Abstract
Green-sulfur bacteria have evolved a unique light-harvesting apparatus, the chlorosome, by which it is perfectly adapted to thrive photosynthetically under extremely low light conditions. We have used single-particle, optical spectroscopy to study the structure-function relationship of chlorosomes each of which incorporates hundreds of thousands of self-assembled bacteriochlorophyll (BChl) molecules. The electronically excited states of these molecular assemblies are described as Frenkel excitons whose photophysical properties depend crucially on the mutual arrangement of the pigments. The signature of these Frenkel excitons and its relation to the supramolecular organization of the chlorosome becomes accessible by optical spectroscopy. Because subtle spectral features get obscured by ensemble averaging, we have studied individual chlorosomes from wild-type Chlorobaculum tepidum by polarization-resolved fluorescence-excitation spectroscopy. This approach minimizes the inherent sample heterogeneity and allows us to reveal properties of the exciton states without ensemble averaging. The results are compared with predictions from computer simulations of various models of the supramolecular organization of the BChl monomers. We find that the photophysical properties of individual chlorosomes from wild-type Chlorobaculum tepidum are consistent with a (multiwall) helical arrangement of syn-anti stacked BChl molecules in cylinders and/or spirals of different size.