Radiation-induced moution of liquid inclusions in alkali halide crystals
The radiation-stimulated behavior of liquid inclusions in KCl crystal was studied. It was shown that due to irradiation the inclusions become movable. It can result in the migration of such objects to the boundary of the material and the release of radioactive elements from the disposal. The traject...
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irk-123456789-1949382023-12-01T20:27:08Z Radiation-induced moution of liquid inclusions in alkali halide crystals Kulik, A.P. Podshyvalova, O.V. Marchenko, I.G. Physics of radiation damages and effects in solids The radiation-stimulated behavior of liquid inclusions in KCl crystal was studied. It was shown that due to irradiation the inclusions become movable. It can result in the migration of such objects to the boundary of the material and the release of radioactive elements from the disposal. The trajectories of spontaneously migrating inclusions of various sizes were investigated in crystals irradiated by electrons and γ-quanta. Вивчено радіаційно-стимульовану поведінку рідких включень у монокристалах KCl. Показано, що під дією опромінення включення стають рухливими. Це може призводити до міграції таких об'єктів на межу матеріалу і виходу радіоактивних елементів із поховання. Досліджено траєкторії самочинної міграції включень різних розмірів у кристалах, опромінених електронами і γ-квантами. Изучено радиационно-стимулированное поведение жидких включений в монокристаллах KCl. Показано, что под действием облучения включения становятся подвижными. Это может приводить к миграции таких объектов на границу материала и выходу радиоактивных элементов из захоронения. Исследованы траектории самопроизвольной миграции включений различных размеров в кристаллах, облученных электронами и γ-квантами. 2019 Article Radiation-induced moution of liquid inclusions in alkali halide crystals / A.P. Kulik, O.V. Podshyvalova, I.G. Marchenko // Problems of atomic science and technology. — 2019. — № 2. — С. 13-19. — Бібліогр.: 17 назв. — англ. 1562-6016 http://dspace.nbuv.gov.ua/handle/123456789/194938 539.534.9:523.23 en Вопросы атомной науки и техники Національний науковий центр «Харківський фізико-технічний інститут» НАН України |
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Physics of radiation damages and effects in solids Physics of radiation damages and effects in solids |
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Physics of radiation damages and effects in solids Physics of radiation damages and effects in solids Kulik, A.P. Podshyvalova, O.V. Marchenko, I.G. Radiation-induced moution of liquid inclusions in alkali halide crystals Вопросы атомной науки и техники |
| description |
The radiation-stimulated behavior of liquid inclusions in KCl crystal was studied. It was shown that due to irradiation the inclusions become movable. It can result in the migration of such objects to the boundary of the material and the release of radioactive elements from the disposal. The trajectories of spontaneously migrating inclusions of various sizes were investigated in crystals irradiated by electrons and γ-quanta. |
| format |
Article |
| author |
Kulik, A.P. Podshyvalova, O.V. Marchenko, I.G. |
| author_facet |
Kulik, A.P. Podshyvalova, O.V. Marchenko, I.G. |
| author_sort |
Kulik, A.P. |
| title |
Radiation-induced moution of liquid inclusions in alkali halide crystals |
| title_short |
Radiation-induced moution of liquid inclusions in alkali halide crystals |
| title_full |
Radiation-induced moution of liquid inclusions in alkali halide crystals |
| title_fullStr |
Radiation-induced moution of liquid inclusions in alkali halide crystals |
| title_full_unstemmed |
Radiation-induced moution of liquid inclusions in alkali halide crystals |
| title_sort |
radiation-induced moution of liquid inclusions in alkali halide crystals |
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Національний науковий центр «Харківський фізико-технічний інститут» НАН України |
| publishDate |
2019 |
| topic_facet |
Physics of radiation damages and effects in solids |
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http://dspace.nbuv.gov.ua/handle/123456789/194938 |
| citation_txt |
Radiation-induced moution of liquid inclusions in alkali halide crystals / A.P. Kulik, O.V. Podshyvalova, I.G. Marchenko // Problems of atomic science and technology. — 2019. — № 2. — С. 13-19. — Бібліогр.: 17 назв. — англ. |
| series |
Вопросы атомной науки и техники |
| work_keys_str_mv |
AT kulikap radiationinducedmoutionofliquidinclusionsinalkalihalidecrystals AT podshyvalovaov radiationinducedmoutionofliquidinclusionsinalkalihalidecrystals AT marchenkoig radiationinducedmoutionofliquidinclusionsinalkalihalidecrystals |
| first_indexed |
2025-07-16T22:37:13Z |
| last_indexed |
2025-07-16T22:37:13Z |
| _version_ |
1837844855121772544 |
| fulltext |
ISSN 1562-6016. PASТ. 2019. №2(120), p. 13-19.
UDC 539.534.9:523.23
RADIATION-INDUCED MOTION OF LIQUID INCLUSIONS
IN ALKALI HALIDE CRYSTALS
A.P. Kulik
1*
, O.V. Podshyvalova
2
, I.G. Marchenko
1,3**
1
V.N. Karazin Kharkov National University, Kharkov, Ukraine
2
N.E. Zhukovsky National Aerospace University
“Kharkov Aviation Institute”. Kharkov, Ukraine;
3
National Science Center “Kharkov Institute of Physics and Technology”, Kharkov, Ukraine
E-mail:
*
kulykop@gmail.com;
**
march@kipt.kharkov.ua
This scientific paper studies the effect of irradiation on the radiation-induced motion of liquid inclusions in
KCl. It was shown that the inclusions exposed to the irradiation become mobile. It can result in the migration of
such inclusions to the material boundary and release of radioactive elements by nuclear waste site. The trajectories
of spontaneous migration of the inclusions of a different size in the crystals exposed to the irradiation with the
electrons and -quanta have been studied.
INTRODUCTION
The irradiation has a substantial influence on a
change in the properties of original material [1]. Many
processes are accelerated under the action of the
neutron, -electron and gamma irradiation. The
phenomena of radiation-accelerated diffusion, creep,
embrittlement, etc. are well-known [2–5].
At the same time, the irradiation can affect not only the
diffusion mobility of individual atoms or clusters but
also the behavior of macroinclusions. Such inclusions
are present in many virgin minerals, in particular in the
depositions of a geological origin. Such minerals can be
used for the nuclear waste disposal [6]. With time,
nuclear reactions progress at nuclear waste sites. It can
result in the activation of the processes of interaction of
the matrix substance with land-buried products, in
particular in the motion of inclusions that occupy vacant
surfaces followed by their discharge into the
atmosphere. In this connection, the studies of the
influence of radioactive defects on the motion processes
of liquid inclusions are of great interest.
The objective of this research paper was to study the
radiation-induced motion of liquid inclusions in KCl
monocrystals exposed to the irradiation with - quanta
and electrons.
SPECIMEN PREPARATION
Liquid inclusions were formed in KCl monocrystals
using the crack healing method [7]. For this purpose the
incomplete crack was formed in the specimen and that
crack was filled with the distilled water exposed to the
action of capillary forces. The specimen has been held
at room temperature for about ten days to heal the crack
and it was accompanied by the formation of the
inclusions of saturated KCl water solution in the mouth
of crack. The dimensions of formed inclusions varied in
the range of 3 to 100 µk.
The motion of liquid inclusions was studied in the
temperature gradient field and the temperature gradient
value varied in the range of 2·10
2
to 2·10
4
K/m. The
temperature gradient was created in the specimen by
contacting its opposite faces with the heater and the
fridge that was cooled by the running water. To define
the temperature gradient value of ( T ) the reference
crystals of the same size as the specimens with
inclusions were annealed. Two thermocouples were
soldered into reference samples. Thermocouples’
readings were taken to calculate the temperature
gradient value for the specimens under certain distance
between the thermocouples.
The motion of inclusions was observed using the
optic microscope with the sight check. For this purpose,
the heater, the specimen and the fridge were fixed on
the microscope stage in such a way that the temperature
gradient was oriented in the plane 100 , parallel to the
direction 100 .
The dislocation structure of studied crystals was
controlled by chemical etching. The saturated methyl
alcohol PlCl2 solution was used as an etching agent.
After the etching the specimen was rinsed by the
mixture of ethyl and amyl alcohols.
DISSOLUTION LAYER SOURCES
It is known that the layer-by-layer growth of crystals
is realized either due to the two-dimensional crystal
nucleation or due to the growth of dislocations that have
a spiral component of the Burgers vector [8]. Assuming
that the inclusion is a negative crystal the process of its
motion can be viewed as a simultaneous growth of the
frontal surface and the dissolution of the rear surface. In
this connection, the dissolution of matrix on the frontal
surface of the inclusion simulates the process of
dislocation growth, because at driving forces that are
realized in these experiments other sources of
dissolution, except for the screw or Burgers dislocation
fail to manifest themselves [2,9]. The growth of crystal
at the rear surface of inclusion occurs due to the motion
of stages that are formed in the angles between the rear
surface and the lateral surface. This process simulates
the dissolution of monocrystal when its edges act as the
source of stages.
A dislocation mechanism of the dissolution of the
frontal surfaces of moving inclusions is immediately
confirmed by the following experiments. The
dislocation structure of the most KCl crystals was
studied to select the crystal with the inhomogeneous
mailto:march@kipt.kharkov.ua
mailto:march@kipt.kharkov.ua
distribution of dislocations. This crystal was used to
chip out the specimen making the inclusions in it. The
chipped off surface of a type (100) with the ensemble of
inclusions near it that was selected for the observation
was etched at the dislocation (Fig. 1,a). Afterwards, the
specimen was placed into the temperature gradient field
oriented in such a way that moving inclusions could
cross both strongly and slightly dislocated areas of the
specimen. The observations showed that moving
inclusions stop as soon as they approach actually non-
dislocated area of the crystal (Fig.1). It is evident that
the inclusions that were not initially crossed by the
dislocations should not move in general. The inclusions
must also be motionless when the distance from the
point of emergence of spiral dislocation to the face edge
or to the point of emergence of the dislocation of an
opposite sign is shorter than the threshold distance at
specified motive forces [9].
EXPERIMENTAL METHODS
The defects can be represented by electron and hole-
type color centers formed under the action of ionizing
radiation on alkali - halide crystals. These color centers
are spot defects and these create no additional sources
of stages on the crystal surface. However, their
presence in the crystal can change the values of the
kinetic characteristics of dissolution processes, in
particular a kinetic coefficient of the stage that results in
a change of the dissolution rate of crystal. In addition,
the energy that was stored in the crystal during its
irradiation should change the conditions of the
thermodynamic equilibrium of the crystal and the
solution. In other words, the solubility of irradiated
crystal must be higher that that of unirradiated crystal.
The experiments were carried out using liquid
inclusions for KCl crystals exposed to the irradiation
with -quanta emitted by the Со
60
source and the
electrons of 10 MeV at the integral current density of
5·10
-2
A/m
2
(a total dose reached the value of 10
21
m
-2
).
The irradiation resulted in colored specimens. The type
and the concentration of color centers were defined
from the spectra of the optic absorption of irradiated
crystals using appropriate methods [10]. For all the
experiments, the basic color centers were electron F-
centers and hole-type V3-centers. The concentrations of
identified R1-, R2- and M-centers turned out to be much
lower. Depending on the dose and the type of irradiation
the concentrations of F- and V3-centers were
approximately the same and varied in the range of
10
21
…10
23
m
-3
.
A scheduled series of experiments was carried out
using liquid inclusions in KCL monocrystals in which
only electron centers were formed due to the additive
coloring in the pairs of alkaline metal [11]. For this
purpose, the plate was chipped out the KCl crystal and it
was placed into the container made of stainless steel at
the bottom of which the metal potassium was located.
The container was tightly closed by the screwed cover.
The temperature was controlled using the built-in
thermocouple. The container was annealed in the argon
atmosphere at a temperature of T = 600
°
C during one
hour. The specimen was cooled to the room temperature
simultaneously with the cooling of the furnace.
Fig. 1. Motion of the inclusions in the temperature
gradient field of KCl crystal with the inhomogeneous
distribution of dislocations:
а is the initial state, b – 11; c – 16; d – 25 h
The inclusions in colored specimens were observed
both in the temperature gradient field and under
isothermal conditions. For additively colored crystals
the direction of temperature gradient was preset
perpendicularly to the crack plane. It is conditioned by
the fact that the inclusions in the additively colored
crystals turn out to be in the recrystallized region that
contains no color centers during the crack healing in
contrast to irradiated crystals (the crystals were exposed
to the irradiation with already formed inclusions).
MOVING AND RESHAPING INCLUSIONS
IN THE CRYSTALS WITH COLOR
CENTERS
Motion of the inclusion in the colored crystal is
accompanied by the dissolution of the crystal with color
centers on its frontal surface and the growth of crystal
that has no such color centers on the rear surface. As a
result, moving inclusions form brightened up traces
behind them (Fig. 2). In this case we observe one more
peculiarity of this process; in particular gas bubbles are
formed inside liquid inclusions. The motion of such an
inclusion can result in its decomposition into the liquid
component and the gas-liquid component with a large
amount of gas. Specifically, it can be explained by that
the electrons localized in anion vacancies transfer to the
solution during the dissolution of the crystal containing
F-centers. These solvated electrons transfer hydrogen in
the atomic state when bonding with H
+
ions available in
the solution [12].
Hydrogen formed in the inclusions saturates and
oversaturates the solution and it forms the bubbles that
can be seen in the inclusions.
b
c d
Fig. 2. Motion of the inclusions in the T field in
irradiated KCl crystals: а is the initial state;
b is the state after 5 hours
Motion of the inclusions both in irradiated
specimens and in additively colored crystals occurred in
the mode of boundary kinetics that is also peculiar for
the motion of the inclusions in the crystals that contain
no color centers [13]. It means that the diffusion transfer
of the matrix substance through the inclusion volume
will not limit the process of its motion. Alongside, the
average values of velocities of the inclusions of the
same size moving in the crystals with color centers turn
out to be 30 to 50% higher in comparison to those in
pure crystals, at other equal conditions. Such an increase
can be related to a change in the crystal-solution
boundary structure of colored crystals. The fact that
such a change takes place confirms indirectly the
difference in the etching patterns of colored and pure
crystals (Fig. 3). It can also be clearly seen when
etching the chipped off part of irradiated crystal over the
inclusion passage plane (Fig. 4). The given patterns are
indicative of the fact that not only the dislocations but
also radiation defects and their clusters are the sites for
the primary etching of the surface of KCl crystal.
Similar etching patterns were observed on the surface
of NaCl monocrystals irradiated with neutrons [14].
In contrast to the irradiation process of crystals that
results in the formation of hole-type color centers in
addition to electron centers the additive coloring of
crystals results only in the formation of electron color
centers. Hence, an increase in the motion velocity of
the inclusions in the specimens of both types is
indicative of the fact that particularly their influence on
a change in the matrix-solution interphase structure can
be considered as a defining factor.
In the absence of the external force fields that affect
the crystal, nonisometric inclusions (the pores)
spontaneously transform their shape approximating it to
the equilibrium one [15,16]. These processes proceed to
the extent of the difference of the chemical potentials of
atoms (molecules) H conditioned by the
difference in the local curvatures of surface H ( is
the surface tension, is the volume falling to one
particle in the crystal). Since typical under saturations
are low, the motion of stages that originate on spiral
dislocations is only possible on condition that the
distance from the point of emergence of the dislocation
to the face edge or to the point of emergence of the
dislocation of an opposite sign exceeds a diameter of the
critical nucleus 2 /cd ( is an effective
surface tension of the stage defined as a ratio of its
linear tension to the height). During the relaxation
process the value of is decreased аnd cd is
increased respectively and the dissolution (evaporation)
process of the stages is stopped.
Hence, the shape relaxation process (equally as the
motion process of inclusions (the pores)) is the
threshold one for the layered mechanism in the crystals
with no color centers. Attention should be paid to the
fact that a motive force of the shape relaxation is
defined by the surface tension , and the process
hampering and its stoppage depend on the value of .
Using the value of the residual degree of nonisometry of
the inclusions (the pores) we can obtain information on
the / ratio [15, 16] required for the understanding of
many phenomena that occur on the crystal surface.
Available color centers have an essential influence
on the relaxation process in isometric conditions of the
shape of inclusions acquired during the motion in the
temperature gradient field. In the pure crystal the
relaxation of the shape of inclusion occurs through the
dissolution of frontal and rear faces and the growth of
lateral edges. In this case, the mass center of inclusion is
not biased. In the irradiated crystal this process occurs
mainly through the dissolution of the frontal edge only
(Fig. 5). In addition, the degree of relaxation of the
shape of inclusions in irradiated crystals is considerably
higher in comparison to that of unirradiated crystals
practically approaching very often the equilibrium
shape.
Such a behavior of the inclusions can be conditioned
at least by two reasons. The calculations and
experiments [14] show that the concentration of
equilibrium solution over the crystal is changed in most
cases insignificantly depending on the extent of its
defectiveness. However, for the liquid inclusion whose
opposite faces are in inequivalent conditions (one face
contains color centers and another face contains no
color centers), and this difference can serve as an
additional motive force ( F ) of dissolution processes
on frontal faces. The second reason can be related to the
fact that the kinetic coefficients of the stages that
characterize the emission rate of crystal particles by the
stage (or the rate of their lining up to form the stage)
b
and define the rate of its motion have different values on
the surfaces contiguous with the irradiated area of the
crystal and with the recrystallized region. A value of the
kinetic coefficient of the stage at other similar
conditions is defined by the concentration of fractures
on the stage. It is evident that the F-centers representing
anion vacancies that captured an electron increase the
values of the kinetic coefficients of elementary stages
when appearing on the surface and increase the
dissolution rate of the face as a whole.
Fig. 3. The structure of the etched surface of KCl crystal
before (а) and after (b) the irradiation
Fig. 4. Etching the crystal chip dislocation in the
inclusion passage plane
Summing up, we can draw a conclusion that the
motion of dissolution stages on the frontal surface
contiguous with the defective area of the crystal will
also be possible at a full relaxation of the inclusion
shape on condition of the sufficient concentrations of
color centers in the crystal. However, in this case the
crystallization will occur on the rear face and it won’t be
observed on lateral faces. In other words, the inclusion
can shift as a whole in the absence of external force
fields.
Fig. 5. Relaxation of the shape of inclusions in the
irradiated crystal. The relaxation time is 34 hours
SPONTANEOUS MIGRATION OF THE
INCLUSIONS IN IRRADIATED CRYSTALS
Let’s give consideration to the liquid inclusion in the
irradiated crystal. Let’s assume that the fluctuation or
short-time external action (for example, that of the
temperature gradient conditioned by the nonuniform
cooling of the specimen and substrate after their
irradiation) resulted in an insignificant recrystallization
of the matrix substance from one surface of the
inclusion to another. Since radiation defects are not
reproduced we can observe the inequivalence of these
surfaces conditioned by the difference in the chemical
potentials of atoms F in the irradiated and
recrystallized regions of crystal. If the value of F is
sufficient to cause the motion of dissolution stages on
any surface contiguous with the defective area of the
crystal the motion of the inclusion as a whole is
possible. The discussed type of the motion of the
inclusions was observed in electron-irradiated KCl
monocrystals in which the concentrations of basic color
centers, i.e. electronic F-centers and hole-type V3-
b
b
centers were approximately the same and these were
equal to
232 10n m
-3
.
After the irradiation, the crystals were matured in
isothermal conditions at room temperature in the
absence of external force fields. It was accompanied by
spontaneous motion of the inclusions (Fig. 6). The
normal dissolution rate of the faces of inclusions given
in Fig. 6 was about one monolayer per second. With
time, the rate of inclusions was decreased and it is
evidently related to the general decrease in the crystal
defectiveness during its long-term maturing after the
irradiation.
Fig. 6. Displacement of the inclusions in the electron-
irradiated crystal in isothermal conditions:
а – 9 days, b – 25 days after the irradiation
A motion trajectory of the inclusions can easily be
judged from the brightened up traces that are formed
behind them (Fig. 7). A chaotic behavior of the
migration is evidently conditioned by the fact that only
one (the rear surface) of six surfaces will be dissolved
and as for the rest five surfaces the surface that has a
more efficient source of the dissolution of stages will be
dissolved. The most favorably located and oriented
spiral dislocation is considered to be such a source.
Different activity of dislocation sources can also explain
an essential spread in the rates of inclusions due to the
values of rates averaged by a sufficiently long time (up
to one month) described in previous papers. Using the
data on the motion kinetics we calculated an increase in
the chemical potential of crystal atoms conditioned by
the irradiation defects of F qn , on the basis of
which we estimated the stored energy q falling per one
F-center.
The obtained value turned out to be much lower than
that of the energy falling to one F-center during the
irradiation of KCl crystal, according to the data of
theoretical and experimental investigations described in
в [14], – 5q eV. A divergence was explained by a
two-order difference in the concentration of color
centers near the dissolution surface in comparison to
that in the crystal volume. This difference was related to
the perturbation effect of the solution on the pre-surface
layer of the crystal of more than 10 nm thick in which
the probability of tunnel recombination of electron and
hole-type centers with each other is increased including
also the donors and accepters situated in the pre-surface
layer of solution [17].
Fig. 7. The traces of spontaneous migration of the
inclusions of a different size in the electron-irradiated
crystal. The after-radiation time is one month
To look into the motive forces and the kinetics of the
spontaneous migration of liquid inclusions in the
crystals with spot defects of a radiation origin in greater
detail we need to carry out additional investigations of
the dynamics of these processes. In conclusion, we
would like to note a fundamental difference in the role
played by the color centers that are formed during the
crystal irradiation and those that are formed during the
additive coloring in the formation of the motive forces
of spontaneous migration of the inclusions. The
attempts made to induce spontaneous migration of the
inclusions in the additively colored specimens turned
out to be ineffective. Evidently, such an outcome is
conditioned by the fact that in the second case the
“matrix-color centers” system is thermodynamically
b
b
stable and in the first case it is thermodynamically
unstable.
CONCLUSIONS
This scientific paper looks into the effect the
irradiation has on the radiation-induced mobility of
liquid inclusions in KCl monocrystals. It is shown that
these inclusions become mobile when exposed to the
irradiation. It can result in the migration of such units to
the material boundary and the release of radioactive
elements from the sites of their disposal. The
trajectories of spontaneous migration of the inclusions
of a different size in the electron-irradiated crystal have
been studied.
The obtained data are of great importance for the
prediction of the properties of the storage sites of
radioactive waste.
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Article received 26.03.2019
РАДИАЦИОННО-ИНДУЦИРОВАННОЕ ДВИЖЕНИЕ ЖИДКИХ ВКЛЮЧЕНИЙ
В ЩЕЛОЧНО-ГАЛОИДНЫХ КРИСТАЛЛАХ
А.П. Кулик, О.В. Подшивалова, И.Г. Марченко
Изучено радиационно-стимулированное поведение жидких включений в монокристаллах KCl. Показано,
что под действием облучения включения становятся подвижными. Это может приводить к миграции таких
объектов на границу материала и выходу радиоактивных элементов из захоронения. Исследованы траектории
самопроизвольной миграции включений различных размеров в кристаллах, облученных электронами и γ-
квантами.
РАДИАЦІЙНО-ІНДУКОВАНИЙ РУХ РІДКИХ ВКЛЮЧЕНЬ
У ЛУЖНО-ГАЛОЇДНИХ КРИСТАЛАХ
О.П. Кулик, О.В. Подшивалова, І.Г. Марченко
Вивчено радіаційно-стимульовану поведінку рідких включень у монокристалах KCl. Показано, що під
дією опромінення включення стають рухливими. Це може призводити до міграції таких об'єктів на межу
матеріалу і виходу радіоактивних елементів із поховання. Досліджено траєкторії самочинної міграції
включень різних розмірів у кристалах, опромінених електронами і -квантами.
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