OPTICALLY nonlinear organic materials show considerable potential for
applications in optical signal processing and telecommunications(1,2).
Most materials are based on the p-nitroaniline template, in which the
optical nonlinearities are intimately associated with quasi-one-dimen
sional charge transfer. But there are problems associated with this co
nventional approach, arising from the strongly dipolar nature of the m
olecules(2). It has recently been recognized(3-5) that two- and three-
dimensional stereochemistry offers new possibilities for the design an
d synthesis of optically nonlinear molecules, in which charge transfer
is multidirectional rather than dipolar in character; octupolar nonli
nearities have now been demonstrated in several molecular systems(5-7)
. Tri-substituted ruthenium complexes(6) appear particularly attractiv
e because intense, multidirectional metal-to-ligand charge transfer le
ads to a significant enhancement of the optical nonlinearity, as quant
ified by the quadratic hyperpolarizability, beta. Here we show that th
e choice of ligand can further increase beta to values in excess of 10
(-27) e.s.u., comparable to the best dipolar optically nonlinear molec
ules.