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

We report on a calibration procedure based on third-harmonic generation, which yields absolute values for chi((3)). By calibrating the nonlinear susceptibility chi((3)) of fused silica against the established, quantum chemically calculated second-order hyperpolarizabilities gamma of various gases at different pressures, we determine reliable absolute values for fused silica. We propose a standard third-order nonlinear optical susceptibilities chi((3)) of fused silica chi((3))(-3 omega,omega,omega,omega) = (2.0+/-0.2) X 10(-22) m(2)/V-2 at the wavelength 1.064 mu m and chi((3))(-3 omega,omega,omega,omega) = (1.6+/-0.2) X 10(-22) m(2)/V-2 at 1.907 mu m. These results are in excellent agreement with the cascading experiments reported by Bosshard et al.