Theory of Hydrogen Migration in Organic–Inorganic Halide Perovskites

Abstract

Solar cells based on organic–inorganic halide perovskites have recently been proven to be remarkably efficient. However, they exhibit hysteresis in their current–voltage curves, and their stability in the presence of water is problematic. Both issues are possibly related to a diffusion of defects in the perovskite material. By using first‐principles calculations based on density functional theory, we study the properties of an important defect in hybrid perovskites—interstitial hydrogen. We show that differently charged defects occupy different crystal sites, which may allow for ionization‐enhanced defect migration following the Bourgoin–Corbett mechanism. Our analysis highlights the structural flexibility of organic–inorganic perovskites: successive iodide displacements, combined with hydrogen bonding, enable proton diffusion with low migration barriers. These findings indicate that hydrogen defects can be mobile and thus highly relevant for the performance of perovskite solar cells.