Tailoring Buried Interface and Minimizing Energy Loss Enable Efficient Narrow and Wide Bandgap Inverted Perovskite...

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.