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Cu2ZnSn(S, Se)4 (CZTSSe) is one of most competitive photovoltaic materialsfor its earth-abundant reserves, environmental friendliness, and highstability.The quality of CZTSSe absorber determines the power-conversionefficiency (PCE) of CZTSSe solar cells. The absorber's quality lies onpost-selenization process, which is the reaction of Cu-Zn-Sn precursor andselenium vapor. And the post-selenization is dependent on various factors (e.g.temperature, precursor composition, reaction atmosphere, etc).However,synergistic regulation of these factors cannot be realized under a widely-usedsingle-temperature zone selenization condition.Here, in our dual-temperaturezone selenization scheme, a solid-liquid and solid-gas (solid precursor andliquid/gas phase Se) synergistic reaction strategy has been developed toprecisely regulate the selenization. Pre-deposited excess liquid Se provideshigh Se chemical potential to drive a direct and fast formation of the CZTSSephase, significantly reducing the amount of binary and ternary compounds withinphase evolution. And organics removal can be accomplished via a synergisticoptimization of Se condensation and subsequent volatilization. We achieve ahigh-performance CZTSSe solar cell with a remarkable PCE of 13.6%, and thehighest large-area PCE of 12.0% (over 1cm2). Our strategy will provide a newidea for further improving efficiency of CZTSSe solar cells via phase evolutionregulation, and also for other complicated multi-compound synthesis.

Controlling selenization equilibrium enables high-quality Cu2ZnSn(S, Se)4 absorbers for efficient solar cells