Rashba Splitting in Two Dimensional Hybrid Perovskite Materials for High Efficient Solar and Heat Energy Harvesting

The physical properties of two-dimensional (2D) lead halide based hybrid perovskites are quite exciting and challenging. Further, the role of organic cations in 2D perovskites is still in a debate. We investigated layered (CH₃(CH₂)₃NH₃)₂(CH₃NH₃)Pb₂I₇ 2D Ruddlesden-Popper (2DRP) phase (M1) and 2D derivative of CH₃NH₃PbI₃ (M2) using density functional theory. The spin orbit coupling mediates the significantly large Rashba splitting energy of 328.5 meV for M2, which is higher than earlier 2D hybrid perovskites. At the picosecond time scale, the dynamical Rashba effect was observed due to organic and inorganic cation dynamics. Two step absorption suggests an indirect optical gap of 2.38 and 2.15 eV for M1 and M2, respectively and solar performance depicts excellent power conversion efficiency of 14.92% and 19.75% for M1 and M2, respectively. For the first time, we explored the thermoelectric properties of 2D hybrid perovskites and perceived high power factor for p-type doping in M2. Our findings suggest that these novel 2D perovskites have the potential to be used in solar and heat energy harvesting.