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We focused on the strategical integration of an electron\u2010donating methoxy group and an electron\u2010withdrawing halogen atom at benzene\u2010fused terminal groups. This combination precisely modulated the dipole moment and electron density of terminal groups, effectively attenuating intramolecular charge transfer effect, and widening the band gap of acceptors. The incorporation of these terminal groups yielded two asymmetric acceptors, named BTP\u20102FClO and BTP\u20102FBrO, both of which exhibited open\u2010circuit voltage (\n                    <jats:italic>V<\/jats:italic>\n                    <jats:sub>oc<\/jats:sub>\n                    ) as high as 0.96\u2005V in binary devices, representing the highest\n                    <jats:italic>V<\/jats:italic>\n                    <jats:sub>OC<\/jats:sub>\n                    s among the asymmetric Y\u2010series small molecule acceptors. More importantly, both BTP\u20102FClO and BTP\u20102FBrO exhibit modest aggregation behaviors and molecular crystallinity, making them suitable as a third component to mitigate excess aggregation of the PM6\u2009:\u2009BTP\u2010eC9 blend and optimize the devices\u2019 morphology. As a result, the optimized BTP\u20102FClO\u2010based ternary organic solar cells (OSCs) achieved a remarkable power conversion efficiency (PCE) of 19.34\u2009%, positioning it among the highest\u2010performing OSCs. Our study highlights the molecular design importance on manipulating dipole moments and electron density in developing medium\u2010band gap acceptors, and offers a highly efficient third component for high\u2010performance ternary OSCs.\n                  <\/jats:p>","DOI":"10.1002\/anie.202415332","type":"journal-article","created":{"date-parts":[[2024,9,8]],"date-time":"2024-09-08T23:05:57Z","timestamp":1725836757000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":34,"title":["Dipole Moment Modulation of Terminal Groups Enables Asymmetric Acceptors Featuring Medium Bandgap for Efficient and Stable Ternary Organic Solar Cells"],"prefix":"10.1002","volume":"64","author":[{"given":"Bosen","family":"Zou","sequence":"first","affiliation":[{"name":"Department of Chemistry and Hong Kong Branch of Chinese National Engineering Research Center for Tissue Restoration and Reconstruction The Hong Kong University of Science and 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