Methylammonium Chloride Induces Intermediate Phase Stabilization for Efficient Perovskite Solar Cells

One of the most effective methods to achieve high-performance perovskite solar cells has been to include additives that serve as dopants, crystallization agents, or passivate defect sites. Cl-based additives are among the most prevalent in literature, yet their exact role is still uncertain. In this work, we systematically study the function of methylammonium chloride (MACl) additive in formamidinium lead iodide (FAPbI(3))-based perovskite. Using density functional theory, we provide a theoretical framework for understanding the interaction of MACl with a perovskite. We show that MACl successfully induces an intermediate to the pure FAPbI(3) alpha-phase without annealing. The formation energy is related to the amount of incorporated MACl. By tuning the incorporation of MACl, the perovskite film quality can be significantly improved, exhibiting a 6 x increase in grain size, a 3 x increase in phase crystallinity, and a 4.3 x increase in photoluminescence lifetime. The optimized solar cells achieved a certified efficiency of 23.48%.