Optical Materials 105 (2020) 109917
Available online 25 April 2020
0925-3467/© 2020 Elsevier B.V. All rights reserved.
Effect of pH treatment on the structural and optical properties of Sn
6
Sb
10
S
21
thin flms facilely synthesized using a spin coating method
Warunee Kumrueng
a
, Khotchanan Sawanthai
a
, Auttasit Tubtimtae
b, *
, Witawat Ponhan
c
a
Department of Chemistry, Faculty of Liberal Arts and Science, Kasetsart University, Kamphaeng Saen Campus, Nakhon Pathom, 73140, Thailand
b
Department of Physics, Faculty of Liberal Arts and Science, Kasetsart University, Kamphaeng Saen Campus, Nakhon Pathom, 73140, Thailand
c
Department of Physics, Faculty of Science and Technology, Sakon Nakhon Rajabhat University, Sakon Nakhon, 47000, Thailand
A R T I C L E INFO
Keywords:
Tin antimony sulfde
Thin flm
pH treatment
Structural and optical properties
Spin coating method
ABSTRACT
This study aimed to examine the effect of pH value for the Sn–Sb–S solution on the growth of tin antimony sulfde
(TAS) thin flms facilely synthesized and deposited on fuorine-doped tin oxide or borosilicate slide glass sub-
strates using a spin coating method. Field-emission scanning electron microscopy (FE-SEM) micrographs
confrmed that some aggregated NPs, the distribution of residuals and larger-sized clusters or non-uniform
surfaces of thin flms on the substrate surface were signifcantly affected by pH alteration. XRD analysis
revealed that the most intense peak of TAS thin flms exhibited a monoclinic Sn
6
Sb
10
S
21
crystal structure with an
orthorhombic Sn
5
Sb
2
S
9
phase. However, the presence of a binary Sb
2
S
3
phase was also observed; its peak in-
tensity gradually reduced with increasing pH value. In addition, the investigation revealed that change in the
structural and optical parameters under the alteration of the pH treatment in a solution had a signifcant impact
on the formation, nucleation and growth of the clusters with increasing residuals and non-uniformity of thin flm.
It could be concluded from the overall results of our demonstration that TAS thin flms with adjusted pH
treatment can be attributed to the growth of TAS thin flms for use as window layers in solar cell devices and may
have potential for use in photodetector, optical communication, and optical dispersion devices in the future.
1. Introduction
Currently, the trends of development for photovoltaic devices
including semiconductor thin flms that are non-toxic, environmentally
friendly, and abundant have attracted much attention. Previously, thin
flm photovoltaics such as cadmium telluride (CdTe) and copper indium
gallium selenide (CIGS) or Cu (In,Ga) Se
2
based solar cells exhibited
power conversion effciency reaching 22.1 and 22.9%, respectively [1,
2], which led to progress in updating photovoltaic technology. However,
both materials contain In and Ga, which are toxic and rare materials
[3–5]. This is a critical issue for further improvement of CIGS-based
solar cells. In this situation, material containing sulfdes and more
earth-abundant materials (Cu, Zn, Sn, Sb, and S) could be used for less
toxicity than material containing selenides. Based on our knowledge,
sulfosalt material belongs to a class of complex sulfdes with the general
formula of A
m
B
n
X
p
, where A means metallic elements like Sn and Pb, B
represents formally trivalent, semi-metallic elements such as As, Sb and
Bi, and X indicates either S or Se [6]. This kind of material has various
advantageous properties such as low cost, non-toxicity, and high
potential for use in many technological applications that can be used in
solid-state and photovoltaic devices [7–10] as well as thermoelectric
energy conversion [11]. Sulfosalts also have direct band gaps in the
range of 1.78–2.5 eV, which are very close to the theoretical value for
power conversion of light into electrical energy for photovoltaic cells
[12,13]. This criterion is preferable as an absorber layer in solar cell
devices [14]. Alternatively, a p-type Cu
2
ZnSnS
4
(CZTS) thin flm was
synthesized as a new absorber for solar cell applications. The CZTS has a
suitable band gap ~1.4–1.5 eV, which is close to the optimal bandgap
required for a single junction solar cell and high absorption coeffcient
(�10
4
cm
1
) [15,16]. For example, a combination of Zn
1x
Sn
x
O (ZTO)
and a short annealing time of CZTS with a Cd-free buffer layer results in
effciency of 9.7% [17]. A Cd-free CZTS solar cell exhibits energy con-
version effciency of 10.2%, resulting from the application of an
aluminum oxide (Al
2
O
3
) passivation layer [18] and a certifed 11% ef-
fciency CZTS solar cell with a high open-circuit voltage of 730 mV, has
been obtained through directly inducing Cd atoms to occupy Zn or Cu
lattice sites by heat treatment to reduce heterojunction recombination
[19]. Moreover, some groups of researchers have synthesized ternary
* Corresponding author.
E-mail address: tubtimtae@gmail.com (A. Tubtimtae).
Contents lists available at ScienceDirect
Optical Materials
journal homepage: http://www.elsevier.com/locate/optmat
https://doi.org/10.1016/j.optmat.2020.109917
Received 17 March 2020; Accepted 13 April 2020