Managing Multiple Halide‐Related Defects for Efficient and Stable Inorganic Perovskite Solar Cells

Halide-related surface defects on inorganic halide perovskite not only induce charge recombination but also severely limit the long-term stability of perovskite solar cells. Herein, adopting density functional theory calculation, we verify that iodine interstitials (I_i ) has a low formation energy similar to that of the iodine vacancy (V_I ) and is also readily formed on the surface of all-inorganic perovskite, and it is regarded to function as an electron trap. We screen a specific 2,6-diaminopyridine (2,6-DAPy) passivator, which, with the aid of the combined effects from halogen-N_pyridine and coordination bonds, not only successfully eliminates the I_i and dissociative I₂ but also passivates the abundant V_I . Furthermore, the two symmetric neighboring -NH₂ groups interact with adjacent halides of the octahedral cluster by forming hydrogen bonds, which further promotes the adsorption of 2,6-DAPy molecules onto the perovskite surface. Such synergetic effects can significantly passivate harmful iodine-related defects and undercoordinated Pb²⁺ , prolong carrier lifetimes and facilitate the interfacial hole transfer. Consequently, these merits enhance the power-conversion efficiency (PCE) from 19.6 % to 21.8 %, the highest value for this type of solar cells, just as importantly, the 2,6-DAPy-treated CsPbI_3-x Br_x films show better environmental stability.