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Non‐fullerene acceptors are currently a hot research area in the development of organic solar cells (OSCs). At present, the‐state‐of‐the‐art power conversion efficiency (PCE) of non‐fullerene organic solar cells (NF‐OSCs) with single and multiple‐junction has surpassed 18% and 19%, respectively. The cathode interlayer (CIL) plays a significant role in the improvement of PCE and the stability of OSCs. Recently, a large number of CIL materials have been employed in OSCs. This review summarizes the recent progress of CIL materials and systematically describes their impact on the device efficiency and stability in single‐junction NF‐OSCs. Firstly, the functions, key requirements, and distinctive features of CILs when used in NF‐OSCs are summarized. Afterward, some big families of materials including metal oxides, metal salts/complexes, small molecules, polymers, composites/hybrids are presented as CIL for NF‐OSCs. Finally, the scale‐up techniques, conclusion, and future challenges regarding CIL in NF‐OSCs are elucidated.

Exhibiting outstanding optoelectronic properties, antimony selenide (Sb 2 Se 3 ) has attracted considerable interest and has been developed as a light absorber layer for thin-film solar cells over the decade. However, current state-of-theart Sb 2 Se 3 devices suffer from unsatisfactory "cliff-like" band alignment and severe interface recombination loss, which deteriorates device performance. In this study, the heterojunction interface of an Sb 2 Se 3 solar cell is improved by introducing effective aluminum (Al 3+ ) cation into the CdS buffer layer. Then, the energy band alignment of Sb 2 Se 3 /CdS:Al heterojunction is modified from a "cliff-like" structure to a "spike-like" structure. Finally, heterojunction interface engineering suppresses recombination losses and strengthens carrier transport, resulting in a high efficiency of 8.41% for the substrate-structured Sb 2 Se 3 solar cell. This study proposes a facile strategy for interfacial treatment and elucidates the related carrier transport enhancement mechanism, paving a bright avenue to overcome the efficiency bottleneck of Sb 2 Se 3 thin-film solar cells.

The cathode interlayer plays a key role in the photovoltaic performance in organic solar cells.