Hyper Rayleigh scattering (HRS) was used to measure the second-order nonlinear susceptibility, χ, for liquid exfoliated WS monolayers. To the best of our knowledge, it is the first reported application of the HRS technique to assess the bulk-like χ of a two-dimensional (2D) material. The concentration-dependent HRS signal indicated a 4.90±0.30×10 esu first hyperpolarizability for 42 nm WS monolayers under 1064 nm laser irradiation using para-nitroaniline as an external reference. The corresponding value of χxxx(2) was calculated to be 460±28 pm V. This was within 46% of independent density functional theory predictions. Agreement with theory was improved over related microscopy-based approaches. These results support the use of HRS to evaluate 2D materials for nonlinear frequency mixing applications.
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