The frequency dispersion of χ(3) of conjugated polyenes is calculated using equations of motion which provide an anharmonic (exciton) oscillator picture. Quantum confinement of the relative electron–hole motion is shown to play an important role in determining the magnitude of χ(3). The nature of the two-photon resonance observed in two-photon absorption and third harmonic generation is discussed, and the electroabsorption spectrum is calculated for a broad range of polyene sizes with up to 160 double bonds.
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Wang et al. (1992) studied this question.
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