Calibration of third-order nonlinear optical susceptibilities via non-phase matched optical third-harmonic generation in noncentrosymmetric media

Summary form only given. One of the great challenges in nonlinear optics is the establishment of reliable absolute values of optical nonlinearities. We here show that frequency-tripling in combination with cascaded second-harmonic and sum-frequency-generation is a veri efficient tool to obtain self-consistent reliable reference values for the third-order nonlinear optical susceptibility /spl chi//sup (3)/. We present our experimental results on the crystals KNbO/sub 3/, quartz, and 4-N-N-dimethylamino-4´-N´-methylstilbazolium toluene-p-sulfonate (DAST) and the glasses BK7, SF59, and fused silica with emphasis on the theoretical analysis of the cascaded phenomena including the boundary conditions, reliable reference materials, wavelength dispersion of the third-order susceptibilities, and structure-property relationships.