Abstract
In recent years, Cu2ZnSn(S1-xSex)4 (CZTSSe) prepared by a two-step process using metal precursors has been reported to exhibit a relatively high power conversion efficiency, and a high efficiency of 12.5% by two-step process contained via sputtering method was recently confirmed by our group. In this study, we proposed formation mechanisms for the CZTSSe double layer, voids and ZnSSe layer, which were observed in the CZTSSe using metal precursor. Due to the persistent dezincification from the metal precursors and preferential reaction between the Zn and chalcogens such as S and Se, almost all Zn is consumed to form the ZnSSe layer; as a result, large voids are produced first under the ZnSSe layer. Cu2Se and SnSe are grown on the ZnSSe layer via migration of the Cu and Sn through the grain boundaries of the ZnSSe layer. Thus, additional small voids are expected to form due to the mass transfer of Cu and Sn. Because of the preferentially formed ZnSSe layer and the chalcogenation of Cu and Sn after the mass transfer, a CZTSSe double layer can be formed, and ZnSSe can exist between these CZTSSe layers. Finally, we propose a method based on the formation mechanism to control the voids and secondary phases, which affect the fill factor and output current.
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