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195-212, 1996
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ELSEVIER
ABSTRACT
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
b)
n- A
bl
SURFACE
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.
Mean depth and mean mass depth for a generalised activity distribution
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):
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
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
TABLE 1
The Regions of Interest for the Series 10PiuSMCA and 3” x 3” NaI(TI) Detector (Tyler,
1994)
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.
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
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
+
0 20 40 60 00 100 120 140
Fig. 5. The change in Q with number of perspex absorber sheets (r2 = 0.991).
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).
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.
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
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%
Columns represent each hexagonal shell, rows represent the arms of each transect from the
centre of the hexagon (see Fig. 3).
Log(~)
=LoP(go
-m/? = 0.1396 - O-0337/? (9)
208 A. N. Tyler et al.
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
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
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).
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
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.
REFERENCES