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Springer Proceedings in Physics 227

Mikhail Korzhik
Alexander Gektin Editors

Engineering
of Scintillation
Materials and
Radiation
Technologies
Selected Articles of ISMART2018
Springer Proceedings in Physics

Volume 227
Indexed by Scopus
The series Springer Proceedings in Physics, founded in 1984, is devoted to timely
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Mikhail Korzhik Alexander Gektin
•

Editors

Engineering of Scintillation
Materials and Radiation
Technologies
Selected Articles of ISMART2018

123
Editors
Mikhail Korzhik Alexander Gektin
Research Institute for Nuclear Problems Institute for Scintillation Materials
Belarusian State University National Academy of Sciences of Ukraine
Minsk, Belarus Kharkiv, Ukraine

ISSN 0930-8989 ISSN 1867-4941 (electronic)

Springer Proceedings in Physics
ISBN 978-3-030-21969-7 ISBN 978-3-030-21970-3 (eBook)
https://doi.org/10.1007/978-3-030-21970-3
© Springer Nature Switzerland AG 2019
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Contents

Part I Fundamental Studies

1 Fast Processes in Scintillators . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 3
Andrei N. Vasil’ev
2 Transient Phenomena in Scintillation Materials . . . . . . . . . . . . . . . 19
G. Tamulaitis, S. Nargelas, A. Vaitkevičius, M. Lucchini, E. Auffray,
A. Fedorov, V. Mechinsky and M. Korjik
3 Fluctuations of Track Structure and Energy Resolution
of Scintillators . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 29
A. Gektin and Andrei N. Vasil’ev
4 New Properties and Prospects of Hot Intraband Luminescence
for Fast timing . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 41
Sergey I. Omelkov, Vitali Nagirnyi and Marco Kirm

Part II Material Science

5 Ceramic Scintillation Materials—Approaches, Challenges
and Possibilities . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 57
P. V. Karpyuk, G. A. Dosovitskiy, D. E. Kuznetsova,
E. V. Gordienko, A. A. Fedorov, V. A. Mechinsky, A. E. Dosovitskiy
and M. V. Korzhik
6 Scintillation Materials with Disordered Garnet Structure
for Novel Scintillation Detectors . . . . . . . . . . . . . . . . . . . . . . . . . . . 75
Y. U. Tratsiak, T. Anniyev, D. Agrawal, M. Vasilyev
and V. Khabashesku
7 Garnet Crystal Growth in Non-precious Metal Crucibles . . . . . . . . 83
O. Sidletskiy, P. Arhipov, S. Tkachenko, Ia. Gerasymov, D. Kurtsev,
V. Jarý, R. Kučerková, M. Nikl, K. Lebbou and E. Auffray

v
vi Contents

Part III Technology and Production

8 Towards New Production Technologies: 3D Printing
of Scintillators . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 99
P. S. Sokolov, G. A. Dosovitskiy, A. E. Dosovitskiy and M. V. Korjik
9 Enriched 40Ca100MoO4 Single Crystalline Material for Search
of Neutrinoless Double Beta Decay . . . . . . . . . . . . . . . . . . . . . . . . . 113
A. Alenkov, O. Buzanov, A. Dosovitskii, V. Kazalov,
V. Kornoukhov and A. Mikhlin
10 Plastic Scintillators with the Improved Radiation
Hardness Level . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 125
P. N. Zhmurin, Yu A. Gurkalenko, V. N. Pereymak, D. A. Eliseev
and O. V. Eliseeva
11 State of the Art of Scintillation Crystal Growth Methods . . . . . . . . 147
V. Taranyuk

Part IV Detector Solutions

12 Application of Scintillation Detectors in Cosmic Experiments . . . . . 165
A. F. Iyudin and S. I. Svertilov
13 Neutron Cross Section Measurements with Diamond Detectors . . . 187
E. Griesmayer, P. Kavrigin and C. Weiss
14 Investigation of the Properties of the Heavy Scintillating Fibers
for Their Potential Use in Hadron Therapy Monitoring . . . . . . . . . 195
K. Rusiecka, J. Kasper, A. Magiera, A. Stahl and A. Wrońska
15 Development of a Submillimeter Portable Gamma-Ray
Imaging Detector, Based on a GAGG:Ce—Silicon
Photomultiplier Array . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 211
S. David and I. Kandarakis
16 Application Scintillation Comparators for Calibration
Low Intense Gamma Radiation Fields by Dose Rate
in the Range of 0.03–0.1 µSv/h . . . . . . . . . . . . . . . . . . . . . . . . . . . . 221
R. Lukashevich, Y. Verhusha, V. Guzov and V. Kozemyakin
17 Antineutrino Detectors . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 237
V. V. Gilewsky, I. S. Satsounkevich, V. M. Dunin and A. S. Lobko
Contents vii

Part V Instrumentation
18 Development of the X-ray Security Screening Systems
at ADANI . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 249
D. A. Bairashewski, G. Yu. Drobychev, V. A. Karas, V. V. Komarov
and M. V. Protsko
19 Optimization of Physico-Topological Parameters of Dual Energy
X-ray Detectors Applied in Inspection Equipment . . . . . . . . . . . . . 261
I. Slavashevich, D. Pozdnyakov, D. Kasiuk and V. Linev
20 Control of Organ and Tissue Doses to Patients During
Computed Tomography . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 271
K. A. Verenich, V. F. Minenko, K. O. Makarevich,
A. A. Khrutchinsky and S. A. Kutsen
21 Information Tool for Multifarious Scientific and Practical
Research . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 281
S. Sytova
22 Calibration and Performance of the CMS Electromagnetic
Calorimeter During the LHC Run II . . . . . . . . . . . . . . . . . . . . . . . 293
Tatyana Dimova (on behalf of the CMS Collaboration)
23 Study the Applicability of Neutron Calibration Facility
for Spectrometer Calibration as a Source of Gamma Rays
with Energies to 10 MeV . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 299
A. Antonov, V. Antonov, Y. Verhusha, V. Guzov, D. Komar
and R. Lukashevich
24 Thermal Neutron Detector Based on LaOBr:Ce/LiF . . . . . . . . . . . . 305
L. Fiserova and J. Janda
25 Specifics of 3D-Printed Electronics . . . . . . . . . . . . . . . . . . . . . . . . . 315
G. Gorokhov, M. Katsemba, A. Liubimau, A. Lobko and A. Melnikau
Contributors

D. Agrawal Baker Hughes a GE Company, Houston, USA

A. Alenkov JSC Fomos-Materials, Moscow, Russia
T. Anniyev Baker Hughes a GE Company, Houston, USA
A. Antonov ATOMTEX Scientific and Production Unitary Enterprise, Minsk,
Belarus
V. Antonov ATOMTEX Scientific and Production Unitary Enterprise, Minsk,
Belarus
P. Arhipov Institute for Scintillation Materials NAS of Ukraine, Kharkiv, Ukraine
E. Auffray CERN, Geneva, Switzerland;
European Organization for Nuclear Research, Geneva 23, Switzerland
D. A. Bairashewski ADANI, Minsk, Belarus
O. Buzanov JSC Fomos-Materials, Moscow, Russia
S. David Department of Biomedical Engineering, University of West Attica,
Athens, Greece
Tatyana Dimova (on behalf of the CMS Collaboration) Novosibirsk State
University, Novosibirsk, Russia
A. Dosovitskii JSC NeoChem, Moscow, Russia
A. E. Dosovitskiy NeoChem JSC, Moscow, Russia
G. A. Dosovitskiy National Research Center “Kurchatov Institute” – IREA,
Moscow, Russia
G. Yu. Drobychev ADANI, Minsk, Belarus
V. M. Dunin JINR, Dubna, Russia

ix
x Contributors

D. A. Eliseev Institute for Scintillation Materials, NAS, Kharkiv, Ukraine

O. V. Eliseeva Institute for Scintillation Materials, NAS, Kharkiv, Ukraine
A. Fedorov Institute for Nuclear Problems of Belarus State University, Minsk,
Belarus
A. A. Fedorov National Research Center “Kurchatov Institute”, Moscow, Russian
Federation;
Institute for Nuclear Problems of Belarussian State University, Minsk, Republic of
Belarus
L. Fiserova NUVIA a.s., Trebic, Czech Republic;
UOPZHN, University of Defence, Vyskov, Czech Republic
A. Gektin Institute for Scintillation Materials, Kharkiv, Ukraine
Ia. Gerasymov Institute for Scintillation Materials NAS of Ukraine, Kharkiv,
Ukraine
V. V. Gilewsky JIPNR-Sosny NAS, Minsk, Belarus
E. V. Gordienko National Research Center “Kurchatov Institute” – IREA,
Moscow, Russian Federation
G. Gorokhov Institute for Nuclear Problems, Belarusian State University, Minsk,
Belarus
E. Griesmayer CIVIDEC Instrumentation GmbH, Vienna, Austria
Yu A. Gurkalenko Institute for Scintillation Materials, NAS, Kharkiv, Ukraine
V. Guzov ATOMTEX Scientific and Production Unitary Enterprise, Minsk,
Belarus
A. F. Iyudin Skobeltsyn Institute of Nuclear Physics, Moscow State University by
Lomonosov M.V, Moscow, Russia
J. Janda UOPZHN, University of Defence, Vyskov, Czech Republic
V. Jarý Institute of Physics AS of Czech Republic, Prague 6, Czech Republic
I. Kandarakis Department of Biomedical Engineering, University of West Attica,
Athens, Greece
V. A. Karas ADANI, Minsk, Belarus
P. V. Karpyuk National Research Center “Kurchatov Institute” – IREA, Moscow,
Russian Federation
D. Kasiuk ADANI, Minsk, Belarus
J. Kasper Physics Institute III. B, RWTH Aachen University, Aachen, Germany
Contributors xi

M. Katsemba Institute for Nuclear Problems, Belarusian State University, Minsk,

Belarus
P. Kavrigin CIVIDEC Instrumentation GmbH, Vienna, Austria
V. Kazalov Baksan Neutrino Observatory INR RAS, Neutrino, KBR, Russia
V. Khabashesku Baker Hughes a GE Company, Houston, USA
A. A. Khrutchinsky Institute for Nuclear Problems, Belarusian State University,
Minsk, Belarus
Marco Kirm Institute of Physics University of Tartu, Tartu, Estonia
D. Komar ATOMTEX Scientific and Production Unitary Enterprise, Minsk,
Belarus
V. V. Komarov ADANI, Minsk, Belarus
M. Korjik Institute for Nuclear Problems of Belarus State University, Minsk,
Belarus
M. V. Korjik National Research Center “Kurchatov Institute”, Moscow, Russia;
Institute for Nuclear Problems of Belarusian State University, Minsk, Belarus
V. Kornoukhov JSC Fomos-Materials, Moscow, Russia;
NRNU MEPhI, Moscow, Russia
M. V. Korzhik National Research Center “Kurchatov Institute”, Moscow, Russian
Federation;
Institute for Nuclear Problems of Belarussian State University, Minsk, Republic of
Belarus
V. Kozemyakin ATOMTEX Scientific and Production Unitary Enterprise, Minsk,
Belarus
R. Kučerková Institute of Physics AS of Czech Republic, Prague 6, Czech
Republic
D. Kurtsev Institute for Scintillation Materials NAS of Ukraine, Kharkiv, Ukraine
S. A. Kutsen Institute for Nuclear Problems, Belarusian State University, Minsk,
Belarus
D. E. Kuznetsova National Research Center “Kurchatov Institute” – IREA,
Moscow, Russian Federation
K. Lebbou Institute of Light and Matter, UMR55306 University Claude Bernard
Lyon 1-CNRS, Villeurbanne Cedex, France
V. Linev ADANI, Minsk, Belarus
A. Liubimau Belarusian State Technological University, Minsk, Belarus
xii Contributors

A. Lobko Institute for Nuclear Problems, Belarusian State University, Minsk,

Belarus
A. S. Lobko INP BSU, Minsk, Belarus
M. Lucchini CERN, Geneva, Switzerland
R. Lukashevich ATOMTEX Scientific and Production Unitary Enterprise, Minsk,
Belarus
A. Magiera Marian Smoluchowski Institute of Physics, Jagiellonian University,
Kraków, Poland
K. O. Makarevich Institute for Nuclear Problems, Belarusian State University,
Minsk, Belarus
V. Mechinsky Institute for Nuclear Problems of Belarus State University, Minsk,
Belarus
V. A. Mechinsky National Research Center “Kurchatov Institute”, Moscow,
Russian Federation;
Institute for Nuclear Problems of Belarussian State University, Minsk, Republic of
Belarus
A. Melnikau Institute for Nuclear Problems, Belarusian State University, Minsk,
Belarus
A. Mikhlin JSC NeoChem, Moscow, Russia
V. F. Minenko Institute for Nuclear Problems, Belarusian State University,
Minsk, Belarus
Vitali Nagirnyi Institute of Physics University of Tartu, Tartu, Estonia
S. Nargelas Institute of Photonics and Nanotechnology, Vilnius University,
Vilnius, Lithuania
M. Nikl Institute of Physics AS of Czech Republic, Prague 6, Czech Republic
Sergey I. Omelkov Institute of Physics University of Tartu, Tartu, Estonia
V. N. Pereymak Institute for Scintillation Materials, NAS, Kharkiv, Ukraine
D. Pozdnyakov ADANI, Minsk, Belarus
M. V. Protsko ADANI, Minsk, Belarus
K. Rusiecka Marian Smoluchowski Institute of Physics, Jagiellonian University,
Kraków, Poland
I. S. Satsounkevich JIPNR-Sosny NAS, Minsk, Belarus
O. Sidletskiy Institute for Scintillation Materials NAS of Ukraine, Kharkiv,
Ukraine
Contributors xiii

I. Slavashevich ADANI, Minsk, Belarus

P. S. Sokolov National Research Center “Kurchatov Institute” – IREA, Moscow,
Russia
A. Stahl Physics Institute III. B, RWTH Aachen University, Aachen, Germany
S. I. Svertilov Faculty of Physics, Moscow State University by Lomonosov M.V,
Moscow, Russia
S. Sytova Institute for Nuclear Problems, Belarusian State University, Minsk,
Belarus
G. Tamulaitis Institute of Photonics and Nanotechnology, Vilnius University,
Vilnius, Lithuania
V. Taranyuk Institute for Scintillation Materials, NAS of Ukraine, Kharkiv,
Ukraine
S. Tkachenko Institute for Scintillation Materials NAS of Ukraine, Kharkiv,
Ukraine
Y. U. Tratsiak Research Institute for Nuclear Problems, Minsk, Belarus
A. Vaitkevičius Institute of Photonics and Nanotechnology, Vilnius University,
Vilnius, Lithuania
Andrei N. Vasil’ev Skobeltsyn Institute of Nuclear Physics of Lomonosov
Moscow State University, Moscow, Russia
M. Vasilyev Baker Hughes a GE Company, Houston, USA
K. A. Verenich Institute for Nuclear Problems, Belarusian State University,
Minsk, Belarus
Y. Verhusha ATOMTEX Scientific and Production Unitary Enterprise, Minsk,
Belarus
C. Weiss CIVIDEC Instrumentation GmbH, Vienna, Austria
A. Wrońska Marian Smoluchowski Institute of Physics, Jagiellonian University,
Kraków, Poland
P. N. Zhmurin Institute for Scintillation Materials, NAS, Kharkiv, Ukraine
 Part I
Fundamental Studies
Chapter 1
Fast Processes in Scintillators

Andrei N. Vasil’ev

Abstract Development of new generation of accelerators for high energy physics

with extremely high luminosity and new demands from medical imaging with PET
requires fast scintillators with response of 10 ps. During last few years the physics
of fast processes in scintillators attracts attention of the community. These processes
include fast emission which occur in parallel with relaxation of electronic excitations
(intraband luminescence, crossluminescence and other types of hot emission) and
fast energy transfer to activators and new ways of fast creation of emission centers
like capture of an electron by Ce4+ ions, and some other phenomena. The paper
reviews the formation of scintillating signal in such systems.

1.1 Introduction. Why Do We Need Fast Timing and How

Fast Should It Be?

Fast decay time of the scintillating response is one of the general demands to “ideal”
scintillator. For many traditional applications of scintillator detectors, the moderate
values of decay time in nanosecond or even microsecond time domain are quite ade-
quate. Nevertheless, some new demands aroused in last years require much faster
scintillator characteristics. One of the examples is future generation of high energy
physics (HEP) devices [1]. The increased number of collisions in future accelerators
demands high precision time stamps of each event. The estimations give the values
for the time resolution about 10 ps. The analogous time resolution for scintillators
can significantly improve the signal-to-noise ratio in positron emission tomogra-
phy (PET) and additionally take the advantages of time-of-flight (TOF) approach
to reconstruction the medical images (see, e.g. [1–9]). The present time resolution
for commercially available scintillators are at least about 10 time worse. Therefore
scintillation scientific community is developing new approaches to improve the time

A. N. Vasil’ev (B)
Skobeltsyn Institute of Nuclear Physics, Lomonosov Moscow State University,
Leninskie Gory 1(2), Moscow, Russia
e-mail: anv@sinp.msu.ru

© Springer Nature Switzerland AG 2019 3

M. Korzhik and A. Gektin (eds.), Engineering of Scintillation Materials
and Radiation Technologies, Springer Proceedings in Physics 227,
https://doi.org/10.1007/978-3-030-21970-3_1
4 A. N. Vasil’ev

resolution of scintillators. The aim of the present paper is to remind how the scintil-
lator rise time problem is connected with physical processes in scintillators and what
effects can be used in order to achieve the ambitious goal of 10 ps time resolution
for estimation of the moment when ionizing particle or X-ray (γ-) photon interacts
with the detecting crystal.

1.2 General Description of Stages of Energy Relaxation

in Scintillators

1.2.1 Interaction of Primary Ionizing Particle with Crystal

The interaction of the high energy particle with the crystal depends on the particle
type and energy and typically starts at the moment when ionizing particle appears
in the crystal. This means that in the case of X- or γ-quantum the interaction starts
within the crystal at the point where this quantum is absorbed with conversion into a
valent or core hole and a photoelectron or where the Compton scattering occur again
with creation of valence or core hole and electron with energy less than in case of
full photoconversion. The analogous situation occurs for the case of interaction of
neutrons or other neutral particles with matter. This means that electronic excitations
start to appear at some point within the crystal at the mean distance from the surface
about minimum of penetration or scattering length or the dimension of the crystal.
In case of penetration length is about or higher than the thickness of the crystal, not
all high-energy particles interact with crystal.
On the contrary, the interaction with charged particles starts at the moment when
the particle passes through the boundary of the crystal. This kind of interaction is
due to the influence of the electric field of the particle and in principle can occur
even without penetration of the particle into the media (for instance, the case of the
interaction of fast electron passing near the nanoparticle can be inelastically scattered
with production of electronic excitations within the nanoparticle). In this case all or
a part of the energy of ionizing particle is converted into the energy of electronic
excitations.
Moreover, the passage of charged particle through the media results in direct
conversion of the energy of this particle into photons. The most known example is
the Cherenkov radiation which is the result of the passage of the charge through the
media with velocity higher than the phase velocity of the low-energy photons. These
“prompt” photons are the best way to fastest detection of the interaction of ionizing
particle with media, but the yield of such process is rater low in the most cases, and
the energy threshold for such process is typically about hundred of keV (63 keV for
crystals with refractive index n = 2.2, 144 keV for n = 1.6). Another example of
the ultrafast conversion into photons is the transient radiation which occur when the
particle crosses the crystal boundary with different refraction indexes at both sides
of the boundary. One additional process to be considered is the Bremsstrahlung. In
1 Fast Processes in Scintillators 5

this case a part of charged particle energy is converted into an X-ray photon, but in
this case this photon should be again converted into electronic excitations in order
to be registered.
The main channel of the interaction of a charged particle with media is the pro-
duction of electron-hole pairs or excitons of different kinds (including core level
excitons) in the events of inelastically scattering the primary particle (see, e.g.
[10–15]). The rate of this process is proportional to so-called “energy loss func-
tion” Im −1 ε̃(ω, q) , depending on energy ω and momentum q transfer in the
inelastic scattering event. Here ε̃(ω, q) is the complex dielectric function of the
crystal. The energy loss function has complicated structure in wide energy region.
The electron scattering with production of new electronic excitations results in the
electron cascade during which secondary excitations are created.
Figure 1.1 shows schematically different relaxation processes and their rates.
Inelastic electron scattering processes e → 2e + h are shown by arrows 1a and 1b.
The rate of this process for an electron with energy well above the threshold (1b)
reaches inverse femtoseconds or higher. These values are in good correspondence
with the more known fact that the mean free path between scatterings for electrons
with energy about 20–50 eV is less than one nanometer. The scattering of electrons
with such energies produce secondary excitations with kinetic energy of several
electronvolts. The scattering of electrons with lower energy (closer to threshold,
case 1a) has lower rate and results in production of electrons and holes with low
kinetic energy. This process has no abrupt threshold, since even electrons with kinetic
energy slightly below exciton energy E ex < E g could produce  electronic excitation
 
at Urbach exciton absorption region where Im(ε̃(ω, q)) ∼ exp (ω − E ex ) σ k B T ,

Fig. 1.1 Rates of different relaxation processes for hot electrons (right panel) and hot holes (left
panel) for BaF2 crystal (E g ≈ 10 eV), schematic representation
6 A. N. Vasil’ev

namely e → e + ex (see the exponential decrease of e → 2e + h rate for electron

energies below 2E g in Fig. 1.1, red curve in the right part of the figure). Here σ is
the Urbach constant and this formula is written for high temperatures.
The analogous cascade h → e + 2 h is created by Auger decay after deep core
hole creation. The corresponding process is shown by arrows 1c, where the transition
of a hole is shown by double line arrow (in direction opposite to electron transition).
This cascade has duration of several femtoseconds and is finished when the its
rate becomes smaller than the rate of another relaxation process—phonon emission.
The cascade results in the formation of electronic excitations with kinetic energy
below the threshold of inelastic electron-electron scattering, i.e. about the forbidden
gap energy E g .
At this stage some amount of energy is converted into photons. There can be X-ray
photons produced as fluorescence due to the filling of deep core holes by electrons
from higher lying core and valence bands, and X-ray photons due to Bremsstrahlung.
The Cherenkov radiation with photons within energy below E g (i.e. in light trans-
parency region) also can be produces by δ-electrons with high energies above the
Cherenkov threshold. We do not consider here the case of high-energy electrons and
positrons (>1 MeV) when the electromagnetic shower is developed.

1.2.2 Thermalization of Electronic Excitations

The rate of phonon emission is presented in Fig. 1.1 by green curves (process 2a for
electrons, 2b for valence holes and 2c for holes in upper core levels or in separated
valence subbands). This rate depends mainly on the value of longitudinal optical
phonon energy LO and is about 1013 –1014 s−1 for carriers with kinetic energy
above this phonon energy. For crystals with light elements (like fluorine, oxygen)
LO is higher than 100 meV and this rate is more than 1014 s−1 , whereas for crystals
without light elements (and, correspondingly, LO about 10–20 meV) it is much
lower (about 1013 s−1 ) (see, e.g. [16–18]). After the thermalization with emission of
longitudinal optical phonons the slower stage of thermalization with scattering by
phonons with lower energies (including acoustical ones) result in the gathering of
thermalized electrons and holes at the bottom of conduction band or at the top of
valence band with kinetic energies about kB T . If densities of states (DOS) for valence
bands have gaps, like in Fig. 1.1, the transition of a hole between different subbands
can occur through the multiphonon process (2d) with much lower rate.  This rate is
exponentially decreased with the increase of the gap as exp − pE LO , p is a
dimensionless parameter about one.
During the thermalization the electrons and holes can emit not only phonons, but
also photons with energies in the light transparent region (below E g ). The rate of this
process is shown schematically in Fig. 1.1 by blue curves and is much lower than the
thermalization rate. The resulting emission is called Intraband luminescence (IBL) of
e-type (process 3a) or h-type (process 3b) (see e.g. [19–21] and references therein).
The rate of this emission can be significant only when a hole is located in energy
1 Fast Processes in Scintillators 7

at the top of the uppermost core band (process 3c) or at the top of a well separated
subband, when this hole cannot emit any more optical phonons and when the rate of
multiphonon process (2d) is about or lower than the radiation rate. In this case the
emission is called crossluminescence (CL) (some authors use the terms core-valence
transitions and Auger-free luminescence for this type of emission). These types of
emission will be discussed below in details.
All the reactions which we have discussed in the present and previous sections
are monomolecular ones, and their rates do not depend on the concentration of other
charge carriers. This is correct for the case when the concentration of excitation is
not too high. If the concentration is above, say, 1020 cm−3 , the additional type of
relaxation can exist (see, e.g. [22–31]). The most important one is the Auger process
due to interaction with neighbor excitations, like 2e + h → e—the process reverse
to the inelastic scattering with multiplication of electronic excitations (e → 2e + h).
The rate of such Auger reaction cubically increases with concentration of carriers
and schematically is shown in Fig. 1.1 by red dashed lines. This kind of process can
compete with weak radiation process and quench CL emission from track regions
with high concentration of excitations. The Auger processes of this type result also in
slowing the relaxation and in radiation-less conversion of some part of electron-hole
pairs into phonons.

1.2.3 Different Types of Emission Centers and Energy

Transfer to Them

In the previous paragraphs we mentioned two types of events which result in pro-
duction of fast photons in processes when the numbers of electrons and holes do not
change (Cherenkov radiation and IBL + CL). All other types of emission are con-
nected with the recombination of electrons and holes. These types of recombination
occur mainly after thermalization of carriers (here we do not consider the case of
recombination of hot carriers). The next step of energy relaxation is the migration
of electrons and holes and interaction of them with production of excitons, capture
by traps, centers of recombination, etc. (see, e.g. [11, 12, 32, 33]). One of the most
important types of excitations is excitons, which are created mainly in the reaction e
+ h → ex. Please note that some excitons are created directly in cascade process e
→ e + ex. The fraction of directly created excitons is typically no more than 5% in
comparison with separated e–h pairs. The reaction of an electron capture by a hole is
bi-molecular, this means that the corresponding term in rate equations is proportional
to the concentration of the other component:

dn e (t)
= · · · − βeh (t)n e (t)n h (t) − · · · ,
dt
dn h (t)
= · · · − βeh (t)n e (t)n h (t) − · · · ,
dt
8 A. N. Vasil’ev

dn ex (t)
= · · · + βeh (t)n e (t)n h (t) − · · · , (1.1)
textdt
where βeh (t) ≈ 4π (De + Dh )ROns for the simplest case, De and Dh are diffusion
2
coefficients for electrons and holes and ROns = 4πε0eεkB T is Onsager radius. In self-
activated crystals these excitons can be self-trapped ex → STE and act as emission
centers. CdWO4 and Bi4 Ge3 O12 (BGO) are such self-activated crystals where STE
is located on oxyanionic complex.
In most activated crystals like Ce3+ - and Tl+ -acivated ones the energy transfer to
the activator is more complicated and depends on the energy location of activator
levels within the forbidden gap. For instance, if 4f Ce3+ level is located far from the
valence band, a hole cannot be captured by the activator due to big energy difference
between activator level and the top of the valence band which cannot be covered by
multiphonon process. The capture of an electron by free 5d Ce3+ level is also not
realized since Ce2+ ion is unstable in most compounds. Therefore the most probable
way to excite Ce3+ ion is the energy transfer from the exciton in the reaction ex +
Ce3+ or STE + Ce3+ The products of these reactions will be discussed below.
On the contrary, thallium ion in alkali halide crystals can participate in all three
reactions: e + Tl+ →Tl0 , h + Tl+ →Tl2+ , and ex + Tl+ →Tl+ *. The excited thal-
lium state is formed directly in third reaction, whereas two other reactions demand
additional capture act like h + Tl0 → Tl+ * or e + Tl2+ →Tl+ *.
The rates of all these reactions depend on the concentration of carriers, and there-
fore we have to discuss how the track region can be described in terms of concentra-
tion of thermalized electronic excitations.

1.2.4 Spatial Distribution of Excitations After Thermalization

Electronic excitations in track region are distributed in a very inhomogeneous way.

Figure 1.2 presents the typical distribution of electrons and holes in CsI crystal after
absorption of 100 keV X-ray photon. Simulation demonstrates the creation of clusters
of excitations due to relaxation of deep core holes and low-energy electrons. CsI is
characterized by significant thermalization length for electrons (up to 100 nm for
5 eV electron kinetic energy before the thermalization), whereas holes are shifted
during themalization on much smaller distances (compare insets b and c in Fig. 1.2).
The simplest way to study different reactions between electronic excitations is the
solving of rate equations for concentration of excitations (electrons, holes, excitons,
different states of traps and activators, etc.). A part of a rate equation set is presented
as Eq. 1.1. Such rate equations are often used for the description of the scintillator
decay kinetics. These equations are nonlinear, and therefore the character of solu-
tions strongly depends on initial conditions for concentrations. We mentioned above
that cascade and thermalization stages are described by monomolecular reactions,
whereas the stage of recombination and interaction demands the account for at least
bi-molecular reactions, and the rate equation’s approach is natural for this stage. So
1 Fast Processes in Scintillators 9

(b)
(a)

(c)

(d) (e)

Fig. 1.2 An example of spatial distribution of electrons (red) and holes (blue) for 100 keV elec-
tron track in CsI after thermalization. Insets: a energy distribution of electrons and holes before
thermalization after the cascade; b distribution of electron (b) and hole (c) thermalization lengths;
zoomed part of the track before (d) and after (e) thermalization

one can use the initial conditions corresponding the distribution of excitations just
after the end of thermalization (see, e.g. [11]).
Let us define the “concentration” of excitations through the distance between the
closest pairs. If the concentration of, say, electrons is n e , then the mean distance
−1 3
between an electron and its neighboring electrons is ree  = n e / . Figure 1.3 shows
the histogram of the “concentrations” calculated as the inverse cube of the mean
distance to three closest neighbors.
This example demonstrates that an electron “feels” surrounding electrons as if
the initial concentrations were distributed between 1014 and 1020 cm−3 . On the other
10 A. N. Vasil’ev

Fig. 1.3 Histogram of electron concentration (blue), hole concentration (yellow) and concentration
of electrons around holes (green) for Monte-Carlo simulation of 100 keV electron track in CsI after
thermalization presented in Fig. 1.2. The histogram is calculated using log(n) equidistant bins

hand, electrons “feel” traps or activators with uniform concentrations equal to the
concentrations of these centers. Therefore the branching between different reac-
tions involving electrons depends on their concentrations, and the results should be
weighted over the distribution of concentrations of excitations similar to that pre-
sented in Fig. 1.3.

1.3 Timing Properties of IBL and CL

Intraband luminescence (IBL) is known to be a result of radiation transitions of

electrons in the conduction bands or holes in the valence band which occurs as a
weak competitive channel of relaxation [19–21]. The decay of this emission differs
significantly from any traditional emission center in scintillators. Its rise time is
in femtosecond region (the time of the cascade of inelastic scattering of electrons
and Auger cascade), and for our purposes it can be regarded as instant. The radiation
transitions have nanosecond radiation time, but due to fast thermalization the lifetime
of emitting states is defined by the thermalization process.
Let us discuss the IBL due to transitions in the conduction band (e-IBL). Before
thermalization the electrons are distributed among the branches of the conduction
band. An example of these branches is presented in Fig. 1.4, left panel. The lower
branches are more populated in comparison with highly lying branches due to the
peculiarities of the distribution of secondary excitations in the cascade. During ther-
malization the electrons from each branch reduce their energy, and therefore highest
branches are depopulated, whereas the population of lower lying branches increases.
1 Fast Processes in Scintillators 11

Fig. 1.4 Scheme of the bands in conduction band in free electron approximation (left panel) with
IBL radiative transitions (blue arrows) and phonon relaxation (red arrows) and the corresponding
emission spectrum for first order transitions (right panel)

In parallel with thermalization electrons can emit photons. The probability of the
photon emission is proportional to the square of the energy of emitting photons,
so more energetic photons are emitted preferably. The corresponding spectrum of
e-IBL is broad and smooth (see Fig. 1.4, right panel) regardless that the transitions
are between individual branches.
The account for the phonon-assisted transitions can add some components to
infrared part of spectrum [21, 34].
The discussed faster depopulation of higher states in the conduction band results in
the modification of the emission spectrum in time. At initial moments after cascade
the spectrum is shifted in blue region (see Fig. 1.5, left panel). With shifting of
the electronic population for lower energies the emission spectrum also shifts to the
infrared region with simultaneous decrease of its intensity (this decrease is connected
with quadratic dependence of the radiation probability with emission energy). This
results in non-typical decay law of this transient emission: decay kinetics is about
linearly and finished when the electrons from different branches go down in energy.

t=0 ps

t=1 ps
hν =4 eV

hν =3 eV
hν=5 eV

t=2 ps
t=3 ps

Fig. 1.5 Evolution of the spectrum of e-IBL with time (left panel) and corresponding decay kinetics
(right panel) for different photon energies for parameters typical for CsI (energy of LO phonon is
10 meV, forbidden gap about 6 eV)
12 A. N. Vasil’ev

These decay curves for different emission energies is presented in Fig. 1.5, right
panel.
The same situation occurs for h-IBL with the only difference that in this case the
spectrum is limited by the width of the valence band.
If there are the gaps in the density of states (that is if the band is spitted into
subbands), the IBL kinetics and their spectra are significantly modified. IBL with
transitions within subband has the properties like described above (with decrease of
the spectral range by the width of the subband and corresponding decrease of the
intensity). The inter-sub-band emission became much closer to crossluminescence.
The standard cross-luminescence occurs when a hole goes to the upper band formed
by the other element. The CL spectrum position and its width is characterized by the
energy position of the accepting band relative to the top of the initially populated band,
since after sub-picosecond relaxation the holes are gathered at the band maximum
(see, e.g. [35]). This picture is correct if the lattice relaxation with presence of core
hole is not strong. If it is strong enough, this relaxation can modify both the core
band and the valence band (resulting, in particular, in temperature dependence of CL
spectrum) [36, 37].
The duration of such inter-sub-band emission is defined by the lifetime of the hole
states at the top of sub-band and is the minimum of two times—radiation time and
the multiphonon transition time. This time is mentioned above when we describe
rates of transitions in Fig. 1.1 and exponentially increases with the increase of the
width of the gap. It is definitely less than radiation time if the gap is about or less than
1 eV. Therefore inter-sub-band IBL should have exponential decay with characteristic
time about few picoseconds up to hundred picoseconds, with corresponding increase
of intensity. From the other hand, CL with relatively narrow gaps between core and
valence band is also quenched due to multi-phonon relaxation of holes from one band
to another and in this case, there is no difference between CL and inter-sub-band IBL.
The quenching of CL can originate not only due to multi-phonon relaxation of core
holes, but also due to transient Auger effect in case of high density of electronic exci-
tations around the core hole. This means that CL results from the transitions mainly
from track regions with low concentration of excitations, i.e. peripheral regions of
the track. It is worth to mention that such high sensitivity of CL to concentration
of surrounding excitations is the reason for good capabilities of discrimination of
different types of ionizing particles [38, 39].

1.4 Rise Profile of Recombination Luminescence Response

The case of energy transfer from the host material to activators is not so prompt
(see, e.g. [40–43]). The activators are excited mostly by recombination process. If
excitation center cannot catch electrons and holes sequentially (an example of Ce3+
ion with 4f Ce3+ level well above the valence band top is mentioned above), the
only way to excite these centers is the energy transfer from excitons. In this case
we can imagine the following sequence of reactions: e + h → ex; ex → STE; STE
1 Fast Processes in Scintillators 13

+ Ce3+ → Ce4+ + e; Ce4+ + e → Ce3+ *; Ce3+ * → Ce3+ + hν. If the energy of

STE is not enough to ionize Ce3+ ion, two intermediate reactions are converted to
one: STE + Ce3+ → Ce3+ *. The rate of the first one is bi-linearly depended on the
concentrations of electrons and holes. The typical kinetics of excited cerium ion are
presented in Fig. 1.6 by solid curves. Curves of different colors represent different
initial concentration of electrons and holes n e (0) = n h (0), measured in units of
critical concentration n c for which the rate of electron-hole recombination equals to
1010 s−1 . Cerium concentration is equal to n c , the rates of ex → STE and STE + Ce3+
reactions equals to 1012 s−1 . These parameters are chosen just to illustrate the effect.
We see that for high electron initial concentration n e (0) = n c the rise time for such
cascade energy transfer is about 100 ps, whereas for lower initial concentration it can
be as high as tens of nanosecond (black curve for n e (0) = 0.001 n c ). The decay for
high initial concentration is exponential with Ce3+ * emission time (we take 30 ns as
typical time for these estimations) except weak deviation at hundreds of nanosecond).
On the contrary, the long-time decay for low concentrations is hyperbolic, and its
level strongly increases with decrease of initial electron and hole concentration.
For the selected parameters both the rising time and long decay are controlled by
bi-molecular coupling of electrons and holes into excitons.
The curves presented in Fig. 1.6 demonstrate the kinetics from different part of the
track with different electron concentration. The total response can be obtained from
these partial responses by weighting with distribution shown in Fig. 1.3. One can
conclude that the fast rise of scintillation is due to the regions with high concentration
of excitations (near the core part of the track and ends of the track branches), whereas

10 -1 ne=nc
ne=0.1 nc
ne=0.01 nc
10 -2
ne=0.001 nc
Response kinetics

10 -3

10 -4

10 -5
w/o Ce 4+
0.1% Ce4+
1% Ce 4+
10 -6
0.0 0.5 1.0 1.5 2.0 2.5 3.0 3.5 200 400 600 800 1000
t, ns

Fig. 1.6 Cerium response kinetics for different initial concentrations of electrons and holes (dif-
ferent colors) without presence of Ce4+ ions (solid curves) and with some amount of conversion
Ce3+ into Ce4+ (dashed and dotted curves)
14 A. N. Vasil’ev

the delayed non-exponential kinetics for times longer than intrinsic radiation time of
the emission center is formed by peripheral parts of the track.
During last few years the extensive study of co-dopants in garnet crystals shows
that even small addition of divalent ions (Mg2+ , Ca2+ ) can significantly reduce the
rise time and the afterglow [44–46]. This effect is connected with several reasons,
one of which is the appearance of Ce4+ ions in the crystal as the consequence of the
shift of the Fermi level in crystals. Figure 1.6 shows also the role of small addition of
Ce4+ ions in the energy transfer from electron-hole pairs to cerium. In this case one-
step reaction e + Ce4+ → Ce3+ *; Ce3+ * → Ce3+ + hν can result in the appearance
of faster emission components. Dashed and dotted curves show the modification of
Ce3+ * kinetics with the conversion of 0.1 and 1% of Ce3+ ions into Ce4+ ions in non-
excited crystal. The effect is strong for concentrations of electrons about or below the
concentration of Ce4+ ions (black and red curves). In this case electrons in regions of
low concentration are captured by Ce4+ ions rather than holes. The overall response
becomes faster and the risetime for emission from regions with low concentration
is much faster than for the case without Ce4+ . The shift of the balance between e +
Ce4+ → Ce3+ * and e + h → ex also suppresses the long components as it was shown
from experiments. Again, this suppression is more prominent for low-concentration
part of the track, which is responsible for long components of the decay.
There can be additional reasons for accelerating cerium decay, since di-valent ions
in garnets modify also the number and the population of shallow defects, which can
significantly reduce the mobility of electrons and holes in the system and therefore
change the reaction constant even for e + h → ex capture process.
The qualitative study of the presented above example of energy transfer from the
host to cerium can be important for engineering of new fast scintillators.

1.5 Additional Delays Due to Finite Track Length

and Light Propagation to the Photon Detector

When we speak about fast processes in scintillators in picosecond and subpicosecond

stages, we should take into account not only time behavior of relaxation processes but
also the difference of the positions of the interaction of fast primary ionizing particle
with matter along the track and the time of the propagation of emitted photons to
the photodetector with account for reflections and scattering of the light from the
crystal boundaries. For relativistic ionizing particles the spread of the moments of
interaction with media can be estimated as the length of the track divided by the
speed of light in vacuum, whereas the typical time of propagation of scintillation
photons is defined by the dimensions of crystals divided by the phase speed of light
in the matter times the mean number of scatterings and reflections form the crystal
surface. The spread of the propagation time even for crystal of 1 mm thickness can
be as high as 0.1 cm/(3 × 1010 cm/s) × 2.2 × 3 = 20 ps for a crystal with refractive
index equal to 2.2 and mean number of reflections about 3.
1 Fast Processes in Scintillators 15

1.6 Conclusions

We discuss physical processes which form the fast response of scintillating materials.
The account for these processes are important to achieve the small values of time
resolution of scintillators.

Acknowledgements This research is carried out in the frame of Crystal Clear Collaboration and is
supported by a European Union’s Horizon 2020 research and innovation program under the Marie
Skłodowska-Curie grant agreement No 644260 (INTELUM) and COST ACTION TD1401 (FAST).

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