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The limitation stems from weak intramolecular charge transfer (ICT) and poor locally excited\/charge\u2010transfer (LE\/CT) state hybridization, which are direct consequences of the canceled dipole moments in symmetric dimer architectures. In this work, we adopt an asymmetric\u2010isomerization strategy to design two novel dual\u2010asymmetric isomeric dimer acceptors QCl\u2010YF and QF\u2010YCl. Compared with QCl\u2010YF, QF\u2010YCl exhibits an enhanced ICT effect as evidenced by a larger electron\u2010hole spatial separation, which promotes LE\/CT hybridization and enables more efficient carrier dynamics. Moreover, the stronger electrostatic potential and dipole moment of QF\u2010YCl enhances the intermolecular interactions to improve donor\/acceptor compatibility and film\u2010forming process in blend film, consequently leading to more ordered film morphology. Consequently, the QF\u2010YCl\u2010based device achieves a record PCE of 20.23% (vs. 19.60% for QCl\u2010YF), achieving the highest efficiency for dimer\u2010based binary OSCs. This work demonstrates that asymmetric\u2010isomerization is a precise and effective design strategy for high\u2010performance dimer acceptors.<\/jats:p>","DOI":"10.1002\/adma.75370","type":"journal-article","created":{"date-parts":[[2026,10,12]],"date-time":"2026-10-12T15:35:10Z","timestamp":1791819310000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Asymmetric\u2010Isomerization Dimer Acceptors via Modular Molecular Design Enable Highly Efficient Binary Organic Solar Cells"],"prefix":"10.1002","author":[{"given":"Lei","family":"Tang","sequence":"first","affiliation":[{"name":"College of Chemistry and Chemical Engineering Film Energy Chemistry for Jiangxi Provincial Key Laboratory (FEC) Nanchang University  Nanchang Jiangxi China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Shiyong","family":"You","sequence":"additional","affiliation":[{"name":"College of Chemistry and Chemical Engineering Film Energy Chemistry for Jiangxi Provincial Key Laboratory (FEC) Nanchang University  Nanchang Jiangxi China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jie","family":"Zhou","sequence":"additional","affiliation":[{"name":"College of Chemistry and Chemical Engineering Film Energy Chemistry for Jiangxi Provincial Key Laboratory (FEC) Nanchang University  Nanchang Jiangxi China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0002-1665-1572","authenticated-orcid":false,"given":"Chao","family":"Yang","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Information Photonic and Optical Communications School of Physical Sciences and Technology Beijing University of Posts and Telecommunications  Beijing 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