2021/10/31 by Cecilia Vona, Vona, Cecilia, Dmitrii Nabok +3 · 2 citations
Engineering · Physics and Astronomy · #Perovskite Materials and Applications #Semiconductor Quantum Structures and Devices #cond-mat.mtrl-sci
paper · pdf · doi:10.48550/arxiv.2111.00503
arxiv created 2021/10/31 · arxiv updated 2021/11/02
Organic-inorganic metal halide perovskites (HaPs) are intensively studied for their light-harvesting properties. Owing to the interplay between strong electron-electron interaction and spin-orbit coupling (SOC), their quantitative theoretical description is still a challenge as evidenced by the wide variety of results available in literature. Here, various methodologies for computing their electronic structure are evaluated, also accounting for SOC. More specific, the GW approach as well as variants of the hybrid functionals PBE0 and HSE are at the center of our investigations. For both functionals, we explore methods to determine the mixing parameter α, and for HSE, we investigate the impact of the screening-parameter ω. An extensive investigation of PbI2, a precursor of many HaPs, leads to the conclusion that hybrid functionals with α tuned by the density-based mixing method are most suitable for obtaining band gaps comparable to G0W0 results. Moreover, this methodology is transferable to CsPbI3, and the same behaviour is expected for the entire family of lead-iodine perovskites.