Abstract

Second-harmonic (SH) generation has attracted much interest because of its simplicity and surface specifity. The SH response of a nonlinear polarization sheet that is isotropic around the z axis normal to the surface can be characterized in terms of three nonvanishing susceptibility components. We demonstrate in this contribution that these complex-valued components can be determined precisely by the evaluation of SH-rotation patterns using Fourier analysis. This procedure has been discussed in detail in a theoretical study.¹ It does not introduce a priori such restrictions as rod-like molecules or the validity of Kleinman’s conjecture.² We have performed angle-of- incidence measurements of the SH response of Langmuir-Blodgett-type monolayers³, prepared from hemicyanine dyes of high second-order nonlinearity.⁴

© 1993 Optical Society of America