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Watching ultrafast barrierless excited-state isomerization of pseudocyanine in real time

Dietzek, Benjamin LU ; Yartsev, Arkady LU orcid and Tarnovsky, Alexander N. (2007) In The Journal of Physical Chemistry Part B 111(17). p.4520-4526
Abstract
The photoinduced excited-state processes in 1,1'-diethyl-2,2'-cyanine iodine are investigated using femtosecond time-resolved pump-probe spectroscopy. Using a broad range of probe wavelengths, the relaxation of the initially prepared excited-state wavepacket can be followed down to the sink region. The data directly visualize the directed downhill motion along the torsional reaction coordinate and suggest a barrierless excited-state isomerization in the short chain cyanine dye. Additionally, ultrafast ground-state hole and excited-state hole replica broadening is observed. While the narrow excited-state wavepacket broadens during pump-probe overlap, the ground-state hole burning dynamics takes place on a significantly longer time-scale.... (More)
The photoinduced excited-state processes in 1,1'-diethyl-2,2'-cyanine iodine are investigated using femtosecond time-resolved pump-probe spectroscopy. Using a broad range of probe wavelengths, the relaxation of the initially prepared excited-state wavepacket can be followed down to the sink region. The data directly visualize the directed downhill motion along the torsional reaction coordinate and suggest a barrierless excited-state isomerization in the short chain cyanine dye. Additionally, ultrafast ground-state hole and excited-state hole replica broadening is observed. While the narrow excited-state wavepacket broadens during pump-probe overlap, the ground-state hole burning dynamics takes place on a significantly longer time-scale. The experiment reported can be considered as a direct monitoring of the shape and the position of the photoprepared wavepacket on the excited-state potential energy surface. (Less)
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publishing date
type
Contribution to journal
publication status
published
subject
in
The Journal of Physical Chemistry Part B
volume
111
issue
17
pages
4520 - 4526
publisher
The American Chemical Society (ACS)
external identifiers
  • wos:000245954800031
  • scopus:34249034210
ISSN
1520-5207
DOI
10.1021/jp066471a
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
4186d490-c6db-47d3-b91a-acfb893c22d1 (old id 663380)
date added to LUP
2016-04-01 15:38:56
date last changed
2022-01-28 06:22:06
@article{4186d490-c6db-47d3-b91a-acfb893c22d1,
  abstract     = {{The photoinduced excited-state processes in 1,1'-diethyl-2,2'-cyanine iodine are investigated using femtosecond time-resolved pump-probe spectroscopy. Using a broad range of probe wavelengths, the relaxation of the initially prepared excited-state wavepacket can be followed down to the sink region. The data directly visualize the directed downhill motion along the torsional reaction coordinate and suggest a barrierless excited-state isomerization in the short chain cyanine dye. Additionally, ultrafast ground-state hole and excited-state hole replica broadening is observed. While the narrow excited-state wavepacket broadens during pump-probe overlap, the ground-state hole burning dynamics takes place on a significantly longer time-scale. The experiment reported can be considered as a direct monitoring of the shape and the position of the photoprepared wavepacket on the excited-state potential energy surface.}},
  author       = {{Dietzek, Benjamin and Yartsev, Arkady and Tarnovsky, Alexander N.}},
  issn         = {{1520-5207}},
  language     = {{eng}},
  number       = {{17}},
  pages        = {{4520--4526}},
  publisher    = {{The American Chemical Society (ACS)}},
  series       = {{The Journal of Physical Chemistry Part B}},
  title        = {{Watching ultrafast barrierless excited-state isomerization of pseudocyanine in real time}},
  url          = {{http://dx.doi.org/10.1021/jp066471a}},
  doi          = {{10.1021/jp066471a}},
  volume       = {{111}},
  year         = {{2007}},
}