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Title: Dark States in the Light-Harvesting complex 2 Revealed by Two-dimensional Electronic Spectroscopy

Abstract

Energy transfer and trapping in the light harvesting antennae of purple photosynthetic bacteria is an ultrafast process, which occurs with a quantum efficiency close to unity. However the mechanisms behind this process have not yet been fully understood. Recently it was proposed that low-lying energy dark states, such as charge transfer states and polaron pairs, play an important role in the dynamics and directionality of energy transfer. However, it is difficult to directly detect those states because of their small transition dipole moment and overlap with the B850/B870 exciton bands. Here we present a new experimental approach, which combines the selectivity of two-dimensional electronic spectroscopy with the availability of genetically modified light harvesting complexes, to reveal the presence of those dark states in both the genetically modified and the wild-type light harvesting 2 complexes of Rhodopseudomonas palustris. In conclusion, we suggest that Nature has used the unavoidable charge transfer processes that occur when LH pigments are concentrated to enhance and direct the flow of energy.

Authors:
 [1];  [1];  [1];  [2];  [2];  [3];  [4];  [1]
+ Show Author Affiliations
  1. Vrije Univ., Amsterdam (Netherlands). Department of Physics and Astronomy
  2. Univ. of Glasgow, Scotland (United Kingdom). Division of Biochemistry and Molecular Biology
  3. Moscow State Univ., Moscow (Russia). A. N. Belozersky Institute of Physico-Chemical Biology
  4. Princeton Univ., NJ (United States). Dept. of Chemistry
Publication Date:
Research Org.:
Vrije Univ., Amsterdam (Netherlands); Energy Frontier Research Centers (EFRC) (United States). Photosynthetic Antenna Research Center (PARC)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1242364
Grant/Contract Number:  
SC0001035
Resource Type:
Accepted Manuscript
Journal Name:
Scientific Reports
Additional Journal Information:
Journal Volume: 6; Journal ID: ISSN 2045-2322
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
59 BASIC BIOLOGICAL SCIENCES

Citation Formats

Ferretti, Marco, Hendrikx, Ruud, Romero, Elisabet, Southall, June, Cogdell, Richard J., Novoderezhkin, Vladimir I., Scholes, Gregory D., and van Grondelle, Rienk. Dark States in the Light-Harvesting complex 2 Revealed by Two-dimensional Electronic Spectroscopy. United States: N. p., 2016. Web. doi:10.1038/srep20834.
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Ferretti, Marco, Hendrikx, Ruud, Romero, Elisabet, Southall, June, Cogdell, Richard J., Novoderezhkin, Vladimir I., Scholes, Gregory D., & van Grondelle, Rienk. Dark States in the Light-Harvesting complex 2 Revealed by Two-dimensional Electronic Spectroscopy. United States. https://doi.org/10.1038/srep20834
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Ferretti, Marco, Hendrikx, Ruud, Romero, Elisabet, Southall, June, Cogdell, Richard J., Novoderezhkin, Vladimir I., Scholes, Gregory D., and van Grondelle, Rienk. Tue . "Dark States in the Light-Harvesting complex 2 Revealed by Two-dimensional Electronic Spectroscopy". United States. https://doi.org/10.1038/srep20834. https://www.osti.gov/servlets/purl/1242364.
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@article{osti_1242364,
title = {Dark States in the Light-Harvesting complex 2 Revealed by Two-dimensional Electronic Spectroscopy},
author = {Ferretti, Marco and Hendrikx, Ruud and Romero, Elisabet and Southall, June and Cogdell, Richard J. and Novoderezhkin, Vladimir I. and Scholes, Gregory D. and van Grondelle, Rienk},
abstractNote = {Energy transfer and trapping in the light harvesting antennae of purple photosynthetic bacteria is an ultrafast process, which occurs with a quantum efficiency close to unity. However the mechanisms behind this process have not yet been fully understood. Recently it was proposed that low-lying energy dark states, such as charge transfer states and polaron pairs, play an important role in the dynamics and directionality of energy transfer. However, it is difficult to directly detect those states because of their small transition dipole moment and overlap with the B850/B870 exciton bands. Here we present a new experimental approach, which combines the selectivity of two-dimensional electronic spectroscopy with the availability of genetically modified light harvesting complexes, to reveal the presence of those dark states in both the genetically modified and the wild-type light harvesting 2 complexes of Rhodopseudomonas palustris. In conclusion, we suggest that Nature has used the unavoidable charge transfer processes that occur when LH pigments are concentrated to enhance and direct the flow of energy.},
doi = {10.1038/srep20834},
journal = {Scientific Reports},
number = ,
volume = 6,
place = {United States},
year = {Tue Feb 09 00:00:00 EST 2016},
month = {Tue Feb 09 00:00:00 EST 2016}
}
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https://doi.org/10.1038/srep20834
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Exciton Relaxation and Polaron Formation in LH2 at Low Temperature
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Mixing of Exciton and Charge-Transfer States in Photosystem II Reaction Centers: Modeling of Stark Spectra with Modified Redfield Theory
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text, January 2012

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text, January 2012

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    Delocalized excitons in natural light-harvesting complexes
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    Studying light-harvesting models with superconducting circuits
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    Introduction to State-of-the-Art Multidimensional Time-Resolved Spectroscopy Methods
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    Studying Light-Harvesting Models with Superconducting Circuits
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    Simulating Fluorescence-Detected Two-Dimensional Electronic Spectroscopy of Multichromophoric Systems
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    • Kunsel, Tenzin; Tiwari, Vivek; Matutes, Yassel Acosta
    • The Journal of Physical Chemistry B, Vol. 123, Issue 2
    • DOI: 10.1021/acs.jpcb.8b10176

    Publisher Correction: Studying light-harvesting models with superconducting circuits
    journal, June 2018

    • Potočnik, Anton; Bargerbos, Arno; Schröder, Florian A. Y. N.
    • Nature Communications, Vol. 9, Issue 1
    • DOI: 10.1038/s41467-018-04655-1

    The molecular mechanisms of light adaption in light-harvesting complexes of purple bacteria revealed by a multiscale modeling
    journal, January 2019

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    • Chemical Science, Vol. 10, Issue 42
    • DOI: 10.1039/c9sc02886b
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