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Here, we demonstrate that tuning the strength of anion\u2013\u03c0\n                    <jats:sup>+<\/jats:sup>\n                    interactions in pyridinium\u2010based contact ion pairs (CIPs) enables exceptionally fast room\u2010temperature phosphorescence (RTP) spanning 540 to 605\u00a0nm and, with radiative rates reaching 5.2\u00d710\n                    <jats:sup>5<\/jats:sup>\n                    s\n                    <jats:sup>\u22121<\/jats:sup>\n                    , places this crystalline material among the fastest known organic phosphors. By systematically tuning electron deficiency, steric confinement, and CIP organization through mono\u2010 and dicarboxyester\u2010functionalized pyridinium iodides, we achieved unusually short and highly polarized I\n                    <jats:sup>\u2212<\/jats:sup>\n                    \u2013\u03c0\n                    <jats:sup>+<\/jats:sup>\n                    tunable contacts that approach 3.50 \u00c5. Structural analysis reveals not only tightly bound, sandwich\u2010like, and columnar\u2010organized ion pairs but also unexpected dynamic behavior, including reversible, thermally activated anion drift in the solid state. Collectively, these solid state features engender strongly coupled iodide \u2192 \u03c0\n                    <jats:sup>+<\/jats:sup>\n                    charge\u2010transfer states with enhanced spin\u2013orbit coupling, thereby promoting ultrafast intersystem crossing. Spectroscopic and theoretical studies identify an intensity\u2010borrowing mechanism within the charge\u2010transfer manifold that underlies the accelerated phosphorescence and\/or thermally stimulated delayed phosphorescence. The resulting materials show promising X\u2010ray scintillation performance. Our work establishes anion\u2013\u03c0\n                    <jats:sup>+<\/jats:sup>\n                    engineering as a general and previously underexploited strategy for achieving high\u2010rate, metal\u2010free phosphorescence.\n                  <\/jats:p>","DOI":"10.1002\/anie.4386683","type":"journal-article","created":{"date-parts":[[2026,8,28]],"date-time":"2026-08-28T16:41:28Z","timestamp":1787935288000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Orchestrating Anion\u2013\u03c0\n                    <sup>+<\/sup>\n                    Interactions to Accelerate Metal\u2010Free Room\u2010Temperature Phosphorescence"],"prefix":"10.1002","volume":"65","author":[{"ORCID":"https:\/\/orcid.org\/0009-0009-2453-4166","authenticated-orcid":false,"given":"Eetu","family":"Hakkarainen","sequence":"first","affiliation":[{"name":"Department of Chemistry and Sustainable Technology University of Eastern Finland  Joensuu Finland"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Corentin","family":"Montagne","sequence":"additional","affiliation":[{"name":"Department of Chemistry and Sustainable Technology University of Eastern Finland  Joensuu Finland"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Hao\u2010Cheng","family":"Lin","sequence":"additional","affiliation":[{"name":"Department of Materials Science and Engineering National Tsing\u2010Hua University  Hsinchu Taiwan"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0008-6976-9551","authenticated-orcid":false,"given":"Chen\u2010Yu","family":"Lin","sequence":"additional","affiliation":[{"name":"Department of Chemistry National Taiwan University  Taipei Taiwan"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Khai\u2010Nghi","family":"Truong","sequence":"additional","affiliation":[{"name":"Rigaku Europe SE  Neu\u2010Isenburg Germany"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Po\u2010Yu","family":"Chen","sequence":"additional","affiliation":[{"name":"Advanced Packaging Instrumentation and Metrology Laboratory Industrial Technology Research Institute  Hsinchu Taiwan"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-0323-3785","authenticated-orcid":false,"given":"Anton","family":"Nechaev","sequence":"additional","affiliation":[{"name":"Department of Chemistry Nanoscience Center University of Jyv\u00e4skyl\u00e4  Jyv\u00e4skyl\u00e4 Finland"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-4487-8707","authenticated-orcid":false,"given":"Fabien B. 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