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By tailoring the geometric connectivity of NDI\u2013pyrene conjugates (NPCs), we control whether CT channels remain confined or segregate into parallel pathways. Confined topologies localize electron\u2013hole pairs to form emissive CT states, while segregated double\u2010cable architectures facilitate long\u2010range charge migration for visible\u2010light\u2010driven H\n                    <jats:sub>2<\/jats:sub>\n                    evolution. Comprehensive structural and photophysical analyses collectively reveal how topology transforms excited\u2010state dynamics into distinct photochemical outcomes. This study highlights the design principle of using geometric confinement to link supramolecular assembly with photocatalytic function.\n                  <\/jats:p>","DOI":"10.1002\/anie.3562192","type":"journal-article","created":{"date-parts":[[2026,4,9]],"date-time":"2026-04-09T10:50:22Z","timestamp":1775731822000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":1,"title":["A Decoupled\u2010Motif Strategy Directs Supramolecular Charge\u2010Transfer Architectures Toward Efficient Photocatalytic H\n                    <sub>2<\/sub>\n                    Evolution"],"prefix":"10.1002","volume":"65","author":[{"given":"Wei\u2010Yuan","family":"Lo","sequence":"first","affiliation":[{"name":"Department of Chemistry National Taiwan University  Taipei Taiwan"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Chin\u2010Hong","family":"Goh","sequence":"additional","affiliation":[{"name":"Department of Chemistry National Taiwan University  Taipei Taiwan"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Chen\u2010Yu","family":"Lin","sequence":"additional","affiliation":[{"name":"Department of Chemistry National Taiwan University  Taipei Taiwan"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Bing\u2010Jun","family":"Zhong","sequence":"additional","affiliation":[{"name":"Department of Chemistry National Taiwan University  Taipei Taiwan"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-8925-7747","authenticated-orcid":false,"given":"Pi\u2010Tai","family":"Chou","sequence":"additional","affiliation":[{"name":"Department of Chemistry National Taiwan University  Taipei Taiwan"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Wei\u2010Tsung","family":"Chuang","sequence":"additional","affiliation":[{"name":"National Synchrotron Radiation Research Center  Hsinchu Taiwan"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-4799-4730","authenticated-orcid":false,"given":"Chien\u2010Lung","family":"Wang","sequence":"additional","affiliation":[{"name":"Department of Chemistry National Taiwan University  Taipei Taiwan"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2026,4,9]]},"reference":[{"key":"e_1_2_8_2_1","doi-asserted-by":"publisher","DOI":"10.1021\/ja00170a016"},{"key":"e_1_2_8_3_1","doi-asserted-by":"publisher","DOI":"10.1002\/(SICI)1099\u20101395(199705)10:5<254::AID\u2010POC875>3.0.CO;2\u20103"},{"key":"e_1_2_8_4_1","doi-asserted-by":"publisher","DOI":"10.1039\/c2sc20045g"},{"key":"e_1_2_8_5_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.chemmater.6b00671"},{"key":"e_1_2_8_6_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.cgd.7b01385"},{"key":"e_1_2_8_7_1","doi-asserted-by":"publisher","DOI":"10.1039\/B615103E"},{"key":"e_1_2_8_8_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.201307756"},{"key":"e_1_2_8_9_1","doi-asserted-by":"publisher","DOI":"10.1039\/C3TC32062F"},{"key":"e_1_2_8_10_1","doi-asserted-by":"publisher","DOI":"10.1002\/ange.202218142"},{"key":"e_1_2_8_11_1","doi-asserted-by":"publisher","DOI":"10.1002\/adma.202406083"},{"key":"e_1_2_8_12_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202412712"},{"key":"e_1_2_8_13_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.5c01841"},{"key":"e_1_2_8_14_1","doi-asserted-by":"publisher","DOI":"10.1002\/cjoc.70088"},{"key":"e_1_2_8_15_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.accounts.7b00124"},{"key":"e_1_2_8_16_1","doi-asserted-by":"publisher","DOI":"10.1039\/C6CP07417K"},{"key":"e_1_2_8_17_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.5b08257"},{"key":"e_1_2_8_18_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.4c00201"},{"key":"e_1_2_8_19_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.ccr.2025.217488"},{"key":"e_1_2_8_20_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.4c13800"},{"key":"e_1_2_8_21_1","doi-asserted-by":"publisher","DOI":"10.1039\/D4SC03359K"},{"key":"e_1_2_8_22_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.201208397"},{"key":"e_1_2_8_23_1","doi-asserted-by":"publisher","DOI":"10.1021\/ja802757w"},{"key":"e_1_2_8_24_1","doi-asserted-by":"publisher","DOI":"10.1039\/b819877b"},{"key":"e_1_2_8_25_1","doi-asserted-by":"publisher","DOI":"10.1002\/adma.201100399"},{"key":"e_1_2_8_26_1","doi-asserted-by":"publisher","DOI":"10.1073\/pnas.0905655106"},{"key":"e_1_2_8_27_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.jpclett.6b02310"},{"key":"e_1_2_8_28_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.201310902"},{"key":"e_1_2_8_29_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.jpcc.7b06660"},{"key":"e_1_2_8_30_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.1c05793"},{"key":"e_1_2_8_31_1","unstructured":"C. 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