Abstract The Raman-enhanced polarization beats (REPB) with phase-conjugation geometry in carbon disulfide are investigated using chaotic and phase-diffusion models. The overall accuracy of using REPB to measure the resonant frequency of Raman-active vibrational mode is determined by the relaxation rates of the Raman mode and the molecular-reorientational grating. Different stochastic models of the laser field only affect the sixth- and fourth-order coherence function. The difference between the REPB and the fourth-order coherence on ultrafast modulation spectroscopy is discussed as well from a physical viewpoint.
Received: 27 April 1999
Revised: 01 July 1999
Accepted manuscript online:
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