Visualizing Buried Local Carrier Diffusion in Halide Perovskite Crystals via Two-Photon Microscopy

Halide perovskites have shown great potential for light emission and photovoltaic applications due to their remarkable electronic properties. Although the device performances are promising, they are still limited by microscale heterogeneities in their photophysical properties. Here, we study the impact of these heterogeneities on the diffusion of charge carriers, which are processes crucial for efficient collection of charges in light-harvesting devices. A photoluminescence tomography technique is developed in a confocal microscope using one- and two-photon excitation to distinguish between local surface and bulk diffusion of charge carriers in methylammonium lead bromide single crystals. We observe a large dispersion of local diffusion coefficients with values between 0.3 and 2 cm²·s^-1 depending on the trap density and the morphological environment - a distribution that would be missed from analogous macroscopic or surface measurements. This work reveals a new framework to understand diffusion pathways, which are extremely sensitive to local properties and buried defects.