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Portrait of Tönu Pullerits; Photo: Kennet Ruona

Tönu Pullerits

Professor

Portrait of Tönu Pullerits; Photo: Kennet Ruona

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

Author

  • Niklas Christensson
  • Franz Milota
  • Alexandra Nemeth
  • Igor Pugliesi
  • Eberhard Riedle
  • Jaroslaw Sperling
  • Tönu Pullerits
  • Harald F. Kauffmann
  • Juergen Hauer

Summary, in English

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.

Department/s

  • Chemical Physics

Publishing year

2010

Language

English

Pages

3366-3370

Publication/Series

The Journal of Physical Chemistry Letters

Volume

1

Issue

23

Document type

Journal article

Publisher

The American Chemical Society (ACS)

Topic

  • Atom and Molecular Physics and Optics

Status

Published

ISBN/ISSN/Other

  • ISSN: 1948-7185