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Two-dimensional action spectroscopy of excitonic systems : Explicit simulation using a phase-modulation technique

Damtie, Fikeraddis A. LU ; Wacker, Andreas LU ; Pullerits, Tõnu LU and Karki, Khadga J. LU (2017) In Physical Review A 96(5).
Abstract

Two-dimensional (2D) spectroscopy has been intensively used to study electronic and vibronic coherences in biological systems and semiconductors. This technique studies coherent as well as incoherent signals that arise from the nonlinear interaction of a sequence of laser pulses. In this paper we present a direct evaluation of the 2D signal based on elementary quantum kinetics in order to compare with the common approximate diagrammatic approaches. Here we consider incoherent action signals such as fluorescence or photocurrent as the observable, which is easily accessible in a measurement. These observables are calculated by solving the time evolution of the density matrix in the Lindblad form, which can take into account all possible... (More)

Two-dimensional (2D) spectroscopy has been intensively used to study electronic and vibronic coherences in biological systems and semiconductors. This technique studies coherent as well as incoherent signals that arise from the nonlinear interaction of a sequence of laser pulses. In this paper we present a direct evaluation of the 2D signal based on elementary quantum kinetics in order to compare with the common approximate diagrammatic approaches. Here we consider incoherent action signals such as fluorescence or photocurrent as the observable, which is easily accessible in a measurement. These observables are calculated by solving the time evolution of the density matrix in the Lindblad form, which can take into account all possible decoherence processes. The phase modulation technique is used to separate the relevant nonlinear signals from the other possible interaction pathways. The approach can be used to calculate 2D spectra of any quantum system. For our model system we find a good agreement for the quantum beating between the coupled states.

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author
organization
publishing date
type
Contribution to journal
publication status
published
subject
in
Physical Review A
volume
96
issue
5
publisher
American Physical Society (APS)
external identifiers
  • scopus:85036611691
  • wos:000414951500024
ISSN
2469-9926
DOI
10.1103/PhysRevA.96.053830
language
English
LU publication?
yes
id
ecd9f408-b855-4fb2-a367-1b3dc9f02e13
date added to LUP
2017-12-18 12:02:31
date last changed
2018-05-29 11:01:27
@article{ecd9f408-b855-4fb2-a367-1b3dc9f02e13,
  abstract     = {<p>Two-dimensional (2D) spectroscopy has been intensively used to study electronic and vibronic coherences in biological systems and semiconductors. This technique studies coherent as well as incoherent signals that arise from the nonlinear interaction of a sequence of laser pulses. In this paper we present a direct evaluation of the 2D signal based on elementary quantum kinetics in order to compare with the common approximate diagrammatic approaches. Here we consider incoherent action signals such as fluorescence or photocurrent as the observable, which is easily accessible in a measurement. These observables are calculated by solving the time evolution of the density matrix in the Lindblad form, which can take into account all possible decoherence processes. The phase modulation technique is used to separate the relevant nonlinear signals from the other possible interaction pathways. The approach can be used to calculate 2D spectra of any quantum system. For our model system we find a good agreement for the quantum beating between the coupled states.</p>},
  articleno    = {053830},
  author       = {Damtie, Fikeraddis A. and Wacker, Andreas and Pullerits, Tõnu and Karki, Khadga J.},
  issn         = {2469-9926},
  language     = {eng},
  month        = {11},
  number       = {5},
  publisher    = {American Physical Society (APS)},
  series       = {Physical Review A},
  title        = {Two-dimensional action spectroscopy of excitonic systems : Explicit simulation using a phase-modulation technique},
  url          = {http://dx.doi.org/10.1103/PhysRevA.96.053830},
  volume       = {96},
  year         = {2017},
}