Various nonlinear optical polarizabilities are derived and evaluated by time dependent Hartree–Fock theory (TDHF). The recursive nature of the TDHF theory is exploited to develop formulas that are applicable in any order. The theory is applied to evaluate dispersion effects for the series of molecules CH4, CH3F, CH2F2, CHF3, and CF4. Comparisons are made with results obtained from dc-induced, second-Harmonic generation, and third-Harmonic generation experiments. Additional applications are reported for H2 and HF.
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Sekino et al. (1986) studied this question.
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