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

Kjellberg, Pär LU and Pullerits, Tönu LU (2006) In Journal of Chemical Physics 124(2).
Abstract
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... (More)
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. (Less)
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Contribution to journal
publication status
published
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in
Journal of Chemical Physics
volume
124
issue
2
publisher
American Institute of Physics (AIP)
external identifiers
  • wos:000234607700011
  • scopus:30744448636
ISSN
0021-9606
DOI
10.1063/1.2150447
language
English
LU publication?
yes
additional info
The information about affiliations in this record was updated in December 2015. The record was previously connected to the following departments: Chemical Physics (S) (011001060)
id
caf6a3e5-dbc5-4023-89ff-5e263bfb0959 (old id 421322)
date added to LUP
2016-04-01 12:27:10
date last changed
2021-10-06 03:06:04
@article{caf6a3e5-dbc5-4023-89ff-5e263bfb0959,
  abstract     = {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.},
  author       = {Kjellberg, Pär and Pullerits, Tönu},
  issn         = {0021-9606},
  language     = {eng},
  number       = {2},
  publisher    = {American Institute of Physics (AIP)},
  series       = {Journal of Chemical Physics},
  title        = {Three-pulse photon echo of an excitonic dimer modeled via Redfield theory},
  url          = {http://dx.doi.org/10.1063/1.2150447},
  doi          = {10.1063/1.2150447},
  volume       = {124},
  year         = {2006},
}