The interference between the contributions of two Raman resonances to the third-order susceptibility χ⁽³⁾ has been observed in a liquid mixture of benzene and cyclohexane. Utilizing three variable laser frequencies, χ⁽³⁾(-ω₃,ω₀,ω₁,-ω₂) was measured in a parametric mixing experiment as a function of the intermediate frequencies ω₀-ω₂ and ω₁-ω₂ which are near different Raman resonances. Detailed Raman spectra are used to give excellent theoretical fits to the experimental curves. The usefulness of this extension of the well-known three-wave mixing, or CARS (coherent anti-Stokes Raman spectroscopy), experiment in calibrating different two-photon cross sections is discussed.
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Lotem et al. (1976) studied this question.
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