Measurement of Vibrationally Resonantχ(3)and the Feasibility of New Vibrational Spectroscopies

In order to determine the feasibility for a new family of nonlinear four-wave-mixing methods based on resonantly enhanced nuclear polarizations, the enhancement of a singly vibrationally resonant, nondegenerate, nonparametric process is measured using an interferometric method. The measurement shows that the resonant nuclear ${\chi }^{\left(3\right)}$ polarization is much larger than the nonresonant electronic ${\chi }^{\left(3\right)}$ polarization for typical infrared transitions and new spectroscopic methods based on vibrational coherences are feasible.