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A semiclassical description of the simultaneous processes of two-photon absorption, two-photon excitation, and second harmonic generation in noncentrosymmetric crystals is presented. The results are generalized to include three-photon processes and third harmonic generation in centrosymmetric media. Consequences for molecular crystal excitation spectroscopy are emphasized. Similar results and observations are made for third-order wave mixing in noncentrosymmetric crystals.
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G. R. Meredith (1981) studied this question.
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