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This design imparts an extended molecular size, elevating the glass transition temperature (<jats:italic>T<\/jats:italic><jats:sub>g<\/jats:sub>) relative to their SMA counterparts. Consequently, it effectively suppresses the thermodynamic relaxation of the acceptor component when blended with polymer donors to construct stable polymer solar cells (PSCs). Despite their merits, the optimization of their chemical structure for further enhancing of device performance remains challenge. Different from previous reports utilizing <jats:italic>p<\/jats:italic>\u2010type linkers, here, we explore an <jats:italic>n<\/jats:italic>\u2010type linker, specifically the benzothiadiazole unit, to dimerize the SMA units via a click\u2010like Knoevenagel condensation, affording BT\u2010DL. In comparison with B\u2010DL with a benzene linkage, BT\u2010DL exhibits significantly stronger intramolecular super\u2010exchange coupling, a desirable property for the acceptor component. Furthermore, BT\u2010DL demonstrates a higher film absorption coefficient, redshifted absorption, larger crystalline coherence, and higher electron mobility. These inherent advantages of BT\u2010DL translate into a higher power conversion efficiency of 18.49\u2009% in PSCs, a substantial improvement over the 9.17\u2009% efficiency observed in corresponding devices with B\u2010DL as the acceptor. Notably, the BT\u2010DL based device exhibits exceptional stability, retaining over 90\u2009% of its initial efficiency even after enduring 1000\u2005hours of thermal stress at 90\u2009\u00b0C. This work provides a cost\u2010effective approach to the synthesis of <jats:italic>n<\/jats:italic>\u2010type linker\u2010dimerized GMAs, and highlight their potential advantage in enhancing intramolecular coupling for more efficient and durable photovoltaic technologies.<\/jats:p>","DOI":"10.1002\/anie.202403005","type":"journal-article","created":{"date-parts":[[2024,2,21]],"date-time":"2024-02-21T21:26:59Z","timestamp":1708550819000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":35,"title":["Dimeric Giant Molecule Acceptors Featuring N\u2010type Linker: Enhancing Intramolecular Coupling for High\u2010Performance Polymer Solar Cells"],"prefix":"10.1002","volume":"63","author":[{"given":"Hongyuan","family":"Fu","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":"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":"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":"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":"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. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Chunfeng","family":"Zhang","sequence":"additional","affiliation":[{"name":"National Laboratory of Solid State Microstructures, School of Physics, and Collaborative Innovation Center for Advanced Microstructures Nanjing University  Nanjing 210093 P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yuanping","family":"Yi","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"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-4341-7773","authenticated-orcid":false,"given":"Zhi\u2010Guo","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"}]}],"member":"311","published-online":{"date-parts":[[2024,3,7]]},"reference":[{"key":"e_1_2_7_1_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.chemrev.1c00955"},{"key":"e_1_2_7_2_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41578-023-00618-1"},{"key":"e_1_2_7_3_1","doi-asserted-by":"publisher","DOI":"10.1007\/s11426-021-1180-6"},{"key":"e_1_2_7_4_1","doi-asserted-by":"publisher","DOI":"10.1039\/D0CS00084A"},{"key":"e_1_2_7_5_1","doi-asserted-by":"publisher","DOI":"10.1002\/adma.201404317"},{"key":"e_1_2_7_6_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.joule.2019.01.004"},{"key":"e_1_2_7_7_1","doi-asserted-by":"publisher","DOI":"10.1093\/nsr\/nwaa189"},{"key":"e_1_2_7_8_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41565-021-01011-1"},{"key":"e_1_2_7_9_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41563-022-01244-y"},{"key":"e_1_2_7_10_1","author":"Liu K.","year":"2024","journal-title":"Joule"},{"key":"e_1_2_7_11_1","doi-asserted-by":"publisher","DOI":"10.1002\/adma.202109516"},{"key":"e_1_2_7_12_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202314420"},{"key":"e_1_2_7_13_1","doi-asserted-by":"publisher","DOI":"10.1002\/adma.202208986"},{"key":"e_1_2_7_14_1","doi-asserted-by":"publisher","DOI":"10.1002\/adma.202307292"},{"key":"e_1_2_7_15_1","doi-asserted-by":"publisher","DOI":"10.1038\/nmat5063"},{"key":"e_1_2_7_16_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41570-022-00409-2"},{"key":"e_1_2_7_17_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41566-018-0104-9"},{"key":"e_1_2_7_18_1","doi-asserted-by":"publisher","DOI":"10.1126\/science.270.5243.1789"},{"key":"e_1_2_7_19_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41563-020-00872-6"},{"key":"e_1_2_7_20_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.201707678"},{"key":"e_1_2_7_21_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202009666"},{"key":"e_1_2_7_22_1","doi-asserted-by":"publisher","DOI":"10.1002\/adma.202005942"},{"key":"e_1_2_7_23_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.nanoen.2020.104718"},{"key":"e_1_2_7_24_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.joule.2020.03.019"},{"key":"e_1_2_7_25_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.chempr.2020.08.003"},{"key":"e_1_2_7_26_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202201844"},{"key":"e_1_2_7_27_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41560-022-01155-x"},{"key":"e_1_2_7_28_1","doi-asserted-by":"publisher","DOI":"10.1007\/s11426-022-1281-0"},{"key":"e_1_2_7_29_1","doi-asserted-by":"publisher","DOI":"10.1002\/advs.202202513"},{"key":"e_1_2_7_30_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.joule.2023.09.001"},{"key":"e_1_2_7_31_1","author":"Lee J.-W.","year":"2024","journal-title":"Adv. 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