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Roscioli JD, Ghosh S, LaFountain AM, et al. Quantum Coherent Excitation Energy Transfer by Carotenoids in Photosynthetic Light Harvesting. J Phys Chem Lett. 2017;8(20):5141-5147doi: 10.1021/acs.jpclett.7b01791.
Roscioli, J. D., Ghosh, S., LaFountain, A. M., Frank, H. A., & Beck, W. F. (2017). Quantum Coherent Excitation Energy Transfer by Carotenoids in Photosynthetic Light Harvesting. The journal of physical chemistry letters, 8(20), 5141-5147. https://doi.org/10.1021/acs.jpclett.7b01791
Roscioli, Jerome D, et al. "Quantum Coherent Excitation Energy Transfer by Carotenoids in Photosynthetic Light Harvesting." The journal of physical chemistry letters vol. 8,20 (2017): 5141-5147. doi: https://doi.org/10.1021/acs.jpclett.7b01791
Roscioli JD, Ghosh S, LaFountain AM, Frank HA, Beck WF. Quantum Coherent Excitation Energy Transfer by Carotenoids in Photosynthetic Light Harvesting. J Phys Chem Lett. 2017 Oct 19;8(20):5141-5147. doi: 10.1021/acs.jpclett.7b01791. Epub 2017 Oct 06. PMID: 28968122.
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J Phys Chem Lett. 2017 Oct 19;8(20):5141-5147. doi: 10.1021/acs.jpclett.7b01791. Epub 2017 Oct 06.

Quantum Coherent Excitation Energy Transfer by Carotenoids in Photosynthetic Light Harvesting.

The journal of physical chemistry letters

Jerome D Roscioli, Soumen Ghosh, Amy M LaFountain, Harry A Frank, Warren F Beck

Affiliations

  1. Department of Chemistry, Michigan State University , East Lansing, Michigan 48824-1322, United States.
  2. Department of Chemistry, University of Connecticut , Storrs, Connecticut 06269-3036, United States.

PMID: 28968122 DOI: 10.1021/acs.jpclett.7b01791

Abstract

It remains an open question whether quantum coherence and molecular excitons created by delocalization of electronic excited states are essential features of the mechanisms that enable efficient light capture and excitation energy transfer to reaction centers in photosynthetic organisms. The peridinin-chlorophyll a protein from marine dinoflagellates is an example of a light-harvesting system with tightly clustered antenna chromophores in which quantum coherence has long been suspected, but unusually it features the carotenoid peridinin as the principal light absorber for mid-visible photons. We report that broad-band two-dimensional electronic spectroscopy indeed reveals the initial presence of exciton relaxation pathways that enable transfer of excitation from peridinin to chlorophyll a in <20 fs, but the quantum coherence that permits this is very short-lived. Strongly coupled excited-state vibrational distortions of the peridinins trigger a dynamic transition of the electronic structure of the system and a rapid conversion to incoherent energy transfer mechanisms.

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