Efficient Pathways of Excitation Energy Transfer from Delocalized S2 Excitons in the Peridinin–Chlorophyll a–Protein Complex

Bricker, William P.; Lo, Cynthia S.

doi:10.1021/jp511766j

Efficient Pathways of Excitation Energy Transfer from Delocalized S₂ Excitons in the Peridinin–Chlorophyll a–Protein Complex

Journal Article · Mon Apr 13 00:00:00 EDT 2015 · Journal of Physical Chemistry. B, Condensed Matter, Materials, Surfaces, Interfaces and Biophysical Chemistry

DOI:https://doi.org/10.1021/jp511766j· OSTI ID:1386218

Bricker, William P. ^[1]; Lo, Cynthia S. ^[1]

Washington Univ., St. Louis, MO (United States)

Excitation energy transfer (EET) in peridinin–chlorophyll–protein (PCP) complexes is dominated by the S₁ → Q_y pathway, but the high efficiencies cannot be solely explained by this one pathway. We postulate that EET from peridinin S₂ excitons may also be important. We use complete active space configuration interaction calculations and the transition density cube method to calculate Coulombic couplings between peridinin and chlorophyll a in the PCP complex of the dinoflagellate Amphidinium carterae and compare monomeric and dimeric delocalized peridinin S₂ excited states. Our calculations show that the S₂ → Q_y EET pathway from peridinin to chlorophyll a is the dominant energy transfer pathway from the S₂ excited state in PCP, with several values in the sub-picosecond range. Here, this result suggests that the S₂ → Q_y EET pathway may be responsible for the reported chlorophyll a bleaching signature seen in experiment at around 200 fs, and not the S₂ → Q_x pathway as previously suggested.

View Accepted Manuscript (DOE)

Research Organization:: Energy Frontier Research Centers (EFRC) (United States). Photosynthetic Antenna Research Center (PARC)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: AC04-94AL85000; AC52-06NA25396; SC0001035

OSTI ID:: 1386218

Journal Information:: Journal of Physical Chemistry. B, Condensed Matter, Materials, Surfaces, Interfaces and Biophysical Chemistry, Journal Name: Journal of Physical Chemistry. B, Condensed Matter, Materials, Surfaces, Interfaces and Biophysical Chemistry Journal Issue: 18 Vol. 119; ISSN 1520-6106

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Fine control of chlorophyll-carotenoid interactions defines the functionality of light-harvesting proteins in plants Balevičius, Vytautas; Fox, Kieran F.; Bricker, William P. Scientific Reports, Vol. 7, Issue 1 https://doi.org/10.1038/s41598-017-13720-6	journal	October 2017
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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
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