Schottky Defects\nSuppress Nonradiative Recombination\nin CH<sub>3</sub>NH<sub>3</sub>PbI<sub>3</sub> through Charge Localization

Hybrid lead halide perovskites are promising materials\nfor photovoltaic\napplications due to their exceptional optoelectronic properties. Here,\nwe investigate the impact of Schottky defectsspecifically\nPbI<sub>2</sub>(V<sub>PbI<sub>2</sub></sub>) and CH<sub>3</sub>NH<sub>3</sub>I (V<sub>MAI</sub>) vacancieson nonradiative recombination\nin CH<sub>3</sub>NH<sub>3</sub>PbI<sub>3</sub> using time-dependent\ndensity functional theory and nonadiabatic (NA) molecular dynamics.\nOur results reveal that Schottky defects do not alter the fundamental\nbandgap or introduce trap states but instead distort the surrounding\nlattice, localizing the hole distribution. This reduces the spatial\noverlap of electron and hole wave functions, weakening NA coupling\nand increasing intensitieis of high-intensity phonon modes that accelerate\ndephasing. Consequently, nonradiative recombination lifetimes extend\nto 2.1 and 2.6 ns for V<sub>PbI<sub>2</sub></sub> and V<sub>MAI</sub>, respectivelyover double that of pristine CH<sub>3</sub>NH<sub>3</sub>PbI<sub>3</sub>. This work demonstrates the potential\nof Schottky defects to enhance perovskite solar cell performance by\nsuppressing nonradiative recombination.