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However, the limited available of electron acceptors with adequate solubility and favorable molecular packing presents a challenge in achieving efficient non\u2010halogenated solvent\u2010processed OSCs. Herein, inspired by the three\u2010dimensional dimeric acceptor CH8\u20104, we employed a molecular isomerization strategy to synthesize its isomers, CH8\u20104A and CH8\u20104B, by tuning the position of fluorine (F) atom in the central unit. The differing intramolecular fluorine\u2010sulfur non\u2010covalent interactions among these isomers led to differences in molecular pre\u2010aggregation abilities (CH8\u20104B&lt;CH8\u20104&lt;CH8\u20104A) in <jats:italic>o<\/jats:italic>\u2010xylene (<jats:italic>o<\/jats:italic>\u2010XY) solution, which significantly influence the film\u2010forming process and the resultant morphological characteristics. Among these, the blend film of CH8\u20104, characterized by moderate molecular pre\u2010aggregation, achieved optimal bi\u2010continuous donor\/acceptor phase separation. Consequently, the <jats:italic>o<\/jats:italic>\u2010xylene processed PM6\u2009:\u2009CH8\u20104 device achieved a power conversion efficiency (PCE) of 18.1\u2009%, outperforming that of two other devices. By incorporating L8\u2010BO\u2010D as a guest acceptor, we attained an impressive PCE of 20.0\u2009% for the CH8\u20104\u2010based ternary device, alongside a high PCE nearing 16\u2009% for the mini\u2010module (13.5\u2005cm<jats:sup>2<\/jats:sup>). Our findings underscore the potential of isomerism in 3D dimer acceptors to enhance the performance of eco\u2010friendly OSCs.<\/jats:p>","DOI":"10.1002\/anie.202423562","type":"journal-article","created":{"date-parts":[[2024,12,26]],"date-time":"2024-12-26T10:19:03Z","timestamp":1735208343000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":95,"title":["Isomerism Effect of 3D Dimeric Acceptors for Non\u2010Halogenated Solvent\u2010Processed Organic Solar Cells with 20\u2009% Efficiency"],"prefix":"10.1002","volume":"64","author":[{"given":"Jia","family":"Wang","sequence":"first","affiliation":[{"name":"School of Materials Science and Engineering National Institute for Advanced Materials Nankai University  Tianjin 300350 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Peiran","family":"Wang","sequence":"additional","affiliation":[{"name":"School of Materials Science and Engineering National Institute for 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