Optical third-harmonic generation of fused silica in gas atmosphere: Absolute value of the third-order nonlinear optical susceptibilityχ(3)

We report on a calibration procedure based on third-harmonic generation, which yields absolute values for ${\chi }^{\mathrm{}\left(3\right)\mathrm{}}.$ By calibrating the nonlinear susceptibility ${\chi }^{\mathrm{}\left(3\right)\mathrm{}}$ of fused silica against the established, quantum chemically calculated second-order hyperpolarizabilities γ of various gases at different pressures, we determine reliable absolute values for fused silica. We propose a standard third-order nonlinear optical susceptibilities ${\chi }^{\mathrm{}\left(3\right)\mathrm{}}$ of fused silica ${\chi }^{\mathrm{}\left(3\right)\mathrm{}}(-3\omega ,\omega ,\omega ,\omega )=(2.0\mathrm{}\pm 0.2)\times {10}^{-22}{\mathrm{m}}^2{/\mathrm{V}}^2$ at the wavelength 1.064 μm and ${\chi }^{\mathrm{}\left(3\right)\mathrm{}}(-3\omega ,\omega ,\omega ,\omega )=(1.6\mathrm{}\pm 0.2)\times {10}^{-22}{\mathrm{m}}^2{/\mathrm{V}}^2$ at 1.907 μm. These results are in excellent agreement with the cascading experiments reported by Bosshard et al. [Phys. Rev. B 61, 10 688 (2000)].