Memory-Assisted Exciton Diffusion in the Chlorosome Light-Harvesting Antenna of Green Sulfur Bacteria

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Memory-Assisted Exciton Diffusion in the Chlorosome Light-Harvesting Antenna of Green Sulfur Bacteria

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Title: Memory-Assisted Exciton Diffusion in the Chlorosome Light-Harvesting Antenna of Green Sulfur Bacteria
Author: Fujita, Takatoshi; Brookes, Jennifer Clare; Saikin, Semion K.; Aspuru-Guzik, Alan

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Citation: Fujita, Takatoshi, Jennifer Clare Brookes, Semion K. Saikin, and Alan Aspuru-Guzik. 2012. “Memory-Assisted Exciton Diffusion in the Chlorosome Light-Harvesting Antenna of Green Sulfur Bacteria.” Journal of Physical Chemistry Letters 3 (17) (September 6): 2357-2361. doi:10.1021/jz3008326. http://dx.doi.org/10.1021/jz3008326.
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Abstract: Chlorosomes are likely the largest and most efficient natural light-harvesting photosynthetic antenna systems. They are composed of large numbers of bacteriochlorophylls organized into supramolecular aggregates. We explore the microscopic origin of the fast excitation energy transfer in the chlorosome using the recently resolved structure and atomistic-detail simulations. Despite the dynamical disorder effects on the electronic transitions of the bacteriochlorophylls, our simulations show that the exciton delocalizes over the entire aggregate in about 200 fs. The memory effects associated to the dynamical disorder assist the exciton diffusion through the aggregates and enhance the diffusion coefficients as a factor of 2 as compared to the model without memory. Furthermore, exciton diffusion in the chlorosome is found to be highly anisotropic with the preferential transfer toward the baseplate, which is the next functional element in the photosynthetic system.
Published Version: doi:10.1021/jz3008326
Other Sources: http://arxiv.org/abs/1206.5812
Terms of Use: This article is made available under the terms and conditions applicable to Open Access Policy Articles, as set forth at http://nrs.harvard.edu/urn-3:HUL.InstRepos:dash.current.terms-of-use#OAP
Citable link to this page: http://nrs.harvard.edu/urn-3:HUL.InstRepos:11643698
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