Abstract
Linear Raman scattering can be described classically when excitation frequencies are used which are far from resonance with electronic absorption frequencies. If this is not the case, the scattering amplitude must be derived by quantum-mechanical calculation of the linear polarizability [1]. Similarly, CARS intensities can be obtained classically by combining the classical theory of the linear Raman effect with a simple damped, field- driven, harmonic oscillator model [2,3], whereas for the case of electronic resonances one has to use again quantum-mechanics for the determination of the CARS amplitude. The latter is given through the third-order non-linear CARS susceptibility [4].
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References
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Kiefer, W. (1982). Application of Classical Theory of CARS to Diatomic Molecules in the Gas Phase. In: Kiefer, W., Long, D.A. (eds) Non-Linear Raman Spectroscopy and Its Chemical Aplications. NATO Advanced Study Institutes Series, vol 93. Springer, Dordrecht. https://doi.org/10.1007/978-94-009-7912-3_12
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