Electronic Double-Quantum Coherences and Their Impact on Ultrafast Spectroscopy: The Example of beta-Carotene
(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)
Please use this url to cite or link to this publication:
https://lup.lub.lu.se/record/1751677
- author
- Christensson, Niklas ; Milota, Franz ; Nemeth, Alexandra ; Pugliesi, Igor ; Riedle, Eberhard ; Sperling, Jaroslaw ; Pullerits, Tönu LU ; Kauffmann, Harald F. and Hauer, Juergen
- organization
- publishing date
- 2010
- 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 (ACS)
- external identifiers
-
- wos:000284991000011
- scopus:78649932563
- pmid:23828724
- ISSN
- 1948-7185
- DOI
- 10.1021/jz101409r
- 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
- e5dd9914-bec2-4cb5-8a67-e64515498273 (old id 1751677)
- date added to LUP
- 2016-04-01 14:52:42
- date last changed
- 2022-02-19 21:20:06
@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 (ACS)}},
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}},
doi = {{10.1021/jz101409r}},
volume = {{1}},
year = {{2010}},
}