual observations range from
about 11 to 27% and thus determine the error on Q. These error contri-
butions could be reduced with increased detector live time.
The relationship between Q and source burial for layered activity
(number of sheets) is shown in Fig. 5. There is a clear exponential rela-
tionship described by eqn (7):

LogN = 1445 - OaO123Q (7)


where N is the number of sheets. Thus Q has a direct quantitative relation-
ship burial of a planar sheet, a geometry which includes angular contribu-
tions not represented in the original point source experiments of Zombori.
The same data set can also be used to simulate other distributions, for
example exponential and gaussian distributions, with the same value of p
and total activity. Such simulations have been undertaken and resulted in
significantly different values of Q, demonstrating the importance of source
burial shape on such potential spectral determinations (Tyler, 1994). Thus,
in the absence of a second spectrally derived parameter to help describe
‘37Cs source burial in salt marshes 205

+
0 20 40 60 00 100 120 140

Fig. 5. The change in Q with number of perspex absorber sheets (r2 = 0.991).

source burial shape, this technique can only be effectively applied to


environments where there are known systematic changes in source burial,
as determined from soil core samples, within a general profile shape.

Evaluation of p from the sediment cores

The ‘37Cs activities per unit area determined from the 31 core samples
taken from Caerlaverock ranged from 26 to 120 kBqm-* with effective
average values for comparison with in situ and airborne observations of
77-84 kBq m-* (Tyler et al., 1996). A substantial proportion of ‘37Cs
activity from all cores was observed below 15cm depth. Figure 2 shows
the vertical activity profiles of the six cores which were selected for more
detailed investigation arranged in sequence of decreasing distance from
the shore. Estimates of mean mass depth (j3) were determined from eqn 6,
and the results are shown in the caption of Fig. 2. All profiles show non-
exponential distributions with a pronounced subsurface maximum, and a
general increase in fi towards the near shore environment reflecting a
greater sediment accretion rate close to the coast. Similar evidence of
systematic variations in source distribution with proximity to the coastal
margins has also been observed on other salt marshes in the Solway
(Allen, 1994, MacKenzie et al., 1994).

Determination of source burial through in situ gamma spectrometry

Table 2 gives the data extracted from in situ spectra measured on the six
transect locations with known fi values, and used to determine Q values.
206 A. N. Tyler et al.

Figure 6 shows the relationship between Q and /?, which is given by


eqn (8):
Loga = 2.39 - 0.0346Q. (8)
The error bars in Fig. 6 are given at 1 0. Ninety-five per cent confidence
limits for the line of best tit are also indicated. The relationship is highly
correlated on a log-linear basis (r2 = O-98) over a range of b from 7 to
26 g cmP2. This confirms that the forward scattering ratio can be used to
estimate source burial parameters across the Caerlaverock site with its
substantial variations in depth distribution.
Use of this relationship enables the mean mass depth (/I?)of the other 25
sampling and in-situ measurement locations at Caerlaverock to be esti-

TABLE 2
Mean Mass Depth (j?) Values from the 6 Transect Locations and Full Energy Peak to Step
Ratios (Q) Derived from Associated In Situ Spectra

P Net peak Mean Mean Valley step Q


(g Cm-2) area valley minimum height
height height

7.2 43.2 f 1.8 1.00 f 0.01 0.038 f 0.026 0.960 f 0.032 44.9 f 5.2
10.78 34.0 ZtI1.3 0.91 f 0.09 0.011 f 0.025 0.898 xt 0.094 37.8 & 4.4
11.24 35.4 i 1.4 0.94 f 0.06 0.030 f 0.036 0.906 f 0.032 39.0 zt 3.6
13.23 35.8 f 2.1 0.96 f 0.11 0.002 zt 0.032 0.960 f 0.032 37.3 f 4.9
20.70 20.1 f 1.2 0.66 f 0.08 0.024 f 0.034 0.638 f 0.078 3 1.5 f 4.7
26.5 10.5 i 0.61 0.36 i 0.07 -0.01 f 0.016 0.372 i O-038 28.2 I!I 5.4

1 -.
25 30 35 40 45 50
cl

Fig. 6. The change in Q with mean mass depth (B) (r2 = 0.983).
13’Cs source burial in salt marshes 201

TABLE 3
The Change in Mean Mass Depth (gcmm2) Derived from Spectral Data, across the Caer-
laverock Calibration Site. 1 Q Errors on Individual Values are Between 10 and 15%

Transect Hexagonal shell number:sample spacing (m)


number
0:o I:2 2:8 3:32 4:128 5.256

1 11.34 12.69 12.39 9.89 7.05 4.65


2 12.84 11.26 9.92 10.60 8.29
3 11.57 12.03 11.32 20.5 20.18
4 14.64 13.56 16.52 26.47 10.10
5 12.47 12.51 12.08 21.87 16.14
6 9.89 14.42 10.30 5.32 5.01

Columns represent each hexagonal shell, rows represent the arms of each transect from the
centre of the hexagon (see Fig. 3).

mated from the measured values of Q, as shown in Table 3. Transect 1


represents the points from the centre of the hexagon north with values of j?
ranging from 12.7 to 4.65 gcmW2. Transect 4 represents the points south
from the centre of the hexagon with /3 values ranging from 11.34 to 26.47.
The other transects represent the remaining arms of the hexagon (Fig. 3).
These results are also generally consistent with an increase in /? towards
the near shore environment. The only exception is provided by position 45
(Fig. 3) (j3 = 10.10gcm-2) where the spectrum was collected over inter-
tidal sediments, rather than from consolidated salt marsh areas. This is
almost certainly due to a very different activity depth profile exhibited by
these intertidal sediments.
Having determined fi from spectral information, a spectrally derived
calibration correction for changes in source burial at the Caerlaverock salt
marsh can be derived.

Caesium-137 calibration correction for changes in mean mass depth (fi)

As shown in Fig. 6, investigations of Q allow the estimates of mean mass


depth (/I) to be made and thus an appropriate calibration correction
coefficient may be established. By regressing the calibration coefficient
(N/A,) determined from each site of known p 137Cs activity and Q, a
spectrally derived calibration coefficient can be readily estimated. This
relationship is shown in Fig. 7 (also showing 95% confidence levels on the
regression) and given in eqn (9):

Log(~)
=LoP(go
-m/? = 0.1396 - O-0337/? (9)
208 A. N. Tyler et al.

Mean Mass Depth 13

Fig. 7. The change in the calibration coefficient (N/A,) with /3 (gem-‘) for the Caerlaver-
ock salt marsh (r* = 0.981).

where N is the stripped counts per second and A, is activity per unit area
(e.g. kBqmm2). Equation (9) in conjunction with the mean mass depth (/3)
values shown in Table 3 was used to determine the b corrected activities
across the Caerlaverock calibration site.
It is instructive to compare estimates of activity per unit area derived
from in situ spectrometry with core results from each of the sampling
locations using both a single calibration value derived from the centre of
the site, and variable calibration factors incorporating corrections based
on Q from each in situ observation.
The comparison between the uncorrected in situ derived inventory esti-
mates and soil core derived estimates (0-30cm), is shown in Fig. 8. The
cluster of points about the 1:l line reflects the number of measurements
made around the centre of the hexagon which is unlikely to demonstrate
any significant change in /?. It is, therefore, the magnitude of the overall
scatter which is important, demonstrating the range of possible mis-
matches in the two techniques of soil sampling and in situ ray spectro-
metry in these salt marsh environments (r2 = O-097). In the worst indivi-
dual cases in situ activity estimates based on a fixed calibration constant
can either underestimate core results by a factor of approximately 3, or in
other cases overestimate activity by a factor of approximately 2.
By contrast, the use of the spectrally derived correction factor is shown
in Fig. 9 demonstrating a substantial improvement in the relationship
between in-situ and soil core derived estimates (r2 = 04301). Error contri-
137Cs source burial in salt marshes 209

0 L ” ” I
0 40000 80000 120000 160000

Soil Core Actiiities (Bq m”)

Fig. 8. The comparison between in situ detector uncorrected calibrations and soil core
derived ‘37Cs activity estimations (Bqme2) across the Caerlaverock site (r2 = O-097).

0.
0 40000 80000 120000 160000

Soil Core Activities (Bq m-2)

Fig. 9. The comparison between in situ detector /I corrected calibrations and soil core
derived ‘37Cs activity estimations (Bqm-‘) across the Caerlaverock site (r2 = 0.801).

butions to this second set of estimates of /? must include the contributions


from stripping and counting statistics in the determination of Q. It should
also be borne in mind that individual core results will not in general be
fully representative of the activities within the field of view of individual
210 A. N. Tyler et al.

in-situ readings, and therefore that Fig. 9 may also include scatter due to
spatial variations of the activity distribution (e.g. Tyler et al., 1996). These
points considered, the overall agreement between the two data sets has
improved such that estimates derived from in-situ spectrometry and core
sampling are in general agreement within 20-30% of each other. An
exception to this is location 45, derived from the intertidal sediments,
which shows evidence of a different activity distribution.

DISCUSSION

These results demonstrate a significant development in the application


of in situ gamma ray spectrometry to salt marsh environments, not only
to predict the mean mass depth (/3) but also to derive a calibration
correction from spectrally derived characteristics for such environments
where the change in mean mass depth is observed to change system-
atically with proximity to the shoreline. Application of this new techni-
que to salt marsh environments will greatly facilitate the speed with
which integrated 13’Cs activity per unit area estimates can be made, and
therefore provide rapid spatial information of activity deposition across
such environments.
The precision of the in situ measurements is shown in Fig. 9, and is of
the order of 20%, with random uncertainties dominated by the statistical
limitations of estimating Q. Residual variations not accounted for could
include contributions from both the spatial mismatch in comparing single
soil cores and in situ measurements, and potentially in small scale
sampling errors of comparable magnitude, as observed subsequently on
similar salt marshes (e.g. Wigtown Bay, Sanderson et al., 1994). The
contribution from changes in profile shape brought about through spatial
differences in depositional history may also have contributed to some of
the residual scatter, as could areas of standing water within the field of
view of the detector. However it is clear, from the improvements achieved
when in situ depth corrections are applied to this site, that the technique is
able to absorb the effects of major variations in mean source burial within
the salt marsh, and that these confounding factors are of secondary
importance relative to such depth variations.
Further work is needed to establish the effect of changes in the shape of
the activity distribution on the performance of such corrections, to exam-
ine the extent to which similar corrections can be applied to other related
sites, and to extend the application of these techniques to airborne gamma
spectrometry. In this last respect it has been noted that step changes due
to forward scattering have been observed in airborne spectra recorded
‘37Cs source burial in salt marshes 211

with both high volume NaI detectors and HPGe detectors in salt marshes
in the Solway (Sanderson et al., 19954).
In addition to improving the quantitative performance of in situ spec-
trometry in complex environments, it may be possible to use these meth-
ods for rapid mapping of spatial variations in mean source burial, of
significance both to directing environmental sampling, and to studies of
salt marsh accretion and sedimentation rates.

ACKNOWLEDGEMENTS

Funding for this research was provided primarily by the Natural Envir-
onmental Research Council. The authors would also like to thank Dr
David Allyson for his useful comments during this work and on the drafts
of this paper, and Mr Simon Murphy for assistance with sampling at
Caerlaverock.

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