The measurement of the antisymmetric components of nonlinear optical susceptibilities of TeO2 crystal

Abstract

The antisymmetric components of the second-order nonlinear optical susceptibility of TeO2 crystal have been measured by the process of sum-frequency mixing between the laser beams at the wavelengths of 1.064 and 0.532 μm. The experimental results were χ123/ (χ123+χ132) =0.59, χ132/(χ123 +χ132) =0.41, and χ312/(χ123+χ132) =−χ321/(χ123+χ132) =−0.18, which imply that χ123 and χ132 are slightly asymmetric and χ312 and χ321 are antisymmetric in the second and third suffices. It is thus concluded that the contribution of the antisymmetric component to the signal at the sum frequency may be comparable with that of the symmetric one forbidden by the Kleinman symmetry relation. Moreover, the symmetric and antisymmetric components of the nonlinear optical polarizabilities of the bond Te-O have been estimated in terms of the scheme of bond additivity by assuming a bond symmetry ∞.