Nonlinear polarization rotation and orthogonal polarization generation experienced in a single-beam configuration

Nonlinear polarization rotation and generation of a polarization component orthogonal to the input beam were observed along fourfold axes of YVO4 and BaF2 crystals. We demonstrate experimentally that in both crystals the angle of rotation is proportional, at low intensities, to the square of the product of the input intensity and the crystal length and is the result of simultaneous action of two third-order processes. This type of nonlinear polarization rotation is driven by the real part of the cubic susceptibility. The recorded energy exchange between the two orthogonal components can exceed 10%. It is to our knowledge the highest energy-conversion efficiency achieved in a single beam nonresonant chi((3)) interaction. A simple theoretical model is elaborated to describe the dependence of nonlinear polarization rotation and orthogonal polarization generation on the intensity of the input beam at both low- and high-intensity levels. It reveals the potential contributions from the real and the imaginary parts of the susceptibility tensor. Moreover, this kind of measurement is designed to permit the determination of the magnitude and the sign of the anisotropy of the real part of third-order nonlinearity in crystals with cubic or tetragonal symmetry on the basis of polarization-rotation measurements. The chi(xxxx)((3)) component of the third-order susceptibility tensor and its anisotropy sign and amplitude value for BaF2 and YVO4 crystals are estimated and discussed. (C) 2004 Optical Society of America.