Pressure-induced core defects and photoluminescent quenching in carbon quantum dots

Abstract

Carbon quantum dots (CDs) with favorable luminescent features for biphotonic applications have attracted much interest in modulating their photoluminescence (PL) efficiency. A surface state with various defects is believed to play a key role in the emissive intensity. Here, pressure-induced quenching of PL is observed in red emissive CDs (R-CDs) and is ascribed to defects in carbon cores upon compression. In the power-law fitting to the excitation power-dependent PL of R-CDs at high pressure, the coefficient k parameter related to the emissive mechanism decreases from 1 under ambient pressure to much less than 1 under the application of pressure, suggesting a transition from single exciton recombination to defect-related emission. With the k parameter decreasing to 0.69 at 1.6 GPa, the pressure-induced defects reduce the PL intensity by approximately one order of magnitude. Furthermore, the attenuation and broadening of the G band characterizing the sp2 hybrid structure of carbon cores in the Raman spectra for R-CDs at high pressure support that the pressure-induced lattice relaxation impairs the crystalline symmetry of the carbon core and results in the dramatic quenching of PL. Our results highlight the importance of the well-crystallized carbon core in designing CDs with high quantum yields.