Accelerated DFT-Assisted Screening of Interfacial Modification Materials for High-Performance Perovskite Solar Cells

• • DFT-based screening identified TZMC as a superior interfacial modifier, achieving a champion PCE of 25.44% in perovskite solar cells, representing a significant improvement over conventional trial-and-error methods. • • TZMC passivates defects via dual coordination: Pb2+ binding through carbonyl oxygen and imidazole nitrogen, and I− stabilization via N–H···I hydrogen bonding, effectively suppressing non-radiative recombination. • • The synergistic mechanism concurrently enhances VOC and FF, leading to a PCE of 25.44%, while operational stability under continuous illumination and resistance to water/oxygen are significantly improved. • • The DFT-assisted screening framework offers a low-cost, efficient pathway for rational design of interface materials, potentially accelerating development of high-performance PSCs and enabling high-throughput screening in artificial intelligence applications.