Abstract

Interference between electronic and lattice contributions to the nonlinear polarization P⁽³⁾ at a Raman resonance can be used to measure the third-order electronic susceptibilities in terms of known Raman cross sections in a coherent anti- Stokes Raman scattering (CARS) experiment.¹ If the experiment is performed with ps-light pulses for excitation and probing, the decay of the coherent vibrational amplitude can be observed by recordirtg the CARS signal as a function of the delay between the probe pulse and the two excitation pulses, The present technology for generation of ultrashort optical pulses allows discriminating the resonant and nonresonant terms owing to their different time dependence.

© 1986 Optical Society of America