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

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, T. Ruchon, H. Soifer, D. Staedter, I. Wilkinson, A. StolowN. Dudovich, Y. Mairesse*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

74 Scopus citations

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.

Original languageEnglish
Article number5952
JournalNature Communications
Volume6
DOIs
StatePublished - 22 Jan 2015
Externally publishedYes

Funding

FundersFunder number
l’Ambassade de France au Canada
Israel Science Foundation
Israeli Centers of Research Excellence program
European Commission
Natural Sciences and Engineering Research Council of Canada
Minerva Foundation
European Research Council
NSERC (Canada)
Crown Photonics Center
Agence Nationale de la RechercheANR-14-CE32-0014
l’Agence Nationale pour la RechercheANR-14-CE32-0014 MISFITS
Seventh Framework Programme228334, 242334
Conseil Régional Aquitaine20091304003, 2.1.3-09010502

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