Molecular Self-Assembly Fabrication and Carrier Dynamics of Stable and Efficient CH3NH3Pb(1-x)SnxI3 Perovskite Solar Cells

The Sn-based perovskite solar cells (PSCs) provide the possibility of swapping the Pb element toward developing toxic-free PSCs. Here, we innovatively employed a molecular self-assembly approach to obtain a series CH3NH3Pb(1-x)SnxI3 (0 <= x <= 1) perovskite thin films with full coverage. The optimized planar CH3NH3Pb0.75Sn0.25I3 PSC with inverted structure was consequently realized with a maximum power conversion efficiency (PCE) over 14%, which displayed a stabilized power output (SPO) over 12% within 200 s at 0.6 V forward bias. Afterward, we investigated the factors that limited the efficiency improvement of hybrid Sn-Pb PSCs, and analyzed the possible reason of the hysteresis effect occurred even in the inverted structure cell. Particularly, the oxidation of hybrid Sn-Pb perovskite thin film was demonstrated to be the main reason that limited its further efficiency improvement. The imbalance of charge transport was intensified, which was associated with the increased hole defect-state density and decreased electron defect-state density after Sn was introduced. This study helps tackle the intractable issue regarding the toxic Pb in perovskite devices and is a step forward toward realizing lead-free PSCs with high stability and efficiency.