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Transfer of vibrational coherence through incoherent energy transfer process in Forster limit

Mancal, Tomas; Dostal, Jakub LU ; Psencik, Jakub and Zigmantas, Donatas LU (2014) In Canadian Journal of Chemistry 92(2). p.135-143
Abstract
We study transfer of coherent nuclear oscillations between an excitation energy donor and an acceptor in a simple dimeric electronic system coupled to an unstructured thermodynamic bath and some pronounced vibrational intramolecular mode. Our focus is on the nonlinear optical response of such a system, i.e., we study both excited state energy transfer and the compensation of the so-called ground-state bleach signal. The response function formalism enables us to investigate a heterodimer with monomers coupled strongly to the bath and by a weak resonance coupling to each other (Forster rate limit). Our work is motivated by recent observation of various vibrational signatures in two-dimensional coherent spectra of energy-transferring systems... (More)
We study transfer of coherent nuclear oscillations between an excitation energy donor and an acceptor in a simple dimeric electronic system coupled to an unstructured thermodynamic bath and some pronounced vibrational intramolecular mode. Our focus is on the nonlinear optical response of such a system, i.e., we study both excited state energy transfer and the compensation of the so-called ground-state bleach signal. The response function formalism enables us to investigate a heterodimer with monomers coupled strongly to the bath and by a weak resonance coupling to each other (Forster rate limit). Our work is motivated by recent observation of various vibrational signatures in two-dimensional coherent spectra of energy-transferring systems including large structures with a fast energy diffusion. We find that the vibrational coherence can be transferred from donor to acceptor molecules provided the transfer rate is sufficiently fast. The ground-state bleach signal of the acceptor molecules does not show any oscillatory signatures, and oscillations in ground-state bleaching signal of the donor prevail with the amplitude, which is not decreasing with the relaxation rate. (Less)
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author
organization
publishing date
type
Contribution to journal
publication status
published
subject
keywords
2D coherent spectroscopy, vibrational coherence, coherence transfer, energy transfer
in
Canadian Journal of Chemistry
volume
92
issue
2
pages
135 - 143
publisher
NRC Research Press
external identifiers
  • wos:000334030500009
  • scopus:84894206161
ISSN
0008-4042
DOI
10.1139/cjc-2013-0351
language
English
LU publication?
yes
id
7712c704-7712-4623-8345-0ceaf7e270cf (old id 4439931)
date added to LUP
2014-05-20 09:55:04
date last changed
2017-09-17 06:53:20
@article{7712c704-7712-4623-8345-0ceaf7e270cf,
  abstract     = {We study transfer of coherent nuclear oscillations between an excitation energy donor and an acceptor in a simple dimeric electronic system coupled to an unstructured thermodynamic bath and some pronounced vibrational intramolecular mode. Our focus is on the nonlinear optical response of such a system, i.e., we study both excited state energy transfer and the compensation of the so-called ground-state bleach signal. The response function formalism enables us to investigate a heterodimer with monomers coupled strongly to the bath and by a weak resonance coupling to each other (Forster rate limit). Our work is motivated by recent observation of various vibrational signatures in two-dimensional coherent spectra of energy-transferring systems including large structures with a fast energy diffusion. We find that the vibrational coherence can be transferred from donor to acceptor molecules provided the transfer rate is sufficiently fast. The ground-state bleach signal of the acceptor molecules does not show any oscillatory signatures, and oscillations in ground-state bleaching signal of the donor prevail with the amplitude, which is not decreasing with the relaxation rate.},
  author       = {Mancal, Tomas and Dostal, Jakub and Psencik, Jakub and Zigmantas, Donatas},
  issn         = {0008-4042},
  keyword      = {2D coherent spectroscopy,vibrational coherence,coherence transfer,energy transfer},
  language     = {eng},
  number       = {2},
  pages        = {135--143},
  publisher    = {NRC Research Press},
  series       = {Canadian Journal of Chemistry},
  title        = {Transfer of vibrational coherence through incoherent energy transfer process in Forster limit},
  url          = {http://dx.doi.org/10.1139/cjc-2013-0351},
  volume       = {92},
  year         = {2014},
}