Theoretical Development of Third-Order Susceptibility as Related to Coherent Antistokes Raman Spectroscopy (CARS).
NAVAL RESEARCH LAB WASHINGTON D C
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The basic theory for coherent anti-stokes Raman spectroscopy has been developed by two methods a classical approach and a quantum mechanical development. Standard methods of perturbation theory, Maxwells equation, harmonic oscillator approximation, and density matrix theory are applied to the third-order nonlinear effect of generating anti-Stokes photons from the mixing of two intense laser beams. Each mathematical step has been explicitly included in the derivations comparisons between the expressions obtained here and those published in the literature are made. Where possible, clarification with respect to differences of factors of 2 or 3 which appear in various references have been included.