Density functional theory study of two-dimensional hybrid organic-inorganic perovskites: frontier level alignment and chirality-induced spin splitting

Abstract Perovskites are a class of semiconductors initially recognized for their exceptional efficiency in solar cell applications. Subsequent research has revealed their diverse and attractive optoelectronic properties. Over the last decades, molecule-level engineering attempts toward the original three-dimensional (“3D”) perovskites have led to the emergence of two-dimensional (“2D”) layered crystals and introduced extensive compositional, structural, and electronic tunability through the incorporation of various organic cations to form hybrid perovskite systems. Consequently, we concentrated on the theoretical investigation of innovative and complex 2D hybrid organic-inorganic perovskites using density functional theory (DFT). A DFT-based simulation protocol has been developed, enabling the efficient simulation of hybrid perovskite systems and providing accurate explanations and predictions of various experimental phenomena. This account article summarizes the recent in-depth DFT study of the structural, electronic, and spin-related properties of 2D hybrid organic-inorganic perovskites.