Advanced

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

Lim, James; Palecek, David LU ; Caycedo-Soler, Felipe; Lincoln, Craig N; Prior, Javier; von Berlepsch, Hans; Huelga, Susana F; Plenio, Martin B; Zigmantas, Donatas LU and Hauer, Jürgen (2015) In Nature Communications 6.
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... (More)
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. (Less)
Please use this url to cite or link to this publication:
author
organization
publishing date
type
Contribution to journal
publication status
published
subject
in
Nature Communications
volume
6
publisher
Nature Publishing Group
external identifiers
  • pmid:26158602
  • wos:000358858500061
  • scopus:84937019662
ISSN
2041-1723
DOI
10.1038/ncomms8755
language
English
LU publication?
yes
id
797bbc72-9762-439b-89e8-0a4bfc53b581 (old id 7750001)
date added to LUP
2015-09-21 15:08:56
date last changed
2017-11-19 03:57:29
@article{797bbc72-9762-439b-89e8-0a4bfc53b581,
  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.},
  articleno    = {7755},
  author       = {Lim, James and Palecek, David and Caycedo-Soler, Felipe and Lincoln, Craig N and Prior, Javier and von Berlepsch, Hans and Huelga, Susana F and Plenio, Martin B and Zigmantas, Donatas and Hauer, Jürgen},
  issn         = {2041-1723},
  language     = {eng},
  publisher    = {Nature Publishing Group},
  series       = {Nature Communications},
  title        = {Vibronic origin of long-lived coherence in an artificial molecular light harvester.},
  url          = {http://dx.doi.org/10.1038/ncomms8755},
  volume       = {6},
  year         = {2015},
}