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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
; and
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
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
f5ba2e18-53a3-4397-a6c3-5e0e58526c04 (old id 398991)
date added to LUP
2016-04-01 16:31:26
date last changed
2022-01-28 20:17:47
@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}},
  doi          = {{10.1103/PhysRevB.74.024303}},
  volume       = {{74}},
  year         = {{2006}},
}