ABSTRACT
Modification of surficial functional groups among carbon quantum dots (CQDs) has been considered an efficient approach to regulate the fluorescence emission of CQDs. However, the mechanism of how surficial functional groups affect fluorescence is vague which fundamentally limits the further applications of CQDs. Here we report the concentration-dependent fluorescence and fluorescence quantum yield of nitrogen-dopped carbon quantum dots (N-CQDs). At high concentrations (≥0.188 g/L), fluorescence redshift occurs accompanied with decrease in fluorescence quantum yield. Fluorescence excitation spectra and HOMO-LUMO energy gaps calculations show that energy levels of excited states of N-CQDs are relocated via the coupling of surficial amino groups among N-CQDs. Furthermore, electron density difference maps and broadened fluorescence spectra obtained from both experimental measurement and theoretical calculation further confirm that the coupling of surficial amino groups dominates the fluorescence property and verify the formation of charge-transfer state of N-CQDs complex at high concentrations which provides pathways for efficient charge transfer. Given that charge-transfer state induced fluorescence loss and fluorescence spectra broadening are the typical characteristics of organic molecules, CQDs exhibit the optical properties of both quantum dots and organic molecules.
