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Two-dimensional electronic spectroscopy of an excitonically coupled dimer

Kjellberg, Pär LU ; Brüggemann, Ben LU and Pullerits, Tönu LU (2006) In Physical Review B (Condensed Matter and Materials Physics) 74(2).
Abstract
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... (More)
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. (Less)
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author
organization
publishing date
type
Contribution to journal
publication status
published
subject
in
Physical Review B (Condensed Matter and Materials Physics)
volume
74
issue
2
publisher
American Physical Society
external identifiers
  • wos:000239426600041
  • scopus:33746439778
ISSN
1098-0121
DOI
10.1103/PhysRevB.74.024303
language
English
LU publication?
yes
id
f5ba2e18-53a3-4397-a6c3-5e0e58526c04 (old id 398991)
date added to LUP
2007-10-07 15:56:08
date last changed
2019-03-17 04:24:41
@article{f5ba2e18-53a3-4397-a6c3-5e0e58526c04,
  abstract     = {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.},
  author       = {Kjellberg, Pär and Brüggemann, Ben and Pullerits, Tönu},
  issn         = {1098-0121},
  language     = {eng},
  number       = {2},
  publisher    = {American Physical Society},
  series       = {Physical Review B (Condensed Matter and Materials Physics)},
  title        = {Two-dimensional electronic spectroscopy of an excitonically coupled dimer},
  url          = {http://dx.doi.org/10.1103/PhysRevB.74.024303},
  volume       = {74},
  year         = {2006},
}