Effects of beam polarization on coherent anti-Stokes Raman scattering using noisy light

The effects of different linear polarization schemes on the noisy light‐based coherent anti‐Stokes Raman scattering [I(2)CARS] signal were investigated. It was found that certain polarization schemes can selectively shut down the contributions from terms represented by various factorized time correlation (FTC) diagrams to the I(2)CARS spectrogram. FTC diagram analysis was used in conjunction with the symmetry properties of the hyperpolarizability to provide a theoretical understanding of this phenomenon and serve as the basis for simulation of the I(2)CARS spectrogram. Striking agreement is seen between the simulations and the experimental results for benzene and several methylated benzene derivatives. Copyright © 2005 John Wiley & Sons, Ltd.