Trace Water in Lead Iodide Affecting Perovskite Crystal Nucleation Limits the Performance of Perovskite Solar Cells

The experimental replicability of highly efficient perovskite solar cells (PSCs) is a persistent challenge faced by laboratories worldwide. Although trace impurities in raw materials can impact the experimental reproducibility of high-performance PSCs, the in situ study of how trace impurities affect perovskite film growth is never investigated. Here, light is shed on the impact of inevitable water contamination in lead iodide (PbI2) on the replicability of device performance, mainly depending on the synthesis methods of PbI2. Through synchrotron-based structure characterization, it is uncovered that even slight additions of water to PbI2 accelerate the crystallization process in the perovskite layer during annealing. However, this accelerated crystallization also results in an imbalance of charge-carrier mobilities, leading to a degradation in device performance and reduced longevity of the solar cells. It is also found that anhydrous PbI2 promotes a homogenous nucleation process and improves perovskite film growth. Finally, the PSCs achieve a remarkable certified power conversion efficiency of 24.3%. This breakthrough demonstrates the significance of understanding and precisely managing the water content in PbI2 to ensure the experimental replicability of high-efficiency PSCs. Material purity impacts optoelectronic properties; trace water in chemicals affects perovskite formation, influencing performance. This study unveils the significance of water content in PbI2, affecting crystallization and texture and ultimately decreasing hole mobility. Imbalanced hole-electron mobility limits device performance. Certified PCEs of 24.3% and 22.9% for small and larger aperture solar cells are achieved by fine-controlling water content in PbI2.image