Control of the Surface Disorder by Ion-Exchange to Achieve High Open-Circuit Voltage in HC(NH₂ )₂ PbI₃ Perovskite Solar Cell

The ionic nature of organic trihalide perovskite leads to structural irregularity and energy disorder at the perovskite surface, which seriously affects the photovoltaic performance of perovskite solar cells. Here, the origin of the perovskite surface disorder is analyzed, and a facial ion-exchange strategy is designed to regulate the surface chemical environment. By the reconstruction of terminal irregular Pb-I bonds and random cations, the repaired surface is characteristic of the reduced band tail states, consequent to the suppression of the uplift of quasi-Fermi level splitting and photocarrier scattering. The optimized device gets a high open-circuit voltage and operational stability. These findings fully elaborate the underlying mechanism concerning perovskite surface problem, giving guidance on tailoring the energy disorder.