Influence of chemical composition on the properties of directly coevaporated Cu–Zn–Sn–S-based thin films and solar cells

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<jats:title>Abstract</jats:title> <jats:p>The influence of the Zn/Sn atomic ratio on the properties of the Cu–Zn–Sn–S-based film microstructure and solar cells was investigated. In addition to a small amount of SnS, Cu<jats:sub>2</jats:sub>SnS<jats:sub>3</jats:sub>, and ZnS coexisted in Zn-poor (Zn/Sn < 1) films, while Cu<jats:sub>2</jats:sub>ZnSnS<jats:sub>4</jats:sub> (CZTS) was not formed. In contrast, the direct growth of a highly crystalline kesterite CZTS phase was evident in Zn-rich (Zn/Sn > 1) films, in which a ZnS phase was inevitably formed as a secondary phase. Despite its coexistence with CZTS in highly Zn-rich films, excess ZnS had a negligible influence on the crystalline quality of CZTS. Solar cells fabricated with more highly Zn-rich films exhibited better device properties, indicating that the ZnS inevitably present in these films positively impacted cell performance, especially the open-circuit voltage and fill factor. The best cell (Zn/Sn = 1.6) yielded an efficiency of 4.61%. The possible ZnS passivation of microstructural defects in CZTS cells is also discussed.</jats:p>

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