Bottom Distribution of F-Based Additives in Perovskite Films and Their Effects on Photovoltaic Performance

Various additives have been introduced to assist in film preparation and defect passivation. Herein, fluoroiodobenzene (FIB) molecules with different numbers of F atoms were incorporated into perovskite films to optimize the film quality as well as passivate defects. Based on the calculation and experimental results, it was found that the FIB additives were inclined to exist at the bottom of the film because of the strong affinity between F atoms stemming from FIB molecules and O atoms stemming from TiO₂, especially for molecules with more F atoms. By optimization of the FIB molecule, the perovskite film crystallinity was significantly improved, the carrier lifetimes were prolonged, and the charge extraction ability was also enhanced. The device with FIB with one F atom achieved a photoelectrical conversion efficiency as high as 22.89% with a V_oc of 1.118 V, fill factor (FF) of 80.44%, and J_sc of 25.45 mA cm^-2, which was much higher than that of the control device with an efficiency of 20.87%. Furthermore, FIB molecules with three and five F atoms also achieved higher efficiency than that of the control device. The devices with FIB molecules showed better stability than the devices without additives. The unencapsulated devices with FIB additives held 90% of their original efficiencies in an ambient environment with a temperature of 15-25 °C and a relative humidity of 20-30%, while the control device dropped to 76% after more than 1000 h.