How the Spacer Influences the Stability of 2D Perovskites?

Abstract Two‐dimensional lead halide perovskites (2D HPs) represent as an emerging class of materials given their tunable optoelectronic properties and long‐term stability in perovskite solar cells. However, the ever‐growing field of optoelectronic devices using 2D HPs requires fundamental understanding of the influence of the spacer on the physiochemical properties and stability of perovskites as well as establish which cation properties are closely related to suppress the halogen ion mobility. This study focuses on investigating the influence of organic spacers with intrinsic properties (e.g., rigidity and flexibility, special groups) and variations of material dimensions on the stability of halogen ions and inorganic frameworks in 2D HPs. It is found that the perovskite structure composed of rigidity molecules owns better stability of halogen ion and inorganic framework than that of flexible molecules. The stability of ions exhibits a negative correlation with the dimensions of perovskite. More importantly, a simple descriptor for measuring the stability of halogen ions in 2D HPs is constructed. By causal discovery algorithms with more physical and chemical significance, the Kappa shape index, number of rotatable bonds, and aromatic carbocycles in organic spacers are identified as causal and important features for the stability of halogen ions in 2D HPs.