Abstract
The frequency dependence of the second hyperpolarizability (γ) of CF4 has been measured in the visible (488 nm<λ<660 nm) by means of gas-phase electric-field-induced second harmonic generation (ESHG). The results of these experiments are compared with the results of other nonlinear optics experiments which have measured γ by third harmonic generation (THG), ESHG, and the dc Kerr effect. In order to make this comparison, expressions for the vibrational contributions to γCF4 have been derived and numerically evaluated for each of these optical processes. This comparison indicates that vibrational contributions to γCF4 are significant for both the dc Kerr effect and ESHG.
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