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Coherent Ro-vibrational Revivals in a Thermal Molecular Ensemble

We report an experimental and theoretical study of the evolution of vibrational coherence in a thermal ensemble of nitrogen molecules. Rotational dephasing and rephasing of the vibrational coherence is detected by coherent anti-Stokes Raman scattering. The existence of ro-vibrational coupling and the discrete energy spectrum of the rotational bath lead to a whole new class of full and fractional ro-vibrational revivals. Following the rich ro-vibrational dynamics on a nanosecond time scale with sub-picosecond time resolution enables us to determine the second-order ro-vibrational constant $gamma_e$ and assess new possibilities of controlling decoherence.