Point defect-mediated hot carrier relaxation dynamics of lead-free FASnI3 perovskites

In search of a promising optoelectronic performance, we herein investigated the hot carrier relaxation dynamics of a lead-free cubic phased bulk formamidinium tin triiodide (FASnI₃) perovskite. To gain detailed theoretical insights, we should estimate the carrier relaxation dynamics of this pristine perovskite. To control the dynamics, point defects like central tin (Sn), iodine(I) anions, and formamidinium (FA) cations were introduced. With the iodine vacancy in the FASnI₃ perovskite, the system seems to be unstable at room temperature, whereas the other three types of FASnI₃ perovskites (pristine, Sn vacancy, and FA vacancy) are significantly stable at 300 K having semiconducting nature and excellent optical absorption in the UV-visible range. The computed electron-hole recombination time for the pristine system is 3.9 nanoseconds, which is in good agreement with the experimental investigation. The exciton relaxation processes in Sn and FA vacancy perovskites require 2.8 and 4.8 nanoseconds, respectively. These variations in the hot carrier relaxation dynamics processes are caused by the generation of significant changes in non-adiabatic coupling between energy levels, electron-phonon coupling, and quantum decoherence in different point defect analogous systems. The results presented here offer deeper insight into the temperature-dependent carrier relaxation dynamics of FASnI₃ perovskites and thus open up opportunities for future exploration of their optoelectronic properties.