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Tönu Pullerits. Portrait.

Tönu Pullerits

Professor

Tönu Pullerits. Portrait.

Two-dimensional electronic spectroscopy of beta-carotene.

Author

  • Niklas Christensson
  • Franz Milota
  • Alexandra Nemeth
  • Jaroslaw Sperling
  • Harald F Kauffmann
  • Tönu Pullerits
  • Jürgen Hauer

Summary, in English

Two-dimensional electronic spectroscopy (2D) has been applied to beta-carotene in solution to shine new light on the ultrafast energy dissipation network in carotenoids. The ability of 2D to relieve spectral congestion provides new experimental grounds for resolving the rise of the excited state absorption signal between 18,000 and 19,000 cm(-1). In this spectral region, the pump-probe signals from ground state bleach and stimulated emission overlap strongly. Combined modeling of the time-evolution of 2D spectra as well as comparison to published pump-probe data allow us to draw conclusions on both the electronic structure of beta-carotene as well as the spectral densities giving rise to the observed optical lineshapes. To account for the experimental observations on all time scales, we need to include a transition in the visible spectral range from the first optically allowed excited state (S(2)-->S(n2)). We present data from frequency resolved transient grating and pump-probe experiments confirming the importance of this transition. Furthermore, we investigate the role and nature of the S* state, controversially debated in numerous previous studies. On the basis of the analysis of Feynman diagrams, we show that the properties of S*-related signals in chi(3) techniques like pump-probe and 2D can only be accounted for if S* is an excited electronic state. Against this background, we discuss a new interpretation of pump-deplete-probe and intensity-dependent pump-probe experiments.

Department/s

  • Chemical Physics

Publishing year

2009

Language

English

Pages

16409-16419

Publication/Series

The Journal of Physical Chemistry Part B

Volume

113

Issue

51

Document type

Journal article

Publisher

The American Chemical Society (ACS)

Topic

  • Atom and Molecular Physics and Optics

Status

Published

ISBN/ISSN/Other

  • ISSN: 1520-5207