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Portrait of Tönu Pullerits; Photo: Kennet Ruona

Tönu Pullerits

Professor

Portrait of Tönu Pullerits; Photo: Kennet Ruona

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

Author

  • Sergey Polyutov
  • Oliver Kuehn
  • Tönu Pullerits

Summary, in English

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.

Department/s

  • Chemical Physics
  • NanoLund: Center for Nanoscience

Publishing year

2012

Language

English

Pages

21-28

Publication/Series

Chemical Physics

Volume

394

Issue

1

Document type

Journal article

Publisher

Elsevier

Topic

  • Atom and Molecular Physics and Optics

Keywords

  • Frenkel excitons
  • Vibronic coupling
  • Dissipation theory

Status

Published

ISBN/ISSN/Other

  • ISSN: 0301-0104