Unveiling Local Current Behavior and Manipulating Grain Homogenization of Perovskite Films for Efficient Solar Cells.

Achieving high power conversion efficiency in perovskite solar cells (PSCs) heavily relies on fabricating homogeneous perovskite films. However, understanding microscopic-scale properties such as current generation and open-circuit voltage within perovskite crystals has been challenging due to difficulties in quantifying intragrain behavior. In this study, the local current intensity within state-of-the-art perovskite films mapped by conductive atomic force microscopy reveals a distinct heterogeneity, which exhibits a strong anticorrelation to the external biases. Particularly under different external bias polarities, specific regions in the current mapping show contrasting conductivity. Moreover, grains oriented differently exhibit varied surface potentials and currents, leading us to associate this local current heterogeneity with the grain orientation. It was found that the films treated with isopropanol exhibit ordered grain orientation, demonstrating minimized lattice heterogeneity, fewer microstructure defects, and reduced electronic disorder. Importantly, devices exhibiting an ordered orientation showcase elevated macroscopic optoelectronic properties and boosted device performance. These observations underscore the critical importance of fine-tuning the grain homogenization of perovskite films, offering a promising avenue for further enhancing the efficiency of PSCs.