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Herein, three global asymmetric SMAs (\n                    <jats:bold>AY2F\u2010ClF<\/jats:bold>\n                    ,\n                    <jats:bold>AY2F\u2010BrF<\/jats:bold>\n                    , and\n                    <jats:bold>AY2F\u2010IF<\/jats:bold>\n                    ) and symmetric\n                    <jats:bold>SY\u20102(FBr)<\/jats:bold>\n                    , featuring one or two regio\u2010regular, locally asymmetric hetero\u2010dihalogenated terminals with successively heavier halogens, were successfully synthesized by applying the dual asymmetric terminal strategy. Asymmetric\n                    <jats:bold>AY2F\u2010BrF<\/jats:bold>\n                    presents a compact 3D molecular packing with the strongest and most multidimensional electronic coupling, which promotes exciton delocalization, and enhanced crystallinity and electron mobility in pure film. Remarkably,\n                    <jats:bold>D18:AY2F\u2010BrF<\/jats:bold>\n                    OSCs deliver a champion binary PCE of 20.26% with energy loss (\n                    <jats:italic>E<\/jats:italic>\n                    <jats:sub>loss<\/jats:sub>\n                    ) of 0.512\u00a0eV, surpassing the PCEs of\n                    <jats:bold>AY2F\u2010ClF<\/jats:bold>\n                    (19.74%),\n                    <jats:bold>AY2F\u2010IF<\/jats:bold>\n                    (19.15%), and\n                    <jats:bold>SY\u20102(FBr)<\/jats:bold>\n                    (19.40%)\u2010based OSCs, setting a new record for asymmetric terminal SMAs\u2010based binary BHJ\u2010OSCs, which is attributed to the optimized phase separation morphology and enhanced and compact crystallinity and faster charge transfer and transport. Our innovative work demonstrates that integrating global asymmetric terminal molecular engineering with a regioisomer\u2010free hetero\u2010fluorinated\/brominated terminal strategy provides an ingenious dual asymmetric terminal strategy for achieving champion PCE and suppressed\n                    <jats:italic>E<\/jats:italic>\n                    <jats:sub>loss<\/jats:sub>\n                    of binary OSCs incorporating asymmetric terminal\u2010based SMAs.\n                  <\/jats:p>","DOI":"10.1002\/anie.3817518","type":"journal-article","created":{"date-parts":[[2026,4,17]],"date-time":"2026-04-17T06:37:26Z","timestamp":1776407846000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":7,"title":["Manipulating Heavy Halogenated Asymmetric Terminals Affords Regio\u2010Regular Hetero\u2010Fluorinated\/Brominated Dual Asymmetric Acceptor With a Binary Photovoltaic Efficiency of 20.3%"],"prefix":"10.1002","volume":"65","author":[{"given":"Aslam\u2010Muhammad","family":"Shahid","sequence":"first","affiliation":[{"name":"Key Laboratory of Cluster Science of the Ministry of Education Beijing Key Laboratory of Intelligent Molecular Materials and High\u2010throughput Manufacturing School of Chemistry and Chemical Engineering Beijing Institute of Technology  Beijing China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Hong\u2010Chen","family":"Rong","sequence":"additional","affiliation":[{"name":"Key Laboratory of Cluster Science of the Ministry of Education Beijing Key Laboratory of Intelligent Molecular Materials and High\u2010throughput Manufacturing School of Chemistry and Chemical Engineering Beijing Institute of Technology  Beijing China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Heng","family":"Zhang","sequence":"additional","affiliation":[{"name":"Key Laboratory of Cluster Science of the Ministry of Education Beijing Key Laboratory of Intelligent Molecular Materials and High\u2010throughput Manufacturing School of Chemistry and Chemical Engineering Beijing Institute of Technology  Beijing China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-5590-0768","authenticated-orcid":false,"given":"Ze\u2010Fan","family":"Yao","sequence":"additional","affiliation":[{"name":"College of Chemistry and Molecular Engineering Peking University  Beijing China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Er\u2010Long","family":"Li","sequence":"additional","affiliation":[{"name":"Key Laboratory of Cluster Science of the Ministry of Education Beijing Key Laboratory of Intelligent Molecular Materials and High\u2010throughput Manufacturing School of Chemistry and Chemical Engineering Beijing Institute of Technology  Beijing 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