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Portrait of Tönu Pullerits; Photo: Kennet Ruona

Tönu Pullerits

Professor

Portrait of Tönu Pullerits; Photo: Kennet Ruona

Photon echo spectroscopy reveals structure-dynamics relationships in carotenoids

Author

  • Niklas Christensson
  • Tomas Polivka
  • Arkady Yartsev
  • Tönu Pullerits

Summary, in English

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.

Department/s

  • Chemical Physics

Publishing year

2009

Language

English

Publication/Series

Physical Review B (Condensed Matter and Materials Physics)

Volume

79

Issue

24

Document type

Journal article

Publisher

American Physical Society

Topic

  • Atom and Molecular Physics and Optics

Keywords

  • organic compounds
  • excited states
  • electron correlations
  • energy gap
  • photon echo
  • time resolved spectra

Status

Published

ISBN/ISSN/Other

  • ISSN: 1098-0121