ARTICLE IN PRESS

Nuclear Instruments and Methods in Physics Research A 529 (2004) 274–279

Scintillation materials for neutron imaging detectors

M. Katagiria,*, K. Sakasaia, M. Matsubayashia, T. Nakamuraa,
Y. Kondob, Y. Chujoc, H. Nantod, T. Kojimae
a
Japan Atomic Energy Research Institute, Tokai, Ibaraki 319-1195, Japan
b
Tohoku University, Aramakiazaaoba, Aoba-ku, Sendai-shi, Miyagi-ken, 980-8579, Japan
c
Kyoto University, Yoshidahoncho, Sakyou-ku, Kyoto-shi, Kyoto-fu, 606-8501, Japan
d
Kanazawa Institute of Technology, Yatsukaho 3-2, Mattou-shi, Ishikawa-ken, 924-0838, Japan
e
Chichibu Fuji Co., Kojikano 755-1, Kojikanocho, Saitama-ken, 368-0193, Japan

Abstract

We have researched scintillation materials for neutron imaging detectors with a photon counting method. The aim of
the research was to develop optimal scintillators, which have the well-balanced performances in detection efficiency,
counting rate, n/g ratio, multi-counting rate, and neutron/g ratio for neutron scattering equipments using high-intensity
pulsed neutron sources. The following scintillation materials were researched: ZnS-series phosphors with neutron
converters, short-life-time phosphors with neutron converters, short-life-time phosphors containing 10B, glass
scintillators containing 10B or 6Li, 6Li-loaded plastic scintillators and organic phosphors containing 10B. The
detection-characteristics of these scintillators were discussed, mainly for their detection efficiency.
r 2004 Elsevier B.V. All rights reserved.

PACS: 29.30.Hs; 29.40.Mc

Keywords: Scintilltor; Phosphor; Neutron; Efficiency; Neutron converter; Pulse height distribution

1. Introduction fications of the various neutron spectrometers, will

The next-generation pulsed neutron source
using a high-intensity proton accelerator (J-PARC
project) has made a great deal of progress in
Japan. At the experimental sites, various kinds of
neutron imaging detectors, which fulfill the speci-
*Corresponding author.
E-mail address: kata@stsp2a0.tokai.jaeri.go.jp
(M. Katagiri).
be used for the neutron scattering experiments.
For this project, we have developed neutron-
imaging detectors using scintillators with a photon
counting method [1–3]. The optimal scintillators
materials should be used according to the specifi-
cations required for the instruments, such as short
decay time, high neutron detection efficiency, high
n/g ratio and low cost.
Therefore, we have researched various scintillat-
ing materials, mainly as follows: ZnS-series phos-
phors with neutron converters, short-life-time

0168-9002/$ - see front matter r 2004 Elsevier B.V. All rights reserved.
doi:10.1016/j.nima.2004.04.165
 ARTICLE IN PRESS
M. Katagiri et al. / Nuclear Instruments and Methods in Physics Research A 529 (2004) 274–279
phosphors with neutron converters, short-life-time
phosphors containing 10B, glass scintillators con-
taining 10B or 6Li, 6Li-loaded plastic scintillators
and organic phosphors containing 10B.
In this paper, the neutron-detection character-
istics of these scintillators will be briefly reviewed,
and discussed their neutron detection efficiency.
2. ZnS:Ag /6LiF scintillators
ZnS:Ag /6LiF scintillator has been widely used
for neutron detectors [4], especially, extensively
developed in ISIS pulsed-neutron facility [5]. The
ZnS:Ag /6LiF scintillator is commercially available.
We have developed ZnS:Ag/6LiF scintillators
aiming to improve their detection efficiency [6].
Fig. 1 shows pulse height distributions of four
ZnS:Ag/6LiF scintillators: JAERI-standard
ZnS:Ag/6LiF, and the products of Bicron (USA),
AST(UK) and Nichia Co.(Japan). These pulse
height distributions were measured by a multi-
channel analyzer after the light was amplified by a
photomultiplier, and a spectroscopy amplifier. An
241
Am–Li of 92.5 GBq was used as a neutron
source. The neutron flux after the thermalization
was B100 n cm 2 s 1.
Each ZnS:Ag/6LiF exhibited different pulse
height distributions. The ZnS:Ag/6LiF scintillators
104
ZnS:AgCl-JAERI-standard
AST:ISIS
Bicron
103
Nichia
Counts/500sec
102
101
100
0 50 100 150
Channel number
Fig. 1. Pulse height distributions of four ZnS:Ag/6LiF scintil-
lators.
275
Table 1
Comparison of the neutron detection efficiencies for thermal
neutrons
Bicron AST:ISIS Nichia JAERI
26.4% 27.3% 25.4% 40.7%
made by Bicron Co. showed a larger number of
counts in the region of low pulse height that in the
higher. On the other hand, the one by AST Co.
exhibited more counts in the higher pulse heights
than that of Bicron. One can see that the JAERI-
standard ZnS:Ag/6LiF scintillator exceeded the
others in counts in all signal height. The pulse
height distribution does strongly depend on
the fabrication method. The measured detection
efficiencies are listed in Table 1. The efficiencies of
ZnS:Ag/6LiF scintillators made by three compa-
nies were similar, 25–27%. The detection efficiency
of the JAERI-standard ZnS:Ag/6LiF scintillator
was 40%, which was about 1.5 times larger than
the others. The reason for this was not clear at this
stage. One possible reason for this might be the
improvement of the light transmission as inferred
from Fig. 1.
3. Comparison with ZnS:Ag/6LiF scintillator and
ZnS:Ag/10B2O3 scintillator
Neutron scintillators composed of ZnS:Ag and
B2O3 were developed, aiming to improve the
neutron detection efficiency because neutron
cross-section of 10B is about four times higher
than that of 6Li. However, the total energy
produced by neutron capture reaction is about
two times lower than that for the reaction in
6
Li [6].
The pulse height distributions of ZnS:Ag/6LiF
scintillators (Bicron, BC-704) and the ZnS:Ag/
10
B2O3 scintillator are compared in Fig. 2. The
maximum channels in the pulse heights for
ZnS:Ag/6LiF and ZnS:Ag/10B2O3 scintillator were
200 170 and 150 channels, respectively. The pulse
height distributions were similar in both distribu-
tions. The neutron detection efficiencies of the
ZnS:Ag/6LiF and the ZnS:Ag/10B2O3 scintillator
 ARTICLE IN PRESS

276 M. Katagiri et al. / Nuclear Instruments and Methods in Physics Research A 529 (2004) 274–279

104 104
ZnS:AgCl+B2O3:600degree ZnS:AgNi5ppm
Bicron
ZnS:AgNi10ppm
103 103
Bicron BC-704
Counts/500sec

Counts/500sec
102 102

101 101

100 100
0 50 100 150 200 250 0 50 100 150 200 250
Channel number Channel number
Fig. 2. Pulse height distributions of ZnS:Ag/6LiF scintillators Fig. 3. pulse height distributions of ZnS:Ag,Ni /6LiF scintilla-
(BC-704) made in Bicron Co. and ZnS:Ag/10B2O3 scintillator. tors and the Bicron BC-704 scintillator.

were 26.4% and 22.0%, respectively. The resultant
detection efficiency of ZnS:Ag/10B2O3 was lower
that that of ZnS:Ag/6LiF, which could be due to
degraded transmittance of the light for the 10B
scintillator. However, it was estimated that the
efficiency of ZnS:Ag/10B2O3 scintillator ap-
proaches relatively the efficiency of ZnS:Ag/6LiF
scintillator with increase of neutron energy be-
cause the absorption efficiency of ZnS:Ag/10B2O3
scintillator calculated based on the cross section of
neutron capture is 61.1%.
4. ZnS:Ag,Ni /6LiF scintillators
It is known that the decay time of ZnS:Ag
decreases by doping killer materials (Ni, Fe, Co)
into the ZnS, although the light intensity de-
creases. We investigated the properties of Ni
doped ZnS:Ag phosphor for a high-counting-rate
neutron scintillation imaging detector. Moreover,
ZnS:Ag, Ni/6LiF scintillators were fabricated to
evaluate the neutron detection efficiency [7].
Fig. 3 shows the pulse height distribution of the
ZnS:Ag,Ni /6LiF scintillators (That of Bicron BC-
704 scintillator was shown as a reference). Samples
containing Ni of 5 and 10 ppm were prepared, and
their decay times of fast component were mea-
sured as 0.230 and 0.210 ms, respectively. The pulse
height for ZnS:Ag,Ni /6LiF scintillators with
10 ppm Ni doping decreased significantly due to
the degradation in transparency of ZnS:Ag,Ni
phosphor. Therefore, the ZnS:Ag,Ni phosphors
should utilize a 10B2O3 neutron converter because
a thin scintillator with the same macroscopic cross
section for neutron capture can be fabricated.
5. ZnO:Zn (P-15) /6LiF scintillator
A ZnO:Zn (P-15) /6LiF scintillator was devel-
oped for high-counting-rate neutron imaging. The
scintillating light of the P-15 exhibited a slightly
longer wavelength (500 nm) than that of ZnS,
however, the decay time of the second component
is faster than that of ZnS:Ag (See Table 2) [8].
Fig. 4 shows the pulse height distributions of the
Table 2
Decay time (ns) of the ZnO and ZnS:Ag,Cl measured by
neutrons
Sample Fast component Slow component
ZnO(P-15) 0.189 1.11
ZnS:Ag, Cl 0.223 1.77
The fast and slow components of the decay time was defined as
the time until the integrated intensity reached the half of
luminescence integrated from 0 to 0.4 and to 4 ms, respectively.

M. Katagiri et al. / Nuclear Instruments and Methods in Physics Research A 529 (2004) 274–279
104
P15(ZnO:Zn, 500nm)
103 BICRON BC-704
Counts/500sec
102
101
100
0 50 100 150 200
Channel number
Fig. 4. Pulse height distributions of the ZnO:Zn (P-15)/6LiF
scintillators and the ZnS:Ag/6LiF scintillators (BC-704).
ZnO:Zn (P-15) /6LiF scintillators and the ZnS:
Ag/6LiF scintillators (Bicron, BC-704). Maximum
peak height for P-15 was about half of that for
BC-704. The detection efficiencies were 24.3 and
26.4% for ZnO:Zn(P-15)/6LiF and BC-704, re-
spectively. It was confirmed that the ZnO:Zn
(P-15)/6LiF can be used in place of ZnS:Ag/6LiF
scintillators where the count rate is rather high.
6. Y2SiO5:Ce3+/6LiF scintillators for high-
counting-rate neutron imaging
It becomes very difficult for ZnS- or ZnS-series-
based scintillation detectors to handle the count
rate of more than 1 Mcps because they have fast
decay time of 0.2 ms and slow component of
prevailing to 1 ms. We have investigated
Y2SiO5:Ce3+ as phosphor with short decay time.
This phosphor exhibited a decay time of 37 ns, and
emitted B104 photons for electrons with the
energy of 1 MeV. Fig. 5 shows the pulse height
distributions of the Y2SiO5:Ce3+/6LiF scintilla-
tors(that of BC-704 as a reference) It was found
that the distribution of Y2SiO5:Ce3+/6LiF were
almost flat in the region from 10 to 60 channels
although the maximum pulse height was about
half of that of BC-704. The amount of light for
Y2SiO5:Ce3+/6LiF was almost identical to that of
conventional 6Li-glass scintillators. The measured
ARTICLE IN PRESS
277
104
YSO/6LiF
Bicron BC-704
103
Counts/500sec
102
101
100
250 0 50 100 150 200
Channel No.
Fig. 5. Pulse height distributions of Y2SiO5:Ce3+/6LiF scintil-
lators and Bicron BC-704 scintillator.
detection efficiency was 37.1%. It was confirmed
that the Y2SiO5:Ce3+/6LiF scintillators can be
used for the high-counting-rate neutron imaging
detectors instead of the 6Li-glass scintillator.
7. 6Li-11B-P Glass scintillators for neutron
detection
We developed Ce-doped glass scintillators com-
posed of lithium, boron and phosphorus as a
substitute 6Li-glass scintillator [9]. A 45% lithium–
20% boron–35% phosphorus (6LBP) glass scintil-
lator loaded with Ce of 1 mol% was fabricated. A
6
Li-enriched Lithium and 11B-enriched Boron
were used in the scintillators. Fig. 6 shows the
pulse height distributions of the 6LBP glass
scintillators with the size of 4 mm  5 mm 
1.0 mmt. The measured neutron detection effi-
ciency was 63.3% for thermal neutrons. The
intensity of luminescence was about one tenth of
that for the 6Li-glass scintillators, but the neutron
events could be separated from the background.
8. Y10BO3:Ce3+ scintillator
C.W.E. van Eijk et al. [10] developed
Y10BO3:Ce3+ scintillator. However, the character-
istics of this scintillator have not been investigated
 ARTICLE IN PRESS

278 M. Katagiri et al. / Nuclear Instruments and Methods in Physics Research A 529 (2004) 274–279

2500 104
Detection area: 4mm x 5mm
2000 YBO3

103 YSO/6LiF
Counts/500sec

Counts/500sec
1500

102
1000

500 101

0
0 50 100 150 200 100
Channel number 0 20 40 60 80 100
Channel No.
Fig. 6. Pulse height distribution for Ce-doped glass scintillators
composed of Lithium, Boron and Phosphorus. Fig. 8. Pulse height distributions of Y10BO3:Ce3+ scintillator
and Y2SiO5:Ce3+/6LiF scintillator.

100
Y10BO3 much smaller than those of Y2SiO5:Ce3+/6LiF.
80 The measured neutron detection efficiency was
5.2% for Y10BO3:Ce3+. The decay time of the
scintillating light was 0.17 ms.
Intensity, a.u.

60

40 9. Other scintillators with fast decay time

20 We attempted to fabricate a ZnO:Zn phosphor

0
200 300 400 500
Wavelength, nm
Fig. 7. Fluorescence spectrum of Y10BO3:Ce3+ phosphor.
enough. We fabricated Y10BO3:Ce3+ phosphor
and evaluated the characteristics.
Fig. 7 shows the fluorescence spectrum of
Y10BO3:Ce3+ phosphor. The phosphor was ex-
cited by 5.4-MeV alpha from the 241Am source.
The peak wavelength of Y10BO3:Ce3+ phosphor
was 395 nm.The intensity was about half of
Y2SiO5:Ce3+ phosphor. The Y10BO3:Ce3+ phos-
phor sheet was made by painting 120 mg of
material on an aluminum plate of 20 mm  20 mm.
Fig. 8 shows the pulse height distribution of the
Y10BO3:Ce3+ phosphor. One can see that the
pulse heights for Y10BO3:Ce3+ phosphor were
that has the peak at the wavelength at 395 nm, for
high-counting-rate neutron imaging because the
600 700 decay time of the ZnO:Zn phosphor was very
short [8]. To fabricate the ZnO:Zn phosphors, a
Spark Plasma Sintering (SPS) method was used.
The ZnO:Zn fabricated by means of the SPS
method had the fast lifetime of 4 ns.
Moreover, we investigated an organic polymer
containing 10B (BP) as the neutron scintillation
material. By evaluation experiments, it is con-
firmed that neutrons can be measured with the
detection efficiency of 2% by the boron polymer
scintillators blended with Polystyrene [11].
10. Conclusion
Many kinds of phosphor/neutron converter
scintillators and neutron scintillators were fabri-
cated and evaluated, especially concerning the
 ARTICLE IN PRESS

M. Katagiri et al. / Nuclear Instruments and Methods in Physics Research A 529 (2004) 274–279 279

detection efficiency, in order to find well-balanced
scintillators for neutron imaging detectors. Con-
sequently, we found that ZnS or ZnS-series
phosphors would be promising ones considering
the detection efficiency and n/g discrimination for
neutron imaging detectors, although their decay
time was rather slow.
References
[1] M. Katagiri, et al., Nucl. Instr. and Meth. A 513 (2003)
374.
[2] M. Katagiri, et al., Appl. phys. A 74 (Suppl.) (2002) S1604.
[3] M. Katagiri, et al., Nucl. Instr. and Meth. A, these
Proceedings.
[4] D.P. Hutchinson, et al.,SPIE, Vol. 3769, Bellingham, WA,
1999 p. 88.
[5] The ISIS Facility, Annual Report 2002–2003, Rutherford
Appleton Laboratory Report, Report Number RAL-TR-
2003-050.
[6] T. Kojima, et al., Nucl. Instr. and Meth. A, these
Proceedings.
[7] M. Matsubayashi, et al., Nucl. Instr. and Meth. A, these
Proceedings.
[8] N. Kubota, et al., Nucl. Instr. and Meth. A, these
Proceedings.
[9] M. Katagiri, et al., Nucl. Instr. and Meth. A, these
Proceedings.
[10] C.W. Eijk, et al., Nucl. Instr. and Meth. A 460
(2001) 1.
[11] H. Kamaya, et al., Nucl. Instr. and Meth. A, these
Proceedings.