Manipulated Crystallization and Passivated Defects for Efficient Perovskite Solar Cells via Addition of Ammonium Iodide

Organic-inorganic metal halide perovskite materials have been widely studied as the light absorber for efficient photovoltaics. However, perovskite layers with defective nature are typically prepared with an uncontrollable crystallization process, intrinsically limiting further advance in device performance, and thus require delicate manipulation of crystallization processes and defect density. Here, we demonstrate an ammonium-assisted crystallization of perovskite absorbers during a two-step deposition to fabricate efficient solar cells. Addition of ammonium iodide (NH₄I) is devised to manipulate the nucleation and crystal growth of perovskite, wherein the formation and transition of intermediate x[NH₄⁺]•[PbI₃]^x- enables high-quality perovskite layers with an enlarged grain and reduced defect density. As a result, the perovskite solar cells (PSCs) achieve an average efficiency of 21.36% with a champion efficiency of 22.15% and improved environmental stability over 30 days in ambient conditions with varied relative humidity. These results with addition of NH₄I provide an available and ingenious way to construct high-quality perovskite layers for efficient solar cells and will advance the commercial application of perovskite-based photovoltaics.