'Octupolar' molecules are of particular interest in the field of nonli
near optics due to their potentially large quadratic nonlinearities. W
ithin this framework, we have designed organic chromophores of tetrahe
dral symmetry and investigated their quadratic nonlinearities by perfo
rming harmonic light scattering (HLS) experiments in solutions. Issues
related to the molecular engineering of the nonlinearity-transparency
trade-off have been addressed. As a result, molecules combining signi
ficant quadratic hyperpolarizabilities and excellent transparency have
been identified. (C) 1998 Elsevier Science B.V.