| Abstract: | The power conversion efficiency of inorganic–organic hybrid lead halide perovskite solar cells (PSCs) is approaching that of those made from single crystalline silicon; however, they still experience problems such as hysteresis and photo/electrical‐field‐induced degradation. Evidences consistently show that ionic migration is critical for these detrimental behaviors, but direct in‐situ studies are still lacking to elucidate the respective kinetics. Three different PSCs incorporating phenyl‐C61‐butyric acid methyl ester (PCBM) and a polymerized form (PPCBM) is fabricated to clarify the function of fullerenes towards ionic migration in perovskites: 1) single perovskite layer, 2) perovskite/PCBM bilayer, 3) perovskite/PPCBM bilayer, where the fullerene molecules are covalently linked to a polymer backbone impeding fullerene inter‐diffusion. By employing wide‐field photoluminescence imaging microscopy, the migration of iodine ions/vacancies under an external electrical field is studied. The polymerized PPCBM layer barely suppresses ionic migration, whereas PCBM readily does. Temperature‐dependent chronoamperometric measurements demonstrate the reduction of activation energy with the aid of PCBM and X‐ray photoemission spectroscopy (XPS) measurements show that PCBM molecules are viable to diffuse into the perovskite layer and passivate iodine related defects. This passivation significantly reduces iodine ions/vacancies, leading to a reduction of built‐in field modulation and interfacial barriers. |
