2242 IEEE TRANSACTIONS ON NUCLEAR SCIENCE, VOL. 59, NO.

5, OCTOBER 2012

Inorganic Scintillators for Thermal Neutron Detection

Carel W. E. van Eijk, Member, IEEE

Abstract—The He shortage is forcing the neutron community to have been discussed [12], [14]–[16]. Inorganic scintillators will
look for other detection methods. The inorganic scintillator may be be an attractive alternative to gas filled detectors in at least some
an alternative. Thermal-neutron detection by means of inorganic of the devices. In the present paper we will discuss the more
scintillators has successfully been realized on a large scale at ISIS,
UK, using LiF/ZnS:Ag mixed with an organic binder. This ma- traditional and the novel inorganic scintillators and their level
terial is now introduced in the security field. For several reasons of implementation.
other traditional neutron scintillators, Li-glass:Ce and LiI:Eu,
and relatively new materials such as Li Gd(BO ) :Ce and elpa- II. TRADITIONAL SCINTILLATORS
solites like Cs LiYCl :Ce and Cs LiLaBr :Ce are hardly used or
did not yet find their way to application. The same applies to more Presently at ISIS, UK, LiF/ZnS:Ag is used on a large scale
recently studied materials of the LICAF group. The pros and cons [4]. This scintillator has the advantage of (Table I) 1) a low
of these inorganic materials for thermal neutron detection will be density and small-atomic-number elements and consequently
discussed. a small gamma-ray sensitivity, 2) a large difference between
Index Terms—Inorganic scintillators, thermal neutron detec- gamma-ray and neutron pulse shape which offers the possi-
tion. bility of pulse-shape discrimination (PSD), and 3) a very high
light yield which facilitates position sensitive light detection.
I. INTRODUCTION A disadvantage is its slow response, which limits the count
rate. Furthermore, ZnS:Ag can only be obtained as a powder.
LiF is admixed to it and the combination is mixed with an or-
T HERMAL neutron detection is of paramount importance
in both neutron scattering and homeland security. In
the preparation for the construction of the spallation neutron
ganic binder to form a scintillating sheet. Due to self absorp-
tion and scattering of the scintillation light (granular structure)
the material is opaque and the effective thickness is limited to
sources in Oak Ridge, USA, (SNS) and Tokai, Japan, (JSNS),
mm whereas the absorption length at 0.18 nm is
and the anticipated construction of the European Spallation
mm. At ISIS this problem has been tackled by using scintillator
Source (ESS), extensive research started on new concepts
sheets tilted over in V-shaped or Venetian-blind geome-
of position-sensitive neutron detection in the nineties of last
tries. Relatively recent studies [17], [18] have shown that the
century [1], [2]. Yet, today the most used detectors are tradi-
detection efficiency for perpendicular incident neutrons of 0.18
tional He gas proportional counters. An example is the ARCS
nm can be increased from % to % by increasing the
instrument at SNS, in which 920 He tubes, diameter 25 mm,
LiF/ZnS mass mixing ratio from 1/4 to 1/2. This improvement
length 1 m, are used [3]. ZnS/LiF:Ag scintillator fibre-coded
has been implemented in commercial scintillators. E.g., Eljen
detectors have been used on a large scale at ISIS, UK [4]. Novel
Technology offers EJ-426-0 and EJ-426HD2, respectively with
scintillators have hardly been introduced in new instruments.
ratios 1/3 and 1/2 [19]. Another consequence of the opaque-
Only new modules with Li Gd(BO ) :Ce have been studied
ness is that LiF/ZnS:Ag has a continuous pulse height spec-
[5], [6]. The development of novel light collection concepts is
trum. Pulse-height discrimination (PHD) is not possible. Em-
limited to small area detectors [7]–[10].
ploying the improved LiF/ZnS composition 2D position sen-
In homeland security we find He tubes on a large scale in
sitive flat panel detectors have been developed for perpendic-
border control radiation portal monitors (RPMs). Typically 2
ular incidence using wavelength shifting fibers (WLS) [7], [8].
tubes of m length are used per module [11], [12]. Although
Another interesting development is the flexible embedded fiber
other concepts have been proposed, these have not been imple-
detector (FEFD), in which WLS fibers are encapsulated in thin
mented in RPMs [13]. In hand-held monitors we do encounter
LiF/ZnS strips that can be bend [9]. Recently, for security ap-
He detectors as well as neutron scintillators.
plication large area LiF/ZnS:Ag detectors that fit into the He
Due to reduction of nuclear weapons—purification of tritium
RPM housing have been introduced by Saint-Gobain [20] and
being the main He source—and the increased use of He in
Symetrica [21], [22]. Read out is done by means of WLS by
security applications a shortage of He has arisen [11], [14].
using fibers or continuous light guides. These detectors are not
Consequently, the neutron detecting community has to look for
position sensitive. The Saint-Gobain design is based on [13]. In
other thermal-neutron detection methods. Several alternatives
these cases the mass mixing ratio is proprietary information.
A scintillator closely related to LiF/ZnS:Ag is
Manuscript received November 17, 2011; revised January 03, 2012, January
B O /ZnS:Ag [18], [23]. This material was developed
13, 2012, January 19, 2012; accepted January 23, 2012. Date of publication
March 05, 2012; date of current version October 09, 2012. as sheet and glass. It has a 20% higher neutron detection
The author is with the Delft University of Technology, 2629JB Delft, The efficiency than 1/4 mass ratio LiF/ZnS:Ag [23].
Netherlands (e-mail: c.w.e.vaneijk@online.nl).
LiI:Eu is a scintillator that is hardly used in neutron scat-
Color versions of one or more of the figures in this paper are available online
at http://ieeexplore.ieee.org. tering [24]. This is due to its hygroscopicity and the fact that
Digital Object Identifier 10.1109/TNS.2012.2186154 PSD is not possible. A point in its favor is the ratio of 0.87

0018-9499/$31.00 © 2012 IEEE

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 VAN EIJK: INORGANIC SCINTILLATORS FOR THERMAL NEUTRON DETECTION
[25]. This is the highest value known. It offers excellent PHD.
In the security field we find reports on handheld monitors em-
ploying LiI:Eu for detection of both gamma-rays and neutrons
[26].
The Li glass:Ce (GS20) scintillator has a poor light yield,
small ratio, and poor energy resolution. However its re-
sponse is fast and both PHD and PSD are possible. In addition
it is transparent to its emitted light. Furthermore, its cost is less
than that of crystal scintillators. In neutron scattering this scin-
tillator is used in Anger cameras [24] and work is in progress
aiming at employing it in an Anger camera with multi-anode
photomultiplier tubes [10]. For security application a study is
made comparing responses of Li glass and Li glass scintilla-
tors, considering that the difference in pulse height spectra will
give the background-free neutron response [27].
Li Gd(BO ) :Ce (LGB) is an interesting material, intro-
duced in 1996 [28]. Due to the different values, i.e., the
high cross sections of the gadolinium isotopes, without special
measures B and Li will hardly contribute to neutron detection.
To use Li, which gives the highest response signal, we need
material enriched in Li and depleted in B and Gd,
i.e., Li Gd( BO ) :Ce. A disadvantage of employing
Li Gd( BO ) :Ce is the high cost of Gd-depleted
material. In one of the experiments in connection with neutron
scattering, mixtures of Li Gd(BO ) :Ce and Y SiO :Ce
powder in a binder were studied. The short-range neutron
reaction products interact primarily in the Li Gd(BO ) :Ce
grains. Electrons resulting from gamma ray interaction (pho-
toelectric effect, Compton scattering, pair formation) do
all have a long range and will produce scintillation in both
Li Gd(BO ) :Ce and Y SiO :Ce grains. The latter has a
shorter scintillation response time (70 ns) than the former (200,
800 ns) and consequently PSD can be applied. Neutron-gamma
discrimination was clearly demonstrated [5]. LGB has also
been employed in studies aiming at application in security [29].
III. ELPASOLITES
Elpasolites of composition A LiMX :Ce (
Y , Br, I) have been studied extensively in
the last decade [30]–[42]. Of the potential neutron/gamma
scintillators among these materials data are summarized in
Table I. Research started with the gamma-ray response of
Cs LiYCl :Ce (CLYC) [30], followed by Cs LiLaCl :Ce
(CLLC) and Cs LiYBr :Ce (CLYB) shortly thereafter [31],
[32]. The first thermal-neutron response pulse-height spectra
of CLYC and CLYB were published in 2004 [33]. The neutron
light yields are relatively high and narrow neutron lines show
up with ratios of respectively 0.73 and 0.78 (Table I),
well suited for PHD. By substituting La for Y the light yields
increase significantly. For neutrons Cs LiLaBr :Ce (CLLB) is
even brighter than LiF/ZnS:Ag [38]. Although the ratios
of CLLC and CLLB are somewhat lower than those of CLYC
and CLYB, the neutron lines are very narrow and PHD is very
well applicable. Note that the gamma-ray energy resolution of
3.0% of CLLB competes with that of LaBr :Ce [38].
It should be noted that Br containing scintillator materials be-
come radioactive under neutron irradiation due to neutron cap-
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2243
ture in Br, resulting in Br, half-life 18 min. The main decay
product is a beta continuum of 2 MeV endpoint. After min.
in a neutron beam production and decay are almost in equilib-
rium (see Fig. 1). The neutron line at MeV is well above
the endpoint of the beta spectrum. Note that the neutron line will
be an order of magnitude more intense if Li enriched material
is used.
An important issue is the high thermal-neutron capture cross
section of 43 barns of Cl (natural abundance 76%). If in CLYC
or CLLC Li of natural composition is used, only % of the
thermal neutron interactions will occur through the capture re-
action with Li and we would have a very inefficient detector
[35]. If we use 95% Li enriched material the efficiency will in-
crease to %. In CLYB and CLLB the detection efficiency
will increase from % for natural Li to % for 95% Li
enriched material. If, in addition, we replace Cs by Rb, i.e., we
use RLYB and RLLB, the efficiencies would further improve
and change from % to 95% upon using enriched material.
We learn from Table I that the specifications of Rb containing
elpasolites are less favorable and consequently this last step in
efficiency improvement is not advisable. It should further be
noted that Rb is radioactive (half-life y; beta con-
tinuum, 280 keV endpoint) [42]. Concluding this paragraph, if
we want to use a large crystal of CLYC, CLLC, CLYB, or CLLB
for detection of both gamma rays and neutrons, we must use Li
enriched material for efficient neutron detection even though
enough Li would be present in a large crystal with nonenriched
material to cover the neutron absorption length.
An interesting aspect of CLYC and CLLC is the presence of
core valence luminescence (CVL) under gamma-ray excitation
[30], [31], [33], [34]. CVL is absent under neutron excitation
and consequently this phenomenon offers the possibility of PSD
[43]. In the nonchloride scintillators of the above composition
CVL is not observed. The gap between conduction and valence
band is relatively small and instead of CVL Auger effect will
occur. The absorption length of thermal neutrons in 95% Li
enriched CLYC is 3.2 mm, which is large compared with this
length in traditional scintillators. In crystals of this depth CVL
scintillation light may be lost due to absorption in the absorption
band of the Ce dopant, implying that PSD will become more dif-
ficult, if not impossible. However, even in a 25 mm diameter, 10
mm thick CLYC: mol% Ce crystal gamma rays and neutrons
do have a different pulse shape, with clear presence of CVL in
the gamma-ray signal [36]. This was also shown for a 25 mm
diameter, 5 mm thick CLLC:0.1 mol% Ce crystal [38]. It is very
interesting that PSD proves to be also possible using CLLB and
CLYB [38], [37]. In these scintillators the pulse shape difference
does not show up in the first ns but at much later times, viz
ns. In Fig. 2 an example is shown of PSD for CLYB. Neu-
trons and gamma rays are well separated.
At present the conclusion appears justified that 100%
Ce doping does not result in crystals with better properties
[40]–[42].
Growing of large crystals of CLYC appears to be well pos-
sible [44], [45]. Collaboration of RMD [46] and Hilger Crys-
tals [47] resulted in commercially available diam. 25 mm 25
mm canned Li enriched CLYC crystals. Larger crystals (diam.
50 mm 50 mm) have been grown [48]. Provided that hygro-
 2244 IEEE TRANSACTIONS ON NUCLEAR SCIENCE, VOL. 59, NO. 5, OCTOBER 2012

TABLE I
TRADITIONAL AND NEW THERMAL-NEUTRON SCINTILLATORS

Fig. 2. PSD of mixed neutron/gamma radiation field of an Am-Be source de-

Fig. 1. Pulse height spectrum of CLYB in a thermal-neutron beam of the TU
Delft reactor. The lower curve on the left reflects the background spectrum with
the neutron beam off. After switching on the beam we recorded spectra for
5 min, starting at 0, 30, 60, and 90 min. After 90 min. the beta decay spec-
trum from Br decay (half-life 18 min., endpoint energy of 2 MeV) is close to
equilibrium intensity.
tected with CLYB. Neutrons and gamma rays are well separated. For details see
[37]. By courtesy of K. S. Shah, RMD [46].
of Tc 140 keV gamma rays in NaI:Tl) will offer excellent
possibilities for use in a neutron Anger camera. Novel light sen-
sors, especially the silicon photomultiplier arrays, may play an
important role in this.

scopicity is not a limiting factor, it is anticipated that large crys- IV. “LICAF” SCINTILLATORS
tals of the other elpasolites can be grown as well. Recently a serious effort started in Japan to develop
A first application of CLYC in a handheld neutron/gamma thermal-neutron scintillators based on crystals of the type
radiation monitor is considered by FLIR [49]. Furthermore, if LiXAlF :Y Ca Sr Y Ce Eu [50]–[53], [55]–[57],
large crystals can be grown the high light yield under neutron [59], [60]. With Ca and Sr, these materials are respectively
interaction (more than an order of magnitude higher than that known as LICAF and LISAF. Doped with Cr or Ce LICAF and

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 VAN EIJK: INORGANIC SCINTILLATORS FOR THERMAL NEUTRON DETECTION
Fig. 3. PSD of mixed neutron/gamma field detected in LICAF:Ce. In spite of
the small light yield PHD and PSD are feasible. By courtesy of T. Yanagida
[55].
LISAF are used as laser crystals and crystal growing is well
developed. LICAF crystals are commercially available from
Tokuyama Corp. [61]. Crystals of 50 mm diameter have been
grown [52].
LICAF:Ce has a very low light yield [50]–[52]. In this mate-
rial Ce is substituded for Ca . Consequently there is a sur-
plus of charge in the unit cell. This is for example compensated
by a Li vacancy next to the Ce ion, thus deforming the lat-
tice and probably decreasing the scintillation light yield. In an
attempt to introduce charge compensation in a more controlled
way, co-doping of Ce and Na is introduced in [53]. The idea
is to substitute these ions for two Ca ions [54]. The light yield
does increase but remains modest. Yet, for for certain applica-
tions LICAF:Ce,Na may be a useful scintillator. Both PHD and
PSD are possible. See Fig. 3. In [51] 50% and 95% Li enriched
samples were used.
The light yield of LICAF:Eu is significantly higher than that
of LICAF:Ce [56]. The neutron light yield is 29 000 photons,
and the gamma ray light yield is photons/MeV. The
latter was extracted from the pulse height spectrum showing
both the Co and the neutron response. The much lower light
yield of 6 300 photons/MeV reported in [56] has been obtained
from a measurement of the 60 keV gamma rays of Am [55].
The difference may be due to a strong nonproportionality effect.
Furthermore, it should be noted that the light yield depends on
the crystal thickness due to the overlap of Eu absorption and
emission bands [58]. In LICAF:Eu the effect of Na co-doping
was also studied [57]. In this case scintillation is due to Eu
at a Ca site and charge surplus is not an issue. However, the
processes are very complex [58]. Interestingly enough the light
yield increases significantly. Also in this case we extracted the
gamma ray light yield from the pulse height spectrum showing
both neutron and Co response. The ratio of is
very small and whether PSD is feasible is not yet clear. The
difference in decay time between LICAF:Ce and LICAF:Eu is
characteristic for Ce (tens of ns) and Eu ( s).
The light yield of LISAF:Ce is much smaller than that of the
Eu doped compound [59]. For both cases it is about the same as
that of their LICAF counterpart.
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2245
It should be noted that the cross section for neutron capture in
Eu is about five times that of Li. Consequently, one is tempted
to conclude that in the 2% doped scintillators % of the neu-
trons interact with Eu if the crystal is fully Li enriched. How-
ever, the quoted concentrations are the concentrations in the
melt, not in the crystal. For LICAF and LISAF the distribu-
tion coefficients, also called segregation coefficients (ratios be-
tween concentrations in the crystal and in the melt), are
[62]. Consequently the effect of Eu on the neutron-detection ef-
ficiency is negligible.
Of the three eutectic composites at the bottom of Table I,
LiF/SrF :Ce is the most promising as for light yield and
ratio [60]. Wafers of 50 mm diameter, 0.5 mm thick were pro-
duced. It was demonstrated that neutron imaging of 2mm struc-
tures is feasible employing an 8 8 channel position sensitive
photomultiplier.
Of the developed scintillators LICAF:Eu has been selected
to be used in a phoswich detector with BGO to detect thermal
neutrons in the balloon-borne PoGOLite experiment [63].
V. CONCLUSION
In this paper we discussed a couple of mainstreams in inor-
ganic scintillator development aimed at introduction in neutron
scattering or security in connection with the He shortage. It
was not the intention to discuss all neutron scintillator studies
presently going on. Of the traditional scintillators, LiF/ZnS:Ag
will clearly have a revival in the security field. This material
is well developed, and its modest cost in comparison with that
of crystals make it attractive for application. This development
may also be beneficial for broader introduction in neutron scat-
tering. Glass scitillators may also find more application in this
field because of its shorter response time. Of the elpasolites
CLYC starts to find its way into the security field. The cost of
these crystals is relatively high and further industrial develop-
ment of crystal growing is required. It is almost inevitable that
a high light yield material like CLLB will eventually follow.
The LICAF group is still in development. More studies are re-
quired for a better understanding of the pro and cons. On the
other hand, the commercial availability of LICAF and its appli-
cation in PoGOLite are clear indications of the potentiality of
these materials.
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