Time-domain coherent active Raman spectroscopy of a free-nitrogen jet

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Abstract
A review of our results in time-domain coherent anti-Stokes Raman spectroscopy (CARS) of N2 molecules cooled in a supersonic jet is given. A full quantitative interpretation of the detected quantum beats, which makes it possible to determine the Trot of N2, is proposed. A noticeable increase of the dephasing cross section with the lowering of temperature is detected. The sensitivity of the CARS spectrometer was radically improved by the development of the injection-locked optical parametric oscillator, which made it possible to register the cooling of N2 to temperatures as low as 8 K.