Dual-interface engineering strategy for optimizing carrier dynamics in perovskite-silicon tandem solar cells

• • Dual-interface modification with EDAI2 yields a champion efficiency of 22.75% in single-junction wide-bandgap (>1.66 eV) perovskite solar cells, representing a significant improvement over unmodified controls and directly addressing the open-circuit voltage deficit that limits tandem performance. • • Perovskite-silicon tandem devices incorporating dual-interface engineering achieve over 31% power conversion efficiency, demonstrating a clear pathway to surpass the single-junction Shockley-Queisser limit and compete with established silicon technologies. • • Time-resolved photoluminescence confirms extended carrier lifetimes and improved spatial homogeneity in dual-modified perovskite films, indicating effective suppression of non-radiative recombination at both interfaces, which is critical for maintaining high fill factors and open-circuit voltages under operational stress. • • The dual-interface strategy enhances operational stability, a key bottleneck for commercialization, by mitigating photoinduced phase segregation and ion migration that typically plague wide-bandgap perovskites, thereby extending device lifetime and reducing levelized cost of energy.