Spin-orbit-coupling-induced band splitting in two-dimensional hybrid organic-inorganic perovskites: Importance of organic cations

Abstract
We investigate how the spin-orbit-coupling-induced lifting of the spin degeneracy depends indirectly on constituting organic motifs in two-dimensional hybrid organic-inorganic perovskites. We examine experimentally synthesized structures using first-principles electronic structure theory. In particular, the effect of the organic spacer cation packing and of the methyl ammonium orientation within the inorganic layer are elucidated. Both the organic spacer packing and subtle changes in methyl ammonium orientations can cause enough distortions of lead iodide octahedral cages to induce the spin splitting. Interestingly, the momentum-independent persistent spin texture splitting rather than the traditional Rashba/Dresselhaus splitting is observed for a structure in which organic spacer molecules are modified with fluorine substitution. Our calculation on these experimentally reported structures highlights the important role of the organic constituents in these hybrid organic inorganic perovskites for the spin splitting.

Citation
Bhattacharya, S., & Kanai, Y. (2023). Spin-orbit-coupling-induced band splitting in two-dimensional hybrid organic-inorganic perovskites: Importance of organic cations. Physical Review Materials, 7(5). https://doi.org/10.1103/physrevmaterials.7.055001