Mapping the Energy Carrier Diffusion Tensor in Perovskite Semiconductors.

Abstract

Understanding energy transport in semiconductors is critical for the design of electronic and optoelectronic devices. Semiconductor material properties, such as charge carrier mobility or diffusion length, are commonly measured in bulk crystals and determined using models that describe transport behavior in homogeneous media, where structural boundary effects are minimal. However, most emerging semiconductors exhibit nano- and microscale heterogeneity. Therefore, experimental techniques with high spatial resolution paired with models that capture anisotropy and domain boundary behavior are needed. We develop a diffusion tensor-based framework to analyze experimental photoluminescence (PL) diffusion maps accounting for material nano- and microstructure. Specifically, we quantify both carrier transport and recombination in single crystal and polycrystalline lead halide perovskites by globally fitting diffusion maps with spatial, temporal, and PL intensity data. We reveal a 29% difference in principal diffusion coefficients and alignment between electronically coupled grains for CH₃NH₃PbI₃ polycrystalline films. This framework allows for understanding and optimizing anisotropic energy transport in heterogeneous materials.