GROUND-STATE ROTATIONAL COHERENCE SPECTROSCOPY OF JET-COOLED MOLECULES BY STIMULATED RAMAN-INDUCED FLUORESCENCE DEPLETION

We report the demonstration of a new technique of rotational coherence spectroscopy that applies to the time-domain measurement of ground-state rotational constants. The technique, stimulated Raman-induced fluorescence depletion, is a picosecond pump-probe scheme in which ground-state rotational coherences prepared via stimulated Raman scattering by the pump pulse are probed via fluorescence induced by the vibronically resonant, variably delayed probe pulse. The scheme is demonstrated with experiments on jet-cooled t-stilbene. The potential of the method and its relation to other techniques are discussed. © 1990.