摘要
Wide-spectrum responsive monolithic perovskite/PbS QD tandem solar cells • RPD-ITO ICL reduces transport barriers and avoids thermal damage to subcells • Monochromatic offset light diagnosis pinpoints subcell photocurrent mismatch • Substrate tandem architecture eliminates solvent-induced perovskite degradation • Substrate perovskite/PbS QD tandems achieves a record efficiency of 21.14%. Emerging tandem photovoltaics offer a promising route for cost-effective solar energy harvesting through high power conversion efficiency (PCE). Although perovskite/PbS quantum dot (QD) tandem solar cells (TSCs) enable broad-spectrum light harvesting, inefficient charge recombination within interconnection layer (ICL) and structural incompatibility cause serve efficiency losses. Herein, we developed monolithic n-i-p perovskite/PbS QD TSCs incorporating a simplified indium tin oxide (ITO)-based ICL. Compared with Au/atomic layer deposition (ALD)‑tin oxide (SnO 2 ) counterpart, the ITO-based ICL exhibits excellent processing compatibility, favorable band alignment, and reduced carrier transport barriers. Compared to the control device, the ITO-based perovskite/PbS QD tandem device demonstrated an improved efficiency from 17.34% to 20.65%, with the fill factor increasing from 65.30% to 72.73%. The corresponding four-terminal tandems also reached a PCE of 26.34%. Furthermore, to address the current mismatch in the superstrate configuration, we engineered a substrate architecture featuring a self-assembled monolayer-integrated ICL. Benefiting from improved current matching, the substrate TSCs achieved a record PCE of 21.14%, with the open-circuit voltage increasing from 1.616 V to 1.718 V. This research demonstrates that matching ICLs and tandem configurations is essential for advancing the performance horizons of solution-processed hybrid perovskite/PbS QD TSCs. Download: Download high-res image (298KB) Download: Download full-size image
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