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Title: Electronic Structure and Dynamics of Higher-Lying Excited States in Light Harvesting Complex 1 from Rhodobacter sphaeroides

Abstract

Light harvesting in photosynthetic organisms involves efficient transfer of energy from peripheral antenna complexes to core antenna complexes, and ultimately to the reaction center where charge separation drives downstream photosynthetic processes. Antenna complexes contain many strongly coupled chromophores, which complicates analysis of their electronic structure. Two-dimensional electronic spectroscopy (2DES) provides information on energetic coupling and ultrafast energy transfer dynamics, making the technique well suited for the study of photosynthetic antennae. Here in this paper, we present 2DES results on excited state properties and dynamics of a core antenna complex, light harvesting complex 1 (LH1), embedded in the photosynthetic membrane of Rhodobacter sphaeroides. The experiment reveals weakly allowed higher-lying excited states in LH1 at 770 nm, which transfer energy to the strongly allowed states at 875 nm with a lifetime of 40 fs. The presence of higher-lying excited states is in agreement with effective Hamiltonians constructed using parameters from crystal structures and atomic force microscopy (AFM) studies. The energy transfer dynamics between the higher- and lower-lying excited states agree with Redfield theory calculations.

Authors:
 [1];  [2];  [3];  [4];  [4];  [2]
+ Show Author Affiliations
  1. Univ. of Chicago, IL (United States)
  2. Univ. of Chicago, IL (United States). Inst. for Biophysical Dynamics, and the James Franck Inst.
  3. Univ. of Chicago, IL (United States). Inst. for Biophysical Dynamics, and the James Franck Inst.
  4. Univ. of Sheffield (United Kingdom)
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC) (United States). Photosynthetic Antenna Research Center (PARC); Washington Univ., St. Louis, MO (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF); Defense Advanced Research Projects Agency (DARPA); Camille and Henry Dreyfus Foundation; Searle Foundation; USDOD; Biotechnology and Biological Sciences Research Council (United Kingdom); European Research Council (ERC)
OSTI Identifier:
1387876
Grant/Contract Number:  
SC0001035; BB/M000265/1
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory
Additional Journal Information:
Journal Volume: 120; Journal Issue: 24; Related Information: PARC partners with Washington University in St. Louis (lead); University of California, Riverside; University of Glasgow, UK; Los Alamos National Laboratory; University of New Mexico; New Mexico Corsortium; North Carolina State University; Northwestern University; Oak Ridge National Laboratory; University of Pennsylvania; Sandia National Laboratories; University of Sheffield, UK; Journal ID: ISSN 1089-5639
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 59 BASIC BIOLOGICAL SCIENCES; solar (fuels); photosynthesis (natural and artificial); biofuels (including algae and biomass); bio-inspired; charge transport; membrane; synthesis (novel materials); synthesis (self-assembly)

Citation Formats

Dahlberg, Peter D., Ting, Po-Chieh, Massey, Sara C., Martin, Elizabeth C., Hunter, C. Neil, and Engel, Gregory S. Electronic Structure and Dynamics of Higher-Lying Excited States in Light Harvesting Complex 1 from Rhodobacter sphaeroides. United States: N. p., 2016. Web. doi:10.1021/acs.jpca.6b04146.
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Dahlberg, Peter D., Ting, Po-Chieh, Massey, Sara C., Martin, Elizabeth C., Hunter, C. Neil, & Engel, Gregory S. Electronic Structure and Dynamics of Higher-Lying Excited States in Light Harvesting Complex 1 from Rhodobacter sphaeroides. United States. https://doi.org/10.1021/acs.jpca.6b04146
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Dahlberg, Peter D., Ting, Po-Chieh, Massey, Sara C., Martin, Elizabeth C., Hunter, C. Neil, and Engel, Gregory S. Fri . "Electronic Structure and Dynamics of Higher-Lying Excited States in Light Harvesting Complex 1 from Rhodobacter sphaeroides". United States. https://doi.org/10.1021/acs.jpca.6b04146. https://www.osti.gov/servlets/purl/1387876.
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@article{osti_1387876,
title = {Electronic Structure and Dynamics of Higher-Lying Excited States in Light Harvesting Complex 1 from Rhodobacter sphaeroides},
author = {Dahlberg, Peter D. and Ting, Po-Chieh and Massey, Sara C. and Martin, Elizabeth C. and Hunter, C. Neil and Engel, Gregory S.},
abstractNote = {Light harvesting in photosynthetic organisms involves efficient transfer of energy from peripheral antenna complexes to core antenna complexes, and ultimately to the reaction center where charge separation drives downstream photosynthetic processes. Antenna complexes contain many strongly coupled chromophores, which complicates analysis of their electronic structure. Two-dimensional electronic spectroscopy (2DES) provides information on energetic coupling and ultrafast energy transfer dynamics, making the technique well suited for the study of photosynthetic antennae. Here in this paper, we present 2DES results on excited state properties and dynamics of a core antenna complex, light harvesting complex 1 (LH1), embedded in the photosynthetic membrane of Rhodobacter sphaeroides. The experiment reveals weakly allowed higher-lying excited states in LH1 at 770 nm, which transfer energy to the strongly allowed states at 875 nm with a lifetime of 40 fs. The presence of higher-lying excited states is in agreement with effective Hamiltonians constructed using parameters from crystal structures and atomic force microscopy (AFM) studies. The energy transfer dynamics between the higher- and lower-lying excited states agree with Redfield theory calculations.},
doi = {10.1021/acs.jpca.6b04146},
journal = {Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory},
number = 24,
volume = 120,
place = {United States},
year = {Fri May 27 00:00:00 EDT 2016},
month = {Fri May 27 00:00:00 EDT 2016}
}
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https://doi.org/10.1021/acs.jpca.6b04146
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    Works referencing / citing this record:

    Communication: Broad manifold of excitonic states in light-harvesting complex 1 promotes efficient unidirectional energy transfer in vivo
    journal, October 2017

    • Sohail, Sara H.; Dahlberg, Peter D.; Allodi, Marco A.
    • The Journal of Chemical Physics, Vol. 147, Issue 13
    • DOI: 10.1063/1.4999057

    Potential pitfalls of the early-time dynamics in two-dimensional electronic spectroscopy
    journal, July 2019

    • Paleček, David; Edlund, Petra; Gustavsson, Emil
    • The Journal of Chemical Physics, Vol. 151, Issue 2
    • DOI: 10.1063/1.5079817
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