Excitation dependence and independence of photoluminescence in carbon dots and graphene quantum dots: insights into the mechanism of emission

Abstract

Excitation-dependent, multicolor emission from different varieties of 0D carbon systems has attracted immense research attention. It is generally accepted that some variants of 0D carbon exhibit excitation dependent emission, while other variants do not. A third variant exhibits both excitation dependent as well as excitation independent emission. In this work we investigate the structure, composition, steady-state emission-excitation and photoluminescence decay dynamics of three distinctly different variants of 0D carbon - amorphous carbon dots (aCDs), graphene quantum dots (GQDs) and nitrogen-doped GQDs (NGQDs). We find that despite significant differences in the structure and composition there is a striking similarity in the excitation energy dependence of the emission characteristics of these three different dots. All of them exhibit excitation energy independent emission below some threshold wavelength (lambda(th)), and above this threshold the emission becomes excitation dependent. We also demonstrate that a similar trend is apparent for nearly all variants of 0D carbon reported in the literature. The threshold wavelength correlates well with the excitation wavelength for the most intense emission and the photoluminescence excitation peaks, suggesting a common origin of light emission in these carbon dots. The findings provide important clues for developing a unified general picture for understanding the light emission mechanism in 0D carbon nanostructures.