Buried‐Interface Regulation of Crystallization and Charge Extraction in Perovskite Solar Cells

This is the authors' abstract. We don't add key points for this paper.

In n–i–p perovskite solar cells, the SnO 2 /perovskite buried interface plays a decisive role in governing crystallization and charge extraction. Here, trisodium methylglycine diacetate (MGDA) is introduced onto SnO 2 to regulate precursor behavior during crystallization. Molecular‐dynamics simulations using PbI 2 ∙DMSO as a representative solvent‐coordinated lead‐iodide species show that MGDA increases interfacial precursor localization while restricting lateral motion and aggregation. This modified precursor state is accompanied by slower but more extended late‐stage growth/reorganization during thermal annealing, leading to larger grains, fewer buried‐interface voids, improved crystallinity, and lower residual tensile stress. The optimized devices deliver a power conversion efficiency of 25.50%, while 7 × 7 cm 2 rigid and 5 × 5 cm 2 flexible mini‐modules reach 22.49% and 17.38%, respectively, with improved ambient‐storage and thermal stability. These results reveal the link between interfacial precursor behavior, subsequent crystallization, and device performance, providing guidance for buried‐interface design in perovskite solar cells.