Abstract
We present the results of a detailed first-principle calculation of the nonlinear susceptibility. The quantum-mechanical expression for χ (3) derived by fourth-order perturbation theory consists of products of the Raman polarizability tensor, each of them representing a two-photon process. By using the well-known molecular constants for the iodine molecule, these tensor components can be calculated numerically “ab initio”. The results are in good agreement with the experimental CARS spectra. We are able to explain the influence of pump laser frequency, temperature, line width, and non-resonant background, respectively.
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