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Intraband dynamics and exciton trapping in the LH2 complex of Rhodopseudomonas acidophila

Thyrhaug, Erling LU ; Schröter, Marco LU ; Bukartė, Eglė LU ; Kühn, Oliver ; Cogdell, Richard ; Hauer, Jürgen and Zigmantas, Donatas LU orcid (2021) In Journal of Chemical Physics 154(4).
Abstract

Over the last several decades, the light-harvesting protein complexes of purple bacteria have been among the most popular model systems for energy transport in excitonic systems in the weak and intermediate intermolecular coupling regime. Despite this extensive body of scientific work, significant questions regarding the excitonic states and the photo-induced dynamics remain. Here, we address the low-temperature electronic structure and excitation dynamics in the light-harvesting complex 2 of Rhodopseudomonas acidophila by two-dimensional electronic spectroscopy. We find that, although at cryogenic temperature energy relaxation is very rapid, exciton mobility is limited over a significant range of excitation energies. This points to the... (More)

Over the last several decades, the light-harvesting protein complexes of purple bacteria have been among the most popular model systems for energy transport in excitonic systems in the weak and intermediate intermolecular coupling regime. Despite this extensive body of scientific work, significant questions regarding the excitonic states and the photo-induced dynamics remain. Here, we address the low-temperature electronic structure and excitation dynamics in the light-harvesting complex 2 of Rhodopseudomonas acidophila by two-dimensional electronic spectroscopy. We find that, although at cryogenic temperature energy relaxation is very rapid, exciton mobility is limited over a significant range of excitation energies. This points to the presence of a sub-200 fs, spatially local energy-relaxation mechanism and suggests that local trapping might contribute substantially more in cryogenic experiments than under physiological conditions where the thermal energy is comparable to or larger than the static disorder.

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author
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organization
publishing date
type
Contribution to journal
publication status
published
subject
in
Journal of Chemical Physics
volume
154
issue
4
article number
045102
publisher
American Institute of Physics (AIP)
external identifiers
  • scopus:85100217179
  • pmid:33514092
ISSN
0021-9606
DOI
10.1063/5.0033802
language
English
LU publication?
yes
id
85963639-1065-486b-8aa0-b9dc384c67ea
date added to LUP
2021-02-09 05:26:26
date last changed
2024-06-13 06:57:40
@article{85963639-1065-486b-8aa0-b9dc384c67ea,
  abstract     = {{<p>Over the last several decades, the light-harvesting protein complexes of purple bacteria have been among the most popular model systems for energy transport in excitonic systems in the weak and intermediate intermolecular coupling regime. Despite this extensive body of scientific work, significant questions regarding the excitonic states and the photo-induced dynamics remain. Here, we address the low-temperature electronic structure and excitation dynamics in the light-harvesting complex 2 of Rhodopseudomonas acidophila by two-dimensional electronic spectroscopy. We find that, although at cryogenic temperature energy relaxation is very rapid, exciton mobility is limited over a significant range of excitation energies. This points to the presence of a sub-200 fs, spatially local energy-relaxation mechanism and suggests that local trapping might contribute substantially more in cryogenic experiments than under physiological conditions where the thermal energy is comparable to or larger than the static disorder. </p>}},
  author       = {{Thyrhaug, Erling and Schröter, Marco and Bukartė, Eglė and Kühn, Oliver and Cogdell, Richard and Hauer, Jürgen and Zigmantas, Donatas}},
  issn         = {{0021-9606}},
  language     = {{eng}},
  number       = {{4}},
  publisher    = {{American Institute of Physics (AIP)}},
  series       = {{Journal of Chemical Physics}},
  title        = {{Intraband dynamics and exciton trapping in the LH2 complex of Rhodopseudomonas acidophila}},
  url          = {{http://dx.doi.org/10.1063/5.0033802}},
  doi          = {{10.1063/5.0033802}},
  volume       = {{154}},
  year         = {{2021}},
}