Coherent anti-Stokes Raman spectroscopy (CARS) selection rules, depolarization ratios and rotational structure

By putting the non-linear susceptibility tensors in irreducible spherical form it is found that orientation averaging, selection rules, and the angular dependence of intensity on field polarizations all follow in a straightforward way. These spherical tensor techniques are used to treat coherent anti-Stokes Raman scattering (CARS) in detail and a comparison is made with conventional Raman scattering. The selection rules for both processes are shown to be the same. The paper concludes with a brief discussion of the rotational structure in CARS