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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28 January 2021
Research Article|
January 27 2021
Intraband dynamics and exciton trapping in the LH2 complex of Rhodopseudomonas acidophila
Erling Thyrhaug
;
Erling Thyrhaug
1
Dynamical Spectroscopy, Department of Chemistry, Technical University of Munich
, Lichtenbergstraße 4, 85748 Garching b. Munich, Germany
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Marco Schröter
;
Marco Schröter
2
Chemical Physics, Department of Chemistry, Lund University
, P.O. Box 124, SE-22100 Lund, Sweden
3
Institute of Physics, University of Rostock
, Albert Einstein Straße 23-24, 18059 Rostock, Germany
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Eglė Bukartė
;
Eglė Bukartė
2
Chemical Physics, Department of Chemistry, Lund University
, P.O. Box 124, SE-22100 Lund, Sweden
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Oliver Kühn
;
Oliver Kühn
3
Institute of Physics, University of Rostock
, Albert Einstein Straße 23-24, 18059 Rostock, Germany
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Richard Cogdell
;
Richard Cogdell
4
Institute of Molecular, Cell and Systems Biology, University of Glasgow
, Room 402 Davidson Building, Glasgow G12 8QQ, Scotland
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Jürgen Hauer
;
Jürgen Hauer
1
Dynamical Spectroscopy, Department of Chemistry, Technical University of Munich
, Lichtenbergstraße 4, 85748 Garching b. Munich, Germany
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Donatas Zigmantas
Donatas Zigmantas
a)
2
Chemical Physics, Department of Chemistry, Lund University
, P.O. Box 124, SE-22100 Lund, Sweden
a)Author to whom correspondence should be addressed: [email protected]
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a)Author to whom correspondence should be addressed: [email protected]
Note: This paper is part of the JCP Special Topic on Excitons: Energetics and Spatio-Temporal Dynamics.
J. Chem. Phys. 154, 045102 (2021)
Article history
Received:
October 19 2020
Accepted:
January 02 2021
Citation
Erling Thyrhaug, Marco Schröter, Eglė Bukartė, Oliver Kühn, Richard Cogdell, Jürgen Hauer, Donatas Zigmantas; Intraband dynamics and exciton trapping in the LH2 complex of Rhodopseudomonas acidophila. J. Chem. Phys. 28 January 2021; 154 (4): 045102. https://doi.org/10.1063/5.0033802
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