Abstract

Flexible Cu2ZnSnSe4 (CZTSe) solar cells gradually attract much attention due to their low-cost, lightweight, and environmentally friendly features. However, the efficiency of flexible CZTSe solar cells obtained through the nonvacuum green electrodeposition process remains sluggish (3.82%), far away from that obtained from other methods (∼10% by magnetron sputtering). Herein, a championed 6.33% efficiency of flexible CZTSe solar cells prepared by the electrodeposition process is achieved through an in situ electrochemical treatment (ET) process. It is found that the ET process drives the formation of a thin MoOx layer, evoking a series of beneficial results, thus accounting for an enhancement in photovoltaic performance. With the ET process, the MoSe2 thickness is compressed and Cu- and Sn-related undesirable defects/secondary phases are inhibited, leading to improved film quality. Additionally, it prolongs the depletion region width and minority lifetime, accelerates the charge separation and collection, relieves the band tails, and favorably reverses the band bending from downward to upward at/near grain boundaries. With these effects, the efficiency increases from 4.21% to 6.33%, far beyond the highest reports on electrodeposited flexible CZTSe solar cells. Our findings offer a promising way to improving Mo foil-based flexible devices and mark a significant breakthrough for the development of electrodeposition-processed flexible CZTSSe-based solar cells.

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