Abstract

Abstract Tin (Sn)‐based perovskites have emerged as promising alternatives to lead (Pb)‐based perovskites in thin‐film photovoltaics due to their comparable properties and reduced toxicity. Strains in perovskites can be tailored to modulate their optoelectronic properties, but mechanisms for the effects of strains on Sn‐based perovskite films and devices are unrevealed and corresponding strain engineering is unexplored. Herein, a strain engineering strategy is developed through incorporating 4‐fluorobenzylammonium halide salts (FBZAX, X = I, Br, Cl) into the perovskite precursor to regulate the strain effects in resultant Sn‐based perovskite films. It is found that a moderate level of compressive strain achieved by FBZABr alleviates the dislocations within perovskites to enhance carrier transport and reduces the defect density to prolong carrier lifetime. These improvements enable a champion efficiency exceeding 14% of Sn‐based perovskite solar cells with excellent operational stability.