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Triplet Exciton Formation as a Novel Photoprotection Mechanism in Chlorosomes of Chlorobium tepidum

Hanyoup Kim ^*, Hui Li , Julia A. Maresca , Donald A. Bryant  and Sergei Savikhin ^*

^* Department of Physics, Purdue University, West Lafayette, Indiana; and Department of Biochemistry and Molecular Biology, The Pennsylvania State University, University Park, Pennsylvania

Correspondence: Address reprint requests to Sergei Savikhin, Tel.: 765-494-3017; Fax: 765-494-0706; E-mail: sergei{at}physics.purdue.edu.

Chlorosomes comprise thousands of bacteriochlorophylls (BChl c, d, or e) in a closely packed structure surrounded by a lipid-protein envelope and additionally contain considerable amounts of carotenoids, quinones, and BChl a. It has been suggested that carotenoids in chlorosomes provide photoprotection by rapidly quenching triplet excited states of BChl via a triplet-triplet energy transfer mechanism that prevents energy transfer to oxygen and the formation of harmful singlet oxygen. In this work we studied triplet energy transfer kinetics and photodegradation of chlorosomes isolated from wild-type Chlorobium tepidum and from genetically modified species with different types of carotenoids and from a carotenoid-free mutant. Supporting a photoprotective function of carotenoids, carotenoid-free chlorosomes photodegrade 3 times faster than wild-type chlorosomes. However, a significant fraction of the BChls forms a long-lived, triplet-like state that does not interact with carotenoids or with oxygen. We propose that these states are triplet excitons that form due to triplet-triplet interaction between the closely packed BChls. Numerical exciton simulations predict that the energy of these triplet excitons may fall below that of singlet oxygen and triplet carotenoids; this would prevent energy transfer from triplet BChl. Thus, the formation of triplet excitons in chlorosomes serves as an alternative photoprotection mechanism.

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