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:
-
- Vrije Univ., Amsterdam (Netherlands). Department of Physics and Astronomy
- Univ. of Glasgow, Scotland (United Kingdom). Division of Biochemistry and Molecular Biology
- Moscow State Univ., Moscow (Russia). A. N. Belozersky Institute of Physico-Chemical Biology
- 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.
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
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.
@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}
}
Web of Science
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