Origin of Long-Lived Coherences in Light-Harvesting Complexes
(2012) In The Journal of Physical Chemistry Part B 116(25). p.7449-7454- Abstract
- A vibronic exciton model is applied to explain the long-lived oscillatory features in the two-dimensional (2D) electronic spectra of the Fenna-Matthews-Olson (FMO) complex. Using experimentally determined parameters and uncorrelated site energy fluctuations, the model predicts oscillations with dephasing times of 1.3 ps at 77 K, which is in a good agreement with the experimental results. These long-lived oscillations originate from the coherent superposition of vibronic exciton states with dominant contributions from vibrational excitations on the same pigment. The oscillations obtain a large amplitude due to excitonic intensity borrowing, which gives transitions with strong vibronic character a significant intensity despite the small... (More)
- A vibronic exciton model is applied to explain the long-lived oscillatory features in the two-dimensional (2D) electronic spectra of the Fenna-Matthews-Olson (FMO) complex. Using experimentally determined parameters and uncorrelated site energy fluctuations, the model predicts oscillations with dephasing times of 1.3 ps at 77 K, which is in a good agreement with the experimental results. These long-lived oscillations originate from the coherent superposition of vibronic exciton states with dominant contributions from vibrational excitations on the same pigment. The oscillations obtain a large amplitude due to excitonic intensity borrowing, which gives transitions with strong vibronic character a significant intensity despite the small Huang-Rhys factor. Purely electronic coherences are found to decay on a 200 fs time scale. (Less)
Please use this url to cite or link to this publication:
https://lup.lub.lu.se/record/2866648
- author
- Christensson, Niklas ; Kauffmann, Harald F. ; Pullerits, Tönu LU and Mancal, Tomas
- organization
- publishing date
- 2012
- type
- Contribution to journal
- publication status
- published
- subject
- in
- The Journal of Physical Chemistry Part B
- volume
- 116
- issue
- 25
- pages
- 7449 - 7454
- publisher
- The American Chemical Society (ACS)
- external identifiers
-
- wos:000305769700007
- scopus:84863007571
- pmid:22642682
- ISSN
- 1520-5207
- DOI
- 10.1021/jp304649c
- 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
- d02b108d-2fa0-4000-bce2-1c8bd6aa2a3f (old id 2866648)
- date added to LUP
- 2016-04-01 13:49:27
- date last changed
- 2023-11-12 22:12:10
@article{d02b108d-2fa0-4000-bce2-1c8bd6aa2a3f,
abstract = {{A vibronic exciton model is applied to explain the long-lived oscillatory features in the two-dimensional (2D) electronic spectra of the Fenna-Matthews-Olson (FMO) complex. Using experimentally determined parameters and uncorrelated site energy fluctuations, the model predicts oscillations with dephasing times of 1.3 ps at 77 K, which is in a good agreement with the experimental results. These long-lived oscillations originate from the coherent superposition of vibronic exciton states with dominant contributions from vibrational excitations on the same pigment. The oscillations obtain a large amplitude due to excitonic intensity borrowing, which gives transitions with strong vibronic character a significant intensity despite the small Huang-Rhys factor. Purely electronic coherences are found to decay on a 200 fs time scale.}},
author = {{Christensson, Niklas and Kauffmann, Harald F. and Pullerits, Tönu and Mancal, Tomas}},
issn = {{1520-5207}},
language = {{eng}},
number = {{25}},
pages = {{7449--7454}},
publisher = {{The American Chemical Society (ACS)}},
series = {{The Journal of Physical Chemistry Part B}},
title = {{Origin of Long-Lived Coherences in Light-Harvesting Complexes}},
url = {{http://dx.doi.org/10.1021/jp304649c}},
doi = {{10.1021/jp304649c}},
volume = {{116}},
year = {{2012}},
}