Exploring the Effects of Ionic Defects on the Stability of CsPbI3 with a Deep Learning Potential

Abstract Inorganic metal halide perovskites, such as CsPbI 3 , have recently drawn extensive attention due to their excellent optical properties and high photoelectric efficiencies. However, the structural instability originating from inherent ionic defects leads to a sharp drop in the photoelectric efficiency, which significantly limits their applications in solar cells. The instability induced by ionic defects remains unresolved due to its complicated reaction process. Herein, to explore the effects of ionic defects on stability, we develop a deep learning potential for a CsPbI 3 ternary system based upon density functional theory (DFT) calculated data for large‐scale molecular dynamics (MD) simulations. By exploring 2.4 million configurations, of which 7,730 structures are used for the training set, the deep learning potential shows an accuracy approaching DFT‐level. Furthermore, MD simulations with a 5,000‐atom system and a one nanosecond timeframe are performed to explore the effects of bulk and surface defects on the stability of CsPbI 3 . This deep learning potential based MD simulation provides solid evidence together with the derived radial distribution functions, simulated diffraction of X‐rays, instability temperature, molecular trajectory, and coordination number for revealing the instability mechanism of CsPbI 3 . Among bulk defects, Cs defects have the most significant influence on the stability of CsPbI 3 with a defect tolerance concentration of 0.32 %, followed by Pb and I defects. With regards to surface defects, Cs defects have the largest impact on the stability of CsPbI 3 when the defect concentration is less than 15 %, whereas Pb defects act play a dominant role for defect concentrations exceeding 20 %. Most importantly, this machine‐learning‐based MD simulation strategy provides a new avenue to explore the ionic defect effects on the stability of perovskite‐like materials, laying a theoretical foundation for the design of stable perovskite materials.