Advanced

Potential surfaces and delocalization of excitons in dimers

Beenken, Wichard LU ; Dahlbom, Mats LU ; Kjellberg, Pär LU and Pullerits, Tönu LU (2002) In Journal of Chemical Physics 117(12). p.5810-5820
Abstract
In the present work we will demonstrate that the nuclear dynamics have a strong influence on the delocalization of an exciton in a dimer, even if they do not effect the excitonic interaction. It will be shown that the internal nuclear conformation of the molecules forming the dimer depends critically on the delocalization of the exciton state in the dimer and vice versa. The resulting closed loop enforces a localization of the lower excitonic state, but, contrary to the commonly accepted view, a delocalization of the upper one. Qualitatively different time-evolution of the delocalization length for the lower and upper excitonic state will be shown. Besides, it will turn out that the nuclear motions inhibit a complete delocalization of the... (More)
In the present work we will demonstrate that the nuclear dynamics have a strong influence on the delocalization of an exciton in a dimer, even if they do not effect the excitonic interaction. It will be shown that the internal nuclear conformation of the molecules forming the dimer depends critically on the delocalization of the exciton state in the dimer and vice versa. The resulting closed loop enforces a localization of the lower excitonic state, but, contrary to the commonly accepted view, a delocalization of the upper one. Qualitatively different time-evolution of the delocalization length for the lower and upper excitonic state will be shown. Besides, it will turn out that the nuclear motions inhibit a complete delocalization of the excitonic state in any case. To accomplish nuclear and exciton dynamics, the nonadiabatic coupling between the two excitonic states will be deduced. This causes a relaxation from the upper to the lower excitonic state, which limits the maximum reachable exciton delocalization. (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
Journal of Chemical Physics
volume
117
issue
12
pages
5810 - 5820
publisher
American Institute of Physics
external identifiers
  • wos:000177825500033
  • scopus:0037159078
ISSN
0021-9606
DOI
10.1063/1.1502647
language
English
LU publication?
yes
id
031b2b92-e8b6-4162-9f4e-3ec1f3d31bf2 (old id 329444)
date added to LUP
2007-08-08 09:53:19
date last changed
2017-12-10 03:41:52
@article{031b2b92-e8b6-4162-9f4e-3ec1f3d31bf2,
  abstract     = {In the present work we will demonstrate that the nuclear dynamics have a strong influence on the delocalization of an exciton in a dimer, even if they do not effect the excitonic interaction. It will be shown that the internal nuclear conformation of the molecules forming the dimer depends critically on the delocalization of the exciton state in the dimer and vice versa. The resulting closed loop enforces a localization of the lower excitonic state, but, contrary to the commonly accepted view, a delocalization of the upper one. Qualitatively different time-evolution of the delocalization length for the lower and upper excitonic state will be shown. Besides, it will turn out that the nuclear motions inhibit a complete delocalization of the excitonic state in any case. To accomplish nuclear and exciton dynamics, the nonadiabatic coupling between the two excitonic states will be deduced. This causes a relaxation from the upper to the lower excitonic state, which limits the maximum reachable exciton delocalization.},
  author       = {Beenken, Wichard and Dahlbom, Mats and Kjellberg, Pär and Pullerits, Tönu},
  issn         = {0021-9606},
  language     = {eng},
  number       = {12},
  pages        = {5810--5820},
  publisher    = {American Institute of Physics},
  series       = {Journal of Chemical Physics},
  title        = {Potential surfaces and delocalization of excitons in dimers},
  url          = {http://dx.doi.org/10.1063/1.1502647},
  volume       = {117},
  year         = {2002},
}