Transfer of structural asymmetry in chiral 2D hybrid perovskites and Rashba-Desselhaus spin splitting in inorganic bands*

Translation of structural patterns between different atomic-scale building blocks plays a fundamental role in nature, enabling unique functionalities in contexts ranging from biological systems to synthetic materials. In this work, we demonstrate the transfer of structural asymmetry from layers of chiral molecules to an originally achiral inorganic component in a group of two-dimensional hybrid perovskites with chiral organic cations. Asymmetric hydrogen-bonding interactions, caused by the orientation preference of R-(+)- or S-(−)-1-(1-naphthyl)ethylammonium organic spacer cations, account for the asymmetric distortion pattern of Pb-Br 2D inorganic framework. Spin-orbit coupled hybrid density-functional theory band structure calculations reveal substantial Rashba-Dresselhaus spin-splitting and spin textures of frontier bands associated with the distorted structures, potentially useful for control of spin properties of carriers in devices.