Third-Order Optical Nonlinearity in Two-Dimensional Transition Metal Dichalcogenides

We present a detailed calculation of the linear and nonlinear optical response of four types of monolayer twodimensional (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 χ_μν⁽¹⁾ (-ω;ω) and nonlinear surface susceptibility tensors χ_μνζη⁽³⁾(-ω_Σ; ω_r; ω_s; ω_t) with ω_Σ=ω_r+ω_s+ω_t. Both non-degenerate and degenerate cases are studied for thirdharmonic 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 highharmonic generation in 2D materials and their heterostructures, thus enabling study of novel functionalities of 2D photonic integrated circuits.