Grain boundary defects passivation by bridging diammonium toward stable and efficient perovskite solar cells

The grain boundary defects of polycrystalline perovskite could induce severe carrier recombination loss to restrict the photovoltaic and stability advancement of perovskite-based solar cells (PSCs). Inserting fixed molar ratio organic cations spacers into halide perovskite slabs to reduce the dimension of the crystal structure is still limited in finding a compromise of efficiency and stability for the widened bandgap and increasing barriers for carrier transport. Here, we select a direct additive bridging engineering to introduce a rationally designed organic amine salt 1,4-Benzene diammonium iodide (BDAI₂) with ammonium group on both terminals of the benzene ring to passivate the grain boundary and interface defects of perovskite. Bridging diammonium could ameliorate the interface contact and achieve electrostatic interactions with negatively charged traps (such as uncoordinated I^-, PbI₃^-, and methylammonium vacancies) to inhibit cation migration, reduce halogen ion vacancy, and then suppress trap-induced recombination in perovskite. As a result, the bridging diammonium could improve the power conversion efficiency (PCE) from 19.86% to 21.91%. This study highlights the importance of rational bridging diammonium for perovskite surface modification and passivation to boost photovoltaic performance and stability.