A Direct Mapping Approach to Understand Carrier Relaxation Dynamics in Varied Regions of a Polycrystalline Perovskite Film

We developed a direct mapping approach to overlay the image of a polycrystalline perovskite film obtained from the transient absorption microscope (TAM) with that from the scanning electron microscope (SEM). By mapping these imaging data pixel by pixel, we are able to observe the relaxation dynamics of the photo‐generated charge carriers on varied regions of the film. The carrier relaxation dynamics contain a dominated single‐exponential decay component owing to the recombination of charge carriers. The lifetime distribution of charge recombination shows a bimodal feature, for which the rapid and slow distributions are assigned as free and trapped carriers, respectively. The charge recombination was slower in the grain boundary (GB) region than in the grain interior (GI) region. The small grains have longer lifetimes than the large grains for the crystal size smaller than 500 nm. Therefore, GB with retarded charge recombination might play a positive role in a perovskite solar cell. Transient absorption microscope (TAM) images can be mapped one to one with the SEM image in grain boundaries and interiors of a perovskite thin film and find correlation between the morphology and carrier relaxation kinetics.