Intercalation of Ammonium Cationic Ligands Enabled Grain Surface Passivation in Sequential‐Deposited Perovskite Solar Cells

Abstract

Solution‐processed formamidinium lead iodide (FAPbI3) perovskite typically contains a high number of ionic defects that are intrinsically formed during film formation. To reduce the defects, postsynthetic surface passivation treatment is widely practiced. However, the practicality of the surface passivation approach is limited by the poor coverage and incomplete adsorption of passivators into the defective sites. Unprecedentedly, the use of 4‐(trifluoromethyl)benzylammonium iodide (CF3BZAI) is demonstrated as a novel passivator additive for sequentially deposited perovskite films. Due to its unique molecular structure and trifluoromethyl (–CF3) moiety, CF3BZAI is expected to have enhanced adsorption with defect sites during the film formation. Owing to grain surface passivation, the CF3BZAI‐intercalated FAPbI3 (target) film has enhanced morphology and crystallinity as well as significantly fewer defects than the normal FAPbI3 film. Interestingly, the intercalation of CF3BZAI passivators does not lead to the formation of a low‐dimensional perovskite phase in FAPbI3 films. The best perovskite solar cell (PSC) device based on the target film achieves a maximum efficiency of ≈22.4%, which is much higher than the efficiency (≈20.7%) of the normal device. CF3BZAI‐assisted grain surface passivation is a facile yet effective strategy to enhance the performance and stability of FAPbI3‐based PSCs.

Revealing Mechanisms and Ultrafast Dynamics of Tetrabutyl Phosphonium Bromide Ionic Liquids Post-Treatment in CsPbBr3 Perovskite Films

“…Perovskite, sharing the same structure as calcium titanate (CaTiO 3 ) and adhering to the ABX 3 general formula, features A representing an organic or inorganic cation (such as methylammonium (MA + ), formamidine (FA + ), Cesium (Cs + ), Rubidium (Rb + ), etc. ), B as a divalent metal cation (lead (Pb 2+ ), Tin (Sn 2+ )), and X as a halogen or pseudohalide anion (chloride (Cl – ), bromide (Br – ), iodide (I – ), thiocyanate (SCN – ), etc.). In the typical three-dimensional (3D) perovskite crystal structure, an angle-shared [BX 6 ] 4– octahedral network houses B at the center of each octahedron, while the cavities between adjacent octahedrons are occupied by A atoms. , Notably, all-inorganic perovskite CsPbX 3 (X = Cl, Br, I) demonstrates remarkable resistance to moisture, heat, and light. − In the past decade, solar cell power conversion efficiency (PCE) has achieved a certified record of 25.7%, signifying significant progress .…”