Journal
CHEMICAL SCIENCE
Volume 10, Issue 41, Pages 9576-9585Publisher
ROYAL SOC CHEMISTRY
DOI: 10.1039/c9sc03712h
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Funding
- Westpac Bicentennial Foundation Research Fellowship
- Australian Government Research Training Program scholarship
- University of Sydney Nano Institute Grand Challenge
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All photosynthetic organisms convert solar energy into chemical energy through charge separation in dimeric reaction centres. It is unknown why early reaction centres dimerised and completely displaced their monomeric ancestors. Here, we discuss several proposed explanations for reaction-centre dimerism and conclude-with only weak assumptions about the primordial dimerisation event-that the most probable explanation for the dimerism is that it arose because it enhanced light-harvesting efficiency by deepening the excitonic trap, i.e., by enhancing the rate of exciton transfer from an antenna complex and decreasing the rate of back transfer. This effect would have outweighed the negative effect dimerisation would have had on charge transfer within the reaction centre. Our argument implies that dimerisation likely occurred after the evolution of the first antennas, and it explains why the lower-energy state of the special pair is bright.
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