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Reversible redox-switching of first hyperpolarizability studied by hyper-Rayleigh scattering

Two examples of efficient and reversible switching of the first hyperpolarizability of charge-transfer metalorganic species are presented. The charge transfer is between a metalorganic donor unit and an organic acceptor. In one case, the donor is a ruthenium(I) pentammine complex, the acceptor is an N-methyl-4,4'-bipyridinium ligand. Oxidizing the ruthenium(II) to ruthenium(III) changes the donor to an acceptor and destroys the charge transfer, as evidence by the disappearance of the charge transfer band in linear absorption spectroscopy. In hyper-Rayleigh scattering, a reduction in first hyperpolarizability of at least an order of magnitude is observed. In a second case, the donor is an octamethylferrocene unit, while the donor is a nitro group on a thiophene. Again, oxidizing the octamethylferrocene to octamethylferrocenium reduces the hyperpolarizability with more than an order of magnitude. Both redox processes are fully reversible.