Journal of Alloys and Compounds 783 (2019) 226e231

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Journal of Alloys and Compounds

journal homepage: http://www.elsevier.com/locate/jalcom

Effect of stress layer on thermal properties of SnSe2 few layers

Xinke Liu a, Zhiwen Li a, Long Min a, Yangfan Peng a, Xinbo Xiong a, Youming Lu a,
Jin-Ping Ao a, Jiangping Fang a, Wei He b, Kuilong Li c, Jing Wu d, Wei Mao e,
Usman Younis a, **, V. Divakar Botcha a, *
a
College of Materials Science and Engineering, Key Laboratory of Optoelectronic Devices and Systems of Ministry of Education and Guangdong Province,
Shenzhen Key Laboratory of Special Functional Materials, Shenzhen Key Laboratory of Microscale Optical Information Technology, Chinese Engineering and
Research Institute of Microelectronics, Shenzhen University, 3688 Nanhai Ave, Shenzhen, 518060, PR China
b
College of Electronic Science and Technology, Shenzhen University, 3688 Nanhai Ave, Shenzhen, 518060, PR China
c
School of Electronic and Information Engineering (Department of Physics), Qilu University of Technology (Shandong Academy of Sciences), Jinan, 250353,
PR China
d
Institute of Materials Research and Engineering (IMRE) 2 Fusionopolis Way, Innovis #08-03, Singapore, 138634, Singapore
e
The Institute of Engineering Innovation, School of Engineering, The University of Tokyo, Yayoi 2-11-16, Bunkyo-ku, Tokyo 113-8656, Japan

a r t i c l e i n f o a b s t r a c t

Article history: Layered SnSe2 have much attention due to their potential novel applications in electronic devices areas,
Received 12 November 2018 such as photo-transistors, solar cells and memory devices. We investigate the thermal properties of few
Received in revised form layer SnSe2 with capping of Al2O3 layer using the temperature and power-dependent Raman spectros-
20 December 2018
copy. The first order temperature coefficient of A1g modes of SnSe2 layers on a SiO2/Si substrate was
Accepted 26 December 2018
found to be
0.01757 cm
1/K, which is much higher than the corresponding value
0.01270 cm
1/K of
Available online 27 December 2018
SnSe2 with Al2O3 layer. The difference in temperature coefficients is attributed to compressive stress
introduced by the Al2O3 stress layer. Meanwhile, the Al2O3 layer significantly increases the thermal
Keywords:
SnSe2
conductivity to 3.102 W/mK, which is larger than that of the SnSe2 films without Al2O3 (~2.378 W/mK).
Thermal properties The first principle calculation using CASTP demonstrated that this improvement of thermal conductivity
Stress layer is attributed to the compressive strain. This work suggests an effective way to improve the performances
Raman spectroscopy of SnSe2 based devices, and also need to understand the vibrational properties and electron-phonon
interactions at the interface of Al2O3 and SnSe2 layers.
© 2018 Elsevier B.V. All rights reserved.

1. Introduction application fields. Among these layered materials, SnSe2, as a

As the pioneer, the success of graphene has raised great con-
cerns about layered two-dimensional (2D) materials, owing to their
unique thermal, electronic, thermo electronic, and optoelectronic
properties [1e3]. Transition metal dichalcogenides (TMDCs) are
extremely attracted nowadays after graphene due to their band
gaps ranging from ~0.5 eV to 2.4 eV [4e10]. Transition metal
dichalcogenides (i.e. MoS2 [6], WS2 [7], and MoSe2 [8]), IIIA-VIA
group (i.e. GaS [11,12], GaSe [9], InSe [10], and In2Se3 [13]), and
IVAeVIA group compounds (i.e. SnS2 [14]) with adjustable band
gap and large surface area have drawn increasing attentions in such
* Corresponding author.
** Corresponding author.
E-mail addresses: usman.younis@gmail.com (U. Younis), divakarbotcha@gmail.
com (V. Divakar Botcha).
typical 2D material which has a similar structure as MoS2, in which
Sn atomic layer is sandwiched between two planes of Se layers to
form a stable “triple-layer” structure. The adjacent layers distance is
about 0.62 nm, which are held together by a weak Van der Waals
forces and these forces facilitated the exfoliation of SnSe2 [15]. The
schematic diagram of the atomic model of SnSe2 is shown in Fig. 1
(a), which has trigonal lattice structure with P3ð一Þm1 space group
[16]. The first principles calculation results have demonstrated that
SnSe2 can rapidly and reversibly switch between amorphous and
crystalline state under laser heating, which implies its bright po-
tential utilization in data storage devices [17]. Meanwhile, being
earth-abundant, environment-friendly, and low-cost, SnSe2 is
particularly desirable for sustainable opto-electronic applications
[15]. Few-layer SnSe2 obtained by mechanical exfoliation have an
excellent photoelectric efficiency, for which the carrier mobility
and photoelectric response efficiency can reach as high as

https://doi.org/10.1016/j.jallcom.2018.12.317
0925-8388/© 2018 Elsevier B.V. All rights reserved.
 X. Liu et al. / Journal of Alloys and Compounds 783 (2019) 226e231 227

Fig. 1. (a) Atomic structure model of a layered SnSe2, (b) the schematic diagram of mechanical exfoliation, (c) AFM image of a SnSe2 flake and the corresponding height profile in the
inset, (d) Raman spectra of few layer SnSe2 on SiO2/Si substrate sample at RT with the vibration modes of different peaks in the inset.

8.6 cm2V
1s
1 and 1.1  103 A/w. [18], respectively, superior to
many other 2D materials [19]. In addition, field effect transistors
(FETs) based on few layer SnSe2 have current on/off ratio about 104
by using 70 nm HfO2 as back-gate dielectric with the combination
of polymer electrolyte layer [20].
However, for nano-electronic and optoelectronic devices, accu-
mulated heat generated during the device operation would be
horrific impact on the performance of the devices. Therefore, it
becomes important for those devices to improve the material
thermal conductivity in order to favor heat dispersion. In recent
studies, it has been reported that Al2O3 passivation layer can not
only protect 2D materials from oxidation and foreign contaminants
but also reduce the current fluctuations effectively and increase the
lifetime of related devices by reducing the surface trap density
[20,21]. In addition, the experimental results of temperature and
power-dependent Raman have shown that the coating of thin Al2O3
profoundly enhances the thermal conductivity of thin film black
phosphorus (BP) [22]. Recently, we also reported on the effect of
high-K Al2O3 substrate on thermal conductivity which is significant
enhanced due to charge-phonon interaction between Al2O3 and
InSe layers [5]. However, there are very few reports on temperature
dependent Raman studies on SnSe2 layers without any passivation
layer and calculated the temperature coefficients for Eg and A1g
vibrational modes [23]. More recently, Lee et al. [24] reported the
first direct experimental demonstration of a SnSe2 few layers,
which is about 2.15 W/m-K. Moreover, the thermal conductivity of
monolayer SnSe2 was calculated to be about 3.27 W/mK by solving
the electron and phonon Boltzmann transport equation (BTE) at RT
[25]. Therefore, it is necessary to shed new light on the thermal
properties of SnSe2 layers coated by a thin layer of Al2O3 in order to
facilitate the design and fabrication of the related devices.
In this work, we expose the thermal properties of SnSe2 few-
layer on SiO2/Si substrate with and without Al2O3 passivation
layer using of Raman spectroscopy. In this work, a ~4 nm thin Al2O3
layer was used as a passivation layer, and which introduce a
uniform stress on few layer SnSe2. Hereafter, the Al2O3 passivation
layer is defined as a ‘stress layer’ in this paper. Mainly, the stress will
be existed at the interface Al2O3 and SnSe2 layers where they are in
contact. It may be due to their different thermal expansion co-
efficients which may change the properties of surface on SnSe2.
Such study is noteworthy to know about material properties such
as, structure, thermal expansion and thermal conductivity. Here,
we also demonstrate a proof-of-concept for change in Raman peak
position for SnSe2 samples with and without Al2O3 stress layer with
a wide range of both temperatures and laser powers. The first
principle calculations were carried out to exploring the phenom-
enon for the improvement of thermal conductivity which is related
to the compressive strain.
2. Experimental details
SnSe2 flakes were purchased from 2D semiconductors and used
as a precursor material. The SnSe2 few layers were transferred onto
SiO2(300 nm)/Si substrates by a classical mechanical exfoliation
using scotch tape as shown in Fig. 1(b). The substrates were initially
go through for standard cleaning process named as RCA-1
(NH4OH:H2O2:H2O-1:1:2) treatment [26]. Atomic force micro-
scopy (AFM) of exfoliated SnSe2 layers was carried out by using a
Bruker Dimension ICON model in tapping mode for thickness
measurements. Fig. 1(c) showed the AFM image of the obtained
sample and the thickness of the SnSe2 layers was about 25.6 nm
which were obtained from the height profile exhibited in the inset.
Here, around 15 samples were prepared by mechanical exfoliation;
most of them were about 25 nm thick and some samples are with
thinner thickness. However, the thickness thinner samples were
not uniform, and the measuring results are relatively random.
Therefore, eight samples with a thickness of about 25 nm were
considered for further experiments which were better in both
uniformity and consistency of measuring results. A confocal Raman
microprobe equipped with a 514 nm Ar þ laser was used for micro-
228 X. Liu et al. / Journal of Alloys and Compounds 783 (2019) 226e231
Raman spectroscopy studies of the SnSe2 few-layers samples.
Thereafter, ~ 4 nm Al2O3 passivation layer was deposited on the
samples via the atomic layer deposition (ALD) system with trime-
thylaluminum (TMA1) and H2O as precursors at 250  C. Further,
temperature and power-dependent Raman measurements were
carried out on both samples with and without passivation Al2O3
layer. In order to avoid the effect of SnSe2 thickness on Raman peak
[20], all the Raman measurement in this work were performed at
the location with same thickness of the sample. Temperature
dependent measurements ranging from RT to 500 K were carried
out using hot plate with well temperature controller, and samples
were allowing for 5 min equilibration time at each temperature
point. The laser power has been maintained below 0.25 mW during
the experiments in order to avoid the heating-induced damage of
the sample.
3. Results and discussion
Raman spectroscopy is a powerful non-destructive technique
and it can be effectively used to explore the properties of materials
such as, structure, nature of the bonds, thermal expansion, and
thermal conductivities [27e30]. The Raman spectra of few layer
SnSe2 recorded at room temperature were shown in Fig. 1(d). These
spectra show the corresponding in-plane (E) and out-of-plane (A)
modes of the sample. Normally, two prominent first-order Raman
active modes are observed and which are related to A1g
(~184 cm
1) and Eg (~117 cm
1), while the other modes are not
appeared due to Raman selection rules or moderately weak due to
degenerate in energy [20]. The corresponding atomic vibration
structures are revealed in the inset of Fig. 1(d). The spectrum shows
the strong Raman peak (A1g) around 184 cm
1, and a weak Raman
peak (Eg) around 117 cm
1.
The atomic vibrational properties obtained from temperature-
dependent Raman spectrum provide an important guidance for
understanding the electron-phonon (e-p) interaction, transport
properties, and structure of materials, which have significant im-
plications for electronic devices. In this work, the temperature-
dependent Raman spectra of SnSe2 few layers with and without
Al2O3 stress layer were carried out for comparison. Fig. 2(a) and (b)
show the Raman spectra of the samples with increasing tempera-
ture from 300 K to 500 K. Obviously, the A1g Raman phonon mode
of both SnSe2 samples exhibited red shift with increasing temper-
ature, as shown in Fig. 2(c). These results were fitted by a linear
equation:
Fig. 2. Temperature-dependent Raman spectra of (a) SnSe2, (b) Al2O3/SnSe2 samples on SiO2/Si substrate from 300 to 500 K, and (c) A1g Raman mode of both samples as a function
of temperature including a linear fit.
u ¼ u0 þ c T D T (1)
[31] Where u0 is the Raman mode frequency at RT, cT is the tem-
perature coefficient, and DT is the temperature difference relative
to 300 K. The measured cT value of A1g mode for the SnSe2 sample
without Al2O3 stress layer is about
0.01757 cm-1/K, which is in
consist with previously reported the value (
0.016 cm
1/K) [32]
and a little higher than the value (0.013 cm
1/K) reported by Taube
et al. [23]. While the cT value of A1g measured for sample with
Al2O3 stress layer is about
0.01270 cm-1/K, much smaller than
that of the SnSe2 sample without Al2O3, signifying a better thermal
stability [33] introduced by Al2O3 stress layer. The peak shift in
Raman modes of SnSe2 with Al2O3 stress layer is smaller than that
observed on sample without Al2O3 due to large difference of the
thermal expansion coefficient between the SnSe2 (1.15  10
4/K)
and Al2O3 (7.5  10
6/K), which will hinders the intrinsic thermal
expansion of the lattice and introduce compressive strain to SnSe2
with increasing temperature. The vibration properties of SnSe2 on
SiO2/Si substrates can be disturbed by the strain introduced owing
to the different thermal expansion coefficients between SnSe2 and
substrate [34,35]. However, this effect tends to weaken with
increasing the film thickness [36]. Therefore, the variation on
thermal coefficient of the samples is attributed to Al2O3 rather than
other environment factors. Similarly, this kind of linear red shift of
Raman peak is also shown in other 2D-materials [5,27,30,34,37].
The thermal conductivity of SnSe2 few layers can be obtained via
taking the laser power-dependent Raman spectroscopy. As shown
in Fig. 3(a), power-dependent Raman spectroscopy of SnSe2 layers
on SiO2/Si substrate have been carried out with a 514 nm Ar þ laser.
During the measurement, the maximum laser power is about
2.5 mW (denoted as P0) and it can be reduced to 0.5P0, 0.1P0, 0.01P0,
and 0.005P0 using an optical attenuator. Due to the local laser
heating effect, obvious frequency red shift of the A1g Raman peak
for SnSe2 few layers was observed with increasing the laser power.
Subsequently the same measurements were carried out for the
sample coated with Al2O3 layer and the results were shown in
Fig. 3(b). Similarly, obvious frequency red shift of the A1g Raman
peak was discovered. In order to compare the degree of red shift for
both samples, the distribution of A1g Raman peak position was
shown in Fig. 3(c) with varying power, where the points were fitted
linearly by equation: Du ¼ cP DP, where cP is the first-order power
dependent coefficient. The cP value for the Al2O3/SnSe2 sample is
about
1.71686 cm
1/W, which (absolute value) is much smaller
than the corresponding value
2.68724 cm
1/W of SnSe2 without
 X. Liu et al. / Journal of Alloys and Compounds 783 (2019) 226e231
Fig. 3. Laser power-dependent Raman spectra of (a) SnSe2, (b) Al2O3/SnSe2 samples on SiO2/Si substrate from 0.05P0 to P0, and (c) A1g Raman mode of both samples as a function of
temperature including a linear fit.
Al2O3 stress layer. However, only part of the laser power was
absorbed by SnSe2 film during the experiments, with a part of laser
was reflected by the air-Al2O3 and Al2O3-SnSe2 interfaces and the
other was transmitted. In fact, the laser reduction factor must be
taken into account by
f ¼ ð1
RÞð1
expð
ahÞÞ
where R is the total reflectance of the air-Al2O3 and Al2O3-SnSe2
interfaces, a is the absorption coefficient of SnSe2 which is about
a ¼ 3:2  104 cm
1 [38], and h is the thickness of SnSe2 film. For the
sample with Al2O3, the reflectance at the Al2O3 surface and the
Al2O3-SnSe2 interface were calculated as 7.73% and 7.05% respec-


tively using R ¼ nn11
n
þn2 with nair ¼ 1, nAl2 O3 ¼ 1:77, nSnSe2 ¼ 3:05
2
[38]. Thus, the laser reduction factor f of the samples with and
without Al2O3 can be calculated to be 0.0585 and 0.0675 respec-
tively. After the calibration that considers the reflectance and ab-
sorption coefficient, is similar to single layer graphene (SLG), the
thermal conductivity has been expressed as
k ¼ f,cT c
1
P ð1=ð2phÞÞ
[39] Where cT and cP are the first temperature and power co-
efficients of the A1g Raman mode. Taking the related values into this
Equation, we obtain the thermal conductivity of SnSe2 without and
with Al2O3 stress layer are about 2.378 W=mK and 3.102 W=mK
respectively, which the former is close to the value reported
[25,40]. The calculations show, the thermal conductivity of few
layer SnSe2 with Al2O3 stress layer is larger than the sample
without Al2O3, which indicates that the covering layer of Al2O3 is
conducive to the heat transfer and diffusion of SnSe2 few layers. The
improvement of the thermal conductivity is mainly attributed to
the e-p interactions at existed the interface charge between Al2O3
and SnSe2 [22,30,41]. There is another possible reason is
compressive strain from the Al2O3 stress layer, which can be modify
the electronic structure of few layer SnSe2. This kind of Al2O3
passivation layer can be suitable for several other 2D materials and
also a similar effect can be obtained by replacing Al2O3 with some
other high-k dielectric oxides.
It is well known that the electron concentration and effective
mass give the main contribution into the thermal conductivity and
it can be written as
ke ¼ p2 Tk2B ne =3m*e ne
229
[42] where T is the temperature, kB is the Boltzmann constant, ne is
the electron concentration, m*e is the effective mass and ne is the
total effective electron collision frequency. The electronic proper-
ties for the four-layers of SnSe2 were investigated by Material
Studio, using the Cambridge Sequential Total Energy Package
(CASTEP) based on density functional theory (DFT) [43] to simulate
(2) the effect of compressive strain on band structure of four-layers of
SnSe2. We use the generalized gradient approximation for the ex-
change and correlation potential, as proposed by Perdew-Burk-
Ernzerhof (PBE) [44], together with the projector augmented
wave potential (PAW) to treat the ion-electron interactions [45].
The plane wave cut-off energy is chosen to be 400 eV, and a
MonkhorstePack k-mesh of 4  4  1 is used to sample the
Brillouin-zone in the structure optimization and total energy
calculation [46]. All the atoms were relaxed to their equilibrium
positions when the total energy changes during the optimization
finally converged to less than 10
4 eV/atom, the force on each atom
in the crystal was converged to 0.003 eV/nm, the stress on each
atom was converged to 0.05 GPa, and the displacement was
converged to 1  10
4 nm. Fig. 4(aed) and (e) exhibit the calcula-
tion of band structures without and with compressive strain from
(3) 1% to 3% for four-layers of SnSe2 and the corresponding measured
electron concentration, respectively. It shows that their band
structure undergoes a significant change as the strain increases
(band gap has been decreased with compressive strain). The
effective mass of the electrons and holes can be calculated through:
, !
v2 E
m* ¼ h2 (5)
v2 k
Subsequently, the 2D-electron concentration (ne ) was estimated
using:

3=2
kB T   
ne ¼ 2 ðme mh Þ3=4 exp
Eg 2kB T (6)
2pħ2
where, Eg is bandgap, ħ is Planck constant. As a result, the 2D-
electron concentration (ne ) is increasing with strain as shown in
Fig. 4(e). This kind of increase on ne implies that k is also increase
according to equation (4). It is well correlating with Raman results.
4. Conclusions
In conclusion, we have reported on thermal conductivity of few
(4)
layers SnSe2 with and without Al2O3 stress layer using temperature
and power dependent Raman studies. With increase in
230 X. Liu et al. / Journal of Alloys and Compounds 783 (2019) 226e231
Fig. 4. Band structures for four-layers of SnSe2 structure at different compressive strain percentages (a) 0%, (b) 1%, (c) 2%, (d) 3%, and (e) the corresponding electron concentration
with compressive strain.
temperature, A1g mode of SnSe2 few layer shows a significant red
shift significantly compared to the other modes. The temperature
coefficients of A1g mode for both SnS2 with and without Al2O3
stress layer were found to be
0.01270 cm-1/K and
0.01757 and
cm
1/K, respectively. The obtained thermal conductivity of SnSe2
with and without Al2O3 stress layer are about 3.102 W=mK and
2.378 W=mK, respectively. The improvement of the thermal con-
ductivity is mainly attributed to the e-p interactions at existed the
interface charge between Al2O3 and SnSe2 and compressive strain
from the Al2O3 layer, which can modify the electronic structure of
thin film SnSe2. The first principle calculation demonstrated that
compressive strain on few layer SnSe2 increases the thermal con-
ductivity due to increasing the electron concentration. This work
will provide a significant direction for the design and fabrication of
SnSe2 based devices.
Acknowledgement
This project is supported by National Natural Science Foundation
of China (61504083, 51872187), Public welfare capacity building in
Guangdong Province (2015A010103016), the Science and Technol-
ogy Foundation of Shenzhen (JCYJ20160226192033020), the Natu-
ral Science Foundation of Guangdong Province (2015A030313559),
The PhD Start-up Fund of Natural Science Foundation of Guangdong
Province (2017A030310424).
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