In this Letter we present a new technique for attaining efficient low-background coherent Raman scattering where the Raman coherence is mediated by a tunable infrared laser in two-photon resonance with a chosen vibrational transition. In addition to the traditional benefits of conventional coherent Raman schemes, this approach offers a number of advantages including potentially higher emission intensity, reduction of nonresonant four-wave mixing background, preferential excitation of the anti-Stokes field, and simplified phase matching conditions. In particular, this is demonstrated in gaseous methane along the ν_{1} (A_{1}) and ν_{3} (T_{2}) vibrational levels using an infrared field tuned between 1400 and 1600  cm^{-1} and a 532-nm pump field. This approach has broad applications, from coherent light generation to spectroscopic remote sensing and chemically specific imaging in microscopy.

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http://dx.doi.org/10.1103/PhysRevLett.120.063602DOI Listing

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