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Herein, we present a rational design strategy to protect photoinduced carbonyl free radical emission through electrostatic interaction and spin delocalization effects. The host\u2010guest system is constructed from tricarbonyl\u2010substituted benzene molecules and a series of imidazolium ionic liquids as the guest and host, respectively, whereby the carbonyl anion radical emission can be in situ generated under the light irradiation and further stabilized by electrostatic interaction. More importantly, the anion species and the alkyl chain length of imidazolium ionic liquids show a noticeable effect on luminescence efficiency, with the highest radical emission efficiency is as high as 53.3\u2009% after optimizing the imidazole ionic liquid's structure, which is about four times higher than the polymer\u2010protected radical system. Theoretical calculations confirm the synergistic effect of strong electrostatic interactions and that the spin delocalization effect significantly stabilizes the radical emission. Moreover, such a radical emission system also could be integrated with a fluorescent dye to induce multi\u2010color or even white light emission with reversible temperature\u2010responsive characteristics. The radical emission system can also be used to detect different amine compounds on the basis of the emission changes and photoactivation time.<\/jats:p>","DOI":"10.1002\/anie.202305925","type":"journal-article","created":{"date-parts":[[2023,6,2]],"date-time":"2023-06-02T13:14:58Z","timestamp":1685711698000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":23,"title":["Bright Free\u2010Radical Emission in Ionic Liquids"],"prefix":"10.1002","volume":"62","author":[{"given":"Wei","family":"Zheng","sequence":"first","affiliation":[{"name":"State Key Laboratory for Modification of Chemical Fibers and Polymer Materials, Science and Technology of Eco-Textile, Ministry of Education, College of Chemistry and Chemical Engineering Donghua University  Shanghai 201620 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"XuPing","family":"Li","sequence":"additional","affiliation":[{"name":"College of Energy Materials and Chemistry Inner Mongolia University  Hohhot 010021 P. 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