Abstract

We demonstrate coherence measurements of single-photon-level collective excitations of vibrational states using transient coherent spontaneous Raman scattering in liquid methanol. We observe the decay of the 1033cm1 mode and coherence oscillations due to simultaneous excitation of the 2834 and 2944cm1 modes. The coherence life-times and oscillation frequencies agree with frequency-domain line-shape measurements and femtosecond coherent anti-Stokes Raman scattering measurements. The demonstrated technique is complementary to and, in some cases, simpler than traditional stimulated spectroscopy techniques in that it does not require more than one laser and is free of nonresonant background.

© 2014 Optical Society of America

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