Organic ammonium salts are widely used for surface passivation to enhance the photovoltaic (PV) performance and stability of perovskite solar cells (PSCs). However, the protic nature of ammonium units results in the quick degradation of perovskites due to the hydrogen bonding interaction with water molecules. Recently, organo-sulfur compounds have attracted growing interest as passivation layers on three-dimensional perovskites due to their moisture-resistive behavior. Herein, trimethylsulfonium iodide (TMSI), an aprotic S-based organic compound, is employed for surface modification of methylammonium lead iodide-based PSCs to impede moisture penetration, improve charge transfer, and passivate surface defects. The TMSI effectively passivates uncoordinated Pb through Pb···S interactions, and the optimized PSC exhibits a power conversion efficiency (PCE) of 21.03% with an open-circuit voltage of ca. 1.13 V under one-sun illumination, while it reached up to 37.58 and 37.69% under low-intensity indoor illuminations, 1000 and 2000 lx with LED 5000 K, respectively. TMSI-treated cells display enhanced device stability by retaining 92.7% of their initial PCE after 50 days of storage in ambient conditions. This study provides a novel and effective surface reconstruction strategy with aprotic materials to improve PV performance and device stability in PSCs.
Keywords: aprotic materials; low-intensity illumination; nonradiative recombination; stable perovskite solar cells; surface reconstruction.