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Exciton coupling induces vibronic hyperchromism in light-harvesting complexes

Schulze, Jan; Torbjörnsson, Magne LU ; Kuehn, Oliver and Pullerits, Tönu LU (2014) In New Journal of Physics 16.
Abstract
The recently suggested possibility that weak vibronic transitions can be excitonically enhanced in light-harvesting complexes is studied in detail. A vibronic exciton dimer model that includes ground-state vibrations is investigated using the multi-configuration time-dependent Hartree method with a parameter set typical to photosynthetic light-harvesting complexes. The absorption spectra are discussed based on the Coulomb coupling, the detuning of the site energies, and the number of vibrational modes. Fluorescence spectra calculations show that the spectral densities obtained from the low-temperature fluorescence line-narrowing measurements of light-harvesting systems need to be corrected for the effects of excitons. For the J-aggregate... (More)
The recently suggested possibility that weak vibronic transitions can be excitonically enhanced in light-harvesting complexes is studied in detail. A vibronic exciton dimer model that includes ground-state vibrations is investigated using the multi-configuration time-dependent Hartree method with a parameter set typical to photosynthetic light-harvesting complexes. The absorption spectra are discussed based on the Coulomb coupling, the detuning of the site energies, and the number of vibrational modes. Fluorescence spectra calculations show that the spectral densities obtained from the low-temperature fluorescence line-narrowing measurements of light-harvesting systems need to be corrected for the effects of excitons. For the J-aggregate configuration, as in most light-harvesting complexes, the true spectral density has a larger amplitude than that obtained from the measurement. (Less)
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author
organization
publishing date
type
Contribution to journal
publication status
published
subject
keywords
coherence, electronic 2D spectroscopy, excitons, vibronic coupling, Huang-Rhys factor, fluorescence line narrowing
in
New Journal of Physics
volume
16
publisher
IOP Publishing Ltd.
external identifiers
  • wos:000334518500001
  • scopus:84899526835
ISSN
1367-2630
DOI
10.1088/1367-2630/16/4/045010
language
English
LU publication?
yes
id
7b6c9e05-c708-4f5d-815a-9e9c8b58ec12 (old id 4488682)
date added to LUP
2014-06-23 13:40:25
date last changed
2017-10-29 03:47:39
@article{7b6c9e05-c708-4f5d-815a-9e9c8b58ec12,
  abstract     = {The recently suggested possibility that weak vibronic transitions can be excitonically enhanced in light-harvesting complexes is studied in detail. A vibronic exciton dimer model that includes ground-state vibrations is investigated using the multi-configuration time-dependent Hartree method with a parameter set typical to photosynthetic light-harvesting complexes. The absorption spectra are discussed based on the Coulomb coupling, the detuning of the site energies, and the number of vibrational modes. Fluorescence spectra calculations show that the spectral densities obtained from the low-temperature fluorescence line-narrowing measurements of light-harvesting systems need to be corrected for the effects of excitons. For the J-aggregate configuration, as in most light-harvesting complexes, the true spectral density has a larger amplitude than that obtained from the measurement.},
  articleno    = {045010},
  author       = {Schulze, Jan and Torbjörnsson, Magne and Kuehn, Oliver and Pullerits, Tönu},
  issn         = {1367-2630},
  keyword      = {coherence,electronic 2D spectroscopy,excitons,vibronic coupling,Huang-Rhys factor,fluorescence line narrowing},
  language     = {eng},
  publisher    = {IOP Publishing Ltd.},
  series       = {New Journal of Physics},
  title        = {Exciton coupling induces vibronic hyperchromism in light-harvesting complexes},
  url          = {http://dx.doi.org/10.1088/1367-2630/16/4/045010},
  volume       = {16},
  year         = {2014},
}