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Exciton-vibrational coupling in molecular aggregates: Electronic versus vibronic dimer

Polyutov, Sergey LU ; Kuehn, Oliver and Pullerits, Tönu LU (2012) In Chemical Physics 394(1). p.21-28
Abstract
The influence of exciton-vibrational coupling on the energy level structure, oscillator strength, and relaxation dynamics is investigated for two different excitonic dimer models. As compared with a purely electronic dimer, the inclusion of local vibrational modes within a vibronic dimer gives rise to a complex energy level structure including avoided crossings and changes of the nature of the exciton states from electronic to vibrational character. Besides these static properties, the dissipative dynamics of the two models is systematically investigated using Redfield relaxation theory. In case of the vibronic dimer this allows to treat selected vibrational degrees of freedom beyond the limits of perturbation theory and Markov... (More)
The influence of exciton-vibrational coupling on the energy level structure, oscillator strength, and relaxation dynamics is investigated for two different excitonic dimer models. As compared with a purely electronic dimer, the inclusion of local vibrational modes within a vibronic dimer gives rise to a complex energy level structure including avoided crossings and changes of the nature of the exciton states from electronic to vibrational character. Besides these static properties, the dissipative dynamics of the two models is systematically investigated using Redfield relaxation theory. In case of the vibronic dimer this allows to treat selected vibrational degrees of freedom beyond the limits of perturbation theory and Markov approximation. It is demonstrated that the vibronic dimer gives rise to transient vibrational population trapping in the one-exciton manifold. (C) 2011 Elsevier B.V. All rights reserved. (Less)
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author
organization
publishing date
type
Contribution to journal
publication status
published
subject
keywords
Frenkel excitons, Vibronic coupling, Dissipation theory
in
Chemical Physics
volume
394
issue
1
pages
21 - 28
publisher
Elsevier
external identifiers
  • wos:000299678900004
  • scopus:84856296994
ISSN
0301-0104
DOI
10.1016/j.chemphys.2011.12.006
language
English
LU publication?
yes
id
a7d8eae9-bb79-40d3-8ad8-be48e447adf5 (old id 2416149)
date added to LUP
2012-03-28 10:19:17
date last changed
2017-10-01 04:13:39
@article{a7d8eae9-bb79-40d3-8ad8-be48e447adf5,
  abstract     = {The influence of exciton-vibrational coupling on the energy level structure, oscillator strength, and relaxation dynamics is investigated for two different excitonic dimer models. As compared with a purely electronic dimer, the inclusion of local vibrational modes within a vibronic dimer gives rise to a complex energy level structure including avoided crossings and changes of the nature of the exciton states from electronic to vibrational character. Besides these static properties, the dissipative dynamics of the two models is systematically investigated using Redfield relaxation theory. In case of the vibronic dimer this allows to treat selected vibrational degrees of freedom beyond the limits of perturbation theory and Markov approximation. It is demonstrated that the vibronic dimer gives rise to transient vibrational population trapping in the one-exciton manifold. (C) 2011 Elsevier B.V. All rights reserved.},
  author       = {Polyutov, Sergey and Kuehn, Oliver and Pullerits, Tönu},
  issn         = {0301-0104},
  keyword      = {Frenkel excitons,Vibronic coupling,Dissipation theory},
  language     = {eng},
  number       = {1},
  pages        = {21--28},
  publisher    = {Elsevier},
  series       = {Chemical Physics},
  title        = {Exciton-vibrational coupling in molecular aggregates: Electronic versus vibronic dimer},
  url          = {http://dx.doi.org/10.1016/j.chemphys.2011.12.006},
  volume       = {394},
  year         = {2012},
}