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.
Two-dimensional materials have attracted significant interest recently for their unique optical properties compared to their bulk counterparts. Specifically, the family of transition metal dichalcogenides (TMD), such as MoS2 and WS2, have large second order nonlinear susceptibility. Extraordinary second harmonic generation and sum frequency generation have been observed. Here we investigate the second order nonlinearity of 2D materials, including TMD layered materials with dopants and defects. Experimental results and preliminary theoretical analysis will be discussed.