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)
Please use this url to cite or link to this publication:
https://lup.lub.lu.se/record/1289533
- author
- Christensson, Niklas
LU
; Dietzek, Benjamin
LU
; Yartsev, Arkady
LU
and Pullerits, Tönu
LU
- organization
- publishing date
- 2009
- type
- Contribution to journal
- publication status
- published
- subject
- in
- Journal of Chemical Physics
- volume
- 130
- issue
- 2
- article number
- 024510
- publisher
- American Institute of Physics (AIP)
- external identifiers
-
- wos:000263112600030
- pmid:19154041
- scopus:58449086136
- pmid:19154041
- ISSN
- 0021-9606
- DOI
- 10.1063/1.2990652
- 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
- 7edffab5-ff1d-43ae-be7a-fa030bf62661 (old id 1289533)
- date added to LUP
- 2016-04-01 11:46:59
- date last changed
- 2022-01-26 18:07:58
@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.}},
author = {{Christensson, Niklas and Dietzek, Benjamin and Yartsev, Arkady and Pullerits, Tönu}},
issn = {{0021-9606}},
language = {{eng}},
number = {{2}},
publisher = {{American Institute of Physics (AIP)}},
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}},
doi = {{10.1063/1.2990652}},
volume = {{130}},
year = {{2009}},
}