Layer Edge States Stabilized by Internal Electric Fields in Two-Dimensional Hybrid Perovskites

Two-dimensional (2D) organic–inorganic hybrid perovskites have been intensively explored in recent years due to their tunable band gaps and exciton binding energies and increased stability with respect to three-dimensional (3D) hybrid perovskites. Experimental observations suggest the existence of localized edge states in 2D hybrid perovskites which facilitate extremely efficient electron–hole dissociation and long carrier lifetimes, while multiple origins for their formation have been proposed. Using first-principles calculations, we demonstrate that layer edge states are stabilized by internal electric fields created by polarized molecular alignment of organic cations in 2D hybrid perovskites when they are two layers or thicker. Our study gives a simple physical explanation of the edge state formation, and facilitating the design and manipulation of layer edge states for optoelectronic applications.