Comparison of the coherent anti-Stokes and coherent Stokes Raman line shapes of the ν1 line of β-carotene near a one photon resonance

Abstract

Experiments to detemine the signs of the imaginary damping factors in the resonance denominators of the expressions for the third order susceptibilities governing coherent anti‐Stokes and coherent Stokes Raman spectroscopy (CARS and CSRS) have been carried out using the ν₁ line of β‐carotene. The experimental results are compared to the two different theoretical results predicted by the fully quantum mechanical and the semiclassical calculations for the third order susceptibilities for CARS and CSRS.