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Stimuli\u2010responsive organic materials utilizing triplet excitons are particularly attractive owing to their pronounced sensitivity to solid\u2010state packing. However, crystallinity\u2010preserving reversible structural switching that enables simultaneous control over X\u2010ray\u2010excited luminescence (scintillation) remains largely unexplored. Herein, donor\u2010acceptor halogen\u2010bonded cocrystals were constructed using\n                    <jats:italic>N<\/jats:italic>\n                    ,\n                    <jats:italic>N<\/jats:italic>\n                    \u2032\u2010bis(n\u2010butyl)pyromellitic diimide (Bu\n                    <jats:sub>2<\/jats:sub>\n                    PMDI) and 3,6\u2010dibromocarbazole (Br\n                    <jats:sub>2<\/jats:sub>\n                    Cz) or 3,6\u2010diiodocarbazole (I\n                    <jats:sub>2<\/jats:sub>\n                    Cz). The green cocrystal Bu\n                    <jats:sub>2<\/jats:sub>\n                    PMDI\u2010Br\n                    <jats:sub>2<\/jats:sub>\n                    Cz\u2010G exhibits room\u2010temperature phosphorescence (RTP) and bright radioluminescence, whereas its orange polymorph is nearly non\u2010emissive. In contrast, the I\n                    <jats:sub>2<\/jats:sub>\n                    Cz\u2010based cocrystal displays thermally activated delayed fluorescence (TADF), representing an alternative triplet exciton utilization pathway. Notably, mild organic\u2010vapor stimulation triggers reversible order\u2010to\u2010order polymorphic interconversion of Bu\n                    <jats:sub>2<\/jats:sub>\n                    PMDI\u2010Br\n                    <jats:sub>2<\/jats:sub>\n                    Cz, which reorganizes halogen\u2010bonding motifs and, thus achieves crystallinity\u2010retained \u201con\/off\u201d switching of radioluminescence. Benefiting from efficient triplet exciton utilization, Bu\n                    <jats:sub>2<\/jats:sub>\n                    PMDI\u2010Br\n                    <jats:sub>2<\/jats:sub>\n                    Cz\u2010G enables high\u2010resolution static X\u2010ray imaging (37\u00a0lp mm\n                    <jats:sup>\u22121<\/jats:sup>\n                    ) and real\u2010time dynamic imaging (2\u00a0K, 60\u00a0fps) with negligible afterglow. Furthermore, the reversible solvent\u2010triggered luminescence switching facilitates rewritable multimodal information encryption by integrating photoluminescence and radioluminescence as orthogonal readout channels. This work demonstrates cocrystal engineering as a powerful strategy for reversibly programming triplet\u2010exciton emission and X\u2010ray scintillation via structural switching in organic solids.\n                  <\/jats:p>","DOI":"10.1002\/anie.3402295","type":"journal-article","created":{"date-parts":[[2026,6,11]],"date-time":"2026-06-11T06:23:13Z","timestamp":1781158993000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":3,"title":["Stimuli\u2010Responsive Triplet Emission and X\u2010Ray Scintillation via Reversible Structural Switching in Pyromellitic Diimide Cocrystals"],"prefix":"10.1002","volume":"65","author":[{"given":"Yuxizi","family":"Guo","sequence":"first","affiliation":[{"name":"State Key Laboratory of Fluorine &amp; Nitrogen Chemicals College of Chemistry Fuzhou University  Fuzhou P. R. 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