Tailored Succinic Acid‐Derived Molecular Structures toward 25.41%‐Efficiency and Stable Perovskite Solar Cells

Abstract Minimizing interfacial charged traps in perovskite films is crucial for reducing the non‐radiative recombination and improving device performance. In this study, succinic acid (SA) derivatives varying active sites and spatial configurations are designed to modulate defects and crystallization in perovskite film. The SA derivative with two symmetric Br atoms, dibromosuccinic acid (DBSA), exhibits the optimal spatial arrangement for defect passivation. Experimental and theoretical results indicate that the carboxyl group and atomic Br in DBSA synergistically interact with the under‐coordinated Pb²⁺. Moreover, the strong electronegativity of Br efficiently stabilizes the formamidinium cation via electrostatic interaction. Consequently, film quality is significantly improved and non‐radiative recombination is markedly depressed, resulting in a photoluminesence lifetime of exceeding 4 µs of and a carrier diffusion length of 3 µm. An exceptional efficiency of 25.41% (certified at 25.00%) along with a high fill factor of 84.39% and excellent long‐term operational stability have been achieved finally.