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Multi-channel electronic and vibrational dynamics in polyatomic resonant high-order harmonic generation

Author

Listed:
  • A. Ferré

    (Université de Bordeaux—CNRS—CEA, CELIA, UMR5107)

  • A. E. Boguslavskiy

    (National Research Council Canada
    University of Ottawa)

  • M. Dagan

    (Weizmann Institute of Science)

  • V. Blanchet

    (Université de Bordeaux—CNRS—CEA, CELIA, UMR5107)

  • B. D. Bruner

    (Weizmann Institute of Science)

  • F. Burgy

    (Université de Bordeaux—CNRS—CEA, CELIA, UMR5107)

  • A. Camper

    (CEA, IRAMIS, Lasers, Interactions and Dynamics Laboratory—LIDyL, CEA-SACLAY)

  • D. Descamps

    (Université de Bordeaux—CNRS—CEA, CELIA, UMR5107)

  • B. Fabre

    (Université de Bordeaux—CNRS—CEA, CELIA, UMR5107)

  • N. Fedorov

    (Université de Bordeaux—CNRS—CEA, CELIA, UMR5107)

  • J. Gaudin

    (Université de Bordeaux—CNRS—CEA, CELIA, UMR5107)

  • G. Geoffroy

    (Université de Bordeaux—CNRS—CEA, CELIA, UMR5107)

  • J. Mikosch

    (National Research Council Canada
    Max-Born-Institute, Max-Born-Strasse 2A)

  • S. Patchkovskii

    (National Research Council Canada
    Max-Born-Institute, Max-Born-Strasse 2A)

  • S. Petit

    (Université de Bordeaux—CNRS—CEA, CELIA, UMR5107)

  • T. Ruchon

    (CEA, IRAMIS, Lasers, Interactions and Dynamics Laboratory—LIDyL, CEA-SACLAY)

  • H. Soifer

    (Weizmann Institute of Science)

  • D. Staedter

    (Université de Toulouse—CNRS, LCAR-IRSAMC)

  • I. Wilkinson

    (National Research Council Canada)

  • A. Stolow

    (National Research Council Canada
    University of Ottawa
    University of Ottawa, 10 Marie Curie)

  • N. Dudovich

    (Weizmann Institute of Science)

  • Y. Mairesse

    (Université de Bordeaux—CNRS—CEA, CELIA, UMR5107)

Abstract

High-order harmonic generation in polyatomic molecules generally involves multiple channels of ionization. Their relative contribution can be strongly influenced by the presence of resonances, whose assignment remains a major challenge for high-harmonic spectroscopy. Here we present a multi-modal approach for the investigation of unaligned polyatomic molecules, using SF6 as an example. We combine methods from extreme-ultraviolet spectroscopy, above-threshold ionization and attosecond metrology. Fragment-resolved above-threshold ionization measurements reveal that strong-field ionization opens at least three channels. A shape resonance in one of them is found to dominate the signal in the 20–26 eV range. This resonance induces a phase jump in the harmonic emission, a switch in the polarization state and different dynamical responses to molecular vibrations. This study demonstrates a method for extending high-harmonic spectroscopy to polyatomic molecules, where complex attosecond dynamics are expected.

Suggested Citation

  • A. Ferré & A. E. Boguslavskiy & M. Dagan & V. Blanchet & B. D. Bruner & F. Burgy & A. Camper & D. Descamps & B. Fabre & N. Fedorov & J. Gaudin & G. Geoffroy & J. Mikosch & S. Patchkovskii & S. Petit &, 2015. "Multi-channel electronic and vibrational dynamics in polyatomic resonant high-order harmonic generation," Nature Communications, Nature, vol. 6(1), pages 1-10, May.
    • Handle: RePEc:nat:natcom:v:6:y:2015:i:1:d:10.1038_ncomms6952
    DOI: 10.1038/ncomms6952
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