Tailoring Buried Interface and Minimizing Energy Loss Enable Efficient Narrow and Wide Bandgap Inverted Perovskite Solar Cells by Aluminum Glycinate Based Organometallic Molecule

Abstract Rational regulation of Me‐4PACz/perovskite interface has emerged as a significant challenge in the pursuit of highly efficient and stable perovskite solar cells (PSCs). Herein, an organometallic molecule of aluminum glycinate (AG) that contained amine (‐NH₂) and aluminum hydroxyl (Al‐OH) groups is developed to tailor the buried interface and minimize interface‐driven energy losses. The Al‐OH groups selectively bonded with unanchored O═P‐OH and bare NiO‐OH to optimize the surface morphology and energy levels, while the ‐NH₂ group interacted specifically with Pb²⁺ to retard perovskite crystallization, passivate buried Pb‐related defects, and release residual interface stress. These interactions facilitate the interface carrier extraction and reduce interface‐driven energy losses, thereby realizing a balanced charge carrier transport. Consequently, AG‐modified narrow bandgap (1.55 eV) PSC demonstrates an efficiency of 26.74% (certified 26.21%) with a fill factor of 86.65%; AG‐modified wide bandgap (1.785 eV) PSC realizes 20.71% champion efficiency with excellent repeatability. These PSCs maintain 91.37%, 91.92%, and 92.00% of their initial efficiency after aging in air atmosphere, the nitrogen‐filled atmosphere at 85 °C, and continuously tracking at the maximum power‐point under one‐sun illumination (100 mW cm⁻²) for 1200 h, respectively.