Applied Radiation and Isotopes 160 (2020) 109124

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Applied Radiation and Isotopes

journal homepage: http://www.elsevier.com/locate/apradiso

Calibration of a CeBr3 based γ-spectrometer for onsite and laboratory

radioactivity measurements in sediment samples
E.G. Androulakaki a, *, C. Tsabaris a, F. Maragkos b, D.L. Patiris a, F.K. Pappa a, G. Eleftheriou a,
S. Alexakis a, M. Kokkoris b, R. Vlastou b
a
Hellenic Centre for Marine Research, Institute of Oceanography, P.O. Box 712, GR-19013, Anavyssos, Greece
b
Department of Physics, National Technical University of Athens, Zografou, Athens, 15780, Greece

A R T I C L E I N F O A B S T R A C T

Keywords: The calibration of an underwater spectrometer, consisting of a CeBr3 crystal, is performed for sediment sample
Monte Carlo simulations measurements, via experimental data and Monte Carlo simulations. The system was implemented for activity
CeBr3 crystal concentration measurements in marine sediment samples in the laboratory. The results were compared with
Marine sediment
corresponding high resolution measurements and showed that the system provides accurate results, but rela­
Marinelli beaker
tively high uncertainties. Different measurement geometries are theoretically studied via Monte Carlo simula­
tions in order to improve the system performance for such measurements.

1. Introduction
The increasing interest in gamma-ray spectrometry measurements,
especially near coastal areas with enhanced industrial activity, along
with a general demand for cost effective surveys have led to the gradual
substitution of high resolution systems with scintillation detectors and
the excessive utilization of the latter for Naturally Occurring Radioactive
Material (NORM) measurements both in the field and in the laboratory.
Low resolution crystals have been employed for measurements of
environmental samples in the laboratory in different applications
(Chiozzi et al., 2000; Kovler et al., 2013; Bezuidenhout, 2013; Safarov
et al., 2017; Pilakouta et al., 2018). Nevertheless, a lot of effort is needed
in terms of spectral analysis and overlapping peak deconvolution (e.g. at
609 keV, convoluted peaks from the emissions of 214Bi (609 keV), 208Tl
(583 keV) and 137Cs (662 keV)). Recently, new medium resolution
spectrometers based on LaBr3:Ce and CeBr3 crystals have become
commercially available and have been used for in situ measurements in
the marine environment (Zeng et al., 2017; Tsabaris et al., 2019; Lee
et al., 2019) and also in the laboratory, for NORM measurements (Peyres
et al., 2017) as well as for radioactivity measurements in water samples
(Naqvi et al., 2016) and steelwork materials (García-Toran ~ o et al.,
2016). Such spectrometers exhibit high full-energy peak efficiency and
can also be applied directly in the field for onsite (on collected samples)
or in situ measurements. Among the different scintillation detectors, the
implementation of CeBr3 based systems for NORM measurements is
increasing, due to their lower intrinsic activity (Quarati et al., 2013;
Naqvi et al., 2016) compared to LaBr3:Ce crystals, which enables them to
be used in low-level activity applications (Lutter et al., 2013).
The GeoMAREA system, utilized in this work, is based on a 200 x 200
CeBr3 crystal enclosed in an acetal mounting cup and is calibrated for in
situ activity concentration measurements of naturally occurring and
anthropogenic radionuclides in a wide energy range (150–2600 keV) in
the aquatic environment (Tsabaris et al., 2019). In the present work the
alternative utilization of the spectrometer GeoMAREA, for onsite and/or
laboratory radioactivity measurements on marine sediment samples, is
examined.
The motivation for this work was to explore the possibility of using a
detection system based on a CeBr3 crystal for radioactivity measure­
ments both in the laboratory and in the field (onsite and/or in situ
measurements), so as to attain a supplementary tool to support radio­
activity mapping activities for site characterization and hot spot iden­
tification in the marine (seabed) and the terrestrial (beach sands and
soil) environment. The aim is to use the onsite measurements for the in
situ results quantification. Moreover, the possibility of utilizing a CeBr3
based system, instead of high resolution cost-consuming laboratory
measurements, is examined and discussed.
To this end, the GeoMAREA system was calibrated for sediment
samples measurements using laboratory data and Monte Carlo (MC)
simulations, via the MCNPX (Pelowitz, 2011) and MCNP-CP (Berlizov,
2006) codes. 152,154Eu and 40K sources were utilized for the sediment

* Corresponding author.
E-mail address: frosso.androulakaki@hcmr.gr (E.G. Androulakaki).

https://doi.org/10.1016/j.apradiso.2020.109124
Received 2 December 2019; Received in revised form 14 February 2020; Accepted 3 March 2020
Available online 4 March 2020
0969-8043/© 2020 Elsevier Ltd. All rights reserved.
E.G. Androulakaki et al.
sample measurements full-energy peak efficiency calibration. The
experimental data were used to optimize the simulation model and
validate the theoretical results. After the simulation evaluation, addi­
tional runs were performed to extend the efficiency calibration in a wide
energy range (150 keV–2600 keV). Additionally, Monte Carlo simula­
tions were performed considering alternative measurement setups to
improve the measurement statistical uncertainty.
The Minimum Detectable Activity (MDA) values were calculated for
the selected measurement geometry, in a wide energy range (238
keV–2614 keV). The proposed methodology was applied for radioac­
tivity measurements in marine sediment samples obtained from a sedi­
ment core collected at a deep sea trench near Samothraki Island in
Greece. The activity concentration results were compared with corre­
sponding measurements using a high resolution system (HPGe).
Moreover, the first results of a theoretical study to optimize the
measurement geometry are presented and discussed in this work. In
more detail, the reduction of the overall measurement statistical un­
certainty is theoretically studied via MC simulations considering
different scenaria, including the removal of the detector mounting cup
and the closer positioning of the sediment sample to the crystal, either
using the same (cylindrical) geometry or a Marinelli beaker.
2. Methodology
2.1. Experimental calibration
The experimental energy and resolution calibration was performed
using 152,154Eu, 60Co, 137Cs calibrated point sources. The full-energy
peak efficiency (ε) calibration was performed using a calibrated
152,154
Eu point source at different source-to-detector window distances,
namely 1.7 cm and 11.2 cm and 25.0 cm and the results (both experi­
mental spectra and ε values) were utilized in the design of the MC model
of the detection system. The experimental full-energy peak efficiency
calibration, for sediment sample measurements, was performed using
extended 152,154Eu and 40K calibrated sources (volume of 65 cm3). The
spectra using the extended calibrated 152,154Eu and 40K sources were
obtained in touch geometry with the detector mounting cup (Fig. 1a).
The geometrical (height) and physical characteristics (source density,
composition) of the calibration sources were different from those of the
sediment samples. Additional ambient background measurements were
performed. The SPECTRW software (Kalfas et al., 2016) was utilized for
the analysis of the spectra. The experimental calibration was deduced
via the following eq. (1):
cps
ε¼ Eq. 1
Ig ⋅m ⋅ A ⋅FTCS ⋅ FSABS
Where:
Fig. 1. MC models of the system GeoMAREA for sediment samples measurements considering four different geometries, a.) a cylindrical sample container in touch
geometry with the mounting cup, b.) a cylindrical sample container in touch geometry with the detector crystal, c.) a commercial Marinelli beaker (Commercial
Marinelli) in touch geometry with the detector crystal and d.) a custom Marinelli beaker (Custom Marinelli) in touch geometry with the detector crystal.
2
Applied Radiation and Isotopes 160 (2020) 109124
ε: The full-energy peak efficiency for a given γ-ray energy in the
studied measurement geometry
cps: The net counting rate attributed to a specific γ-ray, after the
extraction of the ambient background and Compton continuum
contribution, in the corresponding peak
Ig : The emission probability of the gamma-ray in the corresponding
peak
m: The sediment sample mass in kg
A: The activity concentration of the studied radionuclide in Bq/kg
FTCS ⋅FSABS : Correction factors to account for True Coincidence Sum­
ming (TCS) effects (FTCS ) for cascade radionuclides and self absorption
differences (FSABS ) attributed to variations regarding the geometry,
density and composition, among the calibration sources and the sedi­
ment samples.
The correction factors FTCS and FSABS were estimated using the EFF­
TRAN code (Vidmar, 2005). An additional correction was required in
the calculation of the ε value at 121 keV (peak attributed to the emission
of 152Eu convoluted with the gamma-line of 154Eu at 123 keV). For the
analysis of this peak, the number of events attributed to emissions from
the disintegration of the radionuclide 154Eu, were calculated and sub­
tracted from the recorded events under the peak prior to the ε calcula­
tion using Eq. (1).
Moreover, Minimum Detectable Activity (MDA) calculations were
performed in a wide energy range from 351 keV to 2600 keV as
described elsewhere (Naumenko et al., 2018; Zhang et al., 2018; Bag­
atelas et al., 2010). For these calculations an ambient background
spectrum measured for 62,000 s and fitted data to the experimentally
derived ε values were used, with an exception at 2614 keV, for which the
estimated MC value was utilized.
2.2. Monte Carlo simulations
The Monte Carlo N-particle transport code (MCNP) was utilized for
the ε values estimation of the GeoMAREA system for sediment sample
measurements in the laboratory. The MCNP code has been efficiently
applied for the calibration of low and medium resolution spectrometers
for measurements in the seawater as well as on the seabed (Androula­
kaki et al., 2015, 2016a, 2016b; Tsabaris et al., 2018, 2019).
As a first step, the MC code was implemented to reproduce point and
extended calibrated source spectra. The MCNP-CP code (Berlizov, 2006)
was selected for the reproduction of experimental spectra using both
point and extended sources. This code was selected because it accounts
for true coincidence summing effects and performs the direct simulation
of the prominent emitted gamma-rays along with the corresponding
intensities for each radionuclide via a single card. The point source
spectrum was obtained using a152,154Eu calibrated source placed at 1.7
E.G. Androulakaki et al.
cm distance from the detector entrance window (acetal mounting cup).
The spectra using extended calibrated 152,154Eu and 40K sources were
obtained in touch geometry with the detector entrance window (acetal
mounting cup). The same detector model was utilized in all the simu­
lation runs, which was designed according to the manufacturer speci­
fications and optimized via the comparison with the experimental
spectra of the calibrated point and extended sources.
After the MC model evaluation, the ε values for all the studied
measurement setups were estimated using the MCNPX code (Pelowitz,
2011). The simulation results were compared to the corresponding
experimental ones. After achieving a satisfactory agreement, additional
runs were performed to extend the estimated ε values for the Geo­
MAREA system in the energy range from 85 to 2600 keV. The simulated
results are presented along with the corresponding experimental data in
section 3.1.
Both MCNP code versions were additionally utilized in a theoretical
study to optimize the measurement geometry. The MCNPX code was
implemented to estimate the ε values in different measurement geom­
etries, as shown in Fig. 1. These runs were performed in an effort to
improve the measurement statistics for future applications. For these
runs, the experimental geometry setup (Fig. 1a), which includes a cy­
lindrical container exhibiting a volume of 65 cm3, placed in touch ge­
ometry with the detection system mounting cup, is altered without
changing the detector model. In the first selected optimized setup
(Fig. 1b), the full-energy peak efficiency (ε) is improved by removing the
mounting cup and placing the cylindrical container (65 cm3) in touch
geometry with the detector crystal. In this way, the solid angle of the
measurement is maximized, while additionally the attenuation of γ-rays
is reduced with the removal of the mounting cup. In the next two utilized
MC models (Fig. 1c–d), the cylindrical container is substituted by two
Marinelli beakers of different dimensions, while the measurement is
performed again in touch geometry with the crystal. The commercially
available (model 443016) Marinelli beaker (Fig. 1c), exhibits a volume
of 250 cm3 (2.7 cm top thickness, 1.8 cm side thickness, 6.6 cm total
height) and the custom one (Fig. 1d) exhibits the same volume of 250
cm3 but different geometry (1.7 cm top thickness, 2.6 cm side thickness,
6.6 cm total height), so that in this case, the sample effectively surrounds
all the crystal volume (see Fig. 1d). Moreover, the MCNP-CP code was
utilized to derive theoretical spectra of the experimental geometry (cy­
lindrical container) with and without the acetal mounting cup. The re­
sults are presented in section 3.3.
2.3. Sediment sample measurements
The sediment samples were dried sieved (grain diameter < 2 mm)
and stored in the measurement geometry (cylindrical sample container)
in the laboratory, for at least three weeks prior to the measurement, in
order to ensure that equilibrium is reached between radium 226Ra and
radon 222Rn progenies. Details on the sediment preparation procedure
are given in literature (Patiris et al., 2016; Pappa et al., 2016). Two
sediment samples were selected and measured via gamma-ray spec­
troscopy using the system GeoMAREA and also by means of a HPGe
detector, to obtain the activity concentrations for the naturally occur­
ring radionuclides of interest (40K, 214Bi, 214Pb, 228Ac and 208Tl). The
selected samples from the core were the surface sediment sample (0–2
cm) and a shallow one (4–6 cm) and were extracted by slicing the
sediment core. The sediment samples were placed in touch geometry
with the system mounting cup for the medium resolution measurements
(see Fig. 1a). The high resolution measurements were performed by a
p-type coaxial HPGe detector of 67 mm in diameter and 67 mm in length
with an entrance window of a 1 mm thick Al foil (model GC5021,
Canberra®), while the samples were inserted inside a Pb shielding for
the measurement. The purpose of these independent measurements was
to examine the accuracy and sensitivity of the activity concentration
results obtained using the medium resolution system.
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Applied Radiation and Isotopes 160 (2020) 109124
3. Results and discussion
3.1. Full-energy peak efficiency calibration
In Fig. 2 a comparison between experimental and simulated spectra
for a calibrated 152,154Eu point source placed at 1.7 cm from the detector
mounting cup is presented. The simulated spectra were reformed in
order to take into account the experimental energy binning and reso­
lution calibration. The reproduction of the experimental binning and
energy calibration was externally achieved via a user-defined algorithm
assuming a linear energy function, while the energy resolution is applied
using a different algorithm and an appropriate Gaussian broadening
equation which can be found in Pelowitz, 2011. Details on the calibra­
tion procedure are presented in Tsabaris et al. (2019). The higher
counting rate in the experimental spectrum in the low energy region
could be additionally attributed to the presence of scattered events
arising from interactions between the γ-rays and the point source holder
(consisting of aluminum and polyethylene). Such events are absent in
the theoretical spectrum since the holder was not included in the
simulation model. In Figs. 3 and 4, the comparison between the exper­
imental and simulated spectra are presented for sediment sample mea­
surements, using calibrated extended sources of 152,154Eu and 40K
positioned in touch geometry with the detector mounting cup. The
agreement with the simulated spectra in both measurements (152,154Eu
and 40K sources) is very satisfactory over the whole energy range. In the
experimental spectrum of the 152,154Eu extended source (Fig. 3), an
additional energy peak is observed below 100 keV which could be
attributed to differences between the estimated and actual TCS effects.
In Fig. 5 the estimated ε values for point source measurements at 1.7 cm
and 11.2 cm are presented in the energy range from 85 keV to 1780 keV
and compared with the corresponding available experimental data.
Similarly, in Fig. 6 the estimated ε values for sediment measurements
(assuming a sediment density of 1 g cm 3) are presented in the energy
range from 85 keV to 2600 keV and compared with the corresponding
experimental data of the 152,154Eu and 40K extended sources. The
experimental data are obtained using Eq. (1) and are corrected for TCS
effects and for self-absorption differences (due to differences in density,
composition and geometry between the sediment samples and the cali­
brated sources), using the EFFTRAN code. The experimental and theo­
retically estimated efficiency values for point and extended sources are
summarized in Table 1. The ratio between the MC and experimental
values ranged from 0.90 to 1.07 and from 0.92 to 1.07 for the point and
extended sources, respectively, while the statistical uncertainty of the
estimated MC values was kept below the value of 5% in all cases.
The results of the calculated MDA values for the radionuclides 40K,
214
Bi, 214Pb, 208Tl, and 228Ac are presented in Table 2, along with the
γ-ray energy of the utilized peaks and the corresponding emission
probabilities, which were introduced in the calculations. The experi­
mental ε values for sediment measurements (according to Eq. (1), for a
sample container of 65 cm3 volume, a sediment density of 1 g cm 3)
along with an ambient background measurement (62,000 s) were used
in the MDA values calculation, according to the methodology presented
elsewhere (Naumenko et al., 2018; Zhang et al., 2018; Bagatelas et al.,
2010; Done and Ioan, 2016). Only in the case of 208Tl the simulated ε
value at 2614 keV was used due to the absence of an experimental value
at this energy.
3.2. Radioactivity measurements results
The sediment samples were also measured using a HPGe detector of
50% relative efficiency, in touch geometry for the same 24 h acquisition
period. These measurements were performed in order to compare the
activity concentration results of the GeoMAREA system with the ones
from a high resolution detection system. The obtained spectrum (HPGe)
is shown in Fig. 7 and compared with the corresponding one using a
medium resolution detection system (CeBr3 spectrum) with respect to
E.G. Androulakaki et al. Applied Radiation and Isotopes 160 (2020) 109124

Fig. 2. Comparison of the simulated and experimental spectra using a152,154Eu calibrated point source.

Fig. 3. Comparison of the simulated and experimental spectra using a152,154Eu calibrated extended source (cylindrical container in touch geometry with the
mounting cup).

their resolution. The spectrum using the medium resolution system is
normalized to the counting rate of the high resolution spectrum, while in
both spectra the ambient radiation background is not subtracted (nor the
intrinsic activity in the medium resolution spectrum). In Table 3, the
activity concentrations of the detected radionuclides (40K, 214Bi, 214Pb,
208
Tl, and 228Ac) are presented for the two sediment samples, namely s1
and s2, corresponding to core sediment depths of 0–2 cm and 4–6 cm,
respectively. The activity concentrations of the radionuclides 40K, 208Tl,
228
Ac, 214Pb and 214Bi exhibit similar values in both sediment samples.
The measured activity concentration values for 40K, 208Tl, and 228Ac
using the two different detectors are in good agreement, thus the Geo­
MAREA system is applicable for radioactivity measurements not only for
in situ applications in the seawater (Tsabaris et al., 2019) but also for
sediment sample measurements in the laboratory.
The major drawback of the utilization of the GeoMAREA system for
sediment sample measurements in the laboratory is the accompanied

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E.G. Androulakaki et al. Applied Radiation and Isotopes 160 (2020) 109124

Fig. 4. Comparison of the simulated and experimental spectra using a40K calibrated extended source (cylindrical container in touch geometry with the
mounting cup).

Fig. 5. Comparison of the MC derived and corresponding experimental full Fig. 6. Comparison of the MC derived and corresponding experimental full
energy peak efficiency values (ε) for point source measurements at energy peak efficiency values (ε) for sediment source measurements (consid­
different distances. ering a sediment density of 1 g cm 3).

high uncertainties, as shown in Table 3. These high uncertainties orig­ uncertainty, a different setup should be selected, in which a larger
inate from the low ε values of the selected measurement geometry sample amount and increased ε values would be utilized, as discussed in
(sample in touch geometry with the mounting cup) and from the low the next section.
counting statistics, as a reduced sediment mass was used (an amount of
approximately 25 g was utilized due to the lack of the necessary quan­
3.3. Full-energy peak efficiency optimization
tity). Despite this drawback, the selected geometry can be utilized as a
supplementary tool for in situ measurements, while for accurate mea­
The first and most crucial step to improve the performance of the
surements in the laboratory, the utilization of optimized measurement
GeoMAREA system is to increase the ε values for sediment measure­
geometry is mandatory. Therefore, to reduce the measurement
ments in the laboratory. The most straightforward way to accomplish

5
E.G. Androulakaki et al. Applied Radiation and Isotopes 160 (2020) 109124

Table 1
The experimental (εexp.) and theoretically (εМ.C.) estimated efficiency values and the calculated Ratio (εМ.C./εexp.), for a152,154Eu point source at different distances from
the mounting cup and a152,154Eu extended source (sediment source) in touch geometry with the mounting cup. The statistical uncertainty (unc.) is given in %
percentage.
Energy point source at 1.7 cm point source at 11.2 cm sediment source
(keV)
εexp. εМ.C. Ratio εexp. εМ.C. Ratio εexp. εМ.C. Ratio
3 3 3 3 3 3
x 10 x 10 x 10 x 10 x 10 x 10
(unc.%) (unc.%) (unc.%) (unc.%) (unc.%) (unc.%)

121 48.27 (0.2) 48.59 (1) 0.99 6.2 (3) 6 (1) 1.04 46.4 (3) 43.5 (1) 1.07
244 37.81 (1) 38.06 (1) 0.99 5.1 (3) 5.3 (3) 0.94 38.7 (3) 36.8 (1) 1.05
344 28.16 (0.2) 29.81 (1) 0.94 4.0 (3) 4.3 (2) 0.93 28.5 (3) 29.9 (1) 0.95
444 24.92 (2) 24.2 (1) 1.03 3.4 (6) 3.5 (2) 0.96 – – –
778 14.38 (1) 15.08 (2) 0.95 2.2 (3) 2.3 (2) 0.97 15.2 (2) 15.8 (2) 0.97
867 14.53 (2) 13.62 (1) 1.07 2.2 (6) – – – – –
964 11.11 (1) 12.39 (1) 0.90 1.8 (3) 1.9 (1) 0.95 12.8 (3) 13.1 (2) 0.97
1085 10.1 (1) – – 1.7 (3) 1.7 (2) 0.96 11.5 (4) – –
1112 – – – – – – 10.9 (4) 11.8 (2) 0.92
1408 8.54 (1) 8.96 (2) 0.95 1.3 (3) 1.4 (1) 0.93 9.1 (3) 9.9 (2) 0.92

and without the system enclosure (mounting cup) are compared. The
Table 2 removal of the system mounting cup allows for the positioning of the
The calculated Minimum Detectable Activity (MDA) values and accompanied
sediment sample much closer to the CeBr3 crystal (approximately 4 cm)
uncertainties (Unc. (%)) for the radionuclides 40K, 214Bi, 214Pb, 212Pb, 228Ac and
208 and therefore increases the measurement solid angle. An alternative
Tl (* MC derived ε value).
geometry setup which further increases the counting statistics and
Radionuclide Energy Unc. MDA Unc.
ε Іg
additionally reduces the MDA values, compared to the utilized mea­
(keV) (%) (%) (Bq/kg) (Bq/kg) (%) surement geometry (Fig. 1a), is to use a Marinelli beaker in close contact
212
Pb 238 0.035 (3) 43.3 17 (3) with the detector crystal.
214
Pb 352 0.029 (3) 37.6 21 (4) To this end, two different Marinelli geometries are considered as
214
Bi 609 0.019 (4) 46.1 21 (3) shown in Fig. 1, exhibiting different geometrical properties (radius and
228
Ac 911 0.013 (3) 25.8 47 (3)
40 thickness) but the same volume of 250 cm3 which is 3.8 times larger
K 1461 0.008 (3) 10.7 107 (5)
208
Tl* 2614 0.005 (4) 99 4 (16) than the one using a cylindrical sample container. This larger volume
allows for the usage of larger sample masses and therefore leads to the
counting statistics increment by a factor of approximately 5 (assuming a
that is to remove the detector mounting cup, so that the sample is placed sediment density of 1g cm 3).
in close contact with the detector crystal as shown in Fig. 1. This step The MC estimated ε values for the four studied measurement setups,
alone drastically increases the ε values and therefore the counting sta­ namely the experimental geometry utilizing a cylindrical container in
tistics over the whole energy range, as shown in Fig. 8, in which the two touch geometry with the mounting cup (see Fig. 1a), a cylindrical
simulated spectra obtained for a sediment sample measurement with container without the mounting cup in touch geometry with the crystal

Fig. 7. Comparison of the acquired spectra (24h measuring period and no ambient background contribution subtraction) using high resolution (HPGe) and medium
resolution (GeoMAREA) detection systems, for the surface sediment sample (sample s2).

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E.G. Androulakaki et al. Applied Radiation and Isotopes 160 (2020) 109124

Table 3
The activity concentration values (A (Bq/kg)) and the calculated ratio (A_ CeBr3/A_ HPGe), using high (HPGe) and medium (CeBr3) resolution detection systems. The
statistical uncertainty (Unc.) is given in % percentage.
sample depth Energy Radionuclide A (CeBr3) Unc. A (HPGe) Unc. A_CeBr3/A_HPGe

cm (keV) Bq/kg (%) Bq/kg (%)

40
s1 0–2 1461 K 550 (29) 539 (7) 1.02
214
352 Pb <MDA 20 (7) –
214
609 Bi <MDA 20 (9) –
228
911 Ac 61 (40) 58 (9) 1.06
208
2614/583 Tl 21 (33) 20 (8) 1.07
40
s2 4–6 1461 K 544 (29) 546 (7) 1.00
214
352 Pb <MDA 21 (10) –
214
609 Bi <MDA 23 (13) –
228
911 Ac 67 (40) 60 (13) 1.11
208
2614/583 Tl 20 (32) 21 (10) 0.93

Fig. 8. Comparison of two simulated spectra obtained for a sediment sample measurement with and without the mounting cup.

(see Fig. 1b), a custom (see Fig. 1d) and a commercial (see Fig. 1c)
Marinelli beaker again without the mounting cup in touch geometry
with the crystal, are summarized and compared in Fig. 9 in the energy
range from 85 keV to 1760 keV. The results of the three optimized
measurement geometries (cylindrical container, commercial Marinelli,
custom Marinelli in touch geometry with crystal) are compared below
with respect to the experimental one (container with mounting cup).
The utilized measurement setup in this work, exhibits the lowest ε
values. Τhe setup using a cylindrical container in touch geometry with
the detector crystal (Fig. 1b), exhibits the highest ε values due to the
utilization of the optimum solid angle. More specifically, for this mea­
surement geometry, the ε values increase by a factor of 2.3 in the high
energy region, up to a factor of 2.8 in the low energy region (as shown in
Fig. 9). The geometry using a custom Marinelli beaker (designed ac­
cording to the crystal characteristics), exhibits higher ε values compared
to the experimental ones (Fig. 1a), by a factor of 1.9 in the low energy
region that drops down to 1.8 in the high energy part. The counting rate
is also enhanced using the custom Marinelli beaker, due to the larger
sediment mass involved in this measurement. To demonstrate this, the
quantity εm is presented with respect to γ-ray energy in Fig. 10, for the
four studied measurement geometries. The quantity εm is the product of
ε values with the sediment sample mass (ε ⋅ mass, in units of kg),
assuming a sediment density of 1 g cm 3. According to Eq. (1) the
counting rate cps, is proportional to the εm values for a given sediment
sample. Therefore, since large differences in the correction factors
(FTCS ⋅FSABS ) are not expected, the counting rate increases approximately
by a factor of 5 for the custom Marinelli geometry compared to the
experimental one (due to the larger volume of the Marinelli beaker
compared to the cylindrical container). The ambient radiation back­
ground of the measurement is additionally decreased using this setup
(again due to the larger sample mass which acts as a shield for cosmic
radiation). Finally, the full-energy peak efficiency using the commercial
Marinelli beaker exhibits higher values by a factor of 1.5 in the low
energy region that drops down to 1.4 in the high energy part, while
again the counting rate is enhanced (due to the sediment mass increment
using a Marinelli beaker).
The MDA values for the optimized geometries are studied only
qualitatively, taking into account the MC derived efficiency data, due to
the lack of experimental data. Regarding the Marinelli geometries,
comparing to the experimental geometry (cylindrical container in touch
geometry with the mounting cup), the MDA values are decreased by a
factor of at least 1.4 in the whole energy range, while the background

7
E.G. Androulakaki et al.
Fig. 9. Comparison of the MC derived full-energy peak efficiency values (ε) for
sediment measurements using the GeoMAREA system, considering different
measurement geometries, a cylindrical container in touch geometry with the
mounting cup (experimental), a cylindrical container in touch geometry with
the CeBr3 crystal, a commercial and a custom Marinelli beaker in touch ge­
ometry with the CeBr3 crystal.
Fig. 10. Comparison of the quantity εm, which is the product ε ⋅ mass (in units
of kg), for the studied measurement geometries, a cylindrical container in touch
geometry with the mounting cup (experimental), a cylindrical container in
touch geometry with the CeBr3 crystal, a commercial and a custom Marinelli
beaker in touch geometry with the CeBr3 crystal.
radiation is also decreased using Marinelli beakers, further improving
thus the MDA values for these measurement geometries. Regarding the
measurement using a cylindrical sample container in touch geometry
with the crystal (without the mounting cup), the MDA is improved by a
factor of at least 2.3 due to the higher ε values, comparing again with the
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Applied Radiation and Isotopes 160 (2020) 109124
corresponding experimental geometry data.
4. Summary and perspectives
The motivation of this work was to examine the capabilities of a
system consisting of a 200 x 200 CeBr3 crystal, for laboratory radioactivity
measurements of sediment samples. The proposed methodology using a
medium resolution crystal for measuring natural radioactivity in sedi­
ment samples can be successfully applied in the case of small labora­
tories, for which a high resolution HPGe detector is not affordable. The
developed methodology can be utilized to support the on-site calibration
of instrumentation used for in situ applications such as mapping activ­
ities and rapid site characterization in the terrestrial environments, but
also in the marine environment, as the water-tight mounting cup allows
also such measurements. An important result of this work is that a valid
MC model of the GeoMAREA system is obtained, able to reproduce the
experimental ε values in various measurement geometries, such as point
sources in different distances, extended sources (sediment samples) and
in situ measurements in the seawater and thus, it can be applied also to
different measurement geometries providing accurate full-energy peak
efficiency results.
The results of the radioactivity measurements on the collected
sediment samples showed that the system GeoMAREA provides accurate
activity concentrations for the detected radionuclides, while using this
system the separate analysis of the 609 keV (214Bi) and 662 keV (137Cs)
γ-lines is feasible, due to the improved resolution compared to NaI
scintillation crystals. Nevertheless, given that the associated un­
certainties with the utilized setup are high (30–40%), the measurement
setup is optimized through simulation exercises at different measure­
ment geometries (solid angle and sample container selection). The
performed theoretical study via MC simulations showed that the
removal of the detector mounting cup provides high improvement in the
system performance (the ε values increase up to a factor of 2.8). In
addition to this modification, the utilization of a Marinelli beaker in­
creases the counting statistics (by a factor of approximately 5), due to
the much larger sediment mass involved.
Future work also involves the implementation of the presented
methodology for onsite sediment samples measurements using the
optimized geometry (Marinelli beaker) in order to test the system per­
formance in the conditions of real environment. This methodology may
be expanded for radioactivity measurements in environmental matrices
(such as seawater, rainwater, groundwater and surface waters) as well as
for in situ measurements on the seabed, using the proposed MC model.
Declaration of competing interest
The authors declare that they have no known competing financial
interests or personal relationships that could have appeared to influence
the work reported in this paper.
CRediT authorship contribution statement
E.G. Androulakaki: Methodology, Validation, Writing - original
draft, Visualization. C. Tsabaris: Supervision, Methodology, Concep­
tualization, Writing - review & editing. F. Maragkos: Software, Formal
analysis, Writing - review & editing. D.L. Patiris: Supervision, Visuali­
zation, Writing - review & editing. F.K. Pappa: Formal analysis. G.
Eleftheriou: Visualization. S. Alexakis: Software. M. Kokkoris: Su­
pervision, Methodology, Writing - review & editing. R. Vlastou: Su­
pervision, Methodology, Writing - review & editing.
Acknowledgments
Dr. E. G. Androulakaki would like to acknowledge IKY, as part of this
research is implemented through IKY scholarships programme and co-
financed by the European Union (European Social Fund - ESF) and
E.G. Androulakaki et al.
Greek national funds through the action entitled “Reinforcement of
Postdoctoral Researchers”, in the framework of the Operational Pro­
gramme “Human Resources Development Program, Education and
Lifelong Learning” of the National Strategic Reference Framework
(NSRF) 2014–2020. The authors would like to thank ITO Ltd and Mr.
Michael Garyfalos for providing their support to implement all tasks
related to GeoMAREA measurements. The authors would like to
acknowledge Dr A. N. Berlizov for kindly providing the MCNP-CP code
and Dr C. A. Kalfas for supporting the analysis of the γ-ray spectra by
providing the software package SPECTRW.
References
Androulakaki, E.G., Tsabaris, C., Eleftheriou, G., Kokkoris, M., Patiris, D.L., Vlastou, R.,
2015. Seabed radioactivity based on in situ measurements and Monte Carlo
simulations. Appl. Radiat. Isot. 101, 83–92.
Androulakaki, E.G., Kokkoris, M., Tsabaris, C., Eleftheriou, G., Patiris, D.L., Pappa, F.K.,
Vlastou, R., 2016a. In situ γ-ray spectrometry in the marine environment using full
spectrum analysis for natural radionuclides. Appl. Radiat. Isot. 114, 76–86.
Androulakaki, E.G., Tsabaris, C., Eleftheriou, G., Kokkoris, M., Patiris, D.L., Pappa, F.K.,
Vlastou, R., 2016b. Efficiency calibration for in situ γ-ray measurements on the
seabed using Monte Carlo simulations: application in two different marine
environments. J. Environ. Radioact. 164, 47–59.
Bagatelas, C., Tsabaris, C., Kokkoris, M., Papadopoulos, C.T., Vlastou, R., 2010.
Determination of marine gamma activity and study of the minimum detectable
activity (MDA) in 4pi geometry based on Monte Carlo simulation. Environ. Monit.
Assess. 165, 159–168.
Berlizov, A.N., 2006. MCNP-CP a correlated particle radiation source extension of a
general purpose Monte Carlo N particle transport code. In: Semkov, T.M., Pomm�e, S.,
Jerome, S.M. (Eds.), ACS Symposium Series 945. American Chemical Society,
Washington DC, pp. 183–194.
Bezuidenhout, J., 2013. Measuring naturally occurring uranium in soil and minerals by
analysing the 352keV gamma-ray peak of 214Pb using a NaI(Tl)-detector. Appl.
Radiat. Isot. 80, 1–6, 2013.
Chiozzi, P., De Felice, P., Fazio, A., Pasquale, V., Verdoya, M., 2000. Laboratory
application of NaI(Tl) γ-ray spectrometry to studies of natural radioactivity in
geophysics. Appl. Radiat. Isot. 53 (1–2), 127–132.
Done, L., Ioan, M.-R., 2016. Minimum Detectable Activity in gamma spectrometry and its
use in low level activity measurements. Appl. Radiat. Isot. 114, 28–32.
García-Tora~ no, E., Caro, B., Peyr�
es, V., Mejuto, M., 2016. Characterization of a CeBr3
detector and application to the measurement of some materials from steelworks.
Nucl. Instrum. Methods 837, 63–68.
Kalfas, C.A., Axiotis, M., Tsabaris, C., 2016. SPECTRW: a software package for nuclear
and atomic spectroscopy. Nucl. Instrum. Methods 830, 265–274.
Kovler, K., Prilutskiy, Z., Antropov, S., Antropova, N., Bozhko, V., Alfassi, Z.B., Lavi, N.,
2013. Can scintillation detectors with low spectral resolution accurately determine
radionuclides content of building materials? Appl. Radiat. Isot. 77, 76–83.
Applied Radiation and Isotopes 160 (2020) 109124
Lee, Jun-Ho, Byun, Jong-In, Lee, Dong-Myung, 2019. A two-point in situ method for
simultaneous analysis of radioactivity in seawater and sediment. J. Radioanal. Nucl.
Chem. 322, 639–648.
Lutter, G., Hult, M., Billnert, R., Oberstedt, A., Oberstedt, S., Andreotti, E., Marissens, G.,
Rosengård, U., Tzika, F., 2013. Radiopurity of a CeBr3 crystal used as scintillation
detector. Nucl. Instrum. Methods 703, 158–162.
Naqvi, A.A., Khiari, F.Z., Liadi, F.A., Khateeb-ur-Rehman, Isab, A.A., 2016. Performance
tests of a large volume cerium tribromide (CeBr3) scintillation detector. Appl. Radiat.
Isot. 114, 50–56.
Naumenko, A., Andrukhovich, S., Kabanov, V., Kabanau, D., Kurochkin, Yu,
Martsynkevich, B., Shoukavy, Dz, Shpak, P., 2018. Autonomous NaI(Tl) gamma-ray
spectrometer for in situ underwater measurements. Nucl. Instrum. Methods 908,
97–109.
Pappa, F.K., Tsabaris, C., Ioannidou, A., Patiris, D.L., Kaberi, H., Pashalidis, I.,
Eleftheriou, G., Androulakaki, E.G., Vlastou, R., 2016. Radioactivity and metal
concentrations in marine sediments associated with mining activities in Ierissos Gulf,
North Aegean Sea, Greece. Appl. Radiat. Isot. 116 (22–33).
Patiris, D.L., Tsabaris, C., Anagnostou, C.L., Androulakaki, E.G., Pappa, F.K.,
Eleftheriou, G., Sgouros, G., 2016. Activity concentration and spatial distribution of
radionuclides in marine sediments close to the estuary of Shatt al-Arab/Arvand Rud
River, the Gulf. J. Environ. Radioact. 157, 1–15.
Pelowitz, D.B. (Ed.), 2011. MCNPX Users Manual, Version 2.7.0. Los Alamos National
Laboratory Report LA-CP-11-00438, 1–645.
Peyres, V., Crespo, T., Mejuto, M., García-Tora~ no, E., 2017. Measurement of NORM
samples with CeBr3 detectors. Appl. Radiat. Isot. 126, 307–310.
Pilakouta, M., Pappa, F.K., Patiris, D.L., Tsabaris, C., Kalfas, C.A., 2018. A methodology
for expanding the use of NaI(Tl) based spectrometry in environmental radioactivity
measurements. Appl. Radiat. Isot. 139, 159–168.
Quarati, F.G.A., Dorenbos, P., van der Biezen, J., Owens, A., Selle, M., Parthier, L.,
Schotanus, P., 2013. Scintillation and detection characteristics of high-sensitivity
CeBr3 gamma-ray spectrometers. Nucl. Instrum. Methods 729, 596–604.
Safarov, A.A., Safarov, A.N., Azimov, A.N., Darby, I.G., 2017. Rapid assessment
methodology in NORM measurements from building materials of Uzbekistan.
J. Environ. Radioact. 169–170, 186–191.
Tsabaris, C., Androulakaki, E.G., Alexakis, S., Patiris, D.L., 2018. An in-situ gamma-ray
spectrometer for the deep ocean. Appl. Radiat. Isot. 142, 120–127.
Tsabaris, C., Androulakaki, E.G., Prospathopoulos, A., Alexakis, S., Eleftheriou, G.,
Patiris, D.L., Pappa, F.K., Sarantakos, K., Kokkoris, M., Vlastou, R., 2019.
Development and optimization of an underwater in-situ cerium bromide
spectrometer for radioactivity measurements in the aquatic environment. J. Environ.
Radioact. 204, 12–20.
Vidmar, T., 2005. Efftran — a Monte Carlo efficiency transfer code for gamma-ray
spectrometry. Nucl. Instrum. Methods 550, 603–608.
Zeng, Z., Pan, X., Ma, H., He, J., Cang, J., Zeng, M., Mi, Y., Cheng, J., 2017. Optimization
of an underwater in-situ LaBr3:Ce spectrometer with energy self-calibration and
efficiency calibration. Appl. Radiat. Isot. 121, 101–108.
Zhang, Y., Wu, B., Liu, D., Zhang, Y., Cheng, Y., 2018. Development and deployment of
an autonomous sensor for the in-situ radioactivity measurement in the marine
environment. Appl. Radiat. Isot. 142, 181–186.