(385c) Impact of Crystalline Structure on Photodynamics in Halide Perovskites

Metal-halide perovskite (MHP) is a promising material for the next-generation solar cells and/or light emitting diodes (LEDs) due to its outstanding photophysical properties. Of particular, the perovskite structure consists of corner-shared octahedra, of which rotation (i.e., octahedral tilting) yields various polymorphic phases. For example, the CsPbBr₃, which is one of the most promising materials for the LED application, has orthorhombic, tetragonal, and cubic phases, and the polymorphic phase is known to be controlled via nanostructuring. In this study, we investigate the impact of crystalline structure on photodynamics in the MHPs. Using time-domain ab-initio molecular dynamics simulation, we compare the carrier dynamics in different structural phases of CsPbBr₃, and unravel how the lattice vibration of the different structural phase-changes the carrier lifetime. Throughout our current theoretical study, we anticipate providing a mechanistic guideline to enhance the quantum yield of the MHPs via nanostructuring, which will offer a stepping stone towards a successful deployment of MHPs for optoelectronic applications.