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:
https://lup.lub.lu.se/record/7750001
- author
- 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
- organization
- publishing date
- 2015
- type
- Contribution to journal
- publication status
- published
- subject
- in
- Nature Communications
- volume
- 6
- article number
- 7755
- publisher
- Nature Publishing Group
- external identifiers
-
- pmid:26158602
- wos:000358858500061
- scopus:84937019662
- pmid:26158602
- ISSN
- 2041-1723
- DOI
- 10.1038/ncomms8755
- 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
- 797bbc72-9762-439b-89e8-0a4bfc53b581 (old id 7750001)
- date added to LUP
- 2016-04-01 14:32:27
- date last changed
- 2023-11-13 08:54:02
@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.}},
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}},
doi = {{10.1038/ncomms8755}},
volume = {{6}},
year = {{2015}},
}