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Sulfurization free spray deposited kesterite Cu2ZnSnS4 absorber layer for photovoltaic applications

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Abstract

The growth of Cu2ZnSnS4 thin films was optimized via sulfurization free chemical spray pyrolysis technique. The sulfate based precursors were used to prepare the CZTS films with varying sulfur contents ranging from 0.08 to 0.12 M to maintain the stoichiometric and avoid sulfurization or H2S gas. The formation of secondary phases on the CZTS films was minimized by controlling the sulfur concentrations with the 2- methoxyethanol solvent. The CZTS kesterite structure with preferential orientation along (112) plane was confirmed by X-Ray diffraction at the sulfur content of 0.12 M. From the Raman analysis, we observed that the addition of the higher sulfur concentration to the precursor solution resulted in a pure phase CZTS peak at 336 cm−1 and reduces the secondary phase segregation. Scanning electron microscopy confirms that higher sulfur concentrations facilitate the growth of CZTS films with larger grain size and achieved Cu-poor and Zn-rich compositions for 0.12 M sulfur concentration from energy dispersive spectra. The UV analysis revealed the maximum absorption peak in the visible region with increasing sulfur concentration and the measurement of the Hall effect affirmed p-type conductivity with carrier concentrations ranging from 1014 to 1016 cm−3 as sulfur concentration increased. The charge transport property of the deposited films was characterized by electrochemical impedance spectroscopy where higher sulfur concentrations resulted in lower internal charge transfer resistance, which is the ideal absorber layer in thin film photovoltaic cells.

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Acknowledgements

One of the authors R. Anne Sarah Christinal would like to thank UGC-DAE Consortium for Scientific Research, Kalpakkam Node, Tamilnadu, India for the collaborative research work and for providing the financial support (CSR-KN/CRS-77/2015-16/804).

Funding

Author R. Anne Sarah Christinal and A. Leo Rajesh have received research funding from UGC-DAE Consortium for Scientific Research, Kalpakkam Node, Tamilnadu, India (CSR-KN/CRS-77/2015–16/804). Author Sujay Chakravarty is the project collaborator from UGC-DAE Consortium for Scientific Research, Kalpakkam Node, Tamilnadu. Author G. Genifer Silvena has no financial interests.

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Authors and Affiliations

  1. Department of Physics, St. Joseph’s College (Autonomous), Affiliated to Bharathidasan University, Tiruchirappalli, 620002, India

    R. Anne Sarah Christinal, G. Genifer Silvena & A. Leo Rajesh

  2. UGC-DAE Consortium for Scientific Research, Kalpakkam, Tamilnadu, 603104, India

    Sujay Chakravarty

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All authors contributed to the study conception and design. RASC: Material preparation, data collection and analysis were performed. RASC: The first draft of the manuscript was written and all other authors analyzed and commented on previous versions of the manuscript. All authors read and approved the final manuscript.

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Correspondence to A. Leo Rajesh.

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Christinal, R.A.S., Silvena, G.G., Chakravarty, S. et al. Sulfurization free spray deposited kesterite Cu2ZnSnS4 absorber layer for photovoltaic applications. J Mater Sci: Mater Electron 33, 22361–22373 (2022). https://doi.org/10.1007/s10854-022-09014-x

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