Understanding steric-charge-dependence of conjugated passivators on π-Pb2+ bond strength for efficient all-inorganic perovskite solar cells

Intramolecular structure of interfacial passivator highly determines the bond strength with detrimental defects located at perovskite surfaces and grain boundaries. Herein, we investigate the steric-charge-dependence of various π-conjugated pyridine derivatives on electron-donating ability to passivate inorganic CsPbIBr2 perovskite film. The primary results demonstrate that the photovoltaic performances tightly correlate with the multidentate coordination sites and structure-steric hindrance because of their synergistic regulation on intramolecular electron-cloudy density and charge extraction. Comparing to pyridine and terpyridine treated devices, the bipyridine passivated device delivers an increased efficiency of 11.04% with a high open-circuit voltage of 1.301 V and improved stability after persistent irradiation over 20 h and storage for 60 days, which is one of the highest efficiencies for carbon-based all-inorganic CsPbIBr2 solar cells. This work provides a direction to choose ideal passivator for high-efficiency perovskite optoelectronics.