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Photon echo spectroscopy reveals structure-dynamics relationships in carotenoids

Christensson, Niklas LU ; Polivka, Tomas LU ; Yartsev, Arkady LU and Pullerits, Tönu LU (2009) In Physical Review B (Condensed Matter and Materials Physics) 79(24).
Abstract
Based on simultaneous analysis of the frequency-resolved transient grating, peak shift, and echo width signals, we present a model for the third-order optical response of carotenoids including population dynamics and system-bath interactions. Our frequency-resolved photon echo experiments show that the model needs to incorporate the excited-state absorption from both the S-2 and the S-1 states. We apply our model to analyze the experimental results on astaxanthin and lycopene, aiming to elucidate the relation between structure and system-bath interactions. Our analysis allows us to relate structural motifs to changes in the energy-gap correlation functions. We find that the terminal rings of astaxanthin lead to increased coupling between... (More)
Based on simultaneous analysis of the frequency-resolved transient grating, peak shift, and echo width signals, we present a model for the third-order optical response of carotenoids including population dynamics and system-bath interactions. Our frequency-resolved photon echo experiments show that the model needs to incorporate the excited-state absorption from both the S-2 and the S-1 states. We apply our model to analyze the experimental results on astaxanthin and lycopene, aiming to elucidate the relation between structure and system-bath interactions. Our analysis allows us to relate structural motifs to changes in the energy-gap correlation functions. We find that the terminal rings of astaxanthin lead to increased coupling between slow molecular motions and the electronic transition. We also find evidence for stronger coupling to higher frequency overdamped modes in astaxanthin, pointing to the importance of the functional groups in providing coupling to fluctuations influencing the dynamics in the passage through the conical intersection governing the S-2-S-1 relaxation. (Less)
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author
organization
publishing date
type
Contribution to journal
publication status
published
subject
keywords
organic compounds, excited states, electron correlations, energy gap, photon echo, time resolved spectra
in
Physical Review B (Condensed Matter and Materials Physics)
volume
79
issue
24
publisher
American Physical Society
external identifiers
  • wos:000267699700052
  • scopus:67650164987
ISSN
1098-0121
DOI
10.1103/PhysRevB.79.245118
language
English
LU publication?
yes
id
fe262b30-c012-4b90-ad82-fec418ede5f6 (old id 1462360)
date added to LUP
2009-08-20 12:08:57
date last changed
2017-01-01 06:09:11
@article{fe262b30-c012-4b90-ad82-fec418ede5f6,
  abstract     = {Based on simultaneous analysis of the frequency-resolved transient grating, peak shift, and echo width signals, we present a model for the third-order optical response of carotenoids including population dynamics and system-bath interactions. Our frequency-resolved photon echo experiments show that the model needs to incorporate the excited-state absorption from both the S-2 and the S-1 states. We apply our model to analyze the experimental results on astaxanthin and lycopene, aiming to elucidate the relation between structure and system-bath interactions. Our analysis allows us to relate structural motifs to changes in the energy-gap correlation functions. We find that the terminal rings of astaxanthin lead to increased coupling between slow molecular motions and the electronic transition. We also find evidence for stronger coupling to higher frequency overdamped modes in astaxanthin, pointing to the importance of the functional groups in providing coupling to fluctuations influencing the dynamics in the passage through the conical intersection governing the S-2-S-1 relaxation.},
  author       = {Christensson, Niklas and Polivka, Tomas and Yartsev, Arkady and Pullerits, Tönu},
  issn         = {1098-0121},
  keyword      = {organic compounds,excited states,electron correlations,energy gap,photon echo,time resolved spectra},
  language     = {eng},
  number       = {24},
  publisher    = {American Physical Society},
  series       = {Physical Review B (Condensed Matter and Materials Physics)},
  title        = {Photon echo spectroscopy reveals structure-dynamics relationships in carotenoids},
  url          = {http://dx.doi.org/10.1103/PhysRevB.79.245118},
  volume       = {79},
  year         = {2009},
}