Local and nonlocal contributions to the linear spectroscopy of light-harvesting antenna systems

In this paper the circular dichroism and absorption spectra of the LH2 complex of Rhodopseudomonas acidophila, for which the atomic structure is known, are analyzed. We show that an analysis based on the distribution of the excitations in real space, and their correlations, to unravel the relation between the atomic structure of the light-harvesting complex and its excitonic properties, is particularly successful. Starting from molecular expressions for the linear susceptibility, we demonstrate that linear spectra can be viewed as originating from the product of coherence correlation functions and geometric structure factors. Effects of homogeneous and inhomogeneous broadening can be incorporated in a natural way and lead to a definition of exciton length as the distance over which coherence correlation functions decay. 1