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Probing the strength of the system-bath interaction by three-pulse photon echoes.

Christensson, Niklas LU ; Dietzek, Benjamin LU ; Yartsev, Arkady LU and Pullerits, Tönu LU (2009) In Journal of Chemical Physics 130(2).
Abstract
We explore how the width of the three-pulse photon echo signal at long population times can be used to determine the strength of the system-bath interaction. Using simulation with finite pulses we show that a simple relation exist between the width of the echo signal, the coupling strength, and the pulse autocorrelation. The derived model is applied to Rhodamine 6G in alcoholic solution, a paradigm system for the study of solvation dynamics, and the results are compared to conventional methods. The independently determined coupling strength forms the basis for a computationally inexpensive route to determine the entire spectral density, the key parameter when considering system-bath interactions. Our method allows us to accurately estimate... (More)
We explore how the width of the three-pulse photon echo signal at long population times can be used to determine the strength of the system-bath interaction. Using simulation with finite pulses we show that a simple relation exist between the width of the echo signal, the coupling strength, and the pulse autocorrelation. The derived model is applied to Rhodamine 6G in alcoholic solution, a paradigm system for the study of solvation dynamics, and the results are compared to conventional methods. The independently determined coupling strength forms the basis for a computationally inexpensive route to determine the entire spectral density, the key parameter when considering system-bath interactions. Our method allows us to accurately estimate the relative amplitude of fast and slow components in the correlation function using only impulsive limit simulations. We show that the peak shift significantly overestimates the amplitude of the fastest decay component for our experimental data. Changing solvent from methanol to 1-hexanol we observe a narrowing of the width of the echo profile. The changes in the echo width allow us to estimate the changes of the coupling strength in various solvents. (Less)
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author
organization
publishing date
type
Contribution to journal
publication status
published
subject
in
Journal of Chemical Physics
volume
130
issue
2
publisher
American Institute of Physics
external identifiers
  • wos:000263112600030
  • pmid:19154041
  • scopus:58449086136
ISSN
0021-9606
DOI
10.1063/1.2990652
language
English
LU publication?
yes
id
7edffab5-ff1d-43ae-be7a-fa030bf62661 (old id 1289533)
date added to LUP
2009-02-18 12:44:03
date last changed
2017-01-01 04:32:18
@article{7edffab5-ff1d-43ae-be7a-fa030bf62661,
  abstract     = {We explore how the width of the three-pulse photon echo signal at long population times can be used to determine the strength of the system-bath interaction. Using simulation with finite pulses we show that a simple relation exist between the width of the echo signal, the coupling strength, and the pulse autocorrelation. The derived model is applied to Rhodamine 6G in alcoholic solution, a paradigm system for the study of solvation dynamics, and the results are compared to conventional methods. The independently determined coupling strength forms the basis for a computationally inexpensive route to determine the entire spectral density, the key parameter when considering system-bath interactions. Our method allows us to accurately estimate the relative amplitude of fast and slow components in the correlation function using only impulsive limit simulations. We show that the peak shift significantly overestimates the amplitude of the fastest decay component for our experimental data. Changing solvent from methanol to 1-hexanol we observe a narrowing of the width of the echo profile. The changes in the echo width allow us to estimate the changes of the coupling strength in various solvents.},
  articleno    = {024510},
  author       = {Christensson, Niklas and Dietzek, Benjamin and Yartsev, Arkady and Pullerits, Tönu},
  issn         = {0021-9606},
  language     = {eng},
  number       = {2},
  publisher    = {American Institute of Physics},
  series       = {Journal of Chemical Physics},
  title        = {Probing the strength of the system-bath interaction by three-pulse photon echoes.},
  url          = {http://dx.doi.org/10.1063/1.2990652},
  volume       = {130},
  year         = {2009},
}