Organic solar cells (OSCs), a nascent technology in the photovoltaic field, have attracted considerable research interest. Recently, the power conversion efficiency (PCE) of OSCs has significantly improved, thereby demonstrating substantial potential for commercialization. To achieve this, it is crucial to enhance the performance and stability of OSCs, necessitating the development of novel materials and devices. This feature article presents a review of chlorine-mediated photovoltaic materials in our group. By carefully controlling energy levels, molecular stacking and aggregation behavior, significantly improved performance was achieved. Furthermore, single-crystal analysis facilitated a profound comprehension of the influence of chlorine-mediated interactions on molecular stacking. This has enabled the design and synthesis of a series of high-performance non-fullerene acceptors (NFAs) with three-dimensional network stacking structures. Building upon these materials, we developed quasi-planar heterojunction (Q-PHJ) devices with a significant stability advantage. To sum up, the chlorine-mediated materials and the Q-PHJ devices provide valuable guidance and reference for the development of efficient and stable organic solar cells.
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