Room-temperature phosphorescence (RTP) with carbon dots (CDs) can be exploited further if the mechanism of trap-state-mediated triplet-state energy transfer is understood and controlled. Herein, we developed an in situ calcination method for the preparation of a CDs@ZnAlO composite material that exhibits unique UV and visible light-excitable ultra-broad-band RTP. The ZnAlO matrix can protect the triplet emissions of CDs by the confinement effect and spin-orbit coupling. In addition, benefitting from the efficient energy transfer between the inorganic trap state and the triplet state of CDs, the special yellow to red RTP of CDs@ZnAlO composites can be realized. A slow-decaying phosphorescence at 570 nm with a lifetime of 1.05 s and a fast-decaying phosphorescence at 400 nm with a lifetime of 0.41 s were observed with UV irradiation of 290 nm, which originated from the surface and core triplet states of CDs, respectively. Based on the unique RTP performance, anti-counterfeiting and information encryption were successfully realized using the CDs@ZnAlO composites with LED light or UV light.
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