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The frequency dependence of the second hyperpolarizability (γ) of CO2 has been measured in the visible (488<λ<693 nm) by means of gas phase electric-field-induced second-harmonic generation (ESHG). Comparison of these results with the results for several other third-order nonlinear optical processes suggests that there are significant vibrational contributions to γCO2.
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David P. Shelton (1986) studied this question.
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