Linear and Nonlinear Optical Properties of Graphene Quantum Dots: A Computational Study

TL;DR

This computational study systematically analyzes the linear and nonlinear optical properties of 400 graphene quantum dots, revealing how their structure, size, and shape influence their optical behavior for photonic applications.

Contribution

It provides a comprehensive analysis of GQDs' optical properties across various structures, offering design guidelines for photonic device applications.

Findings

GQDs with inequivalent sublattice atoms have lower HOMO-LUMO gaps and higher nonlinear coefficients.

Zigzag edges are common in GQDs with notable optical properties.

Spectral shifts depend on size, shape, and topology of GQDs.

Abstract

Due to the advantage of tunability via size, shape, doping and relatively low level of loss and high extent of spatial confinement, graphene quantum dots (GQDs) are emerging as an effective way to control light by molecular engineering. The collective excitation in GQDs shows both high energy plasmon frequency along with frequencies in the terahertz (THz) region making these systems powerful materials for photonic technologies. Here, we report a systematic study of the linear and nonlinear optical properties of large varieties of GQDs (400 systems) in size and topology utilizing the strengths of both semiempirical and first-principles methods. Our detailed study shows how the spectral shift and trends in the optical nonlinearity of GQDs depends on their structure, size and shape. Among the circular, triangular, stripe, and random shaped GQDs, we find that GQDs with inequivalent sublattice atoms always possess lower HOMO-LUMO gap, broadband absorption and high nonlinear optical coefficients. Also, we find that for majority of the GQDs with interesting linear and nonlinear optical properties have zigzag edges, although reverse is not always true. We strongly believe that our findings can act as guidelines to design GQDs in optical parametric oscillators, higher harmonic generators and optical modulators.