Composite scintillators based on organic grains and their pulse shape discrimination capability
Studies of photoluminescence, relative light output and optical transmission of organic single-layer composite scintillators with different grain sizes have been carried out. The paper presents the dependences of these values on the grain sizes for fractions <0.04; <0.06; 0.06…0.1; 0.1…0.3; 0....
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| Cite this: | Composite scintillators based on organic grains and their pulse shape discrimination capability / I.F. Khromiuk, N.L. Karavaeva, А.V. Krech, І.V. Lazarev, Ye.V. Martynenko, О.А. Tarasenko, S.U. Khabuseva // Problems of Atomic Science and Technology. — 2022. — № 5. — С. 37-41. — Бібліогр.: 11 назв. — англ. |
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| author | Khromiuk, I.F. Karavaeva, N.L. Krech, А.V. Lazarev, І.V. Martynenko, Ye.V. Tarasenko, О.А. Khabuseva, S.U. |
| author_facet | Khromiuk, I.F. Karavaeva, N.L. Krech, А.V. Lazarev, І.V. Martynenko, Ye.V. Tarasenko, О.А. Khabuseva, S.U. |
| citation_txt | Composite scintillators based on organic grains and their pulse shape discrimination capability / I.F. Khromiuk, N.L. Karavaeva, А.V. Krech, І.V. Lazarev, Ye.V. Martynenko, О.А. Tarasenko, S.U. Khabuseva // Problems of Atomic Science and Technology. — 2022. — № 5. — С. 37-41. — Бібліогр.: 11 назв. — англ. |
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| description | Studies of photoluminescence, relative light output and optical transmission of organic single-layer composite scintillators with different grain sizes have been carried out. The paper presents the dependences of these values on the grain sizes for fractions <0.04; <0.06; 0.06…0.1; 0.1…0.3; 0.3…0.5; 0.5…1.0 mm. Possible physical mechanisms of such results are discussed.
Проведено дослідження фотолюмінесценції, відносного технічного світлового виходу та оптичного пропускання органічних одношарових композиційних сцинтиляторів з різними розмірами гранул. Наведено залежності цих значень від розмірів зерен для фракцій <0,04; <0,06; 0,06…0,1; 0,1…0,3; 0,3…0,5; 0,5…1,0 мм. Обговорюються можливі фізичні механізми таких результатів.
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ISSN 1562-6016. Problems of Atomic Science and Technology. 2022. №5(141) 37
https://doi.org/10.46813/2022-141-037
COMPOSITE SCINTILLATORS BASED ON ORGANIC GRAINS AND
THEIR PULSE SHAPE DISCRIMINATION CAPABILITY
I.F. Khromiuk
1,
*, N.L. Karavaeva
1
, А.V. Krech
1
, І.V. Lazarev
1
, Ye.V. Martynenko
1
,
О.А. Tarasenko
1
, S.U. Khabuseva
2
1
Institute for Scintillation Materials of NAS of Ukraine, Kharkiv, Ukraine;
2
State Scientific Institution “Institute for Single Crystals” of NAS of Ukraine,
Kharkiv, Ukraine
*E-mail: ikhromiuk@gmail.com
Studies of photoluminescence, relative light output and optical transmission of organic single-layer composite
scintillators with different grain sizes have been carried out. The paper presents the dependences of these values on
the grain sizes for fractions <0.04; <0.06; 0.06…0.1; 0.1…0.3; 0.3…0.5; 0.5…1.0 mm. Possible physical
mechanisms of such results are discussed.
PACS: 32.50.+d; 78.60.−b; 87.53
INTRODUCTION
The issue of registration of the flow of ionizing
particles in conditions where the flow intensity is
extremely low is very important in modern medical,
geological, environmental, biological problems, for the
border patrol to preclude unauthorized transport of
nuclear materials, during the liquidation of nuclear man-
made disasters, and etc. Radiation with large specific
losses dE/dx of particle energy E per unit length of its
path x in the media are the most harmful to humans and
other living creatures. The harm caused by ionizing
radiation to a living organism can be described as the
product of the absorbed dose and the so-called
radiation-weight factor wR, which characterizes the
long-term effects of such radiation. For photons of
gamma radiation wR = 1, for alpha particles, fast
neutrons with energies En ≤ 2 MeV and
2 MeV ≤ En ≤ 20 MeV, the values wR = 20, 20, and 10,
respectively [1]. Therefore, even the device that can be
used is capable to accurately count the number of
recorded events but does not separate them by the
“type” of radiation, the use of such information is
dangerous and misleads the user.
For fast neutron spectrometry, it is important that the
scintillation medium has a high hydrogen content, so
organic scintillation materials are most relevant in this
case. Moreover, in contrast with inorganic ones, they
have negligible backscattering for charged particles, so
it is increases the efficiency of their registration.
Organic scintillators in the form of single crystals and
liquids efficiently separate high dE/dx radiation from
low dE/dx background radiation as the slow component
of the radioluminescence pulse. [2], which makes these
materials most effective in creating systems for
detecting radiation that is more harmful to living beings
under background radiation conditions with a low dE/dx
value. In particular, for organic molecular crystals, the
ability to separate signals from radiation with different
dE/dx as a consequence of the process of fusion of
triplet molecular excitons is called the pulse shape
discrimination capability (PSD) [2].
However, modern technology for obtaining organic
single crystals limits their maximum size and shape,
besides being quite expensive. The solution to this
problem can be a new type of scintillators – hetero-
structured organic scintillators, that is, media containing
grains of organic scintillators. These grains are
connected by sintering during hot pressing (polycrystals
or the so-called van der Waals ceramics), or introduced
into a transparent gel composition (composite
scintillators) [2].
In the case of continuous media, the PSD capability,
caused by the difference of the mechanisms of spin-
selective processes for excited T-states, has been well
studied, but for heterostructured materials, the results
are still poorly presented. A similar study was initiated
by the authors of the article. The PSD capability for
such samples is currently considered simply as an
experimental fact [3–5].
In addition, there are currently no data on PSD
capabilities of heterostructured organic scintillators
based on grains of different sizes. However, it is
obvious that the size of an elementary cell (crystal
grain), which limits the transport and recombination of
T-states in such systems, must significantly affect this
process. This, in turn, leads to a change in the formation
of the slow component of the scintillation pulse and, as
a consequence, determines the PSD capability of the
scintillator.
The theoretical basis for such studies were presented
by us in [6]. We note that in the case of this article, the
probability of direct excitation to the T1 state was incre-
ased due to the high optical radiation density.
1. TECHNOLOGICAL ASPECTS OF
OBTAINING OF EXPERIMENTAL
SAMPLES
We have chosen trans-stilbene and p-terphenyl as
the scintillation materials for the studies in this article
because of their known scintillation properties.
The single-crystal samples were grown using the
Bridgman-Stockbarger method. More details about
samples preparation technologies can be found in [6].
1.1. SOURCE MATERIALS
To obtain samples based on p-terphenyl, we used
commercially available raw materials, which were
mailto:ikhromiuk@gmail.com
38 ISSN 1562-6016. Problems of Atomic Science and Technology. 2022. №5(141)
thoroughly purified. Unfortunately, trans-stilbene
manufactured by leading companies does not allow
obtaining scintillators with the required high
characteristics [7]. Our preliminary studies (see, for
example, [6]) have found impurities that limit the
characteristics of the material. Therefore, for the
production of samples based on trans-stilbene, we
synthesized this substance of sufficient quality.
1.2. TECHNOLOGICAL FEATURES OF THE
CREATION OF COMPOSITE SCINTILATORS
Two series of composite scintillators have been
created: based on trans-stilbene and p-terphenyl. In each
series, the samples differed in the grain sizes.
To obtain single-layer composite scintillators
crystalline grains obtained by cracking a polycrystalline
ingot in nitrogen were separated (using a set of
calibrated sieves) into fractions of different sizes. The
selected fraction was applied to a layer of polysiloxane
elastomer, which is not a luminescent material [8], in an
amount of about 70…80% of the total sample volume.
The sample size was chosen to be 15×15 mm for the
convenience of the experiments. For the possibility of
irradiation with alpha particles, one of the surfaces of
the grains was not covered with an elastomer layer. The
samples were left at 60 °C for 24 h to solidify.
2. EXPERIMENTAL RESEARCH METHODS
2.1. METHOD OF THE MEASURING OF THE
LUMINESCENCE SPECTRA
Luminescence spectra were obtained on a Cary
Eclipse Fluorescence Spectrometer. For each material,
its own luminescence excitation wavelength (λ) and
wave-length range of the luminescence spectrum were
selected. The excitation and emission slits were 1.5 nm
and 2.5 nm, respectively. The luminescence intensity (I)
was taken as the number of readings in the
luminescence spectrum.
2.2. METHOD OF THE MEASURING OF THE
SPECTRA OF SCINTILATION AMPLITUDES
The amount of light emitted by the scintillator is
characterized by the magnitude of the luminous flux, i.e.
the ratio of the number of photons arising in the
scintillator to the energy lost in it by ionizing radiation.
The essence of the method is to measure the electrical
signal at the output of the photodetector, which fixes the
glow of the scintillator. At the output of the photo-
detector, the electrical signals, caused by the photons of
the scintillation pulse that have arisen in the scintillator,
are summed. The value of this accumulated signal is
proportional to the amplitude of the scintillation pulse
[7, 9]. For organic scintillators, it is better to use photo-
multipliers as a photodetector. We used a 9208A photo-
multiplier manufactured by Electron Tubes Ltd., for
which, according to the passport data, the dark current
has a record low value of 6.8 10
–11
A at an anode
sensitivity of 50 A/Lm [10]. The original
photomultiplier circuit had an electrical signal
generation time τap = 2 μs.
More often, the light output is determined by the
spectrum of scintillation amplitudes. For this task, an
ADC was used, connected to a PC, where the accumu-
lation and processing of the received data was carried
out.
The relative light output can be calculated using the
following formula: С = (J / Jref)·100%, where J is the
value of the maximum amplitude of the spectrum of the
test sample, Jref is the value of the maximum amplitude
of the spectrum of the reference scintillator. Recalcu-
lating the data obtained in relation to the value of the
light output of the reference scintillators in photons per
1 MeV, we obtain the values of the light output of the
studied samples. The error of this method is less than
5% [11]. The setup was calibrated using
22
Na,
60
Co,
137
Cs, and
152
Eu gamma sources.
239
Pu was used as a
source of alpha particles.
2.3. METHOD OF THE MEASURING OF THE
OPTICAL TRANSMISSION
The optical transmission was measured using a
Shimadzu UV-2450 spectrophotometer. The absolute
error in determining the wavelength was 0.4 nm, and the
error in measuring the spectral transmission coefficients
was 0.6% [11]. An integrating sphere was used in the
measurements, which made it possible to collect most of
the scattered light on the photodetector of the spectro-
photometer. The spectrophotometer has two channels.
Before measurements, the device was calibrated, i.e.
100% was taken as the value when the same signal
passed through both channels of the spectrophotometer.
The sample was placed in the path of one of the beams
and tightly pressed against the outer surface of the
sphere with a clamp. Measurements were made relative
to air (one channel remained unfilled). This value in the
formula Т = (Ф/Ф0)·100% was taken as Ф0 = 100%.
3. RESULTS AND DISCUSSION
3.1. RESULTS OF THE MEASUREMENT OF THE
LUMINESCENCE SPECTRA
The samples were excited in the “red” region of the
spectrum (in the region of absorption of their molecular
triplet excitons) when radiation was detected in the
“blue” region, i.e. in the fluorescence region. In this
way, only the light resulting from the fusion of triplet
excitons can be detected.
The energies of the triplet levels for trans-stilbene
and p-terphenyl are 2.2 and 2.5 eV, respectively [6].
Therefore, if light photons have a small amount of
energy (2.37 eV for trans-stilbene), the intensity of
delayed fluorescence increases. The same is true for
other materials.
As an example, Fig. 1 shows the luminescence
curves obtained for samples based on trans-stilbene
when excited directly to the T1 state (i.e. without excess
energy). The same measurements were made for higher
energies (wavelength for trans-stilbene 523 nm) and
showed the expectedly higher intensity. A similar set of
measurements was carried out for p-terphenyl.
ISSN 1562-6016. Problems of Atomic Science and Technology. 2022. №5(141) 39
Fig. 1. Luminescence spectra of a single crystal and
single-layer composite scintillators based on trans-
stilbene grains upon excitation by the light with a
wavelength of 563 nm
In the figure in the band 350…420 nm, we see the
characteristic fluorescence of trans-stilbene, which has
a low intensity due to indirect (through T–T
annihilation) excitation of luminescence centres. Similar
spectra were obtained for all scintillators in the
framework of this article. Two groups of peaks can be
distinguished: (i) delayed fluorescence (DF) peaks and
(ii) reflected excitation light peak. When the excitation
wavelength was changed, the peaks of the DF band did
not change their position.
Fig. 2. Dependences of the relative intensity of the
delayed fluorescence peak of composite scintillators on
the average size of Lav of trans-stilbene grains
compared to trans-stilbene single crystal, when excited
by light with wavelengths of 523 and 563 nm
Based on the data in Fig. 1 and similar data for
excitation at a wavelength of 523 nm, the curves in
Fig. 2 were plotted. Here Lav = (Lj+1 + Lj)/2 is the
average grain size, where Lj+1 and Lj (Lj+1 > Lj) are the
largest and smallest grains in the fraction.
Similar curves for p-terphenyl are shown in Fig. 3.
Fig. 3. Dependences of the relative intensity of the
delayed fluorescence peak of composite scintillators on
the average size of Lav of p-terphenyl grains compared
to p-terphenyl single crystal, when excited by light with
wavelengths of 496 and 600 nm
Similar curves for p-terphenyl activated by 0.1 wt.%
1,4-diphenyl-1,3-butadiene (DPB) are shown in Fig. 4.
Fig. 4. Dependences of the relative intensity of the
delayed fluorescence peak of composite scintillators on
the average size of Lav of p-terphenyl activated by
0.1 wt.% DPB grains compared to p-terphenyl
activated by 0.1 wt.% DPB single crystal, when excited
by light with wavelengths of 496 and 600 nm
From Figs. 2–4, quite high DF values are observed
for fine-grained scintillators. For scintillators with larger
grains, as the grain size increased, the spread of DF
intensity values exceeded their tendency to increase or
decrease. As expected, the lowest value of the DF
intensity was obtained for single crystals, which is most
likely due to the almost unlimited possibility of of T1
states to “run away” from their point of origin, while the
grain size limits the movement of T-excitons. It should
be remembered that that the lifetime of T-excitons in
such media is on the order of 10
–3
…10
–2
s, so they can
repeatedly bounce off grain boundaries, which increases
the probability of T-T annihilation events. It is important
to note that prof. Agranovich predicted this effect.
40 ISSN 1562-6016. Problems of Atomic Science and Technology. 2022. №5(141)
3.2. RESULTS OF MEASUREMENT OF
SCINTILLATION AMPLITUDE SPECTRA
For the purposes of this article, we measured the
scintillation amplitude spectra of single crystals and
composite scintillators based on selected materials. As
noted earlier, the excitation of the samples was carried
out using a standard source of
239
Pu alpha particles.
For the scintillation amplitude spectra, we will give
as an example data for samples based on p-terphenyl
(Fig. 5).
Fig. 5. Scintillation amplitude spectra of samples of
composite scintillators based on p-terphenyl grains
(curves 2–7) and p-terphenyl single crystal (curve 1).
Curve 2 – grain size < 0.04 mm, curve 3 – < 0.06 mm,
curve 4 – 0.06 – 0.1 mm, curve 5 – 0.1 – 0.3 mm, curve
6 – 0.3 – 0.5 mm, curve 7 – 0.5 – 1.0 mm
Fig. 6. Relative light output C for composite
scintillators based on trans-stilbene (curve 1),
p-terphenyl (curve 2) and p-terphenyl with 0,1% DPB
(curve 3)
Based on the data shown in Fig. 5 and data for other
materials used in this article, the curves shown in Fig. 6
were constructed.
As can be seen from the figure, there is a clear
dependence on the grain sizes.
3.3. OPTICAL TRANSMITTANCE OF SINGLE-
LAYER COMPOSITE SAMPLES
To complement the data in this article, optical
transmission measurements of the previously mentioned
materials were carried out in the wavelength range of
190…800 nm. Graphs for trans-stilbene are given as an
example.
Fig. 7. Spectra of optical transmittance T of samples
based on trans-stilbene. Designations as in Fig. 5
Fig. 7 shows that in the luminescence region of the
scintillation materials studied in this article (>390 nm),
the optical transmittance is quite high. Using the data in
Fig. 7, the dependences of the optical transmission in
the luminescence region on the average granule size
were plotted. These curves are shown in Fig. 8.
Fig. 8. Optical transmission of single-layer composite
scintillators based on selected materials at 390 nm.
Dashed lines I, II and III – optical transmission of
single crystals of trans-stilbene, p-terphenyl and
p-terphenyl, with 0.1% DPB, respectively. Other
designations as in Fig. 6
CONCLUSIONS
Based on the data presented in this article, the
following conclusions can be drawn:
1. The dependence of the intensity of the glow on
the size of the granules differed greatly under
photoexcitation and excitation by ionizing radiation.
This effect arises in connection with different
mechanisms of the formation of instantaneous and
delayed fluorescence in these cases.
2. When excited by alpha particles, there was a ten-
dency for the signal to increase with increasing grain
size to the level of single crystals. This is reminiscent of
our previous results on excitation of these materials by
light into the first singlet state [6]. However, for
granules with a fraction <0.06 mm, there is a spike that
requires further analysis.
ISSN 1562-6016. Problems of Atomic Science and Technology. 2022. №5(141) 41
3. Irradiation with light with a wavelength lying in
the absorption region of triplet excitons of these
materials, a fluorescence spectrum was observed,
similar in spectral composition to the spectrum of
instantaneous fluorescence. According to the
experimental conditions, excitation can occur only due
to the fusion of triplet excitons; accordingly, we
observed a spectrum of delayed fluorescence. Since
there is a multiplicity prohibition, the intensity of this
spectrum reached only a few percent of the intensity of
the excitation light. Note that the sample was excited
not by individual light pulses, but in a continuous mode.
In this case, the drop in the DF intensity due to the
inhibition was compensated for by increasing the
density of the photon flux that excites this material.
Single crystals had the lowest DP intensity, which is
most likely due to the possibility of the T1-states moving
away from each other in such scintillators, since their
volume for these states can be considered quasi-infinite.
In this case, in composite scintillators, the effect of
exciton reflection from the granule surface appears,
which increases the probability of their recombination
with a decrease in the granule size. Recall that the
lifetime of T1-states is about ~10
–3
…10
–2
s.
It should also be noted that, upon excitation by light,
the density of occurrence of T1-states is orders of
magnitude lower than the density of their occurrence in
the track of an alpha particle.
ACKNOWLEDGEMENTS
This work was supported by the National Research
Foundation of Ukraine (project No. 2020.01/0133,
«Heterostructured organic scintillators with high pulse
shape discrimination capability for radioecology
problems».
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Article received 16.09.2022
КОМПОЗИЦІЙНІ СЦИНТИЛЯТОРИ НА ОСНОВІ ОРГАНІЧНИХ ГРАНУЛ
ТА ЇХНЯ МОЖЛИВІСТЬ ДО РОЗДІЛЕННЯ ЗА ФОРМОЮ ІМПУЛЬСУ
I.Ф. Хромюк, Н.Л. Караваєва, A.В. Креч, I.В. Лазарєв, Е.В. Мартиненко,
O.A. Тарасенко, С.У. Хабусєва
Проведено дослідження фотолюмінесценції, відносного технічного світлового виходу та оптичного
пропускання органічних одношарових композиційних сцинтиляторів з різними розмірами гранул. Наведено
залежності цих значень від розмірів зерен для фракцій <0,04; <0,06; 0,06…0,1; 0,1…0,3; 0,3…0,5;
0,5…1,0 мм. Обговорюються можливі фізичні механізми таких результатів.
|
| id | nasplib_isofts_kiev_ua-123456789-195802 |
| institution | Digital Library of Periodicals of National Academy of Sciences of Ukraine |
| issn | 1562-6016 |
| language | English |
| last_indexed | 2025-12-07T16:12:27Z |
| publishDate | 2022 |
| publisher | Національний науковий центр «Харківський фізико-технічний інститут» НАН України |
| record_format | dspace |
| spelling | Khromiuk, I.F. Karavaeva, N.L. Krech, А.V. Lazarev, І.V. Martynenko, Ye.V. Tarasenko, О.А. Khabuseva, S.U. 2023-12-07T10:24:32Z 2023-12-07T10:24:32Z 2022 Composite scintillators based on organic grains and their pulse shape discrimination capability / I.F. Khromiuk, N.L. Karavaeva, А.V. Krech, І.V. Lazarev, Ye.V. Martynenko, О.А. Tarasenko, S.U. Khabuseva // Problems of Atomic Science and Technology. — 2022. — № 5. — С. 37-41. — Бібліогр.: 11 назв. — англ. 1562-6016 PACS: 32.50.+d; 78.60.−b; 87.53 DOI: https://doi.org/10.46813/2022-141-037 https://nasplib.isofts.kiev.ua/handle/123456789/195802 Studies of photoluminescence, relative light output and optical transmission of organic single-layer composite scintillators with different grain sizes have been carried out. The paper presents the dependences of these values on the grain sizes for fractions <0.04; <0.06; 0.06…0.1; 0.1…0.3; 0.3…0.5; 0.5…1.0 mm. Possible physical mechanisms of such results are discussed. Проведено дослідження фотолюмінесценції, відносного технічного світлового виходу та оптичного пропускання органічних одношарових композиційних сцинтиляторів з різними розмірами гранул. Наведено залежності цих значень від розмірів зерен для фракцій <0,04; <0,06; 0,06…0,1; 0,1…0,3; 0,3…0,5; 0,5…1,0 мм. Обговорюються можливі фізичні механізми таких результатів. This work was supported by the National Research Foundation of Ukraine (project No. 2020.01/0133, «Heterostructured organic scintillators with high pulse shape discrimination capability for radioecology problems». en Національний науковий центр «Харківський фізико-технічний інститут» НАН України Problems of Atomic Science and Technology Interaction of relativistic particles with crystals and matter Composite scintillators based on organic grains and their pulse shape discrimination capability Композиційні сцинтилятори на основі органічних гранул та їхня можливість до розділення за формою імпульсу Article published earlier |
| spellingShingle | Composite scintillators based on organic grains and their pulse shape discrimination capability Khromiuk, I.F. Karavaeva, N.L. Krech, А.V. Lazarev, І.V. Martynenko, Ye.V. Tarasenko, О.А. Khabuseva, S.U. Interaction of relativistic particles with crystals and matter |
| title | Composite scintillators based on organic grains and their pulse shape discrimination capability |
| title_alt | Композиційні сцинтилятори на основі органічних гранул та їхня можливість до розділення за формою імпульсу |
| title_full | Composite scintillators based on organic grains and their pulse shape discrimination capability |
| title_fullStr | Composite scintillators based on organic grains and their pulse shape discrimination capability |
| title_full_unstemmed | Composite scintillators based on organic grains and their pulse shape discrimination capability |
| title_short | Composite scintillators based on organic grains and their pulse shape discrimination capability |
| title_sort | composite scintillators based on organic grains and their pulse shape discrimination capability |
| topic | Interaction of relativistic particles with crystals and matter |
| topic_facet | Interaction of relativistic particles with crystals and matter |
| url | https://nasplib.isofts.kiev.ua/handle/123456789/195802 |
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