Abstract
We discuss a technique for nonlinear Raman spectroscopy that utilizes two orthogonally polarized, frequency-degenerate pump waves whose relative phase is modulated. A phase-modulated signal wave results from the mixing of the pump waves and a probe wave through the third-order, nonlinear susceptibility χ3. Heterodyne detection of the signal wave yields signals linear in χ3, permits measurement of both the real and the imaginary parts of χ3, and routinely provides shot-noise-limited sensitivities. Expressions for signal voltages are derived and typical spectra quantitatively analyzed.
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