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Portrait of Tönu Pullerits; Photo: Kennet Ruona

Tönu Pullerits

Professor

Portrait of Tönu Pullerits; Photo: Kennet Ruona

Two-dimensional electronic spectroscopy of an excitonically coupled dimer

Author

  • Pär Kjellberg
  • Ben Brüggemann
  • Tönu Pullerits

Summary, in English

The two-dimensional three-pulse photon echo signals from a dimer system are investigated in detail. A perturbative approach is used to calculate the response of the system via a numerical propagation of the density matrix in exciton state representation. Exciton vibrational coupling is modeled by Redfield relaxation theory. The main goal of this paper is to dissect the two-dimensional spectrum of the dimer to give better understanding of how the dynamics influence the spectral features. We will show how different Liouville pathways lead to the appearance/disappearance of diagonal and cross peaks. The inclusion of a Gaussian shaped electric field will be contrasted to the use of delta-pulses in the impulsive limit. The impulsive limit is found to be a satisfactory approximation at long population times, while at shorter times, in the pulse-overlap region, more realistic electric fields are called for.

Department/s

  • Chemical Physics

Publishing year

2006

Language

English

Publication/Series

Physical Review B (Condensed Matter and Materials Physics)

Volume

74

Issue

2

Document type

Journal article

Publisher

American Physical Society

Topic

  • Atom and Molecular Physics and Optics

Status

Published

Research group

  • Pullerits

ISBN/ISSN/Other

  • ISSN: 1098-0121