Revealing Charge Transfer Dynamics in Methylammonium Lead Bromide Perovskites via Transient Photoluminescence Characterization.

Abstract

It is an important but difficult issue to identify charge and energy transfer processes in materials where multiple band gaps coexist. Conventional methods using transient absorption and optoelectrical characterization based on devices could not provide a clear picture of transfer dynamics. According to the bimolecular and monomolecular nature of each process, the carrier dynamics is supposed to solve this issue. In this work, we established a novel, convenient and universal strategy based on the calculation of carrier dynamics to distinguish energy/charge transfer and reveal their transfer dynamics in methylammonium lead bromide (MAPbBr3) films with mixing wide-band gap small grains and narrow-band gap large grains. A highly efficient charge transfer process is confirmed with a high negative nonradiative bimolecular recombination coefficient of −2.12 × 10–7 cm–3 s–1, indicating that free carriers within small grains are efficiently transferred from small grains to large grains. As a result, emission from large grains becomes dominant when increasing the photoexcitation intensity. In addition, current-density-dependent electroluminescence results in emission only from large grains, further verifying the charge transfer process. Moreover, it is interesting to find that when decreasing the size of small grains, the charge transfer process is facilitated, leading to an increased nonradiative bimolecular recombination coefficient from −2.12 × 10–7 to −4.01 × 10–7 cm–3 s–1 in large grains. Our work provides a convenient strategy to identify and quantify energy and charge transfer in metal halide perovskites, which can be used to enrich our understanding of perovskite photophysics.