Trimethyl Ammonium‐Assisted Interfacial Modification for Efficient and Stable Wide‐Bandgap Perovskite Solar Cells

Wide‐bandgap (WBG) perovskite solar cells (PSCs) are acknowledged as promising candidates for tandem solar cells and building photovoltaics. It is well known that cesium‐based all‐inorganic halide WBG perovskites possess the comparable optoelectronic properties as the organic–inorganic counterparts, but exhibit superior thermal stability. Among them, CsPbIBr2 is considered a feasible material for tandem solar cells after balancing the bandgap and stability of the inorganic perovskite. However, CsPbIBr2 PSCs are often subjected to drastic interfacial charge recombination especially in carbon‐based device structure derived from the chemical bonding defects (i.e., uncoordinated Pb2+) naked on CsPbIBr2 soft lattice, which dramatically limits overall efficiency of CsPbIBr2 WBG PSCs. Herein, a trimethyl ammonium salt hexyltrimethylammonium bromide is presented for CsPbIBr2/carbon interfacial modification. Benefiting from the −N+(CH3)3 passivation effect and −C6H13 hydrophobic alkyl chain, the optimal device with highly smooth morphology and sufficient charge extraction exhibits a champion power conversion efficiency of 11.24% and improved long‐term stability with 99.7% and 79.7% efficiency retention under dry air atmosphere and continuous 85 °C thermal stress, indicating the valuable potential application of the lattice solidified CsPbIBr2 WBG PSCs.