Abstract
Despite the rapid increase in the performance of perovskite solar cells (PSC), they still suffer from low lab-to-lab or people-to-people reproducibility. Aiming for a universal condition to high-performance devices, we investigated the morphology evolution of a composite perovskite by tuning annealing temperature and precursor concentration of the perovskite film. Here, we introduce thermal annealing as a powerful tool to generate a well-controlled excess of PbI2 in the perovskite formulation and show that this benefits the photovoltaic performance. We demonstrated the correlation between the film microstructure and electronic property and device performance. An optimized average grain size/thickness aspect ratio of the perovskite crystallite is identified, which brings about a highly reproducible power conversion efficiency (PCE) of 19.5%, with a certified value of 19.08%. Negligible hysteresis and outstanding morphology stability are observed with these devices. These findings lay the foundation for further boosting the PCE of PSC and can be very instructive for fabrication of high-quality perovskite films for a variety of applications, such as light-emitting diodes, field-effect transistors, and photodetectors.