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

Journal Article · · Scientific Reports
DOI:https://doi.org/10.1038/srep20834· OSTI ID:1242364
 [1];  [1];  [1];  [2];  [2];  [3];  [4];  [1]
  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

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.

Research Organization:
Vrije Univ., Amsterdam (Netherlands); Energy Frontier Research Centers (EFRC) (United States). Photosynthetic Antenna Research Center (PARC)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
SC0001035
OSTI ID:
1242364
Journal Information:
Scientific Reports, Vol. 6; ISSN 2045-2322
Publisher:
Nature Publishing GroupCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 61 works
Citation information provided by
Web of Science

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  • Novoderezhkin, Vladimir I.; Cohen Stuart, Thomas A.; van Grondelle, Rienk
  • The Journal of Physical Chemistry A, Vol. 115, Issue 16 https://doi.org/10.1021/jp108187m
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Cited By (16)

The role of charge-transfer states in the spectral tuning of antenna complexes of purple bacteria journal March 2018
Introduction to State-of-the-Art Multidimensional Time-Resolved Spectroscopy Methods journal June 2018
Studying light-harvesting models with superconducting circuits journal March 2018
Spatially-resolved fluorescence-detected two-dimensional electronic spectroscopy probes varying excitonic structure in photosynthetic bacteria journal October 2018
Multiscale modelling of photoinduced processes in composite systems journal April 2019
Before Förster. Initial excitation in photosynthetic light harvesting journal January 2019
The molecular mechanisms of light adaption in light-harvesting complexes of purple bacteria revealed by a multiscale modeling journal January 2019
Electronic coherence lifetimes of the Fenna–Matthews–Olson complex and light harvesting complex II journal January 2019
Delocalized excitons in natural light-harvesting complexes journal August 2018
Studying light-harvesting models with superconducting circuits text January 2018
Introduction to State-of-the-Art Multidimensional Time-Resolved Spectroscopy Methods book June 2018
Studying Light-Harvesting Models with Superconducting Circuits text January 2017
Delocalized excitons in natural light harvesting complexes text January 2018
Simulating Fluorescence-Detected Two-Dimensional Electronic Spectroscopy of Multichromophoric Systems journal December 2018
Publisher Correction: Studying light-harvesting models with superconducting circuits journal June 2018
Spatially-resolved Fluorescence-detected Two-dimensional Electronic Spectroscopy Probes Varying Electronic Couplings in Photosynthetic Bacteria text January 2018