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Near-infrared time-resolved study of the S-1 state dynamics of the carotenoid spheroidene

Polívka, Tornáš LU ; Zigmantas, Donatas LU orcid ; Frank, Harry A. ; Bautista, James A. ; Herek, Jennifer L. LU ; Koyama, Yasushi ; Fujii, Ritsuko and Sundström, Villy LU (2001) In The Journal of Physical Chemistry Part B 105(5). p.1072-1080
Abstract
Using a novel experimental approach based on near-infrared femtosecond absorption spectroscopy, we have determined the energy of the S-1 state of the carotenoid spheroidene. The energy of this state is 13 400 +/- 90 cm(-1) at both 293 and 186 K, showing that there is no temperature-induced shift of the S-1 level. A discrepancy of about 800 cm(-1) between the S-1 energy determined here and that obtained from previous fluorescence and resonance Raman measurements is explained in terms of the different conformational species coexisting in the S-1 excited state. Measurements of kinetics in the near-infrared region revealed that at least three relaxation processes take place after excitation of spheroidene into its S-2 state. Ultrafast S-2... (More)
Using a novel experimental approach based on near-infrared femtosecond absorption spectroscopy, we have determined the energy of the S-1 state of the carotenoid spheroidene. The energy of this state is 13 400 +/- 90 cm(-1) at both 293 and 186 K, showing that there is no temperature-induced shift of the S-1 level. A discrepancy of about 800 cm(-1) between the S-1 energy determined here and that obtained from previous fluorescence and resonance Raman measurements is explained in terms of the different conformational species coexisting in the S-1 excited state. Measurements of kinetics in the near-infrared region revealed that at least three relaxation processes take place after excitation of spheroidene into its S-2 state. Ultrafast S-2 --> S-1 internal conversion occurs within the first 300 fs, followed by vibrational cooling in the SI state, which occurs on a time scale of similar to 700 fs. The S-1 lifetime is 8 ps at 293 K, in good agreement with previous measurements of the S-1 --> S-N transition. A somewhat longer S-1 lifetime of 9.5 ps is observed at 186 K. (Less)
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author
; ; ; ; ; ; and
organization
publishing date
type
Contribution to journal
publication status
published
subject
keywords
long polyenes, crystal-structure, different extents, 2-photon fluorescence excitation, light-harvesting complex, rhodobacter-sphaeroides r-26.1, pi-electron conjugation, all-trans-spheroidene, xanthophyll cycle, energy-transfer
in
The Journal of Physical Chemistry Part B
volume
105
issue
5
pages
9 pages
publisher
The American Chemical Society (ACS)
external identifiers
  • scopus:0038202572
ISSN
1520-5207
DOI
10.1021/jp002206s
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
c391741e-3da7-4f75-8b89-70579ffa1cbf (old id 1432986)
date added to LUP
2016-04-04 09:19:13
date last changed
2022-02-21 00:10:45
@article{c391741e-3da7-4f75-8b89-70579ffa1cbf,
  abstract     = {{Using a novel experimental approach based on near-infrared femtosecond absorption spectroscopy, we have determined the energy of the S-1 state of the carotenoid spheroidene. The energy of this state is 13 400 +/- 90 cm(-1) at both 293 and 186 K, showing that there is no temperature-induced shift of the S-1 level. A discrepancy of about 800 cm(-1) between the S-1 energy determined here and that obtained from previous fluorescence and resonance Raman measurements is explained in terms of the different conformational species coexisting in the S-1 excited state. Measurements of kinetics in the near-infrared region revealed that at least three relaxation processes take place after excitation of spheroidene into its S-2 state. Ultrafast S-2 --> S-1 internal conversion occurs within the first 300 fs, followed by vibrational cooling in the SI state, which occurs on a time scale of similar to 700 fs. The S-1 lifetime is 8 ps at 293 K, in good agreement with previous measurements of the S-1 --> S-N transition. A somewhat longer S-1 lifetime of 9.5 ps is observed at 186 K.}},
  author       = {{Polívka, Tornáš and Zigmantas, Donatas and Frank, Harry A. and Bautista, James A. and Herek, Jennifer L. and Koyama, Yasushi and Fujii, Ritsuko and Sundström, Villy}},
  issn         = {{1520-5207}},
  keywords     = {{long polyenes; crystal-structure; different extents; 2-photon fluorescence excitation; light-harvesting complex; rhodobacter-sphaeroides r-26.1; pi-electron conjugation; all-trans-spheroidene; xanthophyll cycle; energy-transfer}},
  language     = {{eng}},
  month        = {{02}},
  number       = {{5}},
  pages        = {{1072--1080}},
  publisher    = {{The American Chemical Society (ACS)}},
  series       = {{The Journal of Physical Chemistry Part B}},
  title        = {{Near-infrared time-resolved study of the S-1 state dynamics of the carotenoid spheroidene}},
  url          = {{http://dx.doi.org/10.1021/jp002206s}},
  doi          = {{10.1021/jp002206s}},
  volume       = {{105}},
  year         = {{2001}},
}