Solid-state multicolor carbon dots (CDs) have attracted tremendous attention due to their wide applications. However, the fluorescence quenching of solid-state CDs occurs due to the π-π stacking or energy transfer between adjacent carbon dots. In addition, it is difficult to observe the afterglow of solid-state CDs due to their self-quenching and deliquescence. Here, electrochemically prepared multicolor CDs emit the solid-state fluorescence and afterglow emission with lifetimes up to 657 ms by embedding the CDs into urea matrix. More importantly, the surface amino groups and C = O bonds regulate the afterglow emission of CDs from phosphorescence and thermally activated delayed fluorescence at room temperature. Surface amino groups of multicolor CDs can enhance the spin–orbit coupling, increase the intersystem crossing (ISC) and reverse intersystem crossing (RISC). Thus it can promote the generation of triple excited states and regulate the singlet–triplet energy gap value from 0.384 to 0.026 eV. The formation of covalent bonds stabilizes the single and triple excited states and inhibits the non-radiative recombination, which achieves the enhanced fluorescence and visual afterglow of multicolor CDs. The fluorescence and afterglow CDs can be applied to dual signal imaging and anti-counterfeiting, which broadens the practical applications for solid-state CDs via surface state modulation.
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