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Keywords: Cu2SnS3 thin lms, Porous silicon, crystal structure, solar cell, e ciency
DOI: https://doi.org/10.21203/rs.3.rs-3040611/v1
License: This work is licensed under a Creative Commons Attribution 4.0 International License.
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Abstract
In this study, an n-type silicon wafer's diode laser (red-650nm) is used to generate 30 mW n-
type porous silicon by illuminating the surface of n-type substrates. To obtain a 0.785 cm2
etched area, a double-concave lens was used. Cu2SnS3 (CTS) thin films on glass substrates
were deposited using a low-cost spin coating process. X-ray diffraction was used to study the
structural properties of a Cu2SnS3 thin film. The films feature a polycrystalline tetragonal
structure with a preferential orientation along the (112) plane, according to the researchers. As
the annealing temperature was raised, the size of the crystallites grew larger. At temperatures
of 200, 250, and 300ᵒC, FE-SEM pictures revealed that Cu2SnS3's surface was denser, with
fewer voids. The grain size grows larger, and the surface morphology becomes rougher,
according to AFM. As the annealing temperature was increased, the band gap of Cu2SnS3 thin
films fell from 2-1.65 eV. With a high absorption coefficient of 104 cm-1, CTS thin films show
a direct optical band gap. The p-type character of the developed CTS films is confirmed by
hall measurements. For a thin film annealed at 300 oC, the carrier concentration, resistivity,
and mobility are 1.231×1023 cm-3, 9.987 ×10-7 Ω cm and 50.78cm2 V-1 S-1, respectively. The
conversion efficiency of Al/Cu2SnS3/n-PSi/Al was 3.7 percent at 300 oC, according to the
findings.
Keywords: Cu2SnS3 thin films, Porous silicon, crystal structure, solar cell, efficiency.
1. Introduction
Photovoltaic cells convert solar energy into direct current electricity by using p and n type
semiconductors. Typically, silicon-based solid-state junction devices have assumed control of
this sector, owing to semiconductor industry experience and the availability of materials based
on it [1]. The high cost of fabrication is one of the key factors preventing the widespread use
of solar cells. The researchers' current focus is on manufacturing photovoltaic devices, where
they are working to develop cost-effective and ecologically beneficial methods. Choosing
appropriate materials for photovoltaic applications is a huge problem, as the quality of
materials plays a significant influence in determining the efficiency of power conversion. Cu–
Sn–S is one of the materials that has a lot of potential for photovoltaic applications [2, 3].
Porous silicon (PS) is a hydride terminated silicon with a high surface area shape whose
effective room temperature luminescence has piqued attention for a wide range of applications.
The first irritant was in the 1990s, and it was about the potential application of light-emitting
silicon in opto-electronic devices that could readily be coupled with current silicon-based
technology [4]. Various (PS) applications in mono-crystalline and multi-crystalline silicon
solar cells have been examined by authors throughout the last decades, and can be utilized as
an antireflection coating due to the refractive index, which is heavily dependent on porosity
[5]. Apart from these characteristics, PS considers silicon solar cell technology to be an ideal
material. This is due to the porous nature of the material, which decreases reflection losses
while providing a large active surface for light interaction with semiconductors [4, 6]. Cu2SnS3
(CTS) compound has garnered increasing attention in recent years among various materials,
reflecting a good potential and an acceptable materials that may be employed as thin film solar
cells due to their high absorption coefficient and superior direct band-gap for solar energy
conversion. The (CTS) exhibit p-type conductivity, a high absorption coefficient (> 104 cm-1)
and a direct band-gap that is optimum. Because CTS are non-toxic and abundant on the planet,
they could be used as absorber materials in solar cells. The absorbent layer, which plays a
significant role in determining the efficiency of solar cells [7, 8]. Sulfurization [9], chemical
spray pyrolysis [10], spin coating [11], chemical bath deposition [12], and solid-state reaction
[8] are among of the processes used to create CTS thin films in vacuum and nonvacuum. In
this study, a tetragonal CTS thin film was made from a precursor solution utilizing a low-cost
spin coating process. This method is useful because it is versatile and cost-efficient, and it may
be used to make Copper Tin Sulphide thin films. Copper Tin Sulphide thin films were
deposited on soda-lime glass at various substrate temperatures in order to build a low-cost and
environmentally acceptable solar cell.
2 -Experimental
2.1. Fabrication of porous silicon
To be suitable with the dimensions of the holder, pieces of porous silicon wafers were sliced
into (1.5×1.5) cm2 squares. Before beginning, the samples were cleaned with an alcohol
solution, and an ultrasonic bath was used to remove any impurities or residuals from their
surface. The substrates were etched with 10% hydrogen peroxide for 5 minutes to remove all
native oxide. Photo-electrochemical etching was used to create a thin, homogeneous layer of
PSi on the frontal surface of the material (PEC). When a sufficiently bright photon shines on
the n-silicon substrate surface, holes can be produced in the bulk. A diode laser (red-650 nm)
with a power of 30 mW illuminates the surface of n-type substrates. To obtain an etched area
of 0.785 cm2, a double-concave lens was used, as shown in fig. 1.
3. Device Fabrication
The preparation of p-n junction solar cells can enhance the conversion efficiency of porous
silicon cells and the preparation of p-n junction solar cells can improve the conversion
efficiency of porous silicon cells. Figure 2 depicts the Al/Cu2SnS3/n-PSi/Al p-n junction device
structure. p-n junction solar cells were created using porous silicon solar cells as bottom cells.
PSi cells were created using a photochemical etching process to create a Cu2SnS3 layer, which
was subsequently spun coated onto the upper PSi substrate at 300°C. This experiment
employed n-type silicon. On the backside of PSi cells, an aluminum layer was deposited using
a thermal evaporation process. Finally, wires were utilized to connect the Al electrodes to the
Keithley source in order to conduct the efficiency test.
The nanocrystalline nature of the films is shown by the broad XRD peaks, and when the
annealing temperature increased, all Cu2SnS3 thin films improved in order crystallinity. Similar
behavior was observed by Z. T. Khodier et al. for Cu2ZnSnS4 thin films [14]. The strongest peak
is found at 2θ ~ 28.5º, often known as the (112) plane. These spectra were used to calculate
structural parameters such as diffraction angle (2θ), lattice spacing (d), full width at half
maximum (FWHM), and phases identified long with (hkl) planes, which are listed in table 1.
The average crystallite size was calculated using the Scherrer equation [15].
0.9 𝜆
𝐷= (1)
𝛽 𝑐𝑜𝑠θ
where, θ is the Bragg diffraction angle, β is the full width at half maximum (FWHM). The
dislocation density (δ) (crystal defect) is an important parameter, defined as the length of the
dislocation lines per unit volume, which is a measure of the number of defects and vacancies
in the crystal [16].
1
𝛿= (2)
𝐷2
The material's micro strain (ε) was calculate using the following formula [16, 17].
𝛽 𝑐𝑜𝑠𝜃
𝜀= (3)
4
With increasing the temperature from 200 to 300 °C, the average crystallite size (D) of Cu2SnS3
thin films increased from 14.37 to 21.56 nm (Table 2). We notice that when the annealing
temperature rises, the intensity of the (112) orientation improves significantly, whereas other
peaks lose crystallinity. Thus, we note that as the substrate temperature rises, the peak (112)
becomes dominant, with sharper and more powerful peaks appearing, which could be related
to particle grain development [18]. Furthermore, the FWHM of this peak shrinks, indicating
enhanced crystallinity (Table 1, 2 and Fig. 3).
Fig. 4. Dependence of dislocation density (δ) and micro strain (ε) on substrate temperature of Cu2SnS3 thin films.
As the substrate temperature rises, the dislocation density (δ) and micro strain (ε) decrease,
with thin films deposited at 300 °C exhibiting the lowest dislocation density and micro strain.
This could be owing to increased grain growth (Fig. 4). Improved crystallinity could be due to
the reduction in micro-strain [19].
(a) (b)
Fig. 5 (a) FE-SEM image and (b) particle size distribution histogram of Cu2SnS3 thin films annealed at 200 °C.
Figure 6 shows Cu2SnS3 thin films deposited at 250°C (a and b). We noted aggregation of tiny
nanoparticles in a polyhedral shape in this image, with diameters ranging from 40.85 to 125.16
nm and an average diameter of 74.66 nm.
(a) (b)
Fig. 6 (a) FE-SEM image and (b) particle size distribution histogram of Cu2SnS3 thin films annealed at 250 °C.
(a) (b)
Fig. 7 (a) FE-SEM image and (b) particle size distribution histogram of Cu2SnS3 thin films annealed at 300 °C.
The clusters of these particles developed into larger grains, as seen in FE-SEM images, and
this expansion may be attributed to a rise in the crystallinity of Cu2SnS3 thin films. This trend
is consistent with the above-mentioned crystallite size increase as seen in the XRD section.
Harshad D. Shelke et al. [4] described a similar pattern of activity.
Table 3: AFM parameters (Average Diameter, roughness and RMS) of Cu2SnS3 thin films at different
substrate temperatures.
Temperature °C Average Diameter (nm) Roughness Average (nm) RMS (nm)
200 21.42 5.869 7.411
250 27.68 6.330 7.742
300 39.15 15.56 17.71
Fig. 8 AFM images of Cu2SnS3 thin films at different substrate temperatures (a) 200, (b) 250 and (c) 300°C.
5. Optical properties
Fig.9 (a and b) shows the optical absorbance spectra and absorption coefficient (α) of Cu2SnS3
thin films respectively at various annealing temperatures, which was obtained using UV-
Visible spectrophotometer (type Shimadzu, UV1800) in the wavelength range 300–900 nm.
We note that when the temperature rises, the absorbance spectrum of thin films increases, with
visible absorption edges. This suggests that increasing the annealing temperature could
improve the crystallinity of CTS thin films [21].
Fig. 9. Variation of (a) absorbance spectra and absorption coefficient (α) of Cu2SnS3 thin films at different
annealing temperatures
The absorption coefficient (α) of Cu2SnS3 thin films associated to the incident photon energy
(hν) was calculated using the following equation [22].
𝐴
𝛼 = 2.303 (4)
𝑡
where A is the absorption and t the thickness of the film (cm). Fig.9 (b) depicts the difference
curves of optical absorption coefficient against the photo energy of the CTS thin films at
various temperature. One can clearly see, the absorption coefficient reaches values (α) above
104 cm-1 in the visible region at higher photon energy. Indicating, the Cu2SnS3 thin films have
higher values of absorption coefficient as the substrate temperature rises, which could be
attributable to an increase in the crystallinity of the thin film where A is the absorption and t
the thickness of the film (cm).
The differential curves of optical absorption coefficient vs photo energy of CTS thin films at
different temperatures are shown in Fig.9 (b). At increasing photon energies, the absorption
coefficient in the visible area reaches values (α) above 104 cm-1. As the substrate temperature
rises, the absorbance coefficient of Cu2SnS3 thin films increases, possibly due to increased
crystallinity [23]. For solar cell applications, these sorption coefficient values are adequate [7].
The direct optical band-gap energy (Eg) of CTS thin films was obtained via extrapolating the
linear absorption (αhv) edge part-curve to the intercept with horizontal axis (photon energy)
using the following expression [22].
(𝛼ℎ𝑣) = 𝑘(ℎ𝑣 − 𝐸𝑔)𝑛 (5)
where k is a constant depending on the structure of the material, while the exponent (n) depends
on the type of transition (n=1/2) for direct transitions. The decrease in optical band gap energy
of the CTS thin films as a function of increasing temperature can be noticed in Fig 10 (a-c).
The improvement in crystallinity may be responsible for the decrease in optical band gap. Biren
Patel et al. [23]. have corroborated this outcome. The reduction in grain boundaries due to
improved crystalline quality, on the other hand, can reduce electron scattering. The electronic
transition from valence band to conduction band increases easier, leading in a drop in Eg. For
high-efficiency thin-film solar cells, such a perfect band-gap is advantageous [24].
Fig. 10. Variation of direct optical band-gap value of Cu2SnS3 thin films at different annealing temperatures (a)
200, (b) 250 and (c) 300°C.
6. Hall Effect
The Hall measurements were carried out at room temperature utilizing the HMS-3000, VER
3.5 offered by the American company in order to evaluate the electrical properties of the
produced CTS thin films (ECOPIA). Table 4 shows the electrical properties of Cu2SnS3 (CTS)
thin films deposited at temperatures of 200, 250, and 300 °C, including carrier density, hall
coefficient, conductivity, resistivity, and mobility. The Hall effect tests demonstrate that all
CTS thin films have p-type conductivity, with hole mobility increasing from 13.82 to -50.78
cm2V-1S-1 as the substrate temperature rises.
Table 4: Electrical properties of Cu2SnS3 thin films at different annealing temperatures.
Hall
T Carrier Conductivity Resistivity Mobility Type of
sample Coefficient
(ᵒC) density (cm-3) (Ω.cm)-1 (Ω.cm) (cm2V-1S-1) conductivity
(cm3 C-1)
200 1.415×1011 4.410×107 3.133×10-7 3.192×106 13.82 p
Cu2SnS3 250 7.494×10 11
8.329×10 6
4.111×10 -6
2.433×10 5
34.24 P
300 1.231×1023 5. 071×10-5 1. 001×106 9.987×10-7 50.78 P
The carrier concentration, resistivity and mobility are 1.231×1023 cm-3, 9.987×10-7 Ω cm and
50.78 cm2 V-1 S-1 respectively. As the annealing temperatures rise, the increasing crystalline
size due to high crystalline quality (Ostwald ripening effect) causes a decrease in grain
boundaries and an increase in Hall mobility, which reduces the resistivity from 3.192×106-
9.987×10-7 Ω.cm correspondingly. In comparison to the other samples, the sample deposited
at a substrate temperature of 300 °C has the lowest resistance and the highest
mobility. Furthermore, our findings show that CTS thin films produced at high temperatures
are better suited for solar cell applications [24, 25].
7. (J-V) characterization
In order to manufacture full photovoltaic devices, p-n junction solar cells were created as
absorber layers. The solar cell (SC) (J-V) curve for Cu2SnS3/n-PSi/Al p-n junction device is
shown in Fig.11. Using a Keithley 2400 source meter and a light source of 10 mW/m2, the
current–voltage (I-V) characteristics of Al/ Cu2SnS3/n-PSi/Al tandem solar cells were studied.
The fill factor (FF) was determined using the following equation [25] based on the (I–V) curve.
𝐽𝑚𝑎𝑥 . 𝑉𝑚𝑎𝑥 𝑃𝑚𝑎𝑥
𝐅. 𝐅 = = (6)
𝐽𝑆𝐶 . 𝑉𝑂𝐶 𝐽𝑆𝐶 . 𝑉𝑂𝐶
Where 𝑃𝑚𝑎𝑥 is the maximum power, 𝐽𝑆𝐶 and 𝑉𝑂𝐶 are the density of short-circuit photocurrent
and the open-circuit photo voltage respectively.
The overall power conversion efficiency (ɳ) performance can be evaluated using the following
formula [26].
𝐽max . 𝑉𝑚𝑎𝑥 𝑃max 𝐽𝑆𝐶 . 𝑉𝑂𝐶 F. F
ɳ (%) = = = × 100 % (7)
𝑃in 𝑃in 𝑃in
where 𝑃in is the intensity of the incident light (mW cm− 2 )
According to the photo-electric response characterization, the cell has an open-circuit voltage
(Voc) of 28 mV, a short-circuit current density (Jsc) of 0.76×10-2 mA/cm2, a fill factor (F.F %)
of 0.176 %, and an efficiency (ɳ) of 3.7%, (table 5). Figure 11 shows how the p-n junction
solar cells that have been produced can be used as light absorption layers. The open circuit
voltage and fill factor were both low, which is a significant problem with CTS solar cells.
Rather, the VOC was low in comparison to the band gap energy, which is a common issue with
CTS devices. Carrier recombination at grain boundaries may be linked to the device's
efficiency (3.7 percent) efficiency (PCE). The increase in grain size suggests that grain borders,
which serve as carrier recombination sites, have shrunk. The number of shunt pathways and
the degree of carrier recombination associated with grain borders in polycrystalline thin films
with identical defect density within the grains will be reduced for films with greater grain sizes.
Fig. 11. (J-V) curve of solar cell (SC) for Al/Cu2SnS3/ n-PSi/Al
8. Conclusion
To deposit thin CTS films, a spin coating method with solution processible was utilized. The
effect of temperature on the structural, morphological, optical, and electrical properties of CTS
thin films has been investigated. CTS has a tetragonal nanocrystalline structure, according to
XRD measurements. The crystallinity of the film increases as the temperature of the film rises.
With polyhedral and spherical form aggregation of small nanoparticles, the thin films surface
morphology showed a significant fluctuation due to the annealing temperature. The optical
band gap shrinks as the temperature of the CTS film rises, indicating that crystallinity
improves. The absorption coefficient, ideal band gap, carrier concentration, mobility, and
shape of the absorption layer all influence the solar cell's conversion efficiency. The
absorbance coefficient of a CTS thin film annealed at 300 °C was (>10-4cm-1), and the band
gap was excellent (1.65 eV). Hall measurements revealed that the films are p-type, and all of
the deposited films had higher carrier concentrations, greater mobility, and lower resistance.
As a result, CTS thin films could be used as an absorbent layer in thin-film solar cells.
Acknowledgments
The authors are grateful to the Department of Physics-Postgraduate Laboratories, College of
Science, University of Diyala, and Ministry of Science and Technology Laboratories-Iraq for
providing the characterization facility.
Author Contribution Layth A. Saleh: Data collection, Analysis and interpretation of results.
Ziad T. Khodair: Investigation, Software and Writing. Ali M. Mohammad: Methodology,
Funding and Supervision, Final revised. Tahseen H. Mubarak: Validation and Original Draft.
Anees A. Khadom: Formal analysis and Editing.
Funding The work was financially supported by the Researchers, Garmian University, Kalar,
Iraq.
Data availability This manuscript contains all data generated or analyzed during the
investigation.
Declarations
Compliance with ethical standards No, all testing is conducted in this study as per ASTM
standards.
Consent to Participate The authors declare no objection to consent to participate.
Consent for Publication The authors declare no objection to consent to publication.
Research Involving Human Participants and/or Animals Not applicable.
Informed Consent Informed consent was obtained from all individual participants included
in the study.
Conflict of Interest The authors declare no conflict of interest.
Competing Interests The authors declare no competing interests
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