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)
Please use this url to cite or link to this publication:
https://lup.lub.lu.se/record/1462360
- author
- Christensson, Niklas
LU
; Polivka, Tomas
LU
; Yartsev, Arkady
LU
and Pullerits, Tönu
LU
- organization
- publishing date
- 2009
- 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
- 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
- fe262b30-c012-4b90-ad82-fec418ede5f6 (old id 1462360)
- date added to LUP
- 2016-04-01 14:16:17
- date last changed
- 2022-04-22 02:18:12
@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}},
keywords = {{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}},
doi = {{10.1103/PhysRevB.79.245118}},
volume = {{79}},
year = {{2009}},
}