title: Rashba Spin-Orbit Coupling Enhanced Carrier Lifetime in CH₃NH₃PbI₃.
abstract: Organometal halide perovskites are promising solar-cell materials for next-generation photovoltaic applications. The long carrier lifetime and diffusion length of these materials make them very attractive for use in light absorbers and carrier transporters. While these aspects of organometal halide perovskites have attracted the most attention, the consequences of the Rashba effect, driven by strong spin-orbit coupling, on the photovoltaic properties of these materials are largely unexplored. In this work, taking the electronic structure of CH3NH3PbI3 (methylammonium lead iodide) as an example, we propose an intrinsic mechanism for enhanced carrier lifetime in three-dimensional (3D) Rashba materials. On the basis of first-principles calculations and a Rashba spin-orbit model, we demonstrate that the recombination rate is reduced due to the spin-forbidden transition. These results are important for understanding the fundamental physics of organometal halide perovskites and for optimizing and designing the materials with better performance. The proposed mechanism including spin degrees of freedom offers a new paradigm of using 3D Rashba materials for photovoltaic applications.
authors.affiliation: The Makineni Theoretical Laboratories, Department of Chemistry, University of Pennsylvania , Philadelphia, Pennsylvania 19104-6323, United States.
authors.forename: Fan
authors.initials: F
authors.lastname: Zheng
authors.affiliation: The Makineni Theoretical Laboratories, Department of Chemistry, University of Pennsylvania , Philadelphia, Pennsylvania 19104-6323, United States.
authors.forename: Liang Z
authors.initials: LZ
authors.lastname: Tan
authors.affiliation: Geophysical Laboratory Carnegie Institution for Science , Washington, D.C. 20015, United States.
authors.forename: Shi
authors.initials: S
authors.lastname: Liu
authors.affiliation: The Makineni Theoretical Laboratories, Department of Chemistry, University of Pennsylvania , Philadelphia, Pennsylvania 19104-6323, United States.
authors.forename: Andrew M
authors.initials: AM
authors.lastname: Rappe
keywords: Organometal halide perovskite; Rashba spin−orbit coupling; carrier lifetime; electron−phonon coupling; spin-forbidden transition