Relation between quantum and geometric dimensionalities in molecular nonlinear optics: Beyond the two-level model for anisotropic systems

The nonlinear optical susceptibilities of two- or three-dimensional molecular systems exhibit variable anisotropic features depending on their structure and substitution pattern. We show that appropriate geometric (e.g. tensorial) considerations combined with an n-level quantum model (n greater than or equal to 3) are able to account for such nonlinear anisotropy as rigorously defined in an invariant spherical formalism by extension of classical linear anisotropy. We call on two kinds of experiments to investigate these properties: firstly, variation of the incident polarization (VIP) in harmonic light scattering (HLS) experiments is being performed to sort out individual tensorial components of the quadratic hyperpolarizability beta tensor; secondly, wavelength dependence studies in coherent second harmonic generation (SHG) from poled thin film media are shown at a preliminary stage to be able to designate those excited states responsible for the nonlinear anisotropy.