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Herein, a series of dithienopyrrole\u2010based luminophores (DTP\u2010R) are developed as a single\u2010emitter system to investigate aggregation\u2010regulated excited\u2010state dynamics. By tuning the doping concentration in poly(methyl methacrylate) (PMMA), the emission evolves from monomer\u2010like to aggregate\u2010dominated states, accompanied by a continuous red shift of both prompt fluorescence (PF) and DF, as well as the coexistence of DF and RTP in the delayed spectra. Structural analysis reveals that aggregation is governed by cooperative weak intermolecular interactions, particularly S\u22ef\u03c0 interaction, rather than conventional \u03c0\u2010\u03c0 stacking. Theoretical calculations suggest that aggregation induces intermolecular charge separation, reduces the singlet\u2010triplet energy gap (\u0394E\n                    <jats:sub>ST<\/jats:sub>\n                    ), and provides more accessible triplet states, thereby favoring thermally activated RISC\u2010related DF. Temperature\u2010dependent delayed emission and ultralow\u2010concentration system DF further support a RISC\u2010mediated DF process. BPBr\u2010based host\u2010guest system regulates triplet\u2010exciton distribution through TTET, enhancing the phosphorescence contribution. As a single\u2010emitter system with concentration\u2010tunable color\u2010evolving afterglow, this system enables spatiotemporal information storage and dynamic anti\u2010counterfeiting, providing a strategy for designing organic afterglow materials with tunable excited\u2010state dynamics.\n                  <\/jats:p>","DOI":"10.1002\/advs.77357","type":"journal-article","created":{"date-parts":[[2026,8,26]],"date-time":"2026-08-26T08:46:23Z","timestamp":1787733983000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Aggregation\u2010Controlled Triplet Exciton Regulation Enables Single\u2010Emitter Color\u2010Evolving Afterglow"],"prefix":"10.1002","author":[{"ORCID":"https:\/\/orcid.org\/0009-0007-6723-9744","authenticated-orcid":false,"given":"Yu","family":"Zhang","sequence":"first","affiliation":[{"name":"Guangdong Basic Research Center of Excellence for Aggregate Science School of Science and Engineering The 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