Modulating Buried Passivation and Aligned Interface toward High‐Performance Perovskite Modules

Abstract The inferior buried film quality and mismatched energy alignment have significantly limited the efficiency and stability of perovskite solar cells (PSCs), especially for the large area, ambient‐condition fabricated perovskite modules (PSMs). The buried interface engineering is considered the most effective strategy for achieving high‐performance PSMs. Herein, the organic thiazole molecule 2‐Cyaniminothiazolidine (CTH) is introduced, which possesses multiple active sites, to modify the buried interface of PSCs. The introduction of CTH can effectively accelerate the nucleation and delay the crystal growth of perovskite compared to monofunctional group additives. In addition, the multisite functional group in CTH passivates deep energy level defects and shallow energy level defects in the perovskite films. These results can reduce interfacial voids and produce high‐quality perovskite films. Consequently, the champion devices prepared under ambient conditions achieve efficiencies of 24.31% for a small area (0.07 cm ² ) and 22.09% for a large area (1 cm ² ), respectively. The inverted PSMs with an aperture area of 48 cm ² achieve an impressive efficiency of 20.76%, indicating a teeny efficiency loss from 1 to 48 cm ² . In addition, the PSCs with CTH exhibit better long‐term operational stability, maintaining 90% of their initial efficiency after 1200 h under continuous one‐sun illumination.