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Portrait of Tönu Pullerits; Photo: Kennet Ruona

Tönu Pullerits

Professor

Portrait of Tönu Pullerits; Photo: Kennet Ruona

Three-pulse photon echo of an excitonic dimer modeled via Redfield theory

Author

  • Pär Kjellberg
  • Tönu Pullerits

Summary, in English

In this article the third-order response of an excitonically coupled dimer is studied. The three-pulse photon echo signals were calculated by extracting polarization components from the total polarization in the corresponding phase-matched directions. The total nonlinear response was obtained by numeric propagation of the density matrix, with the exciton-vibrational coupling modeled via Redfield relaxation theory. The full two-dimensional three-pulse photon echo signals and the peak shift were analyzed in terms of the density-matrix dynamics of coherence dephasing and population relaxation. The location of the two-exciton state was found to be essential for proper modeling of the three-pulse photon echo. In particular, an oscillation in the three-pulse photon echo peak shift is found if the two-exciton state is displaced. The oscillations can be related to the dynamics of the one-exciton coherences. (c) 2006 American Institute of Physics.

Department/s

  • Chemical Physics

Publishing year

2006

Language

English

Publication/Series

Journal of Chemical Physics

Volume

124

Issue

2

Document type

Journal article

Publisher

American Institute of Physics (AIP)

Topic

  • Atom and Molecular Physics and Optics

Status

Published

Research group

  • Pullerits

ISBN/ISSN/Other

  • ISSN: 0021-9606