Cross-propagating Beam-Deflection measurements of third-order nonlinear optical susceptibility

We extend our recently developed Beam-Deflection (BD) method which we used to determine the sign, magnitude, and ultrafast dynamics of bound electronic and nuclear nonlinear optical responses, to measure elements of the third-order nonlinear optical susceptibility tensor with longitudinal field components. In these measurements, in contrast to the conventional BD technique where excitation and probe beams are nearly collinear, the interaction geometry involves orthogonal propagation of excitation and probe beams. This cross-propagating BD method enables probing with the electric field polarized parallel to the wavevector of the excitation beam as well as conventional parallel and perpendicular polarizations as in most other experimental methods. This technique may be of use in detecting possible magneto-electric contributions to the nonlinear susceptibility. The ratio between parallel and perpendicular bound-electronic responses in this method is shown to be larger than the factor of 3 predicted by theory and measured in the conventional configuration.