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Herein, we report a facile chiral assembly strategy that enables concurrent CPL and three\u2010photon excitation fluorescence (3PEF) through the interaction of achiral pyridinium\u2010based homodimers with calf thymus DNA (\n                    <jats:italic>ct<\/jats:italic>\n                    DNA). Specifically, two homodimers, designated\n                    <jats:bold>LD<\/jats:bold>\n                    and\n                    <jats:bold>FD<\/jats:bold>\n                    , were precisely designed and synthesized to feature distinct spatial configurations. The linear\n                    <jats:bold>LD<\/jats:bold>\n                    , with its narrow molecular thickness, binds preferentially to the minor groove of\n                    <jats:italic>ct<\/jats:italic>\n                    DNA\n                    <jats:italic>via<\/jats:italic>\n                    electrostatic interactions. This association facilitated efficient chirality transfer from the DNA scaffold while simultaneously triggering 3PEF through effective suppression of nonradiative decay, ultimately yielding a pronounced CPL signal. Collectively, this work not only provided a viable strategy for designing achiral small organic molecules compatible with nucleic acid but also elegantly addresses the longstanding challenge of achieving integrated CPL and NIR\u2010window fluorescence imaging.\n                  <\/jats:p>","DOI":"10.1002\/smll.75575","type":"journal-article","created":{"date-parts":[[2026,9,1]],"date-time":"2026-09-01T06:43:11Z","timestamp":1788244991000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["<i>ct<\/i>\n                    DNA\u2010Driven Helical Assembly of Achiral Dimers: Simultaneous Activation of Three\u2010Photon Fluorescence and Circularly Polarized Luminescence"],"prefix":"10.1002","author":[{"given":"Junjun","family":"Wang","sequence":"first","affiliation":[{"name":"Anhui Engineering Laboratory For Medicinal and Food Homologous Natural Resources Exploration Department of Chemistry and Pharmaceutical Engineering Hefei Normal University Hefei People's Republic of China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xuan","family":"Zhao","sequence":"additional","affiliation":[{"name":"School of Chemistry and Chemical Engineering Key Laboratory of Structure and Functional Regulation of Hybrid Materials, Ministry of Education Key Laboratory of Functional Inorganic Materials Chemistry of Anhui Province Key Laboratory of Chemistry for Inorganic\/Organic Hybrid Functionalized Materials of Anhui Province Anhui University Hefei People's Republic of China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-5093-0367","authenticated-orcid":false,"given":"Shengyu","family":"Shi","sequence":"additional","affiliation":[{"name":"School of Chemistry and Environmental Engineering Anhui Province Engineering Research Center of Critical Electronic Materials ; Anhui Polytechnic University Wuhu People's Republic of China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Haoyue","family":"Wu","sequence":"additional","affiliation":[{"name":"Anhui Zhongzhi Technology Co., LTD Hefei People's Republic of China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Liang","family":"Yang","sequence":"additional","affiliation":[{"name":"Anhui Engineering Laboratory For Medicinal and Food Homologous Natural Resources Exploration Department of Chemistry and Pharmaceutical Engineering Hefei Normal University Hefei People's Republic of China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Aidong","family":"Wang","sequence":"additional","affiliation":[{"name":"Key Laboratory of Drug Design Huangshan University Huangshan People's Republic of China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-2906-0125","authenticated-orcid":false,"given":"Bin","family":"Zheng","sequence":"additional","affiliation":[{"name":"Anhui Engineering Laboratory For Medicinal and Food Homologous Natural Resources Exploration Department of Chemistry and Pharmaceutical Engineering Hefei Normal University Hefei People's Republic of China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jinmiao","family":"Zhu","sequence":"additional","affiliation":[{"name":"Anhui Engineering Laboratory For Medicinal and Food Homologous Natural Resources Exploration Department of Chemistry and Pharmaceutical Engineering Hefei Normal University Hefei People's Republic of China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-8128-9402","authenticated-orcid":false,"given":"Xiaojiao","family":"Zhu","sequence":"additional","affiliation":[{"name":"School of Chemistry and Chemical Engineering Key Laboratory of Structure and Functional Regulation of Hybrid Materials, Ministry of Education Key Laboratory of Functional Inorganic Materials Chemistry of Anhui Province Key Laboratory of Chemistry for Inorganic\/Organic Hybrid Functionalized Materials of Anhui Province Anhui University Hefei People's Republic of China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-9583-2595","authenticated-orcid":false,"given":"Hongping","family":"Zhou","sequence":"additional","affiliation":[{"name":"School of Chemistry and Chemical Engineering Key Laboratory of Structure and Functional Regulation of Hybrid Materials, Ministry of Education Key Laboratory of Functional Inorganic Materials Chemistry of Anhui Province Key Laboratory of Chemistry for Inorganic\/Organic Hybrid Functionalized Materials of Anhui Province Anhui University Hefei People's Republic of China"},{"name":"School of Chemistry and Environmental Engineering Anhui Province Engineering Research Center of Critical Electronic Materials ; Anhui Polytechnic University Wuhu People's Republic of China"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2026,8,31]]},"reference":[{"key":"e_1_2_7_2_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.ccr.2025.217173"},{"key":"e_1_2_7_3_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202515768"},{"key":"e_1_2_7_4_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.ccr.2019.06.017"},{"key":"e_1_2_7_5_1","doi-asserted-by":"publisher","DOI":"10.1039\/d4nr03743j"},{"key":"e_1_2_7_6_1","doi-asserted-by":"publisher","DOI":"10.1039\/d5ob00086f"},{"key":"e_1_2_7_7_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.6c03689"},{"key":"e_1_2_7_8_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202407495"},{"key":"e_1_2_7_9_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202523463"},{"key":"e_1_2_7_10_1","doi-asserted-by":"publisher","DOI":"10.1002\/adma.202519007"},{"key":"e_1_2_7_11_1","doi-asserted-by":"publisher","DOI":"10.1042\/bst20253138"},{"key":"e_1_2_7_12_1","doi-asserted-by":"publisher","DOI":"10.1039\/C9TC04508B"},{"key":"e_1_2_7_13_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.9b03305"},{"key":"e_1_2_7_14_1","doi-asserted-by":"publisher","DOI":"10.1021\/accountsmr.4c00374"},{"key":"e_1_2_7_15_1","doi-asserted-by":"publisher","DOI":"10.1002\/agt2.168"},{"key":"e_1_2_7_16_1","doi-asserted-by":"publisher","DOI":"10.1126\/science.2321027"},{"key":"e_1_2_7_17_1","doi-asserted-by":"publisher","DOI":"10.1002\/adfm.202408594"},{"key":"e_1_2_7_18_1","doi-asserted-by":"publisher","DOI":"10.1002\/adfm.202404709"},{"key":"e_1_2_7_19_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.3c05957"},{"key":"e_1_2_7_20_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41583\u2010025\u201000937\u2010y"},{"key":"e_1_2_7_21_1","doi-asserted-by":"publisher","DOI":"10.1002\/smll.202403994"},{"key":"e_1_2_7_22_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41592\u2010020\u20100819\u20107"},{"key":"e_1_2_7_23_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.4c13516"},{"key":"e_1_2_7_24_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.jechem.2025.07.043"},{"key":"e_1_2_7_25_1","doi-asserted-by":"publisher","DOI":"10.1021\/acsnano.5c10093"},{"key":"e_1_2_7_26_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202523661"},{"key":"e_1_2_7_27_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.analchem.4c03788"},{"key":"e_1_2_7_28_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.analchem.5c05382"},{"key":"e_1_2_7_29_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.biomaterials.2018.05.050"},{"key":"e_1_2_7_30_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.molliq.2020.112672"},{"key":"e_1_2_7_31_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.4c03254"},{"key":"e_1_2_7_32_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.201813900"},{"key":"e_1_2_7_33_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.cej.2025.163896"},{"key":"e_1_2_7_34_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.5c20599"},{"key":"e_1_2_7_35_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.201804402"},{"key":"e_1_2_7_36_1","doi-asserted-by":"publisher","DOI":"10.1021\/acsmaterialslett.5c00347"},{"key":"e_1_2_7_37_1","doi-asserted-by":"publisher","DOI":"10.1002\/chem.202300182"}],"container-title":["Small"],"original-title":[],"language":"en","link":[{"URL":"https:\/\/onlinelibrary.wiley.com\/doi\/pdf\/10.1002\/smll.75575","content-type":"application\/pdf","content-version":"vor","intended-application":"text-mining"},{"URL":"https:\/\/onlinelibrary.wiley.com\/doi\/full-xml\/10.1002\/smll.75575","content-type":"application\/xml","content-version":"vor","intended-application":"text-mining"},{"URL":"https:\/\/onlinelibrary.wiley.com\/doi\/pdf\/10.1002\/smll.75575","content-type":"unspecified","content-version":"vor","intended-application":"similarity-checking"}],"deposited":{"date-parts":[[2026,9,1]],"date-time":"2026-09-01T06:43:12Z","timestamp":1788244992000},"score":1,"resource":{"primary":{"URL":"https:\/\/onlinelibrary.wiley.com\/doi\/10.1002\/smll.75575"}},"subtitle":[],"short-title":[],"issued":{"date-parts":[[2026,8,31]]},"references-count":36,"alternative-id":["10.1002\/smll.75575"],"URL":"https:\/\/doi.org\/10.1002\/smll.75575","archive":["Portico"],"relation":{},"ISSN":["1613-6810","1613-6829"],"issn-type":[{"value":"1613-6810","type":"print"},{"value":"1613-6829","type":"electronic"}],"subject":[],"published":{"date-parts":[[2026,8,31]]},"assertion":[{"value":"2026-05-09","order":0,"name":"received","label":"Received","group":{"name":"publication_history","label":"Publication History"}},{"value":"2026-08-25","order":2,"name":"accepted","label":"Accepted","group":{"name":"publication_history","label":"Publication History"}},{"value":"2026-08-31","order":3,"name":"published","label":"Published","group":{"name":"publication_history","label":"Publication History"}}],"article-number":"e75575"}}