A Dynamic Metal‐Organic Radical Emission System

Developing new organic radical emission systems and regulating their luminescence properties presents a significant challenge. Herein, we build dynamic and multi‐emission band radical luminescence systems by co‐assembling inorganic metal salts with carbonyl compounds in ionic liquids. After the assembling, dual‐band, and excitation wavelength‐dependent emission was observed upon light irradiation, one emission band originates from carbonyl radical after light irradiation, the other band from the ligand‐metal charge transfer (LMCT) state, which benefits from the charge transfer from the radicals to the metal salts. The dual emission centers also introduce excitation wavelength‐dependent properties for the molecules. In addition, three‐band emission covering the visible and near‐infrared regions can be shown when two or three kinds of metal ions are simultaneously doped into the radical system driven by the ligand‐metal‐metal charge transfer (LMMCT). Interestingly, visible light can quickly quench the radical emission of systems, thus realizing a dynamic luminescence. The LMMCT effect and strong supramolecular interactions significantly improve the photoluminescence quantum yield by up to 67.2%. Moreover, such materials can be successfully used for detecting radioactive metal ions and information encryption. This study develops a platform for manufacturing various metal‐organic radical emission systems with diverse properties.