The second-order nonlinear optical, (NLO) properties of light-harvesting complexes (LHs) from, the purple photosynthetic bacteria Thermochromatium (Tch.) tepidum were investigated for the first time by means of hyper-Rayleigh scattering (HRS). The carotenoid (Car) molecules bound to the isolated LH1 and LH2 proteins gave rise to second-harmonic Scattering; however, they showed an opposite effect of the collective contribution,from Car, that is, the first hyperpolarizability (beta) reduced substantially from (10 510 +/- 370) X 10(-30) esu for LH1 to (360 +/- 120) X 10(-30) esu for LH2 Chromatophores of Tch. tepidum also Showed a giant hyperpolarizability,of (11 640 +/- 630) x 10(-30) esu, On the basis of the structural information on :bacterial LHs, it is found that the effective, beta of an LH is governed by the microenvironment and orientational correlation among the Car chromophores, which is concluded to be coherently enhanced for LH1. For LH2, however, additional. destructive effects between different Car molecules may account for the small beta value. This work demonstrates that LH1 and native membranes of purple bacteria can be potent NLO materials and that HRS is a promising spectroscopic means for investigating Structural information of pigment-protein supramolecules.