Abstract

Two-dimensional transition metal dichalcogenides (TMD), such as WS2 and MoS2, have been shown to exhibit large second order optical nonlinearity due to their non-centrosymmetric crystalline symmetry in few odd- and mono-layers, and resonance enhancement. Here we study the second-order nonlinear susceptibility of 2D TMDs through second harmonic generation (SHG) and sum frequency generation (SFG). Using a wavelength-tunable femtosecond laser, we can characterize SHG of TMDs to obtain the second-order nonlinear susceptibility at multiple wavelengths. Along with the experimental studies, theoretical investigation of the second-order nonlinear susceptibility is also performed. With this we explore the estimation of the second-order nonlinear susceptibility of 2D TMD layered materials based on their first-order susceptibility through the experimental and theoretical verification of Miller’s Rule for these materials. Additionally, we characterize the second-order nonlinear susceptibility of 2D TMD alloys through the SFG spectroscopy.

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