Tönu Pullerits
Professor
Three-pulse photon echo of an excitonic dimer modeled via Redfield theory
Author
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
ISBN/ISSN/Other
- ISSN: 0021-9606