On the problem of relaxation for radiation-induced optical effects in some ternary chalcogenide glasses
We have investigated the influence of high-energy γ-irradiation on the optical transmission spectra of ternary Ge-As-S chalcogenide glasses of the stoichiometric As₂S₃-GeS₂ and non-stoichiometric As₂S₃-Ge₂S₃ systems. A long-wave shift of the fundamental absorption edge is observed for all glasses...
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Інститут фізики напівпровідників імені В.Є. Лашкарьова НАН України
2007
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irk-123456789-1181172017-05-29T03:05:26Z On the problem of relaxation for radiation-induced optical effects in some ternary chalcogenide glasses Shpotyuk, O.I. Vakiv, M.M. Butkiewicz, B. Kovalskiy, A.P. Golovchak, R.Ya. We have investigated the influence of high-energy γ-irradiation on the optical transmission spectra of ternary Ge-As-S chalcogenide glasses of the stoichiometric As₂S₃-GeS₂ and non-stoichiometric As₂S₃-Ge₂S₃ systems. A long-wave shift of the fundamental absorption edge is observed for all glasses. Two different components of radiation-induced changes were specified: static (residual) and dynamic (time dependent) ones. The dynamic component is mathematically described by the exponential and power functions in respect to post-irradiation periods. It is shown that quantitative features of the observed self-restoration phenomena in the irradiated glasses are closely related to their chemical compositions and stoichiometry. 2007 Article On the problem of relaxation for radiation-induced optical effects in some ternary chalcogenide glasses / O.I. Shpotyuk, M.M. Vakiv, B. Butkiewicz, A.P. Kovalskiy, R.Ya. Golovchak // Semiconductor Physics Quantum Electronics & Optoelectronics. — 2007. — Т. 10, № 3. — С. 23-27. — Бібліогр.: 17 назв. — англ. 1560-8034 PACS 61.80.-x http://dspace.nbuv.gov.ua/handle/123456789/118117 en Semiconductor Physics Quantum Electronics & Optoelectronics Інститут фізики напівпровідників імені В.Є. Лашкарьова НАН України |
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Digital Library of Periodicals of National Academy of Sciences of Ukraine |
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DSpace DC |
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English |
| description |
We have investigated the influence of high-energy γ-irradiation on the optical
transmission spectra of ternary Ge-As-S chalcogenide glasses of the stoichiometric
As₂S₃-GeS₂ and non-stoichiometric As₂S₃-Ge₂S₃ systems. A long-wave shift of the
fundamental absorption edge is observed for all glasses. Two different components of
radiation-induced changes were specified: static (residual) and dynamic (time dependent) ones. The dynamic component is mathematically described by the exponential and power functions in respect to post-irradiation periods. It is shown that quantitative features of the observed self-restoration phenomena in the irradiated glasses are closely related to their chemical compositions and stoichiometry. |
| format |
Article |
| author |
Shpotyuk, O.I. Vakiv, M.M. Butkiewicz, B. Kovalskiy, A.P. Golovchak, R.Ya. |
| spellingShingle |
Shpotyuk, O.I. Vakiv, M.M. Butkiewicz, B. Kovalskiy, A.P. Golovchak, R.Ya. On the problem of relaxation for radiation-induced optical effects in some ternary chalcogenide glasses Semiconductor Physics Quantum Electronics & Optoelectronics |
| author_facet |
Shpotyuk, O.I. Vakiv, M.M. Butkiewicz, B. Kovalskiy, A.P. Golovchak, R.Ya. |
| author_sort |
Shpotyuk, O.I. |
| title |
On the problem of relaxation for radiation-induced optical effects in some ternary chalcogenide glasses |
| title_short |
On the problem of relaxation for radiation-induced optical effects in some ternary chalcogenide glasses |
| title_full |
On the problem of relaxation for radiation-induced optical effects in some ternary chalcogenide glasses |
| title_fullStr |
On the problem of relaxation for radiation-induced optical effects in some ternary chalcogenide glasses |
| title_full_unstemmed |
On the problem of relaxation for radiation-induced optical effects in some ternary chalcogenide glasses |
| title_sort |
on the problem of relaxation for radiation-induced optical effects in some ternary chalcogenide glasses |
| publisher |
Інститут фізики напівпровідників імені В.Є. Лашкарьова НАН України |
| publishDate |
2007 |
| url |
http://dspace.nbuv.gov.ua/handle/123456789/118117 |
| citation_txt |
On the problem of relaxation for radiation-induced optical effects in some ternary chalcogenide glasses / O.I. Shpotyuk, M.M. Vakiv, B. Butkiewicz, A.P. Kovalskiy, R.Ya. Golovchak // Semiconductor Physics Quantum Electronics & Optoelectronics. — 2007. — Т. 10, № 3. — С. 23-27. — Бібліогр.: 17 назв. — англ. |
| series |
Semiconductor Physics Quantum Electronics & Optoelectronics |
| work_keys_str_mv |
AT shpotyukoi ontheproblemofrelaxationforradiationinducedopticaleffectsinsometernarychalcogenideglasses AT vakivmm ontheproblemofrelaxationforradiationinducedopticaleffectsinsometernarychalcogenideglasses AT butkiewiczb ontheproblemofrelaxationforradiationinducedopticaleffectsinsometernarychalcogenideglasses AT kovalskiyap ontheproblemofrelaxationforradiationinducedopticaleffectsinsometernarychalcogenideglasses AT golovchakrya ontheproblemofrelaxationforradiationinducedopticaleffectsinsometernarychalcogenideglasses |
| first_indexed |
2025-07-08T13:23:41Z |
| last_indexed |
2025-07-08T13:23:41Z |
| _version_ |
1837085253287542784 |
| fulltext |
Semiconductor Physics, Quantum Electronics & Optoelectronics, 2007. V. 10, N 3. P. 23-27.
© 2007, V. Lashkaryov Institute of Semiconductor Physics, National Academy of Sciences of Ukraine
23
PACS 61.80.-x
On the problem of relaxation for radiation-induced optical effects
in some ternary chalcogenide glasses
O.I. Shpotyuk1,3, M.M. Vakiv1, B. Butkiewicz2,
A.P. Kovalskiy1, and R.Ya. Golovchak1,4
1Scientific Research Company "Carat", 202, Stryjska str., 29031 Lviv, Ukraine
2Institute of Electronic Systems, Warsaw University of Technology,
15/19, Nowowiejska Str., Warsaw 00-665, Poland
3Physics Institute, Pedagogical University of Czestochowa,
13/15, Al. Armii Krajowej, Czestochowa 42-415, Poland
4Ivan Franko Lviv National University, Physics Department
50, Dragomanov str., 29005 Lviv, Ukraine
Abstract. We have investigated the influence of high-energy γ-irradiation on the optical
transmission spectra of ternary Ge-As-S chalcogenide glasses of the stoichiometric
As2S3-GeS2
and non-stoichiometric As2S3-Ge2S3 systems. A long-wave shift of the
fundamental absorption edge is observed for all glasses. Two different components of
radiation-induced changes were specified: static (residual) and dynamic (time dependent)
ones. The dynamic component is mathematically described by the exponential and power
functions in respect to post-irradiation periods. It is shown that quantitative features of
the observed self-restoration phenomena in the irradiated glasses are closely related to
their chemical compositions and stoichiometry.
Keywords: irradiation, chalcogenide glass, absorption, relaxation.
Manuscript received 07.02.07; accepted for publication 27.09.07; published online 31.10.07.
1. Introduction
The great number of chalcogenide glasses (ChGs), thin
films, and structures based on these inorganic polymer
materials are well known as photosensitive media. The
photoinduced changes of optical properties of these
amorphous semiconductors have been intensively
investigated in recent years. Their microscopic mecha-
nisms as well as physical-chemical features have been
studied and explained quite well for the majority of
known chalcogenide-based compounds [1]. At the same
time, the radiation-induced optical effects (RIOE)
produced by high-energy ionizing irradiation (γ-quanta,
fast electrons, neutrons, etc. with average energies of
more than 1 MeV) have been investigated only for some
types of amorphous semiconductors (mainly for binary
or quasibinary ones) characterized by a relatively simple
two-dimensional structure [2-5]. The systematic
investigations of RIOE in more complicated amorphous
cross-linked ternary 3D systems obtained in the form of
bulk glasses [6, 7] have not been carried out yet.
Our interest in such investigations is caused now by
different circumstances. The most important is the
existence of a topological phase transition at the average
coordination number (calculated as the number of
covalent chemical bonds per formula unit) Z ≈ 2.67 in
some non-stoichiometric ternary ChGs with the so-called
2D-3D mixed structure. At this point, the compositional
dependences of photoinduced effects have well-
expressed peculiarities [7]. As a rule, the extreme values
of photoinduced shifts of the fundamental optical
absorption edges were observed for Z ≈ 2.67. The
analogous compositional dependences of RIOE in such
ChGs with a more complicated mixed 2D-3D structure
have not been completely studied yet.
In addition, the time dependent relaxation
processes in ChGs treated previously by high-energy
ionizing radiation (60Co γ-quanta, for example) need
especial attention from the controversial point
concerning their degradation or, in other words, the
RIOE stability. Despite the widely used conclusion on
the full time stability of the radiation-induced changes in
ChGs (3-5 years) at room temperature, we revealed that
Semiconductor Physics, Quantum Electronics & Optoelectronics, 2007. V. 10, N 3. P. 23-27.
© 2007, V. Lashkaryov Institute of Semiconductor Physics, National Academy of Sciences of Ukraine
24
these effects measured in the visible range of optical
absorption spectra contained two basically different
parts: the static (residual) component being constant at
room temperature after irradiation and the dynamic (time
dependent) one decaying with time at room temperature
[8]. But the compositional dependences of these
restoration processes, their total duration, and the
mathematical description in respect to the post-irra-
diation exposure are the problems for precise experi-
mental investigations.
Taking into account these features, we put forward
the purpose of the detailed study and a mathematical
simulation of the restoration processes for γ-irradiated
ternary ChGs of the Ge-As-S system depending on their
chemical compositions in a wide range of variation of Z
including the point of the 2D-3D topological phase
transition.
2. Experimental procedure
ChGs of the ternary Ge-As-S system with different
average coordination numbers Z are used in the form of
disk-like (1 mm in thickness and 10 mm in diameter)
polished samples of the stoichiometric (As2S3)y(GeS2)1-y
(y = 0.1, Z = 2.63; y = 0.2, Z = 2.59; y = 0.4, Z = 2.52;
y = 0.6, Z = 2.48) and non-stoichiometric
(As2S3)x(Ge2S3)1-x (x = 0.1, Z = 2.76; x = 0.2, Z = 2.72;
x = 0.4, Z = 2.64; x = 0.6, Z = 2.56; x = 0.8, Z = 2.48)
compositions. All investigated samples were prepared by
the melt quenching under natural conditions of a mixture
of high purity (99.9999 %) Ge, As, and S elements. The
initial materials were sealed in quartz ampoules at
10−3 Pa and heated gradually up to 1080 K. The furnace
was rocked for 24h in order to obtain the most
homogeneous samples. Then the ingots were quenched
in air at ambient temperature. All ampoules were
annealed once more at a temperature of 20-30 K below
the softening point (Tg) to remove the mechanical
strains. The amorphous state of the obtained materials
was controlled by the existence of a characteristic
conchoidal fracture and the data of X-ray diffraction and
infrared microscope analyses. Finally, all ingots were
sliced into 1-mm thick disks and polished for precise
optical measurments.
All samples were irradiated from a 60Co source
with a dose of 106 Gy and an average energy of
1.25 MeV.
Optical investigations were performed in the range
of 200-900 nm using a “Specord M40” spectro-
photometer. The transmission spectra τ(hν) at various
photons energies hν were measured before and after
irradiation in different periods of time (up to 6 months).
Then the absorption coefficients α were calculated from
the equation [9]
τ
−
=α
2)1(
ln
1 r
d
, (1)
where d is the sample thickness, and r is the reflectivity.
Table 1. Quantitative parameters of radiation-induced
changes of optical absorption for stoichiometric
(As2S3)y(GeS2)1-y chalcogenide glasses.
y Z
χ 1
=
∆
α
/α
0)
' m
ax
(a
.u
.)
(1
d
ay
a
fte
r γ
, w
ho
le
ef
fe
ct
)
hν'max
(eV)
χ 2
=
(∆
α
/α
0)
'' m
ax
(a
.u
.)
(2
m
on
th
s a
fte
r γ
, s
ta
tic
co
m
po
ne
nt
)
hν''max
(eV)
χ 0
=
χ
1
–
χ 2
(a
.u
.)
(d
yn
am
ic
c
om
po
ne
nt
)
0.1 2.63 0.55 2.410 0.53 2.415 0.02
0.2 2.59 0.52 2.380 0.48 2.390 0.04
0.4 2.52 0.46 2.340 0.36 2.360 0.10
0.6 2.48 0.41 2.210 0.26 2.240 0.15
Radiation-induced optical changes have been
determined by the value of χ = ∆α / α0, where ∆α is the
difference between the α values before and after γ-
irradiation, and α0 is the absorption before γ-irradiation.
To estimate the time dependences of the dynamic
component relaxation, the value of ∆α / α0max was taken
(the value at the maximum points of ∆α/α0(hν)
dependences).
2. Results and discussion
It is well known that γ-irradiation lead to a long-wave
shift of the optical absorption edge of a ChG due to the
specific topological coordination defect formation
processes [9]. Some of these defects are unstable with
time by causing the existence of the dynamic RIOE
component.
The typical spectral χ(hν) dependences for the
RIOE can be presented by characteristic bell-like curves.
Such a dependence is shown in Figure for one of the
investigated samples – (As2S3)0.1(Ge2S3)0.9 with Z = 2.76.
Curves 1 and 2 show the change of the χ parameter with
photon energy registered in 1 day and 2 months after
irradiation, respectively. The wide maximum, sharp
high-energy tail, and wide low-energy one are proper for
all spectra. This asymmetry of the χ(hν) curve becomes
sufficiently less with the self-restoration of the gamma-
induced changes.
One can see that the radiation-stimulated darkening
takes place after γ-treatment. This darkening is unstable
and decays with time to some residual value (the static
component of RIOE). The relaxation of the dynamic
component is considered in this paper in dependence on
the stoichiometry of ChG and the average coordination
number Z. The quantitative parameters of these static
and dynamic RIOE components are presented in
Tables 1 and 2 for the investigated stoichiometric and
non-stoichiometric ChG systems, respectively.
Semiconductor Physics, Quantum Electronics & Optoelectronics, 2007. V. 10, N 3. P. 23-27.
© 2007, V. Lashkaryov Institute of Semiconductor Physics, National Academy of Sciences of Ukraine
25
1.4 1.6 1.8 2.0 2.2 2.4
0
0.2
0.4
0.6
2
1
∆α
/α
0,
a.
u.
E,eV
In stoichiometric (As2S3)y(GeS2)1-y glasses, the
compositional dependence of the dynamic RIOE is
determined by the compactness behavior with variation
in Z. Increasing the GeS2 content in the glass matrix is
accompanied by the compactness decrease (owing to the
decompressing of the covalent linked network of As2S3-
based pyramidal units by two structurally inconsistent
GeS2 forms) [10]. As a result, the relaxation processes
decay too (see Table 1). In the non-stoichiometric
(As2S3)x(Ge2S3)1-x system, this process is complicated by
the presence of homopolar chemical bonds with low
dissociation energy which enlarge sufficiently the
relaxation effects. That is why the compositional
dependence of the dynamic RIOE in non-stoichiometric
ChGs reveals some peculiarities at the higher Z (see
Table 2).
We can see also from Tables 1 and 2 that the
spectral position of χmax correlates with the change of the
band gap Eg of the investigated glasses [11].
In order to mathematically describe the observed
phenomena, we used the exponential and power
functions (see Tables 3 and 4).
Table 2. Quantitative parameters of radiation-induced
changes of optical absorption for non-stoichiometric
(As2S3)x(Ge2S3)1-x chalcogenide glasses.
x
Z
χ 1
=
(∆
α
/α
0)
' m
ax
(a
.u
.)
(1
d
ay
a
fte
r γ
, w
ho
le
ef
fe
ct
)
hν'max
(eV)
χ 2
=
(∆
α
/α
0)
'' m
ax
(a
.u
.)
(2
m
on
th
s a
fte
r γ
,
st
at
ic
c
om
po
ne
nt
)
hν''max
(eV)
χ 0
=
χ
1 –
χ
2
(a
.u
.)
(d
yn
am
ic
o
m
po
ne
nt
)
0.1 2.76 0.77 1.990 0.28 2.060 0.49
3D↑ 0.2 2.72 0.71 2.005 0.35 2.070 0.36
Topological phase transition
2D↓ 0.4 2.64 0.74 2.145 0.36 2.180 0.38
0.6 2.56 0.81 2.200 0.46 2.240 0.35
0.8 2.48 0.87 2.240 0.50 2.270 0.37
Table 3. Parameters of RIOE fitting for stoichiometric
(As2S3)y(GeS2)1-y glasses.
y Z χ = χ0exp[–(t/τ)λ] χ = χ0exp(–t/τ1)
τ
(days)
λ
(a.u.)
Err. τ1 (days) Err.
0.1 2.63 4.75 0.06 0.00003 134.7 0.005
0.2 2.59 3.90 0.10 0.0003 73.1 0.019
0.4 2.52 3.20 0.09 0.00002 88.3 0.006
0.6 2.48 2.65 0.14 0.0001 53.3 0.015
Table 4. Parameters of RIOE fitting for non-stoichiometric
(As2S3)x(Ge2S3)1-x glasses.
x Z χ = χ0exp[–(t/τ)λ] χ =
=χ0exp(–t/τ1)
τ
(days)
λ
(a.u.)
Err. τ1
(days)
Err.
0.1 2.76 0.30 0.16 0.002 32.8 0.081
3D↑ 0.2 2.72 0.40 0.13 0.003 49.2 0.100
Topological phase transition
2D↓ 0.4 2.64 3.30 0.12 0.0005 67.4 0.029
0.6 2.56 3.90 0.15 0.0005 48.3 0.055
0.8 2.48 4.65 0.22 0.0004 35.0 0.018
It is worth to note that similar methods of
simulation were used previously to describe the
temperature dependences of optical reflectivity [12],
different types of structural relaxation processes [13-15],
and the dose dependences of defect concentrations [16]
in various amorphous materials.
The relation
])/(exp[)( 0
λτ−χ=χ tt (2)
is known as the “universal” relation used to describe the
relaxation processes in amorphous solids [16]. The χ
value is the measured quantity, τ is the time constant and
λ is the exponent varying from 0 to 1.
Relation (2) can be considered also as a
consequence of the superposition of different relaxation
processes [17] and can be replaced by the sum of n
exponential functions corresponding to the different
types of coordination defects:
∑
=
τ−χ=χ
n
i
ii tt
1
0 )/exp()( . (3)
In the present paper, we make the first attempt to
apply expression (2) to the description of RIOE in the
investigated ChGs. We also consider separately the case
where λ = 1,
)1/exp(0 τ−χ=χ t , (4)
and compare the obtained results.
Semiconductor Physics, Quantum Electronics & Optoelectronics, 2007. V. 10, N 3. P. 23-27.
© 2007, V. Lashkaryov Institute of Semiconductor Physics, National Academy of Sciences of Ukraine
26
Calculating the optimum τ and λ values for relation
(2), we obtained the results with the lowest error
presented in Tables 3 and 4.
The quantitative parameters of mathematical
simulation for the dynamic RIOE, τ, λ, and τ1, in the
stoichiometric (As2S3)y(GeS2)1-y system reveal a smooth
monotonic dependence on Z (see Table 3) without any
extrema. While the λ(Z) dependence is weakly defined
in these ChGs, the compositional τ and τ1 relations are
close to the linear monotonic increase with Z. The only
exception is the sample with Z = 2.59, where a high error
value was obtained. For the all other investigated
samples, the error value is comparatively low. It testifies
to the good fitting of experimental data by the chosen
expressions. Relation (2) gives a lower error and
therefore is more acceptable for the description of
dynamic effects in the stoichiometric system. Evidently,
this is caused by the complexity of the microstructural
mechanism of relaxation. This relaxation process cannot
be considered as the single integral process described by
the exponential function but as a superposition of several
components.
Compositional dependences of the quantitative
parameters of the dynamic component differ radically in
the non-stoichiometric glasses. They reveal less or more
pronounced extrema at the point Z = 2.67. The quantity
λ has a local minimum at this point changing the value
from 0.12 to 0.22. On the contrary, τ1 reaches the local
maximum changing from 32.8 to 67.4. The τ values
decrease with Z in the whole range, but, at the point of
the topological phase transition, the clear jump of τ is
observed. In 2D compositions, the magnitude of this
jump equals several days. But, in 3D compositions, it is
less than 1 day. At the same time, the all previous
conclusions concerning the effectiveness of the fitting of
the obtained experimental data by the chosen
mathematical formulas remain actual (see the error
values in Table 4). In other words, the fitting by formula
(2) of the data concerning the stoichiometric system is
better.
Thus, the characteristic feature of the non-
stoichiometric glasses in comparison with the
stoichiometric ones is the well-pronounced manifest-
tation of extrema at the point Z = 2.67. We consider that
the specific character of the short- and medium-range
order topologies near the point of the topological phase
transition in these glasses is the reason for such a
behavior. This specific character consists in the
anomalously high content of the homopolar chemical
bonds which are the “outflows” for the annihilation of
radiation-induced coordination defects, by owing to the
low dissociation energies. The specific microstructural
mechanisms for such an annihilation, as well as the
initiating processes of radiation-induced defect forma-
tion, need a more detailed study by the methods of
structural-physical investigations.
4. Conclusions
The relaxation of radiation-induced optical effects in
ternary chalcogenide glasses can be described quite well
by Eq. (2). This result agrees with the previous data
obtained for different types of relaxation in the range of
temperatures below Tg.
The compositional dependences of relaxation
parameters in non-stoichiometric ternary glasses, in
contradistinction to stoichiometric ones, reveal some
peculiarities at the point of the topological phase
transition. These features are related to the types of
defects in the structure and with the value of glass
compactness at different Z.
Acknowledgements
The authors would like to express the thanks to the
colleagues from the Institute of Solid State Physics of
Bulgarian Academy of Sciences for the collaboration
and preparation of samples. This work was supported in
part by the Mianowski Foundation (Warsaw, Poland)
and the Polish State Committee for Scientific Research.
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