Measurement of vibrationally resonant chi((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((3)) polarization is much larger than the nonresonant electronic chi((3)) polarization for typical infrared transitions and new spectroscopic methods based on vibrational coherences are feasible.