The first hyperpolarizability of several ii-like chromophores including Mal
achite Green and Brilliant Green were measured by means of Kleinman-disallo
wed hyper-Rayleigh (harmonic light) scattering (KD-HRS). Such chromophores
are of interest as components of a new class of chiral and axial macroscopi
c materials. Light scattering measurements were carried out in both the non
-resonant and the anomalous dispersion regime in order to compare experimen
tal results with a two-level model that indicates that B-symmetry excited s
tates will contribute. Large hyperpolarizabilities were observed in all cas
es and evidence that the lowest-lying excited state has B-symmetry was foun
d in some molecules. (C) 2001 Elsevier Science B.V. All rights reserved.