Across‐Interface Effect of Alkylamine Salt on the Formation of Intermediate Phase and Defect Passivation in High‐Performance of Perovskite Solar Cells.

High‐quality and low‐defect perovskite active layer (PVK) and electron transport layer (ETL) are essential for high‐performance perovskite solar cells (PSCs). Herein, an alkylamine salt, cyclohexylmethylammonium chloride (CMACl) is introduced into tin oxide (SnO2) ETL. CMACl, possessing protonated −NH3+ group and Cl− ions, not only effectively inhibits the aggregation of SnO2 colloids and enhances the quality of the ETLs, but also reduces and passivates the defects on ETLs. On the other hand, via the across‐interface effect of alkylamine salt by thermal diffusion, the CMACl‐PbI2 intermediate phase is formed and leads to the high quality of PVK, meanwhile, the defect on the buried interfaces and in the bulk of PVK are passivated by CMA+ and Cl− ions. Consequently, the CMACl‐modified PSC achieves a preeminent power conversion efficiency of 25.47% and excellent stability. This work demonstrates a facile and effective approach for synchronous optimization of ETL and PVK for high‐performance PSCs by across‐interface effect. [ABSTRACT FROM AUTHOR]