High-efficiency and thermally stable FACsPbI3 perovskite photovoltaics.

Abstract

α-FA1-xCsxPbI3 is a promising absorber material for efficient and stable perovskite solar cells (PSCs)1,2. However, the most efficient α-FA1-xCsxPbI3 PSCs require the inclusion of methylammonium chloride (MACl) additive3,4, which generates volatile organic residues (i.e., MA) that limit device stability at elevated temperatures5. To date, the highest certified power-conversion efficiency (PCE) of α-FA1-xCsxPbI3 PSCs without MACl was only ~24% (ref.6,7), and has yet to exhibit any stability advantages. Here, we identify interfacial contact loss caused by the Cs+ accumulation for the conventional α-FA1-xCsxPbI3 PSCs, which deteriorates the device performance and stability. Through in-situ GIWAXS analysis and DFT calculations, we demonstrate an intermediate phase-assisted crystallization pathway enabled by acetate surface coordination to fabricate high-quality α-FA1-xCsxPbI3 film, without using MA-additive. We herein report a certified stabilized power output (SPO) efficiency of 25.94% and a reverse-scanning PCE of 26.64% for α-FA1-xCsxPbI3 PSCs, exhibiting negligible contact losses and enhanced operational stability. The devices retain >95% of their initial PCEs after over 2,000 hours operating at maximum power point under 1 sun, 85 °C, and 60% relative humidity (ISOS-L-3).