Li2S doping into CZTSe drives the large improvement of VOC of solar cell

Abstract Alkali metal doping or sulfurization are commonly applied in Cu2ZnSnSe4 (CZTSe) solar cell to improve the open-circuit voltage (VOC). However, alkali metal sulfide affording both alkali metal and sulfur is seldom to be studied, which restrains the development of kesterite solar cells. In this study, we evaporate Li2S during selenization process and hope to provide both alkali metal and sulfur to CZTSe film. The result indicates that Li shows a gradient distribution near the surface of CZTSe film and the content of S is slight. The film quality is improved and the recombination at grain boundaries is decreased after Li2S treatment. Besides, the bandgap of the absorber gets wider. Under the synergy of sulfur and lithium (mainly from lithium), the work function of the treated absorber gets higher and the conduction band offset (CBO) is in the ideal range. Combined with these contributions, the VOC of the champion device treated by Li2S dramatically increase by 120 mV. This study discloses that alkali metal brings the main effect on the performance of the kesterite solar cell even an alkali metal sulfide is evaporated, which deepens the understanding of sulfurization of CZTSe and also promote the progress of kesterite solar cells.