Abstract
Using the femtosecond Raman-induced polarization spectroscopy (RIPS) technique, we have observed ground vibronic state rotational coherence in gaseous N 2, CO 2 and O 2. Both theoretical and experimental studies are reported. The theory is in excellent agreement with experiment. At earlier pump—probe delays, the time evolution of the polarization recurrence is well described by a rigid rotor model. Higher order spectroscopic constants are extracted from longer delay time spectra. The rotational relaxation constants for ground vibronic state N 2 and O 2 are also measured using the real-time technique.
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