Abstract
Metal complexes display interesting properties in terms of molecular optimization of quadratic nonlinear properties, combined with a good thermal stability and a large flexibility of geometrical and electronic properties. The role of dimensionality and intramolecular charge transfer of the pure ligand is investigated here, in particular for Schiff base derivatives. Also, the influence of metal electronic configurations on the quadratic hyperpolarizability is investigated in the series of Ni II, Co II and Cu II atoms, showing the interest of open-shell structures as compared to closed-shell complexes in the case of a weakly nonlinear ligand. Finally, strongly octupolar two-dimensional systems, subphthalocyanines, are shown to present very large second-order nonlinear polarizabilities, with static values as high as measured on a trinitro-substituted SubPc by the harmonic light scattering technique.

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