Controlled Crystal Grain Growth in Mixed Cation-Halide Perovskite by Evaporated Solvent Vapor Recycling Method for...

We developed a new and simple solvent vapor-assisted thermal annealing (VA) procedure which can reduce grain boundaries in a perovskite film for fabricating highly efficient perovskite solar cells (PSCs). By recycling of solvent molecules evaporated from an as-prepared perovskite film as a VA vapor source, named the pot-roast VA (PR-VA) method, finely controlled and reproducible device fabrication was achieved for formamidinium (FA) and methylammonium (MA) mixed cation-halide perovskite (FAPbI₃)_0.85(MAPbBr₃)_0.15. The mixed perovskite was crystallized on a low-temperature prepared brookite TiO₂ mesoporous scaffold. When exposed to very dilute solvent vapor, small grains in the perovskite film gradually unified into large grains, resulting in grain boundaries which were highly reduced and improvement of photovoltaic performance in PSC. PR-VA-treated large grain perovskite absorbers exhibited stable photocurrent-voltage performance with high fill factor and suppressed hysteresis, achieving the best conversion efficiency of 18.5% for a 5 × 5 mm² device and 15.2% for a 1.0 × 1.0 cm² device.