Surface defect passivation of All-Inorganic CsPbI2Br perovskites via fluorinated ionic liquid for efficient Outdoor/Indoor photovoltaics processed in ambient air

Abstract

All-inorganic α-CsPbI2Br perovskite has garnered considerable interest due to its optical bandgap (∼1.92 eV) suitable for tandem architectures and superior thermal stability. However, CsPbI2Br based perovskite solar cells (PSCs) exhibit severe energy loss due to presence of various surface defects like uncoordinated Pb2+ ions, halide ion vacancies and pinholes, which causes serious non-radiative recombination and limit the further improvement in power conversion efficiency (PCE). Surface passivation strategy is an effective approach to produce high quality α-CsPbI2Br film. Herein, we introduce fluorinated ionic liquid, 3-(Trifluoromethyl) benzylamine (CFBA), as surface passivating agent. The chemical analysis shows that the trifluoro (-CF3) and amine groups of CFBA strongly interacted with perovskite surface via forming Pb-F and H-I bonding, respectively. The high electronegative fluoride atoms of -CF3 group allow for electrostatic interaction with uncoordinated Pb2+ ions, which built a robust shield that protected against surrounding moisture as well. In addition, CFBA modification passivates the dangling bonds, enhanced crystallinity, reduced pinholes, improved the surface coverage and compactness, increased hydrophobicity, and decreased non-radiative recombination, leading to high PCE. With optimum concentration of 3 μL-CFBA, CsPbI2Br PSC revealed an impressive PCE of 17.07% with FF of 83.21% as compared to pristine device (PCE of 15.24% with FF of 79.81%). Moreover, champion device showed an excellent thermal stability by retaining ∼ 86.23% of its initial PCE, whereas pristine device maintained ∼ 48.26% of its original PCE after 1440 h aging at 85 ℃ in a dry box without any encapsulation. In addition, optimized PSC showed a decent indoor PCE of 23.24% as compared to pristine device (18.35%) under dim lighting conditions (LED, 3200 K) at 1000 lx. These results suggested that surface passivation strategy with CFBA is a promising approach for developing efficient all-inorganic CsPbI2Br outdoor/indoor PSCs with better thermal stability.