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Spectral Trends in the Fluorescence of Single Bacterial Light-Harvesting Complexes: Experiments and Modified Redfield Simulations

Danielis Rutkauskas ^*, Vladimir Novoderezhkin , Andrew Gall , John Olsen , Richard J. Cogdell , C. Neil Hunter  and Rienk van Grondelle ^*

^* Department of Biophysics and Physics of Complex Systems, Division of Physics and Astronomy, Faculty of Sciences, Vrije Universiteit, 1081 HV Amsterdam, The Netherlands; A. N. Belozersky Institute of Physico-Chemical Biology, Moscow State University, Moscow 119899, Russia; Division of Biochemistry and Molecular Biology, University of Glasgow, Glasgow G12 8QQ, United Kingdom; and Robert Hill Institute for Photosynthesis, Krebs Institute for Biomolecular Research, and Department of Molecular Biology and Biotechnology, University of Sheffield, Sheffield S10 2TN, United Kingdom

Correspondence: Address reprint requests to Danielis Rutkauskas, Fax: 31-20-5987999; E-mail: danielis{at}nat.vu.nl.

In this work we present and discuss the single-molecule fluorescence spectra of a variety of species of light-harvesting complexes: LH2 of Rhodopseudomonas acidophila, Rhodobacter sphaeroides, and Rhodospirillum molischianum and LH1 of Rhodobacter sphaeroides. The emission spectrum of these complexes varies as a function of time as was described in earlier work. For each type of complex, we observe a pronounced and well-reproducible characteristic relationship between the fluorescence spectral parameters of the peak wavelength, width, and asymmetry. This dependence for the LH2 complexes can be quantitatively explained on the basis of a disordered exciton model by varying the static disorder and phonon coupling parameters. In addition, a correlation of the pigment site energies has to be assumed to interpret the behavior of the LH1 complex.

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