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The effect of charge transfer (CT) in such systems, however, is largely ignored for understanding ISC and phosphorescence efficiency. Here, we unveiled a principle for producing highly\u2010efficient room\u2010temperature phosphorescence (RTP) polymer where the role of CT in diarylketone phosphors was a prerequisite. Designed diarylketones with carbonyl group substituted by aromatic rings unsymmetrically achieved superior RTP quantum yield of &gt;30% in copolymer. Detailed investigation indicated that\n                    <jats:sup>1<\/jats:sup>\n                    CT\u2192\n                    <jats:sup>3<\/jats:sup>\n                    LE (locally excited triplet state) transition with small energy gap (\u2206\n                    <jats:italic>E<\/jats:italic>\n                    <jats:sub>ST<\/jats:sub>\n                    ) and strong spin\u2010orbit coupling underlies their ultrafast ISC, as recorded by femtosecond transient absorption (fs\u2010TA) spectroscopy. When single aromatic ring was bonded to carbonyl group, singlet (S\n                    <jats:sub>1<\/jats:sub>\n                    ) and triplet (T\n                    <jats:sub>1<\/jats:sub>\n                    ) states remained LE with large \u2206\n                    <jats:italic>E<\/jats:italic>\n                    <jats:sub>ST<\/jats:sub>\n                    and weak spin\u2010orbit coupling, leading to low RTP efficiency. Finally, manufacturing organic glass in presence of trace diarylketone monomers could generate shape\u2010rich three\u2010dimensional (3D) objects with intense afterglow under room lighting, even at high\u2010temperature and wet conditions. This work advances understanding on structure\u2010property relationship in popular aromatic ketone phosphors, and paves the way for producing afterglow materials with high brightness and stability.\n                  <\/jats:p>","DOI":"10.1002\/anie.202520738","type":"journal-article","created":{"date-parts":[[2025,11,6]],"date-time":"2025-11-06T13:22:54Z","timestamp":1762435374000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":16,"title":["Near\u2010Unity Intersystem Crossing Efficiency and Bright Polymer Phosphorescence Enabled by Charge\u2010Transfer Diarylketones"],"prefix":"10.1002","volume":"64","author":[{"given":"Jiajun","family":"Song","sequence":"first","affiliation":[{"name":"Hefei National Research Center for Physical Sciences at the Microscale University of Science and Technology of China  Hefei 230026 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Physical Sciences at the Microscale University of Science and Technology of China  Hefei 230026 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Biao","family":"Chen","sequence":"additional","affiliation":[{"name":"Hefei National Research Center for Physical Sciences at the Microscale University of Science and Technology of China  Hefei 230026 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xueyu","family":"Li","sequence":"additional","affiliation":[{"name":"Hefei National Research Center for Physical Sciences at the Microscale University of Science and Technology of China  Hefei 230026 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-5187-9084","authenticated-orcid":false,"given":"Meng","family":"Zhou","sequence":"additional","affiliation":[{"name":"Hefei National Research Center for Physical Sciences at the Microscale University of Science and Technology of China  Hefei 230026 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China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-2608-6098","authenticated-orcid":false,"given":"Xuepeng","family":"Zhang","sequence":"additional","affiliation":[{"name":"Hefei National Research Center for Physical Sciences at the Microscale University of Science and Technology of China  Hefei 230026 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