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Energy Transfer in Reconstituted Peridinin-Chlorophyll-Protein Complexes: Ensemble and Single-Molecule Spectroscopy Studies

Sebastian Mackowski ^*, Stephan Wörmke ^*, Tatas H. P. Brotosudarmo ^* , Christophe Jung ^*, Roger G. Hiller , Hugo Scheer  and Christoph Bräuchle ^*

^* Department of Chemistry and Biochemistry and Center for Nanoscience, Ludwig Maximilian University, D-81377 Munich, Germany; Department of Biology 1, Ludwig Maximilian University, D-80638 Munich, Germany; and Biology Department, Division of Environmental and Life Sciences, Macquarie University, North Ryde, NSW 2109, Australia

Correspondence: Address reprint requests to Christoph Bräuchle, Dept. of Chemistry and Biochemistry and Center for Nanoscience (CeNS), Ludwig Maximilian University, Butenandtstrasse 11, D-81377 Munich, Germany. E-mail: christoph.braeuchle{at}cup.uni-muenchen.de.

We combine ensemble and single-molecule spectroscopy to gain insight into the energy transfer between chlorophylls (Chls) in peridinin-chlorophyll-protein (PCP) complexes reconstituted with Chl a, Chl b, as well as both Chl a and Chl b. The main focus is the heterochlorophyllous system (Chl a/b-N-PCP), and reference information essential to interpret experimental observations is obtained from homochlorophyllous complexes. Energy transfer between Chls in Chl a/b-N-PCP takes place from Chl b to Chl a and also from Chl a to Chl b with comparable Förster energy transfer rates of 0.0324 and 0.0215 ps^–1, respectively. Monte Carlo simulations yield the ratio of 39:61 for the excitation distribution between Chl a and Chl b, which is larger than the equilibrium distribution of 34:66. An average Chl a/Chl b fluorescence intensity ratio of 66:34 is measured, however, for single Chl a/b-N-PCP complexes excited into the peridinin (Per) absorption. This difference is attributed to almost three times more efficient energy transfer from Per to Chl a than to Chl b. The results indicate also that due to bilateral energy transfer, the Chl system equilibrates only partially during the excited state lifetimes.

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				T. Polivka, T. Pascher, and R. G. Hiller Energy Transfer in the Peridinin-Chlorophyll Protein Complex Reconstituted with Mixed Chlorophyll Sites Biophys. J., April 15, 2008; 94(8): 3198 - 3207. [Abstract] [Full Text] [PDF]