Abstract
Metal ions such as ruthenium(II) are excellent templates for building 3D octupolar nonlinear optical (NLO)-phores. Their associations with bipyridyl ligands give rise to octahedral metal complexes with large first-order hyperpolarizabilities. The ability to functionalize these octupoles allows their incorporation into macromolecular architectures such as polyimides and metallodendrimers. The quadratic NLO susceptibilities β of these supramolecules are characterized by harmonic light scattering performed at the near-IR 1.91 μm fundamental wavelength, in order to rule out two-photon fluorescence contributions to the harmonic signal. Comparison with a linear polymer clearly demonstrates a quasi-optimized octupolar supramolecular ordering in a dendrimer made of seven ruthenium(II) complexes.