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Generation and Coherent Control of Pulsed Quantum Frequency Combs
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Multi-channel electronic and vibrational dynamics in polyatomic resonant high-order harmonic generation.

A Ferré1, A E Boguslavskiy2, M Dagan3

  • 1Université de Bordeaux-CNRS-CEA, CELIA, UMR5107, F33405 Talence, France.

Nature Communications
|January 23, 2015
PubMed
Summary

Investigating polyatomic molecules with high-harmonic spectroscopy reveals a dominant shape resonance. This resonance impacts ionization channels, harmonic emission phase, and polarization, advancing attosecond dynamics studies.

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Area of Science:

  • Atomic, Molecular, and Optical Physics
  • Quantum Chemistry
  • Spectroscopy

Background:

  • High-order harmonic generation (HHG) in polyatomic molecules is complex due to multiple ionization channels.
  • Assigning resonances is crucial but challenging for high-harmonic spectroscopy.
  • Understanding these resonances is key to interpreting HHG spectra.

Purpose of the Study:

  • To develop and demonstrate a multi-modal approach for investigating unaligned polyatomic molecules using HHG.
  • To identify and characterize resonances influencing HHG in SF6.
  • To extend high-harmonic spectroscopy to complex molecular systems.

Main Methods:

  • Combined extreme-ultraviolet spectroscopy, above-threshold ionization (ATI), and attosecond metrology.
  • Performed fragment-resolved ATI measurements on SF6.
  • Utilized a multi-modal approach to probe molecular dynamics.

Main Results:

  • Identified at least three ionization channels in strong-field ionization of SF6.
  • Discovered a dominant shape resonance in the 20-26 eV range.
  • Observed resonance-induced phase jumps, polarization switching, and altered vibrational responses.

Conclusions:

  • The developed multi-modal approach enables the study of complex attosecond dynamics in polyatomic molecules.
  • Shape resonances significantly influence HHG spectra and molecular dynamics.
  • This work provides a pathway for extending high-harmonic spectroscopy to a broader range of molecular systems.