Regulated Crystallization Through Intermolecular Interactions Bridging for Efficient Tin‐Based Perovskite Solar Cells

Tin halide perovskite (THP) has emerged as a promising lead-free material for high-performance solar cells, attracting significant attention for their potential use for energy conversion. However, the rapid crystallization of THP due to its high Lewis acidity and easy oxidation of Sn²⁺ leads to poor morphology and rampant defects in the resulting perovskite films. These strongly hamper the advances in efficiency and stability in THP solar cells. Herein, a comprehensive crystallization regulation strategy is demonstrated by introducing methyl carbazate (C₂H₆N₂O₂, MeC) to regulate the crystallization kinetics of perovskite through inter-molecular interactions. The coordination bonds (O…Sn) and hydrogen bonds (N─H…O) between MeC and perovskite bridge the perovskite lattice together, helping suppress the oxidation of Sn²⁺, meanwhile, restraining the fast crystallization of perovskite in the precursor solution, by enhancing nucleation sites. More importantly, the connection by MeC can reduce the deep-level trap state defect density, significantly restraining non-radiative recombination and improving the carrier lifetime. Consequently, this facile strategy offers valuable insights into THP crystallization kinetics and allows an enhanced high power conversion efficiency from 10.43% to 14.02% to be achieved with good stability.