Abstract

Knowledge of the ratios between different polarizability tensor elements of a chemical group in a molecule is crucial for quantitative interpretation and polarization analysis of its coherent anti-stokes raman spectra (CARS) and coherent anti-stokes hyper-raman spectra (CAHRS). The hyperpolarizability derivative model along with experimentally obtained Raman and Hyper-Raman depolarization ratios could be used to obtain such tensor ratios for the CH3, CH2, and CH groups. Such treatment can be used to quantitatively analyze and simulate the intensity and field polarization dependence in the CARS and CAHRS spectra for the symmetric and asymmetric stretching modes of CH3 groups, respectively.

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