Abstract
The incoherent probing of nonequilibrium vibrational population via antiStokes Raman scattering served as the first tool for direct measurements of vibrational lifetimes in liquids.1 Small Raman scattering cross sections and ultrafast relaxation time constants made these experiments very difficult and hindered the exploitation of the full potential of this technique, especially in the frequency domain. For a limited frequency range this shortcut has been overcome recently.2 We report on an experimental setup allowing the detection of rather complete relaxation pathways after resonant infrared excitation of a specific vibrational mode in a pure liquid by simultaneously monitoring all involved Raman active modes. Intense tunable infrared excitation and green probing pulses giving a time resolution of 1.5 ps are derived from a modelocked allsolid-state laser.3 Information about the reorientation dynamics is obtained using different Pump-Probe polarization schemes.
© 1996 Optical Society of America
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