Abstract
Wide-bandgap (WBG) perovskite solar cells (PSCs) play a fundamental role in perovskite-based tandem solar cells. However, the efficiency of WBG PSCs is limited by significant open-circuit voltage losses, which are primarily caused by surface defects. In this study, we present a novel method for modifying surfaces using the multifunctional S-ethylisothiourea hydrobromide (SEBr), which can passivate both Pb-I and FA-I terminated surfaces. Moreover, the SEBr upshifted the Fermi level at the perovskite interface, thereby promoting carrier collection. This proposed method was effective for both 1.67 and 1.77 eV WBG PSCs, achieving power conversion efficiencies (PCEs) of 22.47% and 19.90%, respectively, with VOC values of 1.28 and 1.33 V, along with improved film and device stability. With this advancement, we were able to fabricate monolithic all-perovskite tandem solar cells with a champion PCE of 27.10%. This research offers valuable insights for passivating the surface trap states of WBG perovskite through rational multifunctional molecular engineering.
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