Impact of Interfaces and Laser Repetition Rate on Photocarrier Dynamics in Lead Halide Perovskites

We studied charge carrier recombination in methylammonium lead iodide (MAPbI₃) perovskite and the impact of interfaces on the charge carrier lifetime using time-resolved photoluminescence. Pristine films and those covered with organic electron and hole transport materials (ETM and HTM) were investigated at various laser repetition rates ranging from 10 kHz to 10 MHz in order to separate the bulk and interface-affected recombination. We revealed two different components in the PL decay. The fast component (shorter than 300 ns) is assigned to interfacial processes and the slow one to bulk recombination. A high repetition pulse train was shown to shorten PL decay in pristine perovskite while significantly prolonging the photocarrier lifetime in MAPbI₃ covered by TMs. This effect can be qualitatively explained with a kinetic model taking interface traps into account. We demonstrate a significant influence of the excitation repetition rate on photocarrier lifetime, which should be considered when studying charge carrier dynamics in perovskites.