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Vibronic origin of long-lived coherence in an artificial molecular light harvester.

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Title: Vibronic origin of long-lived coherence in an artificial molecular light harvester.
Authors: Lim, J
Paleček, D
Caycedo-Soler, F
Lincoln, CN
Prior, J
von Berlepsch, H
Huelga, SF
Plenio, MB
Zigmantas, D
Hauer, J
Item Type: Journal Article
Abstract: Natural and artificial light-harvesting processes have recently gained new interest. Signatures of long-lasting coherence in spectroscopic signals of biological systems have been repeatedly observed, albeit their origin is a matter of ongoing debate, as it is unclear how the loss of coherence due to interaction with the noisy environments in such systems is averted. Here we report experimental and theoretical verification of coherent exciton-vibrational (vibronic) coupling as the origin of long-lasting coherence in an artificial light harvester, a molecular J-aggregate. In this macroscopically aligned tubular system, polarization-controlled 2D spectroscopy delivers an uncongested and specific optical response as an ideal foundation for an in-depth theoretical description. We derive analytical expressions that show under which general conditions vibronic coupling leads to prolonged excited-state coherence.
Issue Date: 9-Jul-2015
Date of Acceptance: 4-Jun-2015
URI: http://hdl.handle.net/10044/1/25393
DOI: https://dx.doi.org/10.1038/ncomms8755
ISSN: 2041-1723
Publisher: Nature Publishing Group
Journal / Book Title: Nature Communications
Volume: 6
Copyright Statement: © 2015, Rights Managed by Nature Publishing Group. This work is licensed under a Creative Commons Attribution 4.0 International License. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in the credit line; if the material is not included under the Creative Commons license, users will need to obtain permission from the license holder to reproduce the material. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/
Publication Status: Published
Article Number: 7755
Appears in Collections:Quantum Optics and Laser Science
Faculty of Natural Sciences

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