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Here, using a donor\u2013acceptor aggregation-induced-emission probe, we show that the onset concentration of assembly (below 200 nM) controls packing density and thereby the photophysical properties of the metastable states via different kinetic routes at room temperature. High-sensitivity ensemble photoluminescence spectroscopy and single-particle fluorescence lifetime imaging reveal pathway-dependent emission peak positions and lifetimes that both remain stable over several days. Fluorescence correlation spectroscopy shows that size distributions are largely decoupled from these photophysical changes, while all-atom molecular dynamics (MD) simulations confirm that higher onset concentrations produce denser packing, accounting for the observed redshift and longer lifetime. These results establish molecular packing density as a key determinant of the photophysics of kinetically trapped hydrophobic aggregates and provide a general room-temperature route to interrogate otherwise inaccessible nonequilibrium intermediates.<\/jats:p>","DOI":"10.1021\/acs.jpclett.6c02718","type":"journal-article","created":{"date-parts":[[2026,10,8]],"date-time":"2026-10-08T16:02:22Z","timestamp":1791475342000},"page":"12076-12083","source":"Crossref","is-referenced-by-count":0,"title":["Single-Particle\nPhotophysics Reveals Pathway-Dependent\nPacking in Kinetically Trapped Hydrophobic Aggregates"],"prefix":"10.1021","volume":"17","author":[{"given":"Miaomiao","family":"Wang","sequence":"first","affiliation":[{"name":"University of Science and Technology of China , , , ,","place":["Hefei, Anhui, China, 230026"]},{"name":"University of Science and Technology of China , , , ,","place":["Hefei, Anhui, China, 230026"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jing","family":"Zhang","sequence":"additional","affiliation":[{"name":"University of Science and Technology of China , , , ,","place":["Hefei, Anhui, China, 230026"]},{"name":"University of Science and Technology of China , , , ,","place":["Hefei, Anhui, China, 230026"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Weijian","family":"Xing","sequence":"additional","affiliation":[{"name":"University of Science and Technology of China , , , ,","place":["Hefei, Anhui, China, 230026"]},{"name":"University of Science and Technology of China , , , ,","place":["Hefei, Anhui, China, 230026"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-6509-228X","authenticated-orcid":true,"given":"Jie","family":"Zhang","sequence":"additional","affiliation":[{"name":"University of Science and Technology of China , , , ,","place":["Hefei, Anhui, China, 230026"]},{"name":"University of Science and Technology of China , , , ,","place":["Hefei, Anhui, China, 230026"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,10,8]]},"reference":[{"issue":"11","key":"2026102208023891900_cit1","doi-asserted-by":"publisher","first-page":"1304","DOI":"10.1002\/anie.199013041","article-title":"Perspectives\nin Supramolecular Chemistry\u2500From Molecular Recognition towards\nMolecular Information Processing and Self-Organization","volume":"29","author":"Lehn","year":"1990","journal-title":"Angew. 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Chem.\nLett."},{"issue":"10","key":"2026102208023891900_cit33","doi-asserted-by":"publisher","first-page":"1975","DOI":"10.1364\/AO.8.001975","article-title":"The Use\nof Photomultiplier\nTubes for Photon Counting","volume":"8","author":"Foord","year":"1969","journal-title":"Appl. Opt., AO"},{"key":"2026102208023891900_cit34","doi-asserted-by":"publisher","first-page":"3","DOI":"10.1016\/j.medpho.2014.12.001","article-title":"Fluorescence Lifetime Imaging (FLIM): Basic Concepts\nand Some Recent Developments","volume":"27","author":"Suhling","year":"2015","journal-title":"Medical Photonics"},{"issue":"6","key":"2026102208023891900_cit35","doi-asserted-by":"publisher","first-page":"377","DOI":"10.1016\/j.cocis.2012.09.003","article-title":"Fluorescence Correlation\nSpectroscopy in Colloid and\nInterface Science","volume":"17","author":"Koynov","year":"2012","journal-title":"Curr. Opin. 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