Third-Order Optical Nonlinearity in Two-Dimensional Transition Metal Dichalcogenides**Supported in part by Laboratory of Photonics and Quantum Measurements (LPQM) at EPFL and European Graphene Flagship under Grant No. 696656, as well as Research Deputy of Sharif University of Technology

Abstract

We present a detailed calculation of the linear and nonlinear optical response of four types of monolayer two-dimensional (2D) transition-metal dichalcogenides (TMDCs), having the formula MX2 with M = Mo, W and X = S, Se. The calculations are based on 6-band tight-binding model of TMDCs, and then performing a semi-classical perturbation analysis of response functions. We numerically calculate the linear and nonlinear surface susceptibility tensors with ωΣ = ωr + ωs + ωt. Both non-degenerate and degenerate cases are studied for third-harmonic generation and nonlinear refractive index, respectively. Computational results obtained with no external fitting parameters are discussed regarding two recent reported experiments on MoS2, and thus we can confirm the extraordinarily strong optical nonlinearity of TMDCs. As a possible application, we demonstrate generation of a π/4-rotated squeezed state by means of nonlinear response of TMDCs, in a silica micro-disk resonator covered with the 2D material. Our proposed method will enable accurate calculations of nonlinear optical response, such as four-wave mixing and high-harmonic generation in 2D materials and their heterostructures, thus enabling study of novel functionalities of 2D photonic integrated circuits.