Determination of fundamental optical constants of Zn₂SnO₄ films
Examined in this paper have been optical properties of polycrystalline films Zn₂SnO₄ deposited using the spray pyrolysis method within the range of substrate temperatures 250 °C to 450 °C in increments of 50 °C. The spectral dependences have been found for the following physical quantities: k(λ), n(...
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Інститут фізики напівпровідників імені В.Є. Лашкарьова НАН України
2017
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| Cite this: | Determination of fundamental optical constants of Zn₂SnO₄ films / A.O. Salohub, A.A. Voznyi, O.V. Klymov, N.V. Safryuk, D.I. Kurbatov, A.S. Opanasyuk // Semiconductor Physics Quantum Electronics & Optoelectronics. — 2017. — Т. 20, № 1. — С. 79-84. — Бібліогр.: 19 назв. — англ. |
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| author | Salohub, A.O. Voznyi, A.A. Klymov, O.V. Safryuk, N.V. Kurbatov, D.I. Opanasyuk, A.S. |
| author_facet | Salohub, A.O. Voznyi, A.A. Klymov, O.V. Safryuk, N.V. Kurbatov, D.I. Opanasyuk, A.S. |
| citation_txt | Determination of fundamental optical constants of Zn₂SnO₄ films / A.O. Salohub, A.A. Voznyi, O.V. Klymov, N.V. Safryuk, D.I. Kurbatov, A.S. Opanasyuk // Semiconductor Physics Quantum Electronics & Optoelectronics. — 2017. — Т. 20, № 1. — С. 79-84. — Бібліогр.: 19 назв. — англ. |
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| description | Examined in this paper have been optical properties of polycrystalline films Zn₂SnO₄ deposited using the spray pyrolysis method within the range of substrate temperatures 250 °C to 450 °C in increments of 50 °C. The spectral dependences have been found for the following physical quantities: k(λ), n(λ), ε1(λ), ε2(λ), and are defined as they change under the influence of substrate temperature Тs. Moreover, using the model by Wemple–DiDomenico, it was calculated the dispersion energy Ео and Ed for this oxide. Two independent methods defined band gaps Zn₂SnO₄, which decrease from 4.21…4.22 eV down to 4.04…4.05 eV with increasing Тs from 250 °C up to 450 °C.
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Semiconductor Physics, Quantum Electronics & Optoelectronics, 2017. V. 20, N 1. P. 79-84.
doi: https://doi.org/10.15407/spqeo20.01.079
© 2017, V. Lashkaryov Institute of Semiconductor Physics, National Academy of Sciences of Ukraine
79
PACS 78.20.-e, 78.66.-w
Determination of fundamental optical constants of Zn2SnO4 films
A.O. Salohub1, A.A. Voznyi1, O.V. Klymov2, N.V. Safryuk3, D.I. Kurbatov1, A.S. Opanasyuk1
1Sumy State University,
2, Rymskogo-Korsakova str., 40007 Sumy, Ukraine
E-mail: annkasalohub@gmail.com, opanasyuk_sumdu@ukr.net
2ISOM and Dpto. de Ingeniería Electrónica
Universidad Politecnica de Madrid, Ciudad Universitaria s/n, 28040 Madrid, Spain
3V. Lashkaryov Institute of Semiconductor Physics, NAS of Ukraine
41, prospect Nauky, 03680 Kyiv, Ukraine
Abstract. Examined in this paper have been optical properties of polycrystalline films
Zn2SnO4 deposited using the spray pyrolysis method within the range of substrate
temperatures 250 °C to 450 °C in increments of 50 °C. The spectral dependences have
been found for the following physical quantities: k(λ), n(λ), ε1(λ), ε2(λ) and defined as
they change under the influence of substrate temperature Тs. Moreover, using the model by
Wemple–DiDomenico it was calculated the dispersion energy Ео and Ed for this oxide.
Two independent methods defined band gaps Zn2SnO4, which decreases from
4.21…4.22 eV down to 4.04…4.05 eV with increasing Тs from 250 °C up to 450 °C.
Keywords: thin film, stannate zinc, spray pyrolysis, optical property, band gap,
dispersion parameters.
Manuscript received 21.11.16; revised version received 23.01.17; accepted for
publication 01.03.17; published online 05.04.17.
1. Introduction
In recent years, zinc stannate through its low cost, high
optical transparency and low resistivity has been
considered as alternative to the binary oxides (ITO,
SnO2, ZnO) and can have potential applications in a
number of optoelectronic devices and solar energetics. In
particular, ZTO thin films have found wide usage in
photoelectrics. It should be emphasized that Zn2SnO4
consists of nontoxic and widespread elements in the
earth’s crust, which have the low cost of extraction [1].
Furthermore, the conductive contact with SnO2 is
replaced by more efficient zinc stannate, as a result, it
allows increasing the energy conversion efficiency from
16.5 % up to 20.4 % in thin-film solar cells based on the
heterojunction CdS/CdTe. Nowadays, all well-known
photovoltaic devices with record parameters on the basis
of the heterojunction necessarily have transparent front
contact with ZTO [2]. The next step is to improve the
performance of devices transparent oxide by way
streamline the optical and electrical characteristics of the
functional layers of the solar cell.
Today, for preparing ZTO thin films different
methods are used: sputtering [3], chemical deposition
from the gas phase [4], sol-gel [5], spray pyrolysis [6]
etc. Among these techniques, the spray pyrolysis is an
effective and inexpensive method for obtaining high-
quality layers of oxides, due to operational simplicity,
cost-efficiency, and the capability for large-scale
production. A striking feature compared with the
techniques given above is non-vacuum system of
deposition. In the works [7-10] great attention is paid to
studies of structural and physical properties of ZTO, and
it is seen that significantly less studies are aimed at
obtaining the zinc stannate by using spray pyrolysis [10-
13]. It has been found that only in [11] the results of
studying the optical properties of ZTO films are
presented.
Semiconductor Physics, Quantum Electronics & Optoelectronics, 2017. V. 20, N 1. P. 79-84.
doi: https://doi.org/10.15407/spqeo20.01.079
© 2017, V. Lashkaryov Institute of Semiconductor Physics, National Academy of Sciences of Ukraine
80
It was this that played a key role in setting the goal
of our work: first, to obtain thin films of Zn2SnO4 with
high performances and, secondly, to investigate their
structural and optical properties.
2. Materials and methods
ZТО films were deposited on glass substrates by using
the spray pyrolysis in a laboratory setup that described in
detail in [14]. The glass substrates were cleaned by
ultrasound, then rinsed in distilled water and ethanol.
Individually prepared precursor with of an aqueous
solution of salts, pentahydrate tin tetrachloride (0.25 M)
and the hexahydrate of zinc nitrate (0.5 M), also added a
few drops of nitric acid to enhance solubility of salts.
Herewith, the volume of this solution (6 ml), velocity of
spraying the precursor (0.2 ml/min) and distance from
spray nozzle to substrate surface (23 cm) were kept
constant throughout all the experiment. Air was used as
the carrier gas that supplied from the compressor under
the pressure 0.2 MPa. The substrate temperature during
deposition of the thin films were varied from Ts =
250 °C up to 450 °C by the steps of 50 °C, and it was
controlled using a thermocouple.
The structural properties of Zn2SnO4 were analyzed
using X-ray diffraction. In particular, a Bruker D8
Avance A25 diffractometer equipped with a Lynxeye
fast detector and employing copper Kα radiation in the
θ–θ configuration were used to obtain diffraction
patterns within the angle range 2θ from 10° to 90°,
where 2θ is the Bragg angle. During the research, we
used focused X-ray radiation in accord with the Bragg–
Brentano scheme.
Optical studies of semiconductor films were carried
out using spectrophotometer Solid Spec-3700 UV-VIS-
NIR within the range of wavelengths λ = 250…1500 nm.
As a result, it was measured the spectra of the reflection
coefficient R(λ) and transmittance T(λ). In this case, with
using the respective console, we reached double
reflection of light from the surface of experimental
samples, taking into account its reflection from the
reference sample. Being based on the light reflection
spectra R(λ) in the region of low absorption of radiation,
we calculated spectra of the refractive index n(λ) and
extinction k(λ) for ZTO.
( ) π
αλ
=−
−
+
−
+
=
4
,
1
4
1
1 2
2
kk
R
R
R
Rn . (1)
Following the obtained above equation (1), from
the values of the coefficients of refraction and extinction
we determined the real ε1 and imaginary ε2 parts of the
dielectric constant of the material using the according
relationships [15, 16]:
22
1 kn −=ε , ,22 nk=ε (2)
where 2
21 )( ikn +=ε+ε=ε .
The dissipation factor [16] of the incident light was
calculated using the following expression:
1
2tan
ε
ε
=δ . (3)
3. Results and discussion
3.1. Structural properties
The data obtained in the previous studies indicated results
of studying the surface morphology, chemical
composition and some optical properties of ZTO films
deposited using the spray pyrolysis were presented in
[17]. Generally speaking, we examined a growth
mechanism of the films and size of their grains in
dependence on the substrate temperature. Using the
method of X-ray spectral microanalysis (ЕDАX), we
determined chemical composition of thin films, after that
confirmed the presence of elements Zn, Sn and O in the
films. Anyway, other doped components were not
detected in the studied samples. Also, we evaluated the
ratios of atomic concentrations СZn /СSn, СZn /CO and
СZn+Sn /CO with increasing Ts for ZTO.
Fig. 1 illustrates the diffraction patterns of ZTO
thin films deposited at various temperatures. As we can
see from the picture, in the patterns at 250 °С and
300 °С the lines at the angles 11.16…11.32° dominate.
Also, there are less intense lines at the angles (16.20°,
22.51°…22.83°, 34.06°, and 46.15°). Nevertheless,
nature of the peaks in diffractogram shows that the film
of zinc stannate has a polycrystalline structure.
Unfortunately, X-ray analysis was carried out partially.
This is with account of disadvantage in the required
number of diffraction lines for full analysis of the pattern
of ZTO.
3.2. Optical properties
Optical spectra for the coefficients of reflection R(λ) and
transmittance Т(λ) inherent to the studied samples are
shown in Fig. 2. Preliminary results of these
investigations were published in [17].
Fig. 1. X-ray diffraction pattern of the as-deposited ZТO films,
where Ts, °C: 250 (1), 300 (2), 350 (3), 400 (4), 450 (5).
Semiconductor Physics, Quantum Electronics & Optoelectronics, 2017. V. 20, N 1. P. 79-84.
doi: https://doi.org/10.15407/spqeo20.01.079
© 2017, V. Lashkaryov Institute of Semiconductor Physics, National Academy of Sciences of Ukraine
81
Fig. 2. Dependences for the coefficients of reflection (а) and
transmittance (b) corresponding to ZТО thin films at Ts, °C:
250 (1), 300 (2), 350 (3), 400 (4), 450 (5).
By using the above mentioned results and
expressions (1), we received values of the extinction
coefficients k and the refractive index n for various λ, as
illustrated by Fig. 3. As we can see from this figure, the
extinction coefficient (Fig. 3a) decreases with increasing
the wavelength, but this value increases with increasing
the deposition temperature Ts. Thus, at the wavelengths
λ > 380 nm, which correspond to the red boundary of the
photoelectric effect, attenuation of the incident light is
almost absent (k → 0).
The dependence of the refractive index n against
medium λ has falling in the wavelength range λ =
400…650 nm (Fig. 3b). It is important to reiterate that
this range corresponds to the region of low light
absorption. Furthermore, when λ = 400 nm, the value of
n changes from 2.23 down to 1.96, which is in good
agreement with the literature data [4] and [18].
Also, using the equation (2) we received the real ε1
and imaginary ε2 parts of the optical dielectric function
for ZTO. Wavelength dependences for these parameters
are given in Fig. 4. The obtained spectral distribution
curves have a similar nature as for the previously
described spectra of k and n.
Note that the imaginary part of the dielectric
function ε2 of the material is 2-fold lower than the real
part ε1. In addition, at the wavelength λ = 400 nm the
value of the real part of optical dielectric function lies
within the range ε1 = 4.8…3.8, while that of the
imaginary part lies within the interval ε2 = 0.019…0.051
(λ = 290 nm).
Respectively to the found values of ε1 and ε2, we
plotted the dependence of the dissipation factor by using
the equation (3). It can be seen from Fig. 5 that with
increasing the frequency (energy of incident photons)
the value of tan δ also increases. Moreover, the higher
the substrate temperature, the greater the scattering
coefficient.
Using the values of the absorption coefficients (that
were determined and described in [17]) we plotted the
spectral dependence of the coefficients of optical
conductivity (σ) for the films of zinc stannate. The
expression for σ has the following look [16]:
π
α
=σ
4
nc , (4)
where σ is the optical conductivity of thin films, α –
absorption coefficient, с – light velocity in vacuum.
Fig. 3. Dependences of the coefficients of extinction k (а) and
refraction n (b) for ZТО thin films at Ts, °C: 250 (1), 300 (2),
350 (3), 400 (4), 450 (5).
b
a
Semiconductor Physics, Quantum Electronics & Optoelectronics, 2017. V. 20, N 1. P. 79-84.
doi: https://doi.org/10.15407/spqeo20.01.079
© 2017, V. Lashkaryov Institute of Semiconductor Physics, National Academy of Sciences of Ukraine
82
Fig. 4. Dependences of real ε1 and imaginary ε2 parts of the
optical dielectric function corresponding to the ZTO thin films
at Ts, °C: 250 (1), 300 (2), 350 (3), 400 (4), 450 (5).
These results are given in Fig. 5b. As it follows
from the above relationships for the region of low light
absorption, the values of σ decrease with increasing λ.
Furthermore, it was discovered that the optical
conductivity of ZTO thin films increases with increasing
Ts, and the maximum value of this magnitude equals to
1.9·1015 s–1.
It is known [16] that the real part of the dielectric
constant can be evaluated using the relation:
2
1 λ−ε=ε ∞ B , (5)
where *
0
22
2
4 mc
NеB
επ
= , here е is the electron charge, N
– free charge carrier concentration, ε∞ – high frequency
dielectric constant, ε0 – electrical constant of vacuum, m∗
– effective mass of the charge carrier.
Linearization of these dependences in the
coordinates 2
1 n=ε against λ2 allows to find the value ε∞
by fitting a straight line with the y axis, and the angle of
slope to the x axis values. The above equation for the
parameter B contains the ratio of the concentration of
free charge carriers to the effective mass of charge
carriers N/m∗ in the material. As a result, one can easy
find the value of the parameter B.
Fig. 5. Dependences of the dissipation factor (а) and optical
conductivity (b) for ZTO thin films at Ts, °C: 250 (1), 300 (2),
350 (3), 400 (4), 450 (5).
According to Fig. 6, we obtained linear parts in the
region 2.55·105 < λ2 < 4.25·105 nm2. The straight line to
x axis formed some angle, which allowed us to
determine the ratio N/m∗, and the point of crossing with
the ordinate axis – values ε∞ (see Table).
The next step in interpretation of our results is
application of the mathematical model of a harmonic
oscillator [19]. With this model, one can determine optical
dispersion parameters of these oscillators. It may be found
from the relationship between the refractive index of the
medium and the energy of harmonic oscillator:
22
2
)(
1)(
hvE
EEhvn
o
od
−
⋅
+= , (6)
where Ed is the dispersion energy that is a measure of the
average strength of the interband optical transitions; Ео –
effective energy of single oscillator.
Using the relation (6), one can find the dispersion
energy parameters of material Ео and Ed. For this
purpose, it was built the experimental dependence
depicted in (Fig. 6). The value (Ео Ed)–1 and angle of the
Ео /Ed were determined by extrapolation of linear parts.
The oscillator energy Eo is related with average
values of the optical band gap Eg of the thin film, which is
consistent with the model by Wemple–DiDomenico [19].
Therefore, using Eo one can obtain the following value:
Semiconductor Physics, Quantum Electronics & Optoelectronics, 2017. V. 20, N 1. P. 79-84.
doi: https://doi.org/10.15407/spqeo20.01.079
© 2017, V. Lashkaryov Institute of Semiconductor Physics, National Academy of Sciences of Ukraine
83
2
o
g
E
E = . (7)
Summarizes in Table are the calculated energy
parameters obtained for the zinc stannate. By using two
independent methods, we determined the values of band
gap for this material (dependences (αhν)2–hν [17] and
the model by Wemple–DiDomenico), which correlate
well among themselves. It was ascertained that the
dispersion energy of oscillators rapidly increased with
growing the substrate temperature. However, the
efficient dispersion energy decreases with increasing Ts.
Table. Optical parameters for thin films ZТO.
Ts, °C N/m∗,
m–3 ε∞ Eo, eV Ed, eV Eg, eV Eg
opt, eV
[17]
250 2.45·1037 3.65 8.44 22.08 4.22 4.21
300 9.93·1036 3.54 8.39 20.58 4.19 4.18
350 6.03·1037 3.86 8.23 24.56 4.11 4.15
400 1.27·1038 4.13 8.13 27.18 4.06 4.05
450 8.94·1037 4.06 8.12 26.01 4.05 4.04
Fig. 6. Dependences of ε1 against λ2 (а) and (n2–1)–1 against
(hν)2 (b) for ZTO thin films at Ts, °C: 250 (1), 300 (2), 350 (3),
400 (4), 450 (5).
Fig. 7. Dependence τ versus hν for ZТО thin film at Ts =
250 °C (а) and 350°C (b).
The aforementioned calculations of the values ε∞
gave the opportunity to estimate the dielectric relaxation
time of carriers in the material and to build its spectral
dependence [16]:
2
1
ωε
ε−ε
=τ ∞ , (8)
where ω is the cyclic frequency.
A typical dependence τ against the energy of
incident light were obtained at temperatures Ts = 250 °C
and 350 °C as it is evident from Fig. 7. It is seen that the
higher the substrate temperature, the lower the value of τ
in the samples.
We can conclude, therefore, were first identified a
different of optical material constants of ZTO films
deposited by using spray pyrolysis. As a result, they can
be used in development of a number of optoelectronic
devices.
4. Conclusions
The optical properties of polycrystalline ZTO films
deposited using spray pyrolysis. In addition, we plotted
the following spectral dependences of the quantities:
k(λ), n(λ), ε1(λ) and ε2(λ) for various temperatures of
film deposition Ts. Using the model by Wemple–
DiDomenico enabled to calculate dispersion energies Eo
Semiconductor Physics, Quantum Electronics & Optoelectronics, 2017. V. 20, N 1. P. 79-84.
doi: https://doi.org/10.15407/spqeo20.01.079
© 2017, V. Lashkaryov Institute of Semiconductor Physics, National Academy of Sciences of Ukraine
84
and Ed of this oxide. It is also worth noting that two
independent methods allowed identification of the band
gap for this material. It is reduced from 4.21…4.22 eV
down to 4.04…4.05 eV at Ts varying within the range
250…450 °C. Also, we have calculated the optical
conductivity of this material at different wavelengths. It
has been ascertained that the dielectric relaxation time of
carriers in the films decreases with increasing Ts.
Overall, we have investigated the fundamental optical
parameters of ZTO films, which can be used in
designing the devices of optoelectronics and solar
energetics.
Acknowledgement
The work has been performed under the financial support
of the Ministry of Education and Science of Ukraine
(state registration numbers 0116U002619,
0115U000665c).
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| id | nasplib_isofts_kiev_ua-123456789-214908 |
| institution | Digital Library of Periodicals of National Academy of Sciences of Ukraine |
| issn | 1560-8034 |
| language | English |
| last_indexed | 2026-03-21T19:35:42Z |
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| publisher | Інститут фізики напівпровідників імені В.Є. Лашкарьова НАН України |
| record_format | dspace |
| spelling | Salohub, A.O. Voznyi, A.A. Klymov, O.V. Safryuk, N.V. Kurbatov, D.I. Opanasyuk, A.S. 2026-03-03T11:05:46Z 2017 Determination of fundamental optical constants of Zn₂SnO₄ films / A.O. Salohub, A.A. Voznyi, O.V. Klymov, N.V. Safryuk, D.I. Kurbatov, A.S. Opanasyuk // Semiconductor Physics Quantum Electronics & Optoelectronics. — 2017. — Т. 20, № 1. — С. 79-84. — Бібліогр.: 19 назв. — англ. 1560-8034 PACS: 78.20.-e, 78.66.-w https://nasplib.isofts.kiev.ua/handle/123456789/214908 https://doi.org/10.15407/spqeo20.01.079 Examined in this paper have been optical properties of polycrystalline films Zn₂SnO₄ deposited using the spray pyrolysis method within the range of substrate temperatures 250 °C to 450 °C in increments of 50 °C. The spectral dependences have been found for the following physical quantities: k(λ), n(λ), ε1(λ), ε2(λ), and are defined as they change under the influence of substrate temperature Тs. Moreover, using the model by Wemple–DiDomenico, it was calculated the dispersion energy Ео and Ed for this oxide. Two independent methods defined band gaps Zn₂SnO₄, which decrease from 4.21…4.22 eV down to 4.04…4.05 eV with increasing Тs from 250 °C up to 450 °C. The work has been performed under the financial support of the Ministry of Education and Science of Ukraine (state registration numbers 0116U002619, 0115U000665c). en Інститут фізики напівпровідників імені В.Є. Лашкарьова НАН України Semiconductor Physics Quantum Electronics & Optoelectronics Determination of fundamental optical constants of Zn₂SnO₄ films Article published earlier |
| spellingShingle | Determination of fundamental optical constants of Zn₂SnO₄ films Salohub, A.O. Voznyi, A.A. Klymov, O.V. Safryuk, N.V. Kurbatov, D.I. Opanasyuk, A.S. |
| title | Determination of fundamental optical constants of Zn₂SnO₄ films |
| title_full | Determination of fundamental optical constants of Zn₂SnO₄ films |
| title_fullStr | Determination of fundamental optical constants of Zn₂SnO₄ films |
| title_full_unstemmed | Determination of fundamental optical constants of Zn₂SnO₄ films |
| title_short | Determination of fundamental optical constants of Zn₂SnO₄ films |
| title_sort | determination of fundamental optical constants of zn₂sno₄ films |
| url | https://nasplib.isofts.kiev.ua/handle/123456789/214908 |
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