Two-Photon Infrared Resonance Can Enhance Coherent Raman Scattering

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 nu(1) (A(1)) and nu(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.