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

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DOIResolve DOI: http://doi.org/10.1038/ncomms6952
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TypeArticle
Journal titleNature Communications
ISSN2041-1723
Volume6
Article number5952
Subjectionization; polarization; ultraviolet spectroscopy; vibration
AbstractHigh-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.
Publication date
PublisherNature Publishing Group
LanguageEnglish
AffiliationNational Research Council Canada; Security and Disruptive Technologies
Peer reviewedYes
NPARC number21277399
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Record identifier7495f42a-a41b-4620-b6a9-7ba93780f1e7
Record created2016-03-09
Record modified2016-05-09
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