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Of particular interest is a single molecular species simultaneously featuring in multiple imaging and synergistic phototherapies; the development of such a molecular species is nevertheless a formidably challenging task. Herein, we innovatively designed and synthesized three aggregation-induced emission (AIE)-active molecules with emission in the second near-infrared (NIR-II) window, by employing 10H-indeno[1,2-b][1,2,5]thiadiazolo[3,4-g]quinoxalin-10-one as the electron acceptor, 4-(tert-butyl)-N-(4-(tert-butyl)phenyl)-N-phenylaniline as the electron donor, and different \u03c0-bridge moieties. One of those molecules, namely 4,12-bis(7-(4-(bis(4-(tert-butyl)phenyl)amino)phenyl)-2,3-dihydrothieno[3,4-b][1,4]dioxin-5-yl)-10H-indeno[1,2-b][1,2,5]thiadiazolo[3,4-g]quinoxalin-10-one (OTTITQ), is capable of affording long absorption and emission wavelengths, efficient type I reactive oxygen species generation, and high photothermal conversion efficiency. Quantum chemical calculations and molecular dynamics simulations substantiated the structure\u2013activity relationship of the molecules, the excited-state energy dissipation pathways and the impact of intramolecular motions on photophysical properties, while elucidating the mechanism of the AIE phenomenon. Moreover, OTTITQ nanoparticles offer unprecedented performance on fluorescence\u2013photoacoustic\u2013photothermal trimodal imaging-navigated photodynamic\u2013photothermal synergistic therapies for bladder cancer.<\/jats:p>","DOI":"10.1093\/nsr\/nwaf254","type":"journal-article","created":{"date-parts":[[2025,6,23]],"date-time":"2025-06-23T07:23:55Z","timestamp":1750663435000},"source":"Crossref","is-referenced-by-count":31,"title":["Unveiling photophysical mechanisms of NIR-II AIE luminogens for multimodal imaging-navigated synergistic therapies"],"prefix":"10.1093","volume":"12","author":[{"given":"Jun","family":"Zhu","sequence":"first","affiliation":[{"name":"Center for AIE Research, Shenzhen Key Laboratory of Polymer Science and Technology, Guangdong Provincial Key Laboratory of New Energy Materials Service Safety, College of Material Science and Engineering, Shenzhen University , Shenzhen 518060 ,","place":["China"]},{"name":"College of Physics and Optoelectronic Engineering, Shenzhen University , Shenzhen 518060 ,","place":["China"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yiqi","family":"Zhu","sequence":"additional","affiliation":[{"name":"The Fourth Affiliated Hospital of Soochow University, Medical Center of Soochow University, Suzhou Dushu Lake Hospital Department of Urology, , Suzhou 215123 ,","place":["China"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yuxun","family":"Ding","sequence":"additional","affiliation":[{"name":"Center for AIE Research, Shenzhen Key Laboratory of Polymer Science and Technology, Guangdong Provincial Key Laboratory of New Energy Materials Service Safety, College of Material Science and Engineering, Shenzhen University , Shenzhen 518060 ,","place":["China"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jianhong","family":"Huang","sequence":"additional","affiliation":[{"name":"Center for AIE Research, Shenzhen Key Laboratory of Polymer Science and Technology, Guangdong Provincial Key Laboratory of New Energy Materials Service Safety, College of Material Science and Engineering, Shenzhen University , Shenzhen 518060 ,","place":["China"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jiangao","family":"Li","sequence":"additional","affiliation":[{"name":"Center for AIE Research, Shenzhen Key Laboratory of Polymer Science and Technology, Guangdong Provincial Key Laboratory of New Energy Materials Service Safety, College of Material Science and Engineering, Shenzhen University , Shenzhen 518060 ,","place":["China"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jianquan","family":"Hou","sequence":"additional","affiliation":[{"name":"The Fourth Affiliated Hospital of Soochow University, Medical Center of Soochow University, Suzhou Dushu Lake Hospital Department of Urology, , Suzhou 215123 ,","place":["China"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Lei","family":"Wang","sequence":"additional","affiliation":[{"name":"Center for AIE Research, Shenzhen Key Laboratory of Polymer Science and Technology, Guangdong Provincial Key Laboratory of New Energy Materials Service Safety, College of Material Science and Engineering, Shenzhen University , Shenzhen 518060 ,","place":["China"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-0293-964X","authenticated-orcid":false,"given":"Ben Zhong","family":"Tang","sequence":"additional","affiliation":[{"name":"School of Science and Engineering, Guangdong Basic Research Center of Excellence for Aggregate Science, Shenzhen Institute of Aggregate Science and Technology, The Chinese University of Hong Kong , Shenzhen (CUHK-Shenzhen), Shenzhen 518172 ,","place":["China"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Dong","family":"Wang","sequence":"additional","affiliation":[{"name":"Center for AIE Research, Shenzhen Key Laboratory of Polymer Science and Technology, Guangdong Provincial Key Laboratory of New Energy Materials Service Safety, College of Material Science and Engineering, Shenzhen University , Shenzhen 518060 ,","place":["China"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"286","published-online":{"date-parts":[[2025,6,24]]},"reference":[{"key":"2025090406414410100_bib1","doi-asserted-by":"publisher","first-page":"209","DOI":"10.3322\/caac.21660","article-title":"Global cancer statistics 2020: GLOBOCAN estimates of incidence and mortality worldwide for 36 cancers in 185 countries","volume":"71","author":"Sung","year":"2021","journal-title":"CA Cancer J 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