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.
© 1985 Optical Society of America
S. A. Akhmanov, N. I. Koroteev, S. A. Magnitskii, V. B. Morozov, A. P. Tarasevich, and V. G. Tunkin, "Time-domain coherent active Raman spectroscopy of a free-nitrogen jet," J. Opt. Soc. Am. B 2, 640-648 (1985)