Pure-Phase, Large-Grained Wide-Band-Gap Perovskite Films for High-Efficiency, Four-Terminal Perovskite/Silicon Tandem Solar Cells

High-quality, stable perovskite films with a wide band gap between 1.65 and 1.80 eV are highly suitable for efficient and cost-competitive silicon-based tandem solar cells. Herein, we demonstrate that the combined strategies of the Pb(SCN)₂ additive and air annealing can enable the Cs_0.22FA_0.78Pb(I_0.85Br_0.15)₃ films with a wide band gap of 1.65 eV and favored properties including pure composition, high crystallinity, micro-sized grains, and reduced defects. With these desired films, the average efficiencies of semitransparent perovskite solar cells (PSCs) are boosted from (18.13 ± 0.31) to (20.35 ± 0.28)%. Further, the semitransparent PSC is used to assemble the four-terminal perovskite/TOPCon tandem solar cell. Benefiting from its excellent performance and preferred optical properties, the obtained tandem solar cell yields a milestone efficiency of 30.32%.