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Electronic Double-Quantum Coherences and Their Impact on Ultrafast Spectroscopy: The Example of beta-Carotene

Christensson, Niklas; Milota, Franz; Nemeth, Alexandra; Pugliesi, Igor; Riedle, Eberhard; Sperling, Jaroslaw; Pullerits, Tönu LU ; Kauffmann, Harald F. and Hauer, Juergen (2010) In The Journal of Physical Chemistry Letters 1(23). p.3366-3370
Abstract
The energy level structure and dynamics of biomolecules are important for understanding their photoinduced function. In particular, the role of carotenoids in light-harvesting is heavily studied, yet not fully understood. The conventional approach to investigate these processes involves analysis of the third-order optical polarization in one spectral dimension. Here, we record two-dimensional correlation spectra for different time-orderings to characterize all components of the transient molecular polarization and the optical signal. Single- and double-quantum two-dimensional experiments provide insight into the energy level structure as well as the ultrafast dynamics of solvated beta-carotene. By analysis of the lineshapes, we obtain the... (More)
The energy level structure and dynamics of biomolecules are important for understanding their photoinduced function. In particular, the role of carotenoids in light-harvesting is heavily studied, yet not fully understood. The conventional approach to investigate these processes involves analysis of the third-order optical polarization in one spectral dimension. Here, we record two-dimensional correlation spectra for different time-orderings to characterize all components of the transient molecular polarization and the optical signal. Single- and double-quantum two-dimensional experiments provide insight into the energy level structure as well as the ultrafast dynamics of solvated beta-carotene. By analysis of the lineshapes, we obtain the transition energy and characterize the potential energy, surfaces of the involved states. We obtain direct experimental proof for an excited state absorption transition in the visible (S-2 -> S-n2). The signatures of this transition in pump-probe transients are shown to lead to strongly damped oscillations with characteristic pump and probe frequency dependence. (Less)
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author
organization
publishing date
type
Contribution to journal
publication status
published
subject
in
The Journal of Physical Chemistry Letters
volume
1
issue
23
pages
3366 - 3370
publisher
The American Chemical Society
external identifiers
  • wos:000284991000011
  • scopus:78649932563
ISSN
1948-7185
DOI
10.1021/jz101409r
language
English
LU publication?
yes
id
e5dd9914-bec2-4cb5-8a67-e64515498273 (old id 1751677)
date added to LUP
2010-12-29 13:59:36
date last changed
2018-05-29 11:56:29
@article{e5dd9914-bec2-4cb5-8a67-e64515498273,
  abstract     = {The energy level structure and dynamics of biomolecules are important for understanding their photoinduced function. In particular, the role of carotenoids in light-harvesting is heavily studied, yet not fully understood. The conventional approach to investigate these processes involves analysis of the third-order optical polarization in one spectral dimension. Here, we record two-dimensional correlation spectra for different time-orderings to characterize all components of the transient molecular polarization and the optical signal. Single- and double-quantum two-dimensional experiments provide insight into the energy level structure as well as the ultrafast dynamics of solvated beta-carotene. By analysis of the lineshapes, we obtain the transition energy and characterize the potential energy, surfaces of the involved states. We obtain direct experimental proof for an excited state absorption transition in the visible (S-2 -> S-n2). The signatures of this transition in pump-probe transients are shown to lead to strongly damped oscillations with characteristic pump and probe frequency dependence.},
  author       = {Christensson, Niklas and Milota, Franz and Nemeth, Alexandra and Pugliesi, Igor and Riedle, Eberhard and Sperling, Jaroslaw and Pullerits, Tönu and Kauffmann, Harald F. and Hauer, Juergen},
  issn         = {1948-7185},
  language     = {eng},
  number       = {23},
  pages        = {3366--3370},
  publisher    = {The American Chemical Society},
  series       = {The Journal of Physical Chemistry Letters},
  title        = {Electronic Double-Quantum Coherences and Their Impact on Ultrafast Spectroscopy: The Example of beta-Carotene},
  url          = {http://dx.doi.org/10.1021/jz101409r},
  volume       = {1},
  year         = {2010},
}