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)
Please use this url to cite or link to this publication:
https://lup.lub.lu.se/record/2859514
- author
- Dostal, Jakub
LU
; Mančal, Tomáš
; Augulis, Ramunas
LU
; Vácha, František
; Pšenčík, Jakub
and Zigmantas, Donatas
LU
- organization
- publishing date
- 2012
- 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 (ACS)
- external identifiers
-
- wos:000306457900050
- pmid:22690836
- scopus:84863893911
- pmid:22690836
- ISSN
- 1520-5126
- DOI
- 10.1021/ja3025627
- language
- English
- LU publication?
- yes
- additional info
- The information about affiliations in this record was updated in December 2015. The record was previously connected to the following departments: Chemical Physics (S) (011001060)
- id
- ce0712c5-07fd-457b-ab5e-57ff79538d30 (old id 2859514)
- date added to LUP
- 2016-04-01 12:53:06
- date last changed
- 2023-11-12 08:33:49
@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 (ACS)}},
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}},
doi = {{10.1021/ja3025627}},
volume = {{134}},
year = {{2012}},
}