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Semiconducting Transition Metal Dichalcogenides (TMDs) have significantnonlinear optical effects. In this work we have used second-harmonic generation(SHG) and the four-wave mixing (FWM) spectroscopy in resonance with theexcitons in MoS2, MoSe2, and WS2 monolayers to characterize the nonlinearoptical properties of these materials. We show that trions and excitons areresponsible for enhancing the nonlinear optical response, and determine theexciton and trion energies by comparing with the photoluminescence spectra.Moreover, we extract the second and third order optical sheet susceptibilitynear exciton energies and compare with values found in the literature. We alsodemonstrate the ability to generate different nonlinear effects in a widespectral range in the visible region for monolayer MoS2, opening thepossibility of using two-dimensional materials for nonlinear optoelectronic andphotonic applications.

Second- and third-order optical susceptibilities in bidimensional semiconductors near excitons states