Structural and optical studies of Cu₆PSe₅I-based thin film deposited by magnetron sputtering
Cu₅.₅P₁.₂Se₅.₀I₁.₃ thin film was deposited onto silicate glass substrate by non-reactive radio frequency magnetron sputtering. Structural studies were carried out using X-ray diffraction and SEM techniques. Spectrometric studies of transmission spectra of Cu₅.₅P₁.₂Se₅.₀I₁.₃ thin film in the temperat...
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Інститут фізики напівпровідників імені В.Є. Лашкарьова НАН України
2017
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| Cite this: | Structural and optical studies of Cu₆PSe₅I-based thin film deposited by magnetron sputtering / I.P. Studenyak, M.M. Kutsyk, A.V. Bendak, V.Yu. Izai, V.V. Bilanchuk, P. Kúš, M. Mikula // Semiconductor Physics Quantum Electronics & Optoelectronics. — 2017. — Т. 20, № 1. — С. 64-68. — Бібліогр.: 16 назв. — англ. |
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Digital Library of Periodicals of National Academy of Sciences of Ukraine| _version_ | 1860279371389992960 |
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| author | Studenyak, I.P. Kutsyk, M.M. Bendak, A.V. Izai, V.Yu. Bilanchuk, V.V. Kúš, P. Mikula, M. |
| author_facet | Studenyak, I.P. Kutsyk, M.M. Bendak, A.V. Izai, V.Yu. Bilanchuk, V.V. Kúš, P. Mikula, M. |
| citation_txt | Structural and optical studies of Cu₆PSe₅I-based thin film deposited by magnetron sputtering / I.P. Studenyak, M.M. Kutsyk, A.V. Bendak, V.Yu. Izai, V.V. Bilanchuk, P. Kúš, M. Mikula // Semiconductor Physics Quantum Electronics & Optoelectronics. — 2017. — Т. 20, № 1. — С. 64-68. — Бібліогр.: 16 назв. — англ. |
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| container_title | Semiconductor Physics Quantum Electronics & Optoelectronics |
| description | Cu₅.₅P₁.₂Se₅.₀I₁.₃ thin film was deposited onto silicate glass substrate by non-reactive radio frequency magnetron sputtering. Structural studies were carried out using X-ray diffraction and SEM techniques. Spectrometric studies of transmission spectra of Cu₅.₅P₁.₂Se₅.₀I₁.₃ thin film in the temperature interval 77 to 300 K were investigated. It is shown that the temperature behaviour of the optical absorption edge is described by the Urbach rule. Temperature dependences of optical parameters of the Urbach absorption edge and refractive index have been analyzed. The influence of temperature and structural disordering on the Urbach tail has been studied. The comparison of optical parameters of Cu₆PSe₅I crystal and Cu₅.₅P₁.₂Se₅.₀I₁.₃ thin film has been performed.
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| first_indexed | 2026-03-21T13:44:17Z |
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Semiconductor Physics, Quantum Electronics & Optoelectronics, 2017. V. 20, N 1. P. 64-68.
doi: https://doi.org/10.15407/spqeo20.01.064
© 2017, V. Lashkaryov Institute of Semiconductor Physics, National Academy of Sciences of Ukraine
64
PACS 78.40.Ha, 77.80.Bh
Structural and optical studies of Cu6PSe5I-based thin film deposited
by magnetron sputtering
I.P. Studenyak1, M.M. Kutsyk1, A.V. Bendak1, V.Yu. Izai1, V.V. Bilanchuk1,
P. Kúš2, M. Mikula2
1Uzhhorod National University, Faculty of Physics,
3, Narodna Sq., 88000 Uzhhorod, Ukraine
2Comenius University, Faculty of Mathematics, Physics and Informatics,
Mlynska dolina, 84248 Bratislava, Slovakia
E-mail: studenyak@dr.com
Abstract. Cu5.5P1.2Se5.0I1.3 thin film was deposited onto silicate glass substrate by non-
reactive radio frequency magnetron sputtering. Structural studies were carried out using
X-ray diffraction and SEM techniques. Spectrometric studies of transmission spectra of
Cu5.5P1.2Se5.0I1.3 thin film in the temperature interval 77 to 300 K were investigated. It is
shown that the temperature behaviour of optical absorption edge is described by the
Urbach rule. Temperature dependences of optical parameters of the Urbach absorption
edge and refractive index have been analyzed. The influence of temperature and
structural disordering on the Urbach tail has been studied. The comparison of optical
parameters of Cu6PSe5I crystal and Cu5.5P1.2Se5.0I1.3 thin film has been performed.
Keywords: thin film, magnetron sputtering, optical absorption, Urbach rule, refractive
index.
Manuscript received 20.10.16; revised version received 26.01.17; accepted for
publication 01.03.17; published online 05.04.17.
1. Introduction
Cu6PSe5I crystals belong to an argyrodite family of
tetrahedrally close-packed structures [1]. These materials
are known as superionic conductors or solid electrolytes.
They have attracted great interest not only in the view of
the possibility to apply them in a high-energy-density
batteries and sensors, but also due to their remarkable
properties.
Cu6PSe5I crystals, by analogy with Cu6PS5I, have
the cubic syngony (space group mF 34 ) at room
temperature [1]. The stepwise change of the total
electrical conductivity in Cu6PSe5I crystals, a sudden
increase in ionic conductivity as well as a decrease of the
activation energy have shown the existence of the
superionic first-order phase transition (PT), which
occurs within the temperature range Ts = 260…268 K
[2]. This PT is related with the structural topological
disorder of copper-cation sublattice, resulting in copper-
ion migration and drastic growth of the ionic component
in the electric conductivity. Temperature behaviour of
the dielectric permeability and absorption edge of
Cu6PSe5I crystal in the vicinity of the superionic PT has
been presented in Ref. [3].
Temperature behaviour of optical properties of
Cu6PSe5I crystals were studied in Refs. [4-6]. The long-
wave side of absorption edge in Cu6PSe5I crystal in the
non-superionic (T < Ts) and superionic (T > Ts) phases
exhibits exponential dependence on photon energy. The
Semiconductor Physics, Quantum Electronics & Optoelectronics, 2017. V. 20, N 1. P. 64-68.
doi: https://doi.org/10.15407/spqeo20.01.064
© 2017, V. Lashkaryov Institute of Semiconductor Physics, National Academy of Sciences of Ukraine
65
temperature studies have shown that the exponential
parts obey the Urbach rule in both phases, though the
convergence point coordinates of the Urbach edge are
different for the two phases. In the temperature range of
superionic PT, a stepwise behaviour of the optical
parameters are observed. The temperature dependence of
the optical pseudogap and Urbach energy were described
in the framework of the Einstein single oscillator model.
Thus, the physical properties of Cu6PSe5I single
crystals are well known, while the investigation of
physical properties of thin films on their basis only
begins. It should be noted that Cu6PS5I thin films for the
first time were obtained and studied in Ref. [7]. The
influence of annealing on the optical absorption edge
parameters of Cu6PS5I thin films was investigated in
Ref. [8]. Electrical and optical studies of Cu6PS5I-based
thin films with a different copper atoms content were
performed in Ref. [9].
Here, we report on the deposition, structural
investigation, and spectrometric studies of the
transmission spectra in Cu6PSe5I-based thin film.
Besides, we would like to analyze the temperature
behaviour of the Urbach absorption edge, to study
disordering processes in Cu6PSe5I-based thin film as
well as to compare the optical parameters of Cu6PSe5I
single crystal and thin films under investigation.
2. Experimental
Thin films were deposited from synthesized poly-
crystalline Cu6PSe5I onto silicate glass substrate by non-
reactive radio-frequency magnetron sputtering; the film
growth rate was close to 3 nm/min. Deposition was
carried out at room temperature in Ar atmosphere. The
structure of the deposited film was analyzed using X-ray
diffraction; the diffraction pattern obtained using
DRON-3 diffractometer (conventional θ–2θ scanning
technique, Bragg angle 2θ ≅ 10–60°, Cu Kα, Ni filtered
radiation) shows the films to be amorphous. Structural
studies were performed for the thin film (Fig. 1) by
using the scanning electron microscopy (SEM)
technique (Hitachi S-4300); the thin film chemical
composition (Cu5.5P1.2Se5.0I1.3) was determined using
energy-dispersive X-ray spectroscopy (EDX) studies,
which enabled us to check the chemical composition in
different points of the film surface. The deposited thin
films were observed to be depleted by copper and
enriched with phosphorous and iodine.
Optical transmission spectra of Cu5.5P1.2Se5.0I1.3 thin
films were studied in the interval of temperatures
77…300 K by an MDR-3 grating monochromator, a
UTREX cryostat was used for low-temperature studies.
From the temperature studies of interferential
transmission spectra, the spectral dependences of the
absorption coefficient as well as dispersion dependences
of the refractive index were derived [10].
Fig. 1. SEM image of Cu5.5P1.2Se5.0I1.3 thin film.
3. Results and discussion
The interferential transmission spectra of
Cu5.5P1.2Se5.0I1.3 thin films at various temperatures are
shown in Fig. 2. With temperature, a red shift of both the
short-wave part of the absorption spectrum (related to
the temperature behaviour of the absorption edge) and
the interferential maxima are observed. Besides, Fig. 2
presents the temperature isoabsorption dependence of
the characteristic energy α
gE from the short-wave part of
the absorption spectrum, corresponding to the fixed ab-
sorption coefficient value α = 4200 cm–1. No anomalies
in the isoabsorption dependence within the temperature
interval 77…300 K were revealed, which is the evidence
of the absence of PTs in this temperature range.
Fig. 2. Spectral dependences of transmission coefficient for
Cu5.5P1.2Se5.0I1.3 thin film at various temperatures: (1) 77, (2)
150, (3) 200, (4) 250, (5) 300 K. The inset shows the
temperature dependences of the absorption edge energy
position α
gE (α = 4200 cm–1) obtained in the heating mode.
Semiconductor Physics, Quantum Electronics & Optoelectronics, 2017. V. 20, N 1. P. 64-68.
doi: https://doi.org/10.15407/spqeo20.01.064
© 2017, V. Lashkaryov Institute of Semiconductor Physics, National Academy of Sciences of Ukraine
66
It is seen (Fig. 3) that the optical absorption edge
spectra within the range of their exponential behaviour
in amorphous Cu5.5P1.2Se5.0I1.3 thin films, similarly to
those in the Cu6PSe5I single crystal, are described by the
Urbach rule [11]
( ) ( )
( ) ⎥⎦
⎤
⎢
⎣
⎡ −ν
α=⎥⎦
⎤
⎢⎣
⎡ −νσ
α=να
TE
Eh
kT
EhTh
U
0
0
0
0 expexp, , (1)
where EU is the Urbach energy, σ is the absorption edge
steepness parameter, α0 and E0 are the convergence point
coordinates of the Urbach bundle. The coordinates of the
Urbach bundle convergence point α0 and E0 for the
Cu5.5P1.2Se5.0I1.3 thin films are given in Table. The latter
also presents the α0 and E0 values for Cu6PSe5I single
crystal.
The temperature behaviour of the Urbach absorption
edge in Cu5.5P1.2Se5.0I1.3 thin film is explained by electron-
phonon interaction (EPI) that is strong in the thin films
under investigation. The EPI parameters were obtained
from the temperature dependence of absorption edge
steepness parameter (Fig. 3) using the Mahr formula [12]
⎟⎟
⎠
⎞
⎜⎜
⎝
⎛ ω
⋅⎟
⎟
⎠
⎞
⎜
⎜
⎝
⎛
ω
⋅σ=σ
kT
kTT p
p 2
tanh2)( 0
h
h
, (2)
where pωh is the effective phonon energy in a single
oscillator model, describing the EPI, and σ0 – parameter
related to the EPI constant g as 1
0 )3/2( −=σ g
(parameters pωh and σ0 are given in Table). For the
Cu5.5P1.2Se5.0I1.3 thin film σ0 < 1, which is the evidence
for the strong EPI [13]. It should be noted that in the thin
film, as compared to the single crystal, the EPI is
substantially enhanced (it corresponds to a decrease of
the σ0 parameter) and the energy pωh of the effective
phonon, taking part in absorption edge formation,
increases (Table).
Fig. 3. Spectral dependences of the absorption coefficient for
Cu5.5P1.2Se5.0I1.3 thin film at various temperatures: (1) 77, (2)
150, (3) 200, (4) 250, (5) 300 K. The insert shows the
temperature dependence of the steepness parameter σ.
Table. The parameters of Urbach absorption edge and EPI
for Cu6PSe5I single crystal and Cu5.5P1.2Se5.0I1.3 thin film.
Material Single crystal Thin film
α0 (cm–1) 2.78×105 7.65×105
E0 (eV) 1.211 2.532
α
gE (eV) 1.059
(α = 103 cm–1)
2.053
(α = 5×104 cm–1)
EU (meV) 27.1 175.6
σ0 1.359 0.243
pωh (meV) 60.3 77.6
θE (K) 700 900
( )0UE (meV) 22.2 156.3
( )1UE (meV) 44.1 312.2
)0(α
gE (eV) 1.089 2.105
α
gS 4.61 4.11
For the spectral characterization of the Urbach
absorption edge in Cu5.5P1.2Se5.0I1.3 thin film, we use
their energy position α
gE at a fixed absorption
coefficient α = 5×104 cm–1 (Table). The temperature
dependences of α
gE and the Urbach energy EU for
Cu5.5P1.2Se5.0I1.3 thin film are summarized in Fig. 4. The
temperature behaviour of α
gE and EU can be described
in the Einstein model by the following relations [14, 15]
( ) ⎥
⎦
⎤
⎢
⎣
⎡
−θ
θ−= ααα
1exp
1)0()(
E
E T
kSETE ggg , (3)
( ) ( ) ( ) ⎥
⎦
⎤
⎢
⎣
⎡
−θ
+=
1exp
1
E
1U0UU T
EEE , (4)
where )0(α
gE and α
gS are the energy gap at 0 K and a
dimensionless constant, respectively; θE is the Einstein
temperature, corresponding to the average frequency of
phonon excitations of a system of non-coupled
oscillators, ( )0UE and ( )1UE are constants. The
obtained )0(α
gE , α
gS , θE, ( )0UE , and ( )1UE parameters
for the thin film are given in Table, and the temperature
dependences of α
gE and the Urbach energy EU for the
Cu5.5P1.2Se5.0I1.3 thin film calculated from Eqs. (3) and
(4) are shown in Fig. 5 as solid and dashed lines,
respectively. Besides, in Table we listed the values of
)0(α
gE , α
gS , θE, ( )0UE , and ( )1UE parameters for
Cu6PSe5I single crystal.
Semiconductor Physics, Quantum Electronics & Optoelectronics, 2017. V. 20, N 1. P. 64-68.
doi: https://doi.org/10.15407/spqeo20.01.064
© 2017, V. Lashkaryov Institute of Semiconductor Physics, National Academy of Sciences of Ukraine
67
Fig. 4. Temperature dependences of the absorption edge
energy position α
gE at α = 5×104 cm–1 (1) and the Urbach
energy EU (2) for Cu5.5P1.2Se5.0I1.3 thin film.
Fig. 5. Refractive index dispersions for Cu5.5P1.2Se5.0I1.3 thin
film at various temperatures: (1) 77, (2) 150, (3) 200, (4) 250
and (5) 300 K. The inset shows the temperature dependence of
refractive index.
It should be noted that in Cu5.5P1.2Se5.0I1.3 thin film
the Urbach behaviour of the absorption edge is observed
in the whole temperature interval under investigation,
while in the single crystal it is observed in non-
superionic and superionic phases separately. An
essential characteristic of the absorption edge spectra
inherent to the thin films under investigation is a lengthy
Urbach tail, which results in the Urbach energy EU
increase by the factor over than 6 in comparison with
that of the single crystal.
In Ref. [16], it was shown that both temperature
and structural disordering affect the Urbach absorption
edge shape, i.e., the Urbach energy EU is described by
the equation
( ) ( ) ( ) ( ) ( ) dynXstatXTXT EEEEEE ,U,UUUUU ++=+= ,
(5)
where ( )TEU and ( )XEU are the contributions of
temperature and structural disordering to EU,
respectively; ( ) statXUE , and dynXUE ,)( – contributions
of static structural disordering and dynamic structural
disordering to ( )XEU , respectively. It should be noted
that the first term in the right-hand side of Eq. (4)
represents static structural disordering, and the second
one represents temperature-related types of disordering:
temperature disordering due to thermal lattice vibrations
and dynamic structural disordering due to the presence
of mobile ions in the superionic conductor.
The static structural disordering ( ) statXE ,U in
Cu5.5P1.2Se5.0I1.3 thin film as well as in Cu6PSe5I single
crystal is caused by structural imperfectness due to the
high concentration of disordered copper vacancies.
Moreover, the static structural disordering in
Cu5.5P1.2Se5.0I1.3 thin film, unlike to that in Cu6PSe5I
single crystal, increases due to: (1) the absence of long-
range order in the atomic arrangement and chemical
bond breakdown; (2) lower density of the atomic
structure packing due to the presence of pores; (3) the
transition from the three-dimensional bulk structure to
the two-dimensional planar structure. Thus, the absolute
value of contribution of static structural disordering into
the thin film Urbach energy increases by the factor over
than 7 in comparison with that in the single crystal,
while its relative value grows from 82% in the single
crystal to 89% in the thin film.
The dynamic structural disordering ( ) dynXE ,U is
related to the intense motion of mobile copper ions,
participating in ion transport, and is responsible for the
ionic conductivity. Preliminary electrical studies have
shown that the total electric conductivity of the thin film
at T = 295 K is σt = 3.9×10–3 S/cm at the frequency close
to 1 MHz, while the total electric conductivity for the
single crystal is σt = 5.6×10–2 S/cm at 1 kHz [2].
The dispersion dependences of the refractive index
for the Cu5.5P1.2Se5.0I1.3 thin film were obtained from the
interferential transmission spectra (Fig. 5). The slight
dispersion of the refractive index is observed in the
transparency region, but it increases when approaching
to the optical absorption edge region. With temperature
increase, the nonlinear growth of the refractive index in
Cu5.5P1.2Se5.0I1.3 thin film has been revealed.
4. Conclusions
Cu5.5P1.2Se5.0I1.3 thin films were deposited onto silicate
glass substrate by non-reactive radio frequency
magnetron sputtering. X-ray diffraction pattern shows
the films to be amorphous. Structural studies were
performed using SEM technique, which gives the
evidence for the formation of a homogeneous two-
dimensional structure. Temperature variation of the
transmission spectra as well as the temperature variation
of the absorption edge spectra within the range of its
Semiconductor Physics, Quantum Electronics & Optoelectronics, 2017. V. 20, N 1. P. 64-68.
doi: https://doi.org/10.15407/spqeo20.01.064
© 2017, V. Lashkaryov Institute of Semiconductor Physics, National Academy of Sciences of Ukraine
68
exponential behaviour have been studied. A typical
Urbach bundle has been observed, temperature
dependences of the optical parameters of the Urbach
absorption edge have been analyzed. In two-dimensional
Cu5.5P1.2Se5.0I1.3 thin films, the Urbach absorption edge is
formed by strong EPI. The influence of temperature and
structural disordering on the Urbach tail is studied and a
comparative analysis of the Urbach absorption edge
parameters for Cu6PSe5I single crystal and
Cu5.5P1.2Se5.0I1.3 thin film has been performed. It should
be noted that the transfer from Cu6PSe5I single crystal to
Cu5.5P1.2Se5.0I1.3 thin film causes the substantial increase
of the Urbach energy EU, enhances EPI (decrease of σ0
parameter) and increases the effective phonon energy
pωh as well as the relative contribution of static
structural disordering into EU from 82% to 89%. The
dispersion dependences of the refractive index for the
Cu5.5P1.2Se5.0I1.3 thin film have been obtained from the
interferential transmission spectra; the nonlinear increase
of refractive index with temperature increase has been
revealed.
Acknowledgements
Mykhailo Kutsyk (contract number 51602011) is
strongly grateful to the International Visegrad Fund
scholarship for funding the project.
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| institution | Digital Library of Periodicals of National Academy of Sciences of Ukraine |
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| language | English |
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| publisher | Інститут фізики напівпровідників імені В.Є. Лашкарьова НАН України |
| record_format | dspace |
| spelling | Studenyak, I.P. Kutsyk, M.M. Bendak, A.V. Izai, V.Yu. Bilanchuk, V.V. Kúš, P. Mikula, M. 2026-03-03T11:07:03Z 2017 Structural and optical studies of Cu₆PSe₅I-based thin film deposited by magnetron sputtering / I.P. Studenyak, M.M. Kutsyk, A.V. Bendak, V.Yu. Izai, V.V. Bilanchuk, P. Kúš, M. Mikula // Semiconductor Physics Quantum Electronics & Optoelectronics. — 2017. — Т. 20, № 1. — С. 64-68. — Бібліогр.: 16 назв. — англ. 1560-8034 PACS: 78.40.Ha, 77.80.Bh https://nasplib.isofts.kiev.ua/handle/123456789/214911 https://doi.org/10.15407/spqeo20.01.064 Cu₅.₅P₁.₂Se₅.₀I₁.₃ thin film was deposited onto silicate glass substrate by non-reactive radio frequency magnetron sputtering. Structural studies were carried out using X-ray diffraction and SEM techniques. Spectrometric studies of transmission spectra of Cu₅.₅P₁.₂Se₅.₀I₁.₃ thin film in the temperature interval 77 to 300 K were investigated. It is shown that the temperature behaviour of the optical absorption edge is described by the Urbach rule. Temperature dependences of optical parameters of the Urbach absorption edge and refractive index have been analyzed. The influence of temperature and structural disordering on the Urbach tail has been studied. The comparison of optical parameters of Cu₆PSe₅I crystal and Cu₅.₅P₁.₂Se₅.₀I₁.₃ thin film has been performed. Mykhailo Kutsyk (contract number 51602011) is strongly grateful to the International Visegrad Fund scholarship for funding the project. en Інститут фізики напівпровідників імені В.Є. Лашкарьова НАН України Semiconductor Physics Quantum Electronics & Optoelectronics Structural and optical studies of Cu₆PSe₅I-based thin film deposited by magnetron sputtering Article published earlier |
| spellingShingle | Structural and optical studies of Cu₆PSe₅I-based thin film deposited by magnetron sputtering Studenyak, I.P. Kutsyk, M.M. Bendak, A.V. Izai, V.Yu. Bilanchuk, V.V. Kúš, P. Mikula, M. |
| title | Structural and optical studies of Cu₆PSe₅I-based thin film deposited by magnetron sputtering |
| title_full | Structural and optical studies of Cu₆PSe₅I-based thin film deposited by magnetron sputtering |
| title_fullStr | Structural and optical studies of Cu₆PSe₅I-based thin film deposited by magnetron sputtering |
| title_full_unstemmed | Structural and optical studies of Cu₆PSe₅I-based thin film deposited by magnetron sputtering |
| title_short | Structural and optical studies of Cu₆PSe₅I-based thin film deposited by magnetron sputtering |
| title_sort | structural and optical studies of cu₆pse₅i-based thin film deposited by magnetron sputtering |
| url | https://nasplib.isofts.kiev.ua/handle/123456789/214911 |
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