Modeling of Charge Dynamics in Low-Dimensional Halide Perovskites

Hybrid organic−inorganic perovskites (HOPs) have demonstrated an extraordinary potential for clean sustainable energy technologies and low-cost optoelectronic devices. For example, crystalline two-dimensional (2D) layered perovskites demonstrate exceptional properties for light emission and x-ray detection. The photophysics of 2D materials is defined by an interplay of strongly bound excitons and lower-energy states associated with the edges of the perovskite layers. Using molecular dynamics with time-domain density functional theory methods at room temperature, we compare the dominant non-radiative electron-hole recombination and dephasing processes in several low-dimensional lead halide perovskite materials. Our study demonstrates that performance limiting nonradiative carrier recombination processes greatly depends on the electron–phonon interactions induced by structural fluctuations and instantaneous charge localization in these materials. Overall, our results provide insights towards the material design principles for 2D perovskites to strategically tune their optoelectronic properties.