Abstract
Ruddlesden–Popper halide perovskites are highly versatile quasi-two-dimensional energy materials with a wide range of tunable optoelectronic properties. Here we use the all-inorganic CsPb n X Ruddlesden–Popper perovskites with X = I, Br, and Cl to systematically model the effect of octahedral tilting distortions on the energy landscape, band gaps, macroscopic polarization, and the emergence of Rashba-/Dresselhaus splitting in these materials. We construct all unique n = 1 and n = 2 structures following from octahedral tilts and use first-principles density functional theory to calculate total energies, polarizations and band structures, backed up by band gap calculations using the GW approach. Our results provide design rules for tailoring structural distortions and band-structure properties in all-inorganic Ruddlesden–Popper perovskites through the interplay of the amplitude, direction, and chemical character of the antiferrodistortive distortion modes contributing to each octahedral tilt pattern. Our work emphasizes that, in contrast to three-dimensional perovskites, polar structures may arise from a combination of octahedral tilts, and Rashba-/Dresselhaus splitting in this class of materials is determined by the direction and Pb-I orbital contribution of the polar distortion mode.
Talk to us
Join us for a 30 min session where you can share your feedback and ask us any queries you have
Disclaimer: All third-party content on this website/platform is and will remain the property of their respective owners and is provided on "as is" basis without any warranties, express or implied. Use of third-party content does not indicate any affiliation, sponsorship with or endorsement by them. Any references to third-party content is to identify the corresponding services and shall be considered fair use under The CopyrightLaw.