摘要： Intrinsic defect density in polycrystalline halide perovskite films are required to be low enough to suppress charge recombination loss for improvement in performance of perovskite solar cells (PeSCs). In this paper, we propose the use of amphoteric imidazole to achieve high crystalline quality of CH3NH3PbI3 perovskite absorption layer. The imidazole additive plays a synergistic role in controlling the perovskite crystal growth for large grain size and passivating the uncoordinated ions (e.g., Pb2+) defects, resulting in improved carrier transport/lifetime and suppressed non-radiative recombination. The champion power conversion efficiency (PCE) of PeSCs with imidazole is improved to 16.88%, from the control device with a PCE value of 14.65%. Besides, the stability of imidazole modified perovskite films is further improved by limiting ion immigration at grain boundaries against moisture and heat stresses. The findings pave an avenue for synergistically modulating crystallization and healing defect in perovskite to achieve efficient and stable solar cells.