Efficient Perovskite/Organic Tandem Photovoltaic Devices and Large‐area Modules Featuring Thick‐Film Organic Solar Cells

Abstract Perovskite‐organic tandem solar cells (TSCs) possess significant potential due to their unique features, such as orthogonal processing solvents, tunable bandgap, and infinite molecular designs. However, their device performance is often hindered by the limited series current density, which is constrained by the absorption of the rear organic solar cell (OSC). Here, a fine‐grained sub‐cell matching model has been developed that enables rapid screening of material combinations based on practical sub‐cell device parameters. The model indicates that increasing the thickness of the OSC layer is an effective approach to boost efficiency, while also reducing manufacturing challenges for large‐scale production. To mitigate the charge collection issues arising from excessive thickness, a contact passivation technique based on a self‐assembled monolayer has been developed, which minimizes non‐radiative recombination and reduces the Schottky barrier at the interface, enabling more balanced hole‐electron transport. As a result, the thick‐film (300 nm) has achieved a record‐high efficiency of 18.08% (certified as 17.80%), enhancing the efficiency of TSCs to 24.31% (certified at 24.00%). Furthermore, a large‐area tandem photovoltaic module with an efficiency exceeding 18.54% (18.48 cm 2 ) has been demonstrated. To the knowledge, this represents the first module demonstration for perovskite‐organic TSCs.