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    Dependence of CZTS thin film properties and photovoltaic performance on heating rate and sulfurization time
    (Elsevier Science Sa, 2023) Olgar, M. A.; Erkan, S.; Zan, R.
    In this study, effect of heating rate and sulfurization time on the properties of CZTS thin films and their photovoltaic performances was investigated. CZTS layers were prepared by a two-stage technique comprising deposition of precursor films by sputtering on Mo-foil substrates (Mo-foil/ZnS/CuSn/Cu) and a sulfurization process utilizing Rapid Thermal Annealing (RTA) approach. Heating rates and sulfurization times at 550 degrees C were changed to determine the best conditions. CZTS films were characterized by several techniques. All samples showed Cu-poor and Zn-rich chemical composition regardless of the heating rate and annealing time of the sulfurization process. XRD diffraction patterns showed that only kesterite CZTS phase was formed in all samples. Although Raman spectroscopy measurements confirmed formation of kesterite CZTS phase in all samples, forming of Cu2SnS3 (CTS) secondary phase was detected in all films except for the sample prepared utilizing a relatively low heating rate of 1 degrees C/s and 60 s sulfurization time (CZTS-I-60). The largest crystallite size and the less micro strain and dislocation density were also found in this sample. All CZTS thin films displayed dense and compact polycrystalline surface microstructure. Optical characterizations showed that the optical band gaps of the films were in the range of 1.48-1.58 eV. PL emission spectra of the films exhibited transition from conduction band to acceptor/defect levels instead of band-to-band transition. Solar cells were fabricated and the highest Voc and conversion efficiency (4.39%) were achieved employing the film obtained with ramp rate of 1 degrees C/s and the sulfurization time of 60 s, because of better structural properties and purer crystal structure determined for this sample.
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    Fabrication of Cu-rich CZTS thin films by two-stage process: Effect of gas flow-rate in sulfurization process
    (Elsevier, 2021) Olgar, M. A.; Altuntepe, A.; Erkan, S.; Zan, R.
    In this study, CZTS thin films were prepared using a two-stage process consisting of sputter deposition of Cu, Sn and ZnS layers on the glass substrates to form CuSn/ZnS/Cu stacked precursor films followed by sulfurization process under various flow-rate (0, 20, 40, 60, 80, 100 sccm) of Ar+ H-2 mix gas in a tubular furnace. The EDX measurements of the precursor and reacted films are Cu-rich and Zn-rich composition. However, Zn and Sn loss was observed for samples annealed under the flow-rate of gas above the 60 sccm. The XRD pattern of the samples showed diffraction peaks of pure kesterite CZTS structure and the FWHM values extracted from their XRD patterns and W-H plot calculations demonstrated that CZTS-40 thin film had a more desired crystallite size. The Raman spectra of the samples confirmed the formation of CZTS phase for all samples and indicated the formation of some secondary phases such as Cu2SnS3, SnS2, Sn2S3 except for CZTS-40 thin film. All the samples displayed dense and polycrystalline microstructure according to their SEM images. The optical band gap values of CZTS samples showed variation between 1.40 and 1.48 eV. The room-temperature PL spectra of the samples revealed a broad band that had a peak value at around 1.36-1.40 eV that are close to the optical band gap values for prepared CZTS samples. (C) 2021 Elsevier B.V. All rights reserved.
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    Impact of the ZnS layer position in a stacked precursor film on the properties of CZTS films grown on flexible molybdenum substrates
    (Elsevier, 2023) Yagmyrov, A.; Erkan, S.; Basol, B. M.; Zan, R.; Olgar, M. A.
    In the present study, CZTS thin films were prepared by annealing and reaction of Cu-Sn-ZnS precursor layers. First, sputter deposition was carried out on flexible molybdenum (Mo) foil to form Mo-foil/CuSn/ZnS/Cu, Mo-foil/CuSn/Cu/ZnS and Mo-foil/ZnS/CuSn/Cu stacked precursor structures. Annealing process was performed in sulfur atmosphere using Rapid Thermal Processing (RTP) method to obtain kesterite CZTS phase in the reacted layers. All prepared precursors and CZTS thin films displayed Cu-poor and Zn-rich chemical composition, as targeted. XRD patterns of CZTS samples showed that the kesterite phase was obtained in all samples regardless of the stacking order of the precursor films. However, the full width at half maximum (FWHM) values of the (112) preferential peaks extracted from the XRD patterns, and the corresponding structural parameters (crystallite size and microstrain), indicated that the Mo-foil/ZnS/CuSn/Cu precursor structure yielded more promising crystal-line quality. The occurrence of kesterite phase in all samples and existence of low amount of CTS phase were verified by Raman spectroscopy measurements. The CZTS sample prepared employing the Mo-foil/ZnS/CuSn/Cu precursor film structure presented more prominent, homogenous and compact surface microstructure as observed in SEM images. Optical band gap values were found to be in the range of 1.44-1.50 eV. The room temperature photoluminescence (PL) measurements showed that the transitions from the conduction band to intrinsic defect levels dominated the spectra instead of the band-to-band transitions. Electrical characterization of the films showed that Mo-foil/CuSn/ZnS/Cu and Mo-foil/ZnS/CuSn/Cu precursor films yielded lower elec-trical resistivity and higher carrier concentration due to better crystalline quality. Overall, it was seen that the CZTS thin films produced using the Mo-foil/ZnS/CuSn/Cu stacked precursor layers displayed better properties in terms of crystalline quality, surface microstructure, and optical and electrical properties, which are favorable for photovoltaic applications.
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    Integration of single layer graphene into CZTS thin film solar cells
    (Elsevier Science Sa, 2022) Erkan, S.; Yagmyrov, A.; Altuntepe, A.; Zan, R.; Olgar, M. A.
    In this study, CZTS samples were produced on Mo and graphene/Mo coated glass substrates using qua-ternary target. The CZTS thin films deposited by RF magnetron sputtering were annealed using rapid thermal processing (RTP) method in sulphur atmosphere at 500, 525, and 550 degrees C so as to obtain glass/Mo/ CZTS and glass/Mo/graphene/CZTS (g-CZTS) structures. The obtained CZTS and g-CZTS thin films were then characterized by several methods such as EDX, XRD, Raman spectroscopy, SEM etc. The EDX data demon-strated that all CZTS thin films had Cu poor composition regardless of the sulfurization temperature and increasing the temperature led to Sn loss from the films. Diffraction peaks of kesterite CZTS phase were observed in all the samples; additionally, SnS and CuS secondary phases were also observed in CZTS samples annealed at 500 degrees C. The crystallite size of the CZTS thin films were found to be increasing with both increasing annealing temperature and use of graphene film as an inter-layer. The creation of kesterite phase with a very small CTS phase in all the samples were verified by the Raman spectroscopy measurement. The SEM images of the samples indicated that using graphene improves the crystalline quality of the CZTS films and contributes to forming more compact, homogenous and larger crystal structure. The determined optical band gap values varied from 1.41 to 1.44 eV depending on the Sn-content of the samples. The produced solar cells selected from the more promising absorber layers showed that implementing graphene in CZTS cell structure enhanced the conversion efficiency from 2.40% to 3.52% due to improvement of crystalline quality of the absorber layer. (c) 2022 Elsevier B.V. All rights reserved.