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To tackle this issue, tethered SMAs, wherein multiple SMA\u2010subunits are connected to the aromatic\u2010core via flexible chains, are proposed. This design aims to an elevated glass transition temperature (<jats:italic>T<\/jats:italic><jats:sub>g<\/jats:sub>) for a dynamical control. However, attaining an elevated <jats:italic>T<\/jats:italic><jats:sub>g<\/jats:sub> value with additional SMA subunits introduces complexity to the molecular packing, posing a significant challenge in realizing both high stability and power conversion efficiency (PCE). In this study, we initiate isomer engineering on the benzene\u2010carboxylate core and find that meta\u2010positioned dimeric <jats:bold>BDY\u2010\u03b2<\/jats:bold> exhibits more favorable molecular packing compared to its para\u2010positioned counterpart, <jats:bold>BDY\u2010\u03b1<\/jats:bold>. With this encouraging result, we expand our approach by introducing an additional SMA unit onto the aromatic core of <jats:bold>BDY\u2010\u03b2<\/jats:bold>, maintaining a meta\u2010position relative to each SMA unit location in the tethered acceptor. This systematic aromatic\u2010core engineering results in a star\u2010shaped C<jats:sub>3h<\/jats:sub>\u2010positioned molecular geometry. The supramolecular interactions of SMA units in the trimer contribute to enhancements in <jats:italic>T<\/jats:italic><jats:sub>g<\/jats:sub> value, crystallinity, and a red\u2010shifted absorption compared to dimers. These characteristics result in a noteworthy increase in PCE to 18.24\u2009%, coupled with a remarkable short\u2010circuit current density of 27.06\u2005mA\u2009cm<jats:sup>\u22122<\/jats:sup>. More significantly, the trimer\u2010based devices delivered an excellent thermal stability with over 95\u2009% of their initial efficiency after 1200\u2005h thermal degradation. Our findings underscore the promise and feasibility of tethered trimeric structures in achieving highly ordered aggregation behavior and increased <jats:italic>T<\/jats:italic><jats:sub>g<\/jats:sub> value in PSCs, simultaneously improving in device efficiency and thermal stability.<\/jats:p>","DOI":"10.1002\/anie.202400590","type":"journal-article","created":{"date-parts":[[2024,2,7]],"date-time":"2024-02-07T06:00:20Z","timestamp":1707285620000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":41,"title":["Tethered Trimeric Small\u2010molecular Acceptors through Aromatic\u2010core Engineering for Highly Efficient and Thermally Stable Polymer Solar Cells"],"prefix":"10.1002","volume":"63","author":[{"given":"Bowen","family":"Chang","sequence":"first","affiliation":[{"name":"State Key Laboratory of Chemical Resource Engineering Beijing Advanced Innovation Center for Soft Matter Science and Engineering Beijing University of Chemical Technology  Beijing 100029 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yaogang","family":"Zhang","sequence":"additional","affiliation":[{"name":"Beijing National Laboratory for Molecular Sciences CAS Key Laboratory of Organic Solids Institute of Chemistry Chinese Academy of Sciences  Beijing 100190 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Cen","family":"Zhang","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Chemical Resource Engineering Beijing Advanced Innovation Center for Soft Matter Science and Engineering Beijing University of Chemical Technology  Beijing 100029 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ming","family":"Zhang","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Chemical Resource Engineering Beijing Advanced Innovation Center for Soft Matter Science and Engineering Beijing University of Chemical Technology  Beijing 100029 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Qingyuan","family":"Wang","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Chemical Resource Engineering Beijing Advanced Innovation Center for Soft Matter Science and Engineering Beijing University of Chemical Technology  Beijing 100029 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zheng'ao","family":"Xu","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Chemical Resource Engineering Beijing Advanced Innovation Center for Soft Matter Science and Engineering Beijing University of Chemical Technology  Beijing 100029 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Qi","family":"Chen","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Chemical Resource Engineering Beijing Advanced Innovation Center for Soft Matter Science and Engineering Beijing University of Chemical Technology  Beijing 100029 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yang","family":"Bai","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Chemical Resource Engineering Beijing Advanced Innovation Center for Soft Matter Science and Engineering Beijing University of Chemical Technology  Beijing 100029 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Hongyuan","family":"Fu","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Chemical Resource Engineering Beijing Advanced Innovation Center for Soft Matter Science and Engineering Beijing University of Chemical Technology  Beijing 100029 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Shixin","family":"Meng","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Chemical Resource Engineering Beijing Advanced Innovation Center for Soft Matter Science and Engineering Beijing University of Chemical Technology  Beijing 100029 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Lingwei","family":"Xue","sequence":"additional","affiliation":[{"name":"Yaoshan Laboratory Pingdingshan University  Pingdingshan Henan 467000 P. 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