Summary
A diagrammatic perturbative approach is adopted to derive the expression for the third-order polarization,P (3) which originates the anti-Stokes emission in a time-resolved CARS experiment. The various contributions toP (3) are calculated assuming that laser fields are off-resonance with respect to any electronic level of material system. The resonant part of the polarization consists of two terms, in which the roles of the pump and probe pulses at frequency ω1 are exchanged. The global expression allows the direct calculation of the signal time profile in a transient CARS experiment once a model is assumed for the laser pulse shape.
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Torre, R., Righini, R., Angeloni, L. et al. Diagrammatic representation of the third-order polarization in transient CARS. Il Nuovo Cimento D 13, 809–819 (1991). https://doi.org/10.1007/BF02452227
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DOI: https://doi.org/10.1007/BF02452227