Boosting All-Perovskite Tandem Solar Cells by Revitalizing the Buried Tin-Lead Perovskite Interface

Narrow-bandgap (NBG) mixed tin-lead (Sn-Pb) perovskite solar cells (PSCs) serve as crucial top subcells in all-perovskite tandem solar cells (TSCs). However, the prevalent use of poly(3,4-ethylenedioxythiophene): poly(styrenesulfonate) (PEDOT: PSS) hole transport layers (HTLs) in NBG PSCs compromises device efficiency and stability. To address this, the study proposes a revitalizing strategy for the buried interface of Sn-Pb perovskites by directly immersing acetylcholine chloride (ACh) into PEDOT: PSS. ACh acts as a proficient "diver," not only modulating the bottom PEDOT: PSS HTLs but also facilitating the reconstruction of the buried interface and significantly enhancing the quality of the top perovskite layers. This intervention with ACh prevents Sn²⁺ oxidation, mitigates buried defects, and encourages the growth of large, densely packed grains within Sn-Pb perovskites. Consequently, the optimized NBG PSCs exhibit significantly improved hole transport and reduced carrier recombination, achieving a steady-state efficiency of 22.98% with enhanced stability. Furthermore, these optimized NBG Sn-Pb cells enable highly efficient two-terminal and four-terminal all-perovskite TSCs, boasting steady-state efficiencies of 27.54% (certified at 26.41%) and 28.01%, respectively. This study emphasizes the importance of optimizing NBG PSCs through buried interface reconstruction, propelling the advancement of all-perovskite TSCs.