In Situ Management of Ions Migration to Control Hysteresis Effect for Planar Heterojunction Perovskite Solar Cells

Abstract As one of the most promising photovoltaic materials, the efficiency of inorganic–organic hybrid halide perovskite solar cells (PSCs) has reached 25.5% in 2020. However, the stability and hysteresis remain primary challenges before it can become a commercial photovoltaic technology. Therefore, those issues have drawn significant attention for photovoltaic applications. In this work, a study of the PSCs hysteresis improvement is presented based on a combination of first‐principles simulations, scanning electron microscopy images, and time‐dependent photocurrent measurements. It indicates the hysteresis led by the ion migration and accumulation is mainly localized at the two interfaces: one is between electron transport layer and active layer, and the other is between active layer and hole transport layer. Considering the massive defects at the grain boundaries (GBs), they lower the potential barriers significantly. The defect density at GBs is therefore reduced via the in situ passivation of PbI 2 crystals. The hysteresis index is decreased from 22.43% down to 1.04%, and results in an improvement in efficiency from 17.12% up to 20.10%. Following the understanding of defect‐induced hysteresis, an approach to improve the hysteresis is provided, which can be integrated into the fabrication process and widely applied to enhance the performance of PSCs.