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Here, we report two naphthalene\u2010based RTP luminophores whose phosphorescence emission is enabled by radiative decay of high\u2010lying triplet excitons. In contrast, upon cooling the dominant phosphorescence originates from the lowest\u2010lying triplet excited state, which is manifested by a red\u2010shifted emission. Photophysical and theoretical studies reveal that the unusual RTP results from thermally activated excitonic coupling between different conformations of the compounds. Aggregation\u2010regulated excitonic coupling is observed when increasing the doping concentration of the emitters in poly(methylmethacrylate) (PMMA). Further, the RTP quantum efficiency improves more than 80\u2010fold in 1,3\u2010bis(\n                    <jats:italic>N<\/jats:italic>\n                    \u2010carbazolyl)benzene (mCP) compared to that in PMMA. This design principle offers important insight into triplet excited state dynamics and has been exploited in afterglow\u2010indicating temperature sensing.\n                  <\/jats:p>","DOI":"10.1002\/anie.202206681","type":"journal-article","created":{"date-parts":[[2022,6,10]],"date-time":"2022-06-10T02:03:57Z","timestamp":1654826637000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":57,"title":["Thermally Activated and Aggregation\u2010Regulated Excitonic Coupling Enable Emissive High\u2010Lying Triplet Excitons**"],"prefix":"10.1002","volume":"61","author":[{"ORCID":"https:\/\/orcid.org\/0000-0003-4200-3712","authenticated-orcid":false,"given":"Tao","family":"Wang","sequence":"first","affiliation":[{"name":"Organic Semiconductor Centre EaStCHEM School of Chemistry University of St Andrews St Andrews KY16 9ST UK"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Joydip","family":"De","sequence":"additional","affiliation":[{"name":"Organic Semiconductor Centre EaStCHEM School of Chemistry University of St Andrews St Andrews KY16 9ST UK"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Sen","family":"Wu","sequence":"additional","affiliation":[{"name":"Organic Semiconductor Centre EaStCHEM School of Chemistry University of St Andrews St Andrews KY16 9ST UK"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Abhishek Kumar","family":"Gupta","sequence":"additional","affiliation":[{"name":"Organic Semiconductor Centre EaStCHEM School of Chemistry University of St Andrews St Andrews KY16 9ST UK"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-7183-6022","authenticated-orcid":false,"given":"Eli","family":"Zysman\u2010Colman","sequence":"additional","affiliation":[{"name":"Organic Semiconductor Centre EaStCHEM School of Chemistry University of St Andrews St Andrews KY16 9ST UK"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2022,7,4]]},"reference":[{"key":"e_1_2_8_1_1","doi-asserted-by":"publisher","DOI":"10.1021\/ja01240a030"},{"key":"e_1_2_8_2_1","unstructured":"\u00a0"},{"key":"e_1_2_8_3_2","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202011957"},{"key":"e_1_2_8_3_3","doi-asserted-by":"publisher","DOI":"10.1002\/ange.202011957"},{"key":"e_1_2_8_4_2","doi-asserted-by":"publisher","DOI":"10.1002\/adma.201904273"},{"key":"e_1_2_8_5_2","doi-asserted-by":"publisher","DOI":"10.1021\/acs.jpclett.9b02513"},{"key":"e_1_2_8_6_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.7b01574"},{"key":"e_1_2_8_7_1","unstructured":"\u00a0"},{"key":"e_1_2_8_8_2","doi-asserted-by":"publisher","DOI":"10.1002\/anie.201906312"},{"key":"e_1_2_8_8_3","doi-asserted-by":"publisher","DOI":"10.1002\/ange.201906312"},{"key":"e_1_2_8_9_2","doi-asserted-by":"publisher","DOI":"10.1002\/anie.201808861"},{"key":"e_1_2_8_9_3","doi-asserted-by":"publisher","DOI":"10.1002\/ange.201808861"},{"key":"e_1_2_8_10_2","doi-asserted-by":"publisher","DOI":"10.1016\/j.cej.2021.129167"},{"key":"e_1_2_8_11_1","unstructured":"\u00a0"},{"key":"e_1_2_8_12_2","doi-asserted-by":"publisher","DOI":"10.1002\/adma.202006752"},{"key":"e_1_2_8_13_2","doi-asserted-by":"publisher","DOI":"10.1002\/anie.201705945"},{"key":"e_1_2_8_13_3","doi-asserted-by":"publisher","DOI":"10.1002\/ange.201705945"},{"key":"e_1_2_8_14_2","doi-asserted-by":"publisher","DOI":"10.1038\/nmat2509"},{"key":"e_1_2_8_15_1","unstructured":"\u00a0"},{"key":"e_1_2_8_16_2","doi-asserted-by":"publisher","DOI":"10.1002\/adma.201807887"},{"key":"e_1_2_8_17_2","doi-asserted-by":"publisher","DOI":"10.1021\/accountsmr.1c00084"},{"key":"e_1_2_8_18_1","unstructured":"\u00a0"},{"key":"e_1_2_8_19_2","doi-asserted-by":"publisher","DOI":"10.1038\/s41566-020-00744-0"},{"key":"e_1_2_8_20_2","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202200236"},{"key":"e_1_2_8_20_3","doi-asserted-by":"crossref","first-page":"e202200236","DOI":"10.1002\/ange.202200236","volume":"134","year":"2022","journal-title":"Angew. 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