VIBRATIONAL QUANTUM BEATS OBSERVED BY RAMAN-INDUCED OPTICAL KERR-EFFECT

Ultra fast molecular motion in liquids may be studied in the time domain with the pump/probe optical heterodyne-detected (OHD) Raman-induced optical Kerr effect (RIKE) technique, which makes use of ultra short pulses from a mode-locked laser. The oscillatory signal observed is attributed to vibrational quantum interference, and a detailed theoretical account is provided. Tn the framework of linear response theory, the theoretical development of this work follows two different approaches: the density matrix formalism in the Schrodinger representation and the Hellwarth formalism involving the evaluation of the time correlation of linear susceptibility tensors. An unambiguous explanation of the decay, in addition to the oscillation, observed in OHD-RIKE is also provided.