Precise characterization of the Raman nonlinearity in benzene using nonlinear interferometry

Abstract

Using a newly developed technique which we term two-beam nonlinear interferometry, we report accurate self-consistent determinations of both the real and imaginary parts of the third-order nonlinear optical susceptibility χ11113(−ω,ω,ωo,−ωo) in benzene including resonant Raman contributions from the 992-cm−1 mode. These measurements provide accurate values for the peak Raman cross section, nonlinear refractive index, and electronic hyperpolarizability, thus enabling the direct comparison of Raman, nonlinear refractivity, and frequency-mixing studies.