Surface Sn(IV) Hydrolysis Improves Inorganic Sn–Pb Perovskite Solar Cells

Cesium tin-lead (Sn-Pb) perovskites are exceptional for their combined capabilities in unlocking ideal bandgaps for solar cells and mitigating the stability issue faced by their hybrid organic-inorganic counterparts. But the development of high-performance solar cells using these materials is retarded by their inherent high density of detrimental Sn(IV) defects. Herein, we demonstrate a sequential surface treatment method, which entails a Sn(II) halide treatment to displace the buried Sn(IV) ions underneath the film surface, followed by a H2O treatment to hydrolyze the displaced Sn(IV) ions. The surface treatment induces chemical and microstructural reconstructions that significantly improve the optoelectronic properties and stability of perovskites. As a result, a power conversion efficiency of 16.79% and a T90 stability of 958 h are achieved, topping all previously reported performance parameters for inorganic Sn-Pb PSCs. This achievement further shortens the performance gap between all-inorganic and hybrid organic-inorganic Sn-Pb PSCs with sub-1.4 eV bandgaps. © 2023 American Chemical Society.