Electronic and Optical Properties of Graphene Quantum Dots: The Role of Many-Body Effects

Abstract

The electronic structure and optical properties of hexagonal armchair and zigzag-edged graphene quantum dots (GQDs) are investigated within the framework of many-body perturbation theory. Many-body effects are significant due to quantum confinement and reduced screening. The quasi-particle corrections and exciton binding energies can be several eV, much larger than those of other carbon allotropes with higher dimensionality. All the GQDs show similar absorption spectra when electron–hole interaction is included, with a prominent peak emerging below the absorption onset of the noninteracting spectrum. This peak is contributed by a pair of double-degenerate excited states originating from the transitions between degenerate frontier orbitals. The spin singlet–triplet splitting is closely related to the electron–hole overlap, which can be approximately measured by the overlap between frontier orbitals involved in the optical transitions. The strong many-body effects in GQDs should be of great importance in optoelectronic applications.