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The mechanism of the surface chemistry of carbon dots (CDs) is revealed in the solid state by X.‐C. Shen and co‐workers in the Full Paper on page 18993 ff. Red‐emitting CDs (RCDs) are prepared, and further used to serve as solid‐state fluorescence sensory material for gaseous ammonia. More importantly, they confirm that the fluorescence response of the RCDs results from ammonia‐induced Michael addition via insertion of N into the CC group and deprotonation of the carboxyl group. [ABSTRACT FROM AUTHOR]