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Portrait of Tönu Pullerits; Photo: Kennet Ruona

Tönu Pullerits

Professor

Portrait of Tönu Pullerits; Photo: Kennet Ruona

Weakly chirped pulses in frequency resolved coherent spectroscopy.

Author

  • Niklas Christensson
  • Yuri Avlasevich
  • Arkady Yartsev
  • Klaus Müllen
  • Torbjörn Pascher
  • Tönu Pullerits

Summary, in English

The role of weakly chirped pulses (time bandwidth product, DeltanuDeltatau<0.61) on three-pulse photon echo signals has been systematically studied. Pulses with varying chirp were characterized with frequency resolved optical gating (FROG) and used to measure spectrally resolved three-pulse photon echoes of a dye in solution. The weakly chirped pulses give rise to markedly different echo signals for population times below approximately 100 fs. The chirped pulses can decrease or enhance spectral signatures of an excited state absorption transition in the echo signal. Furthermore, the observed dephasing dynamics depend on the phase of the electric fields. Simulations based on a three-level model and the electric fields retrieved from the FROG traces give a good agreement for photon echo experiments with both transform limited and chirped pulses. The simulations also allow for a numerical investigation of effects of chirp in two-dimensional spectroscopy. For a two-level system, the chirped pulses result in nonelliptical two-dimensional spectra that can erroneously be interpreted as spectral heterogeneity with frequency dependent dephasing dynamics. Furthermore, chirped pulses can give rise to "false" cross peaks when strong vibrational modes are involved in the system-bath interaction.

Department/s

  • Chemical Physics
  • NanoLund: Center for Nanoscience

Publishing year

2010

Language

English

Pages

1-174508

Publication/Series

Journal of Chemical Physics

Volume

132

Issue

17

Document type

Journal article

Publisher

American Institute of Physics (AIP)

Topic

  • Atom and Molecular Physics and Optics

Status

Published

ISBN/ISSN/Other

  • ISSN: 0021-9606