Time-Resolved Two-Color Optical Coherence Experiments

Abstract

Coherent Raman experiments have been shown to be very effective in studying the vibrational dynamics of molecules in the condensed phase (1). When in the excitation process two different frequencies are being used, vibrational mode selectivity can be achieved,and quite often electronic resonances can be used to enhance the Raman scattering cross-section (2). It is also well known that such coherence Raman experiments can be performed in either the frequency — or time-domain and that the choice of technique depends on the particular problem. These techniques are therefore complementary in the same way as holeburning and photon echoes for the study of electronic transitions. We note that time-domain experiments are mandatory for those cases where we wish to study a transient species.