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In the current stage, the main focus is to balance the performance and stability. It has been shown that all\u2010polymer formulation can improve device stability, however, PCE is not in satifsfaction, and the batch\u2010to\u2010batch variation leads to quality control issues. In this work, we constructed monodispersed tetramer NFA materials named G\u20101 and G\u20102, to best integrate the merits of small molecule and polymer. Density functional theory (DFT) calculations and experimental results showed that different connecting units at the centre could significantly affect the molecular planarity and thin film morphology. The alkene\u2010bonded tetramer G\u20101 had a more regioregular structure, which leads to better molecular planarity, and more ordered packing in thin film. More importantly, the oligomeration induced a favourable face\u2010on orientation, achieved a lower binding energy and exhibited a higher photoluminescence yield. As a result, the exciton and charge carrier kinetics was optimized with reduced non\u2010radiative energy loss. The OSC based on PM6\u2009:\u2009G\u20101 achieved a PCE of 19.6\u2009%, which is the highest PCE reported so far for oligomer\u2010based binary OSC. In addition, the device stability was largely improved, showing a lifetime over 10000\u2005hours in the inverted OSC device.<\/jats:p>","DOI":"10.1002\/anie.202420453","type":"journal-article","created":{"date-parts":[[2025,1,2]],"date-time":"2025-01-02T22:33:52Z","timestamp":1735857232000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":30,"title":["Construction of Linear Tetramer\u2010Type Acceptors for High\u2010Efficiency and High\u2010Stability Organic Solar Cells"],"prefix":"10.1002","volume":"64","author":[{"given":"Rui","family":"Zeng","sequence":"first","affiliation":[{"name":"School of Chemistry and Chemical Engineering Frontiers Science Center for Transformative Molecules Shanghai Key Laboratory of Electrical Insulation and Thermal Aging Shanghai Jiao Tong University  Shanghai 200240 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jiawei","family":"Deng","sequence":"additional","affiliation":[{"name":"School of Chemistry and Chemical Engineering Frontiers Science Center for Transformative Molecules Shanghai Key Laboratory of Electrical Insulation and Thermal Aging Shanghai Jiao Tong University  Shanghai 200240 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xiaonan","family":"Xue","sequence":"additional","affiliation":[{"name":"Shanghai OPV Solar New Energy Technology Co. 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