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Two-Dimensional Electronic Spectroscopy Reveals Ultrafast Energy Diffusion in Chlorosomes.

Dostal, Jakub LU ; Mančal, Tomáš; Augulis, Ramunas LU ; Vácha, František; Pšenčík, Jakub and Zigmantas, Donatas LU (2012) In Journal of the American Chemical Society 134(28). p.11611-11617
Abstract
Chlorosomes are light-harvesting antennae that enable exceptionally efficient light energy capture and excitation transfer. They are found in certain photosynthetic bacteria, some of which live in extremely low-light environments. In this work, chlorosomes from the green sulfur bacterium Chlorobaculum tepidum were studied by coherent electronic two-dimensional (2D) spectroscopy. Previously uncharacterized ultrafast energy transfer dynamics were followed, appearing as evolution of the 2D spectral line-shape during the first 200 fs after excitation. Observed initial energy flow through the chlorosome is well explained by effective exciton diffusion on a sub-100 fs time scale, which assures efficiency and robustness of the process. The... (More)
Chlorosomes are light-harvesting antennae that enable exceptionally efficient light energy capture and excitation transfer. They are found in certain photosynthetic bacteria, some of which live in extremely low-light environments. In this work, chlorosomes from the green sulfur bacterium Chlorobaculum tepidum were studied by coherent electronic two-dimensional (2D) spectroscopy. Previously uncharacterized ultrafast energy transfer dynamics were followed, appearing as evolution of the 2D spectral line-shape during the first 200 fs after excitation. Observed initial energy flow through the chlorosome is well explained by effective exciton diffusion on a sub-100 fs time scale, which assures efficiency and robustness of the process. The ultrafast incoherent diffusion-like behavior of the excitons points to a disordered energy landscape in the chlorosome, which leads to a rapid loss of excitonic coherences between its structural subunits. This disorder prevents observation of excitonic coherences in the experimental data and implies that the chlorosome as a whole does not function as a coherent light-harvester. (Less)
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author
organization
publishing date
type
Contribution to journal
publication status
published
subject
in
Journal of the American Chemical Society
volume
134
issue
28
pages
11611 - 11617
publisher
The American Chemical Society
external identifiers
  • wos:000306457900050
  • pmid:22690836
  • scopus:84863893911
ISSN
1520-5126
DOI
10.1021/ja3025627
language
English
LU publication?
yes
id
ce0712c5-07fd-457b-ab5e-57ff79538d30 (old id 2859514)
date added to LUP
2012-07-06 15:57:05
date last changed
2017-10-29 03:45:46
@article{ce0712c5-07fd-457b-ab5e-57ff79538d30,
  abstract     = {Chlorosomes are light-harvesting antennae that enable exceptionally efficient light energy capture and excitation transfer. They are found in certain photosynthetic bacteria, some of which live in extremely low-light environments. In this work, chlorosomes from the green sulfur bacterium Chlorobaculum tepidum were studied by coherent electronic two-dimensional (2D) spectroscopy. Previously uncharacterized ultrafast energy transfer dynamics were followed, appearing as evolution of the 2D spectral line-shape during the first 200 fs after excitation. Observed initial energy flow through the chlorosome is well explained by effective exciton diffusion on a sub-100 fs time scale, which assures efficiency and robustness of the process. The ultrafast incoherent diffusion-like behavior of the excitons points to a disordered energy landscape in the chlorosome, which leads to a rapid loss of excitonic coherences between its structural subunits. This disorder prevents observation of excitonic coherences in the experimental data and implies that the chlorosome as a whole does not function as a coherent light-harvester.},
  author       = {Dostal, Jakub and Mančal, Tomáš and Augulis, Ramunas and Vácha, František and Pšenčík, Jakub and Zigmantas, Donatas},
  issn         = {1520-5126},
  language     = {eng},
  number       = {28},
  pages        = {11611--11617},
  publisher    = {The American Chemical Society},
  series       = {Journal of the American Chemical Society},
  title        = {Two-Dimensional Electronic Spectroscopy Reveals Ultrafast Energy Diffusion in Chlorosomes.},
  url          = {http://dx.doi.org/10.1021/ja3025627},
  volume       = {134},
  year         = {2012},
}