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Identification and quantification of a Co
137
radiation source under an intense Cs radiation
field using an application-specific CeBr3
spectrometer suited for use in intense radiation
fields

Masaaki Kaburagi, Kenji Shimazoe, Masahiro Kato, Tadahiro Kurosawa &

Hiroyuki Takahashi

To cite this article: Masaaki Kaburagi, Kenji Shimazoe, Masahiro Kato, Tadahiro Kurosawa &
60
Hiroyuki Takahashi (2022) Identification and quantification of a Co radiation source under
137
an intense Cs radiation field using an application-specific CeBr3 spectrometer suited for
use in intense radiation fields, Journal of Nuclear Science and Technology, 59:8, 983-992, DOI:
10.1080/00223131.2022.2026833

To link to this article: https://doi.org/10.1080/00223131.2022.2026833

© 2022 The Author(s). Published by Informa

UK Limited, trading as Taylor & Francis
Group.

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JOURNAL OF NUCLEAR SCIENCE AND TECHNOLOGY
2022, VOL. 59, NO. 8, 983–992
https://doi.org/10.1080/00223131.2022.2026833

ARTICLE

Identification and quantification of a 60Co radiation source under an intense

137
Cs radiation field using an application-specific CeBr3 spectrometer suited
for use in intense radiation fields
a
Masaaki Kaburagi , Kenji Shimazoeb, Masahiro Katoc, Tadahiro Kurosawac and Hiroyuki Takahashib
a
Collaborative Laboratories for Advanced Decommissioning Science, Japan Atomic Energy Agency, Ibaraki, Japan; bSchool of Engineering,
University of Tokyo, Tokyo, Japan; cNational Metrology Institute of Japan, National Institute of Advanced Industrial Science and
Technology, Ibaraki, Japan

ABSTRACT ARTICLE HISTORY

Passive γ-ray spectroscopy is a useful technique for surveying the radioactive wastes and spent Received 18 August 2021
nuclear fuels under nuclear decommissioning. However, this method depends on material Accepted 28 December 2021
properties such as the activity, density, element, scale, and (especially) for low-energy γ rays KEYWORDS
from 235U and 239Pu. The γ-decay lines of 134Cs, 137Cs, 60Co, and 154Eu occur at greater energies Passive γ-ray spectroscopy;
(than those of 235U and 239Pu), and these nuclides provide significant information on spent identification and
nuclear fuel and radioactive wastes. A CeBr3 spectrometer with a small-volume crystal has been quantification of
previously developed for use in intense radiation measurements. We exposed the spectro­ radionuclide; CeBr3; nuclear
meter to radiation dose rates of 0.025, 0.151, 0.342, 0.700, and 0.954 Sv/h under a standard decommissioning
137
Cs radiation field. A 6.38 MBq 60Co calibration source was placed in front of the detector
surface. Identification of the full energy peak at 1173 keV was impossible at dose rates higher
than 0.700 Sv/h. However, subtraction of the 137Cs radiation spectra from the γ-ray spectra
enabled the identification of the full energy peaks at 1173 and 1333 keV at dose rates of up to
0.954 Sv/h; the relative energy resolution at 1173 and 1333 keV was only slightly degraded at
this dose rate.

1. Introduction (30 years). Furthermore, the space in these facilities is

Recently, an increasing number of nuclear facilities
worldwide have been decommissioned. However,
some of these facilities present several difficulties. In
the United Kingdom, the Sellafield nuclear facility,
which was one of the first nuclear facilities in the
world [1], stores large amounts of high-level nuclear
waste. The decommissioning of this facility is a long
and ongoing process. The Chernobyl nuclear power
station suffered a catastrophic accident in April 1986
[2], and large amounts of radionuclides, which were
released into the atmosphere, spread through Eastern
Europe [3]; the nuclear power station is still covered
with stone coffins and large shelters requiring periodic
renewals. Regarding the Tokyo Electrical Power
Company Holding’s (TEPCO’s) Fukushima Daiichi
Nuclear Power Station, the fifth version of ‘Mid-and-
Long-Term Roadmap toward the Decommissioning of
TEPCO’s Fukushima Daiichi Nuclear Power Station’
[4] has been published. This roadmap suggested that
complete decommissioning of the facilities will take 30
to 40 years [5]. In these nuclear facilities, intense
radiation fields are distributed due to large amounts
of radioactive contamination resulting (especially)
from 137Cs nuclide, which has large fission yields for
235
U and 239Pu nuclides, and has a long decay time
insufficient for the installation of large devices due to
broken buildings or systematic design errors. Under
the abovementioned severe environments, manage­
ment of radioactive wastes and spent nuclear fuels
will be required until the end of the decommissioning
process.
Passive γ-ray spectroscopy is a useful technique for
this management. However, this technique depends on
material properties, such as the activity, density, ele­
ment identity, and size. In particular, low-energy γ
rays emitted from 235U or 239Pu nuclides are susceptible
to self-shielding effects, and are easily buried within
background radiations. The γ-decay lines of other
nuclides such as 134Cs, 137Cs, 60Co, and 154Eu nuclides
occur at greater energies (than those of the lines asso­
ciated with 235U or 239Pu nuclides), which provide
beneficial information on spent nuclear fuel and radio­
active wastes. The amounts of 134Cs, 154Eu, and 137Cs in
spent nuclear fuels are characterized by an initial
enrichment, a burnup, and a cooling time [6].
Moreover, 60Co nuclide can be considered a burnup
indicator [7] and radioactive-waste evaluator.
CeBr3 [8–12], which is suitable for use in intense
radiation fields, has become a popular scintillator for
γ-ray spectroscopy. The material exhibits good

CONTACT Masaaki Kaburagi kaburagi.masaaki@jaea.go.jp Collaborative Laboratories for Advanced Decommissioning Science, Japan Atomic
Energy Agency, Ibaraki, Japan
© 2022 The Author(s). Published by Informa UK Limited, trading as Taylor & Francis Group.
This is an Open Access article distributed under the terms of the Creative Commons Attribution-NonCommercial-NoDerivatives License (http://creativecommons.org/licenses/by-
nc-nd/4.0/), which permits non-commercial re-use, distribution, and reproduction in any medium, provided the original work is properly cited, and is not altered, transformed, or
built upon in any way.
984 M. KABURAGI ET AL.
energy resolution (FWHM: full width at half max­
imum 4%–5% at 662 keV) and a fast decay time (~20
ns), although LaBr3(Ce) is characterized by better
energy resolution and faster decay time (16–25 ns).
However, the self-activity of LaBr3(Ce) is larger than
that of CeBr3, and the minimum detection limit of
CeBr3 is better than that of LaBr3(Ce), with γ-ray
spectral lines of 500‒3000 keV [13]. The spectral
range covers the prominent γ-ray decay lines of
134
Cs, 137Cs, 154Eu, and 60Co nuclides. Under intense
γ-ray fields, the amount of a targeted radionuclide
can be small, and the minimum detection limit is
important for identifying small amounts of radionu­
clides under intense radiation fields mainly contrib­
uted by other radionuclides.
Under a 60Co radiation field at dose rates of up
to 0.750 Sv/h, with increasing exposure dose, the
spectral shifts for a small-volume CeBr3 scintillator
increased due to the gain shift of a photomultiplier
tube (PMT) [12]. Therefore, an application-specific
PMT was developed, and its divider circuit was
equipped with individual power supplies to resis­
tors and capacitors between the dynodes at the last
three stages [14]. A small-volume CeBr3 coupled
to the PMT was covered with an aluminum case,
thereby serving a γ-ray spectrometer suited for use
in intense radiation fields. Under 137Cs and 60Co
radiation fields at exposure dose rates of greater
than 1 Sv/h, the energy resolution met the require­
ment for resolving the principal γ-ray decay spec­
tral lines of 137Cs (662 keV) and 134Cs (734 keV)
nuclides under the 137Cs radiation field. The reso­
lution requirement was also met for 60Co
(1333 keV) and 154Eu (1274 keV) nuclides under
the 60Co radiation field. However, this demonstra­
tion yielded insufficient confirmation of the applic­
ability to radiation fields associated with nuclear
decommissioning, where radiation fields consist of
various radionuclides (rather than a single
nuclide). Furthermore, γ-ray spectroscopy for
small amounts of radionuclides under intense
radiation fields is required for surveying radioac­
tive wastes and spent nuclear fuels in nuclear
facilities.
In this study, using an γ-ray spectrometer suited
for use in intense radiation fields [14], identifica­
tion and quantification of a radionuclide via γ-ray
spectroscopy were investigated under
a background-radiation field with various intensi­
ties. We obtained γ-ray spectra of a 137Cs standard
radiation field (background-radiation field) and a
60
Co calibration source under the background-
radiation field. The exposure dose rates of the
background-radiation field ranged from 0.000 to
0.957 Sv/h. Furthermore, the influence of the back­
ground radiations on the identification and quanti­
tation of the source was investigated.
2. Materials and methods
2.1. Measurement system
A small-volume 5 mm × 5 mm × 5 mm CeBr3 crystal
was encapsulated in an aluminum package with
a quartz window. The small scintillator was coupled
to a photomultiplier (H11934-203: Hamamatsu
Photonics K. K., Hamamatsu City, Japan) with an
application-specific divider circuit. This enabled the
use of individual power supplies for the resistors and
capacitors between the last three dynodes at the 8‒10th
stages [14]. Furthermore, the scintillator and photo­
multiplier were covered with an aluminum case for
shielding against light and electrical noise. The supply
voltages to the cathode (Vc) and the three dynodes
(V8–10) were 649, 180, 144, and 46.2 V, respectively.
Using a 137Cs standard calibration source, the energy
resolution was 4.3% at 662 keV.
A digital pulse process unit (APU-8104: Techno-
AP, Hitachinaka City, Japan) was adopted to produce
a readout. The pulse signals from the PMT anode were
inserted directly into an analog-digital converter that
acquired the pulse amplitudes at 109 Hz and with a 14-
bit resolution. The digitalized pulse data was pro­
cessed by a field-programmable gate array. The values
were averaged over eight points, owing to the internal
clock frequency (125 MHz). Furthermore, the average
values were filtered using a digital low-pass filter with
a 10-ns time constant. The areas of the digital-
processed waveforms were integrated over 136 ns,
starting at 8 ns before the pulse signals exceeded the
set threshold. Values of the integrations were then
converted into charge equivalent values as charge-to-
digital converter (QDC) values. Subsequently, the data
was transferred into a personal computer via an ether­
net cable.
2.2. Experimental
The detector was exposed to a standard 137Cs radiation
field (background-radiation field) at the National
Institute of Advanced Industrial Science and
Technology (Tsukuba City, Japan). The institute pro­
vides the national radiation field standard for Japan.
The exposure dose rate was determined in units of air
kinetic energy released per mass, defined in the
International Commission on Radiation Units and
Measurements report 85 [15]. In addition, the inten­
sity of the background-radiation field was indicated by
the 10 mm ambient dose equivalent rate [H � ð10Þ],
which is referred to as the ‘dose rate’ in this study.
Exposure dose rates of 0.025, 0.151, 0.342, 0.474,
0.700, and 0.954 Sv/h were produced by adjusting the
distance between the 137Cs source and the detector, or
by using an attenuator, as shown in Table 1. The
detector was set up such that the center of the detector
entrance surface was located at the center of the
 JOURNAL OF NUCLEAR SCIENCE AND TECHNOLOGY 985

137
Table 1. Distance and attenuator used in the standard Cs
radiation field.
H*(10) [Sv/h] Distance [m] Attenuator and thickness
0.025 4.0 Iron 20 mm
0.151 3.0 None
0.342 2.0 None
0.474 1.7 None
0.700 1.4 None
0.954 1.2 None

standard radiation field. Furthermore, a 60Co calibra­

tion source (462CE, Japan Radioisotope Association)
was placed at the front of the detector surface, and the 60
Figure 1. Schematic showing the detector and the Co cali­
distance between the center of the source and the bration source: top view (i) and side view (II).
detector surface was 2.5 mm (Figures 1 and 2). The γ-
ray spectrum of the 60Co source was obtained in the
absence of the background-radiation, expressed as
a dose rate of 0.000 Sv/h (< 1 µSv/h). All experimental Table 2. List of the experimental parameters: experimental
conditions are listed in Table 2. number [No], background-radiation intensity [H*(10)], radia­
tion source, and symbols (as expressed in Figure 4).
No H*(10) [Sv/h] Radionuclide and activity Symbol
60
2.3. Data analysis 1 0.000 Co 6.38 MBq (a)
2 0.025 None (b)
60
3 0.025 Co 6.38 MBq (b)
The intensity of the 60Co calibration source was given 4 0.151 None (c)
by the exposure rate (X0 [C·kg−1·h−1]) at a position 5 0.151 60
Co 6.38 MBq (c)
1-m away from the reference time. A rate of 8.50 × 108 6 0.342
60
None (d)
7 0.342 Co 6.38 MBq (d)
[C·kg−1·h−1] was determined. The activity of the 60Co 8 0.474 None (e)
60
calibration source for a given time (A0 [MBq]) is 9 0.474 Co 6.38 MBq (e)
10 0.700 None (f)
calculated using Equation 1. 11 0.700 60
Co 6.38 MBq (f)
12 0.954 None (g)
60
X0 � Wair 13 0.954 Co 6.38 MBq (g)
A0 ¼ (1)
Γ 60 Co

Here, Wair is the W-value of air (34.0 [eV]), and
Γ 60 Co is the effective dose rate constant of 60Co
(0.305 [µGy·MBq−1·h−1]). The activity of the 60Co
calibration source was 6.38 MBq at the time of the
experiment. Furthermore, the subtracted spectra
(D) were obtained from absolute values by sub­
tracting the background spectra from the γ-ray
spectra at each exposure dose rate [H*(10)] as
shown in Equation 2.
DðQDC; H� ð10ÞÞ ¼ jns ðQDC; H� ð10ÞÞ nðQDC; H � ð10ÞÞj
(2)
Here, n(QDC, H*(10)) is the count rate per QDC value
at an exposure dose rate [H*(10)] under the back­
ground-radiation field; ns(QDC, H*(10)) is the count
rate per QDC value at the exposure dose rate [H*(10)]
for the γ-ray spectra of the 60Co calibration source
under the background-radiation field.

Figure 2. Experimental photographs: the 137Cs irradiation device (a) and detector setup (b).
986 M. KABURAGI ET AL.

To evaluate the properties, such as position (µ),

relative energy resolution (RE), and detection effi­
ciency, of full energy peaks a fitting was applied to the
ns and D values around the full energy peaks of 60Co.
A fitting function, Fit(QDC), which was defined as
a Gaussian pulse linear function of the QDC value in
Equation 3.
!
ðQDC μÞ2
Fit ðQDCÞ ¼ A exp þ C1 � QDC
2σ
þ C0
(3)
Figure 3. Schematic showing the effective area of the energy
Here, A and σ are the amplitude and standard devia­ peak (Speak).
tion of the Gaussian, respectively, and C1 and C0 are
the gradient and constant of the linear component,
respectively. The relative energy resolution (RE) asso­ 3. Results
ciated with the FWHM of the full energy peaks was 3.1. γ-Ray spectra
estimated using Equation 4.
The γ-ray spectra of the 137Cs standard radiation
2:35σ field and the 60Co calibration source at dose rates
RE ¼ � 100½%� (4) of 0.025, 0.151, 0.342, 0.474, 0.700, and 0.954 Sv/h
μ
were obtained, as shown in Figure 4(b)‒(g).
To evaluate the detection efficiency, the effective area Figure 4(a) shows a spectrum of the 60Co calibra­
of the full energy peaks (Speak) was defined as the tion source in the absence of the 137Cs standard
effective area of the Gaussian component ranging radiation irradiation (No. 1 in Table 2), which is
characterized by a dose rate of 0.000 Sv/h. The
from µ – 2σ to µ + 2σ, as shown in Equation 5 and
spectra of the 137Cs standard radiation field
Figure 3.
(No. 2, 4, 6, 8, 10, and 12 in Table 2) reveal
μþ2σ a full energy peak of 137Cs (137mBa) at 662 keV
Speak ¼ ò ½Fit ðQDCÞ C1 � QDC C0 �dðQDCÞ and a sum energy peak at 1324 keV. These peaks
μ 2σ
were observed across all dose rates, and the sum
(5) peak increased with the dose rate. In γ-ray spectra

Figure 4. γ-ray spectra at 0.000 Sv/h (a), 0.025 Sv/h (b), 0.151 Sv/h (c), 0.342 Sv/h (d), 0.474 Sv/h (e), 0.700 Sv/h (f), and 0.954 Sv/h (g).

of the 60Co calibration source under the standard
radiation field (No. 3, 5, 7, 9, 13 in Table 2), a full
energy peak of 137Cs (137mBa) at 662 keV was
observed across all dose rates and two other peaks
were observed at dose rates as high as 0.474 Sv/h.
The two peaks corresponded to full energy peaks of
60
Co at 1173 and 1333 keV, regarding the spectrum
of the 60Co calibration source at 0.000 Sv/h (No. 1
in Table 2) shown in Figure 4(a). As the exposure
dose rate increased to 0.700 and 0.954 Sv/h, the
peak at 1173 keV was buried within continuum
spectra associated with energy levels exceeding
662 keV. The energy resolution of the γ-ray spec­
trometer was inadequate for resolving the full
energy peak of 60Co at 1333 keV and the sum
energy peak of 137Cs at 1324 keV. Therefore,
a superimposed peak (rather than the individual
peaks) was observed.
3.2. Subtracted spectra (D)
The subtracted spectra (D), mentioned in Section 2.3,
at dose rates of 0.025, 0.151, 0.342, 0.474, 0.700, and
0.954 Sv/h and the γ-ray spectrum of the 60Co cali­
bration source are shown in Figure 5. The full energy
peaks of the 60Co calibration source at 1173 and
1333 keV were observed across all dose rates. In
addition to the two full energy peaks at these ener­
gies, sharp pseudospectral peaks occurred at spectral
values around the full energy peak, the Compton
edge, and the backscattering peak of 137Cs.
3.3. Properties of the full energy peaks
3.3.1. Fitting result
To observe the properties of the full energy peaks at
1173 and 1333 keV, the γ-ray spectra and D were
fitted with the Fit(QDC) function mentioned in
Figure 5. Subtracted γ-ray spectra (d): the log scale plot (main) and linear scale plot around the full energy peaks (sub).
JOURNAL OF NUCLEAR SCIENCE AND TECHNOLOGY 987
Section 2.3. The full energy peak at 1333 keV was
successfully fitted for the γ-ray spectra and D across
all dose rates. The full energy peak at 1173 keV was
also successfully fitted for the D across all dose rates.
However, fitting for the spectra was successful at dose
rates of 0.025, 0.151, 0.342, and 0.474 Sv/h, but failed
at 0.700 and 0.954 Sv/h. Furthermore, the full energy
peaks at 1173 and 1333 keV in the γ-ray spectrum of
the 60Co calibration source (in the absence of 137Cs
irradiation) were also fitted. The corresponding spec­
tra and D at 0.000 Sv/h are shown in Figure 4(a).
3.3.2. Peak position
The peak positions (μ) of the γ-ray spectra and D at
1173 and 1333 keV are shown in Figure 6, and the
numerical values are listed in Tables 3 and 4. The full
energy peak at 1173 keV was positioned by a μ value of
179.6 pico-coulombs (pC) at 0.000 Sv/h. The μ values
for the spectra and D were the same at dose rates of up
to 0.474 Sv/h, and the values of 181.6, 181.8, 181.3, and
181.8 pC occurred at 0.025, 0.151, 0.342, and 0.474 Sv/
h, respectively. No μ values could be obtained at 0.700
and 0.954 Sv/h for the spectra, but corresponding
values of 182.1 and 183.0 pC, respectively, were
obtained for the D.
For the full energy peak at 1333 keV, the μ value at
0.000 Sv/h was 203.6 pC. The μ values for the γ-ray
spectra and D increased to the same values of 205.9
and 206.2 pC at 0.025 and 0.151 Sv/h. At dose rates of
0.342, 0.474, and 0.700 Sv/h, the μ values were 205.4,
205.8, and 205.7 pC for the spectra, and 205.6, 206.2,
and 206.3 pC for the D, respectively. At 0.954 Sv/h, the
μ values for the spectra and D were 206.6 and 208.1
pC, respectively.
Slight spectral shifts occurred at dose rates of 0.000‒
0.025 Sv/h and 0.700‒0.954 Sv/h for the full energy
peaks at 1173 and 1333 keV.
988 M. KABURAGI ET AL.

Figure 6. Peak positions (µ) for the γ-ray spectra and D: the full energy peaks at 1173 keV (a) and 1333 keV (b).

3.3.3. Relative energy resolution
The relative energy resolution (RE) at 1173 and
1333 keV for the γ-ray spectra and D is shown in
Figure 7, and the numerical values are listed in Tables
5 and 6. The RE value at 1173 keV was 3.1% at
0.000 Sv/h, and the values for the γ-ray spectra were
3.2, 3.1, 3.2, and 3.0% at 0.025, 0.151, 0.342, and
0.474 Sv/h, respectively. No values could be obtained
at 0.700 and 0.954 Sv/h. The RE values for the D at
1173 keV were 3.2, 3.1, 3.2, 3.1, 2.9, and 3.3% at 0.025,
0.151, 0.342, 0.474, 0.700, and 0.954 Sv/h,
respectively.
For the full energy peak at 1333 keV, the RE value
for the γ-ray spectra was 3.0% at 0.000 Sv/h, and the RE
values for the D were equal to or better than those of
the spectra across all dose rates. For dose rates of
0.025, 0.151, 0.342, 0.474, 0.700, and 0.954 Sv/h, the
RE values were 2.9, 3.0, 3.1, 3.2, 3.1, and 3.3%, respec­
tively, for the spectra and 2.9, 3.0, 3.0, 3.0, 3.1, and
3.1%, respectively, for the D.
3.3.4. Effective peak area
The effective peak areas (Speak) of the full energy peaks
at 1173 and 1333 keV for the γ-ray spectra and D are
presented in Figure 8, and the numerical values are
listed in Tables 7 and 8. As the exposure dose rate
increased to 0.954 Sv/h, the Speak values decreased with
the exception of the full energy peak at 1333 keV for
the γ-ray spectra at 0.151 and 0.954 Sv/h. The Speak
values of the full energy peak at 1173 keV for the
D surpassed the values for the spectra at dose rates of
0.342‒0.474 Sv/h. At dose rates higher than these
levels, no Speak values could be obtained for the spec­
tra. However, at dose rates of 0.342‒0.954 Sv/h, the
values at 1333 keV for the spectra were larger than
those for the D.
4. Discussion
Slightly systematic spectral shifts occurred at dose
rates of 0.000‒0.025 Sv/h and 0.700‒0.954 Sv/h.
Previously, using an ordinary PMT with a normal
resistor voltage divider circuit (R7600U-200 and
E5966: Hamamatsu Photonics K. K., Hamamatsu
City, Japan), spectral shifts began at a dose rate of
a few tens of mSv/h [12]. In contrast, the spectrometer
with individual power supplies to the resistors and
capacitors between dynodes at the last three stages
provided gain stability, and no systematic position
shifts were observed at dose rates of 0.025‒0.700 Sv/

Table 3. Peak position (µ) of the full energy peak at 1173 keV. Table 4. Peak position (µ) of the full energy peak at 1333 keV.
H*(10) [Sv/h] µ for γ-ray spectra [pC] µ for D [pC] H*(10) [Sv/h] µ for γ-ray spectra [pC] µ for D [pC]
0.000 179.6 179.6 0.000 203.6 203.6
0.025 181.6 181.6 0.025 205.9 205.9
0.151 181.8 181.8 0.151 206.2 206.2
0.342 181.3 181.3 0.342 205.4 205.6
0.474 181.8 181.8 0.474 205.8 206.2
0.700 None 182.1 0.700 205.7 206.3
0.954 None 183.0 0.954 206.6 208.1
 JOURNAL OF NUCLEAR SCIENCE AND TECHNOLOGY 989

Figure 7. Relative energy resolutions (RE) for the γ-ray spectra and D: the full energy peaks at 1173 keV (a) and 1333 keV (b).

Table 5. Relative energy resolution (RE) of the full energy peak radiations consisted of direct γ rays emitted from
137
at 1173 keV. Cs (137mBa) nuclides and the corresponding scatter,
H*(10) [Sv/h] RE for γ-ray spectra [%] RE for D [%] and these energy values were smaller than 662 keV.
0.000 3.1 3.1 Thus, the continuum spectra associated with energy
0.025 3.2 3.2
0.151 3.1 3.1 levels exceeding 662 keV were generated by multiple γ
0.342 3.2 3.2 rays (rather than a single γ ray). This occurred when
0.474 3.0 3.1
0.700 None 2.9 more than one γ ray interacted with the CeBr3 crystal
0.954 None 3.3 during time intervals shorter than the rising times of
the pulse signals, and these signals were superimposed
as single pulses (multiple γ-ray event). When the
Table 6. Relative energy resolution (RE) of the full energy peak exposure dose rate increased, the continuum spectra
at 1333 keV.
increased due to the increasing intensity of the multi­
H*(10) [Sv/h] RE for γ-ray spectra [%] RE for D [%]
0.000 3.0 3.0
ple γ-ray event, which buried the γ-ray spectrum of
0.025 2.9 2.9 the 60Co calibration source. Fittings of the full energy
0.151 3.0 3.0 peak at 1173 keV were unsuccessful at dose rates of
0.342 3.1 3.0
0.474 3.2 3.0 0.700 and 0.954 Sv/h. However, for the D, successful
0.700 3.1 3.1 fitting at 1173 keV was realized at dose rates of up to
0.954 3.3 3.1
0.954 Sv/h. The full energy peak at 1333 keV was
successfully fitted for the γ-ray spectra and D at dose
rates of up to 0.954 Sv/h. That is, the peak was also
h. The individual power supply started at dose rates of buried within the background γ-ray spectra but the
0.000‒0.025 Sv/h, which could cause slight gain shifts sum energy peak of 662 keV at 1324 keV intensified
of the PMT. In contrast, the individual supply was the superimposed peak at high dose rates, thereby
applied to resistors and capacitors associated with allowing successful fitting. However, the D also pro­
the last three dynode stages (rather than all dynode vided pseudospectral peaks around the backscattering
stages), but the potentials of the other front dynodes peak, Compton edge, and full energy peak of 137Cs
could change with large pulse current flows at dose (sharp spectral points). The values for both ns(QDC,
rates of 0.700‒0.954 Sv/h. H*(10)) and n(QDC, H*(10)), defined in Section 2.3,
The γ-ray spectrum of the 60Co calibration source changed significantly around the sharp spectral points.
was buried within continuum γ-ray spectra, owing to Therefore, even if the differences between the sharp
the background-radiation. The continuum spectra spectral points of ns(QDC, H*(10)) and n(QDC, H*
were greater than the full energy peak of 137Cs (10)) are small, the D values around the sharp points
(137mBa) at 662 keV. However, the background increased, thereby leading to the pseudospectral peaks.
990 M. KABURAGI ET AL.

Figure 8. Effective peak areas (Speak) of the full energy peaks at 1173 keV (a) and 1333 keV (b) for the γ-ray spectra and D.

Table 7. Effective peak areas (Speak) of the full energy peak at In γ-ray spectroscopy, the detection efficiencies are
1173 keV. often determined by the areas of the full energy peaks
H*(10) [Sv/h] Speak for γ-ray spectra Speak for D
[16], associated with the quantifications of radionu­
0.000 14.9 14.9
0.025 14.6 14.6 clides. For the full energy peak of 1173 keV, the Speak
0.151 13.1 13.0 value for D at 0.954 Sv/h was 4.4 times smaller than
0.342 8.8 9.5
0.474 6.0 6.7
that at 0.000 Sv/h. For the full energy peak of
0.700 None 4.5 1333 keV, the Speak values for the γ-ray spectra and
0.954 None 3.4 D were 1.9 and 3.6 times smaller than those at
0.000 Sv/h. This suggested that the background-
radiation led to an underestimation of the 60Co cali­
bration source. When the dose rate due to background
Table 8. Effective peak areas (Speak) of the full energy peak at
1333 keV. radiations increased, the live-time of the spectrometer
H*(10) [Sv/h] Speak for γ-ray spectra Speak for D decreased. The resulting decrease in the ratio of γ-ray
0.000 12.4 12.4 fluence rate due to the 137Cs radiation fields to that due
0.025 11.2 11.1 to the 60Co calibration source led to a reduction in the
0.151 11.5 11.4
0.342 9.0 7.4 detection rate of the γ rays emitted from the 60Co
0.474 8.3 6.1 calibration source.
0.700 6.5 3.6
0.954 6.7 3.4
At dose rates higher than 0.151 Sv/h, the Speak
values of the full energy peak at 1173 keV for the
D surpassed those for the γ-ray spectra; the opposite
trend was observed for the Speak values of the full
At dose rates of 0.000‒0.954 Sv/h, the RE values at energy peak at 1333 keV. The background-
1173 keV ranged from 3.0 to 3.2%, and the values at subtraction radiation spectra resolved the two spectra
1333 keV ranged from 2.9 to 3.3%. The short pulse generated by the 137Cs radiation field and the 60Co
signals of the CeBr3 spectrometer reduced distortions calibration source, thereby revealing the degradation
of the waveforms, without deterioration of the RE effect of the Speak due to the background-radiation.
values at dose rates higher than 0.000‒0.954 Sv/h. So, However, the sum energy peak of 137Cs at 1324 keV
the RE values were better (by 8.6% at 1173 keV and intensified the superimposed energy peak with the full
4.4% at 1333 keV) than the energy resolution required energy peak at 1333 keV and the sum energy peak,
for identifying 60Co (1173 and 1333 keV) and 154Eu leading to an increase in the Speak values.
(1274 keV). The D associated with dose rates exceed­ Subtraction of the background-radiation spectra was
ing 0.700 Sv/h could only provide an RE value at helpful in identifying small amounts of radioactive
1173 keV. sources. For this subtraction, background-radiation

spectra were required at each place, and hence template
spectra were obtained by measuring γ-ray spectra cor­
responding to major radionuclides. A maximum-
likelihood spectrum for a background spectrum was
then reconstructed using the template spectra.
Nuclear facilities under severe nuclear decommis­
sioning have radiation fields at extremely high dose
rates (10–1000 Sv/h) [1–5]. In this study, γ-ray spec­
troscopy for a 6.38 MBq 60Co radionuclide was con­
ducted at dose rates of up to 0.957 Sv/h (~1 Sv/h).
However, this was insufficient for use in the manage­
ment of radioactive wastes and spent nuclear fuels
under intense radiation fields in nuclear facilities
under decommissioning.
5. Summary
In this study, a small-volume CeBr3 spectrometer
already developed for use under intense radiation fields
was employed, and γ-ray spectroscopy for a 6.38 MBq
60
Co radionuclide was performed under a 137Cs stan­
dard radiation field (background-radiation fields) at
dose rates of up to 0.957 Sv/h (~1 Sv/h). The full energy
peak at 1173 keV was buried with the γ-ray spectra of
multiple γ-ray interactions due to the background
radiations, and identification of the full energy peak
was impossible at dose rates higher than 0.700 Sv/h.
Subtraction of the background radiations from the γ-
ray spectra enabled the identification at dose rates of up
to 0.954 Sv/h, but also generated pseudospectral peaks.
Background radiations resulted in underestimation of
radionuclides. The detection efficiency of the full energy
peak at 1173 keV at 0.954 Sv/h for the background-
subtracted spectra was 4.4 times smaller than that at
0.000 Sv/h, and those at 1333 keV were 1.9 and 3.6 times
smaller for the obtained γ-ray spectra and background-
subtracted spectra, respectively.
In the future, reconstruction algorithms of back­
ground γ-ray spectra at each place should be devel­
oped in order to complete the background-subtracting
technique. The identification of full energy peaks can
be done under more intense radiation fields at dose
rates of 10–1000 Sv/h. The effect of background-
radiation interfaces on the identification of radionu­
clides must be taken into consideration. Finally, to
show the practicality, demonstrations of γ-ray spectro­
scopy under radiation fields with more complex spec­
tra (than those considered here).
Acknowledgments
The authors are grateful for the helpful suggestions from
I. Wakaida, K. Takasaki, and K. Okumura who work at the
Collaborative Laboratory for the Advanced Decommissioning
Sciences (CLADS) at Japan Atomic Energy Agency.
JOURNAL OF NUCLEAR SCIENCE AND TECHNOLOGY 991
Disclosure statement
No potential conflict of interest was reported by the author(s).
ORCID
Masaaki Kaburagi http://orcid.org/0000-0002-8845-4933
References
[1] The Nuclear Decommissioning Authority. The
nuclear decommissioning authority: progress with
reducing risk at Sellafield (House of Commons, HC
1126). Victoria, London: National Audit Office; 2018.
[2] Anspaugh LR, Catlin RJ, Goldman M. The global
impact of the Chernobyl reactor accident. Science.
1988;242(4885):1513–1519.
[3] Lewis HW. The accident at the Chernobyl’ nuclear
power plant and its consequences. Environ Sci Policy
Sustain Dev. 1986;28(9):25–27.
[4] METI [Internet]. Mid-and-long-term road map
towards the decommissioning of TEPCO’s
Fukushima Daiichi Nuclear Power Station. Available
from: https://www.meti.go.jp/english/earthquake/
nuclear/decommissioning/;2019.
[5] International Atomic Energy Agency. The
Fukushima Daiichi accident (Vienna, Austria:
Marketing and Sales Unit, Publishing Section
International Atomic Energy Agency Vienna
International Centre). 2015.
[6] Favalli A, Vo D, Grogan B, et al. Determining
initial enrichment, burnup, and cooling time of
pressurized-water-reactor spent fuel assemblies by
analyzing passive gamma spectra measured at the
Clab interim-fuel storage facility in Sweden. Nucl
Instrum Methods Phys Res A. 2016;820:102–111.
[7] Hawari AI, Chen J, Su B, et al. Assessment of
on-line burnup monitoring of pebble bed reactor
fuel using passive spectrometry 2001 IEEE
Nuclear Science Symposium Conference 4-10
Nov. 2001 San Diego, CA, USA. 2002;(IEEE):
398–402.
[8] Shah KS, Glodo J, Higgins W, et al. CeBr3 scintillators
for gamma-ray spectroscopy. IEEE Trans Nucl Sci.
2005;52(6):3157–3159.
[9] Guss P, Reed M, Yuan D, et al. CeBr3 as a
room-temperature, high-resolution gamma-ray
detector. Nucl Instrum Methods Phys Res A.
2009;608(2):297–304.
[10] Quarati FGA, Dorenbos P, Van Der Biezen J, et al.
Scintillation and detection characteristics of
high-sensitivity CeBr3 gamma-ray spectrometers.
Nucl Instrum Methods Phys Res A.
2013;729:596–604.
[11] Fraile LM, Mach H, Vedia V, et al. Fast timing study
of a CeBr3 crystal: time resolution below 120 ps at
60
Co energies. Nucl Instrum Methods Phys Res A.
2013;701:235–242.
[12] Kaburagi M, Shimazoe K, Otaka Y, et al. A cubic
CeBr3 gamma-ray spectrometer suitable for the
decommissioning of the Fukushima Daiichi Nuclear
Power Station. Nucl Instrum Methods Phys Res A.
2020;971:164118.
992 M. KABURAGI ET AL.
[13] Kozyrev A, Mitrofanov I, Owens A, et al.
A comparative study of LaBr3(Ce3+) and CeBr3
based gamma-ray spectrometers for planetary remote
sensing applications. Rev Sci Instrum. 2016;87
(8):085112.
[14] Kaburagi M, Shimazoe K, Kato M, et al. Gamma-ray
spectroscopy with a CeBr3 scintillator under intense
γ-ray fields for nuclear decommissioning. Nucl
Instrum Methods Phys Res A. 2021;988:164900.
[15] Seltzer SM, Bartlett DT, Burns DT, et al. The
international commission on radiation units and
measurements. J ICRU [Internet]. 2011;11(1):
NP.1–NP. Available from: https://academic.oup.
com/jicru/article-lookup/doi/10.1093/jicru/ndr011
[16] Knoll GF. Radiation detection and measurement.
Chichester: Wiley; 2010.