Optoelectronic Properties of Nitrogen-Doped Hexagonal Graphene Quantum Dots: A First-Principles Study

Graphene quantum dots have been widely studied owing to their unique optical, electrical, and optoelectrical properties for various applications in solar devices. Here, we investigate the optoelectronic properties of hexagonal and nitrogen-doped graphene quantum dots using the first-principles method. We find that doping nitrogen atoms to hexagonal graphene quantum dots results in a significant red shift toward the visible light range as compared to that of the pristine graphene quantum dots, and the doped nitrogen atoms also induce a clear signature of anisotropy of the frontier orbitals induced by the electron correlation between the doped nitrogen atoms and their adjacent carbon atoms. Moreover, time-dependent density functional theory calculations with the M06-2X functional and 6-311++G(d,p) basis set reproduce well the experimental absorption spectra reported recently. These results provide us with a novel approach for more systematic investigations on next-generation solar devices with assembled quantum dots to improve their light selectivity as well as efficiency. © 2024 The Authors. Published by American Chemical Society.