title: Multi-channel electronic and vibrational dynamics in polyatomic resonant high-order harmonic generation.
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.
authors.affiliation: Université de Bordeaux-CNRS-CEA, CELIA, UMR5107, F33405 Talence, France.
authors.forename: A
authors.initials: A
authors.lastname: Ferré
authors.affiliation: 1] National Research Council Canada, 100 Sussex Drive, Ottawa, K1A 0R6 Ontario, Canada [2] Department of Physics, University of Ottawa, 150 Louis Pasteur, Ottawa, K1N 6N5 Ontario, Canada.
authors.forename: A E
authors.initials: AE
authors.lastname: Boguslavskiy
authors.affiliation: Department of Physics of Complex Systems, Weizmann Institute of Science, Rehovot 76100, Israel.
authors.forename: M
authors.initials: M
authors.lastname: Dagan
authors.affiliation: Université de Bordeaux-CNRS-CEA, CELIA, UMR5107, F33405 Talence, France.
authors.forename: V
authors.initials: V
authors.lastname: Blanchet
authors.affiliation: Department of Physics of Complex Systems, Weizmann Institute of Science, Rehovot 76100, Israel.
authors.forename: B D
authors.initials: BD
authors.lastname: Bruner
authors.affiliation: Université de Bordeaux-CNRS-CEA, CELIA, UMR5107, F33405 Talence, France.
authors.forename: F
authors.initials: F
authors.lastname: Burgy
authors.affiliation: CEA, IRAMIS, Lasers, Interactions and Dynamics Laboratory-LIDyL, CEA-SACLAY, F-91191 Gif-sur-Yvette, France.
authors.forename: A
authors.initials: A
authors.lastname: Camper
authors.affiliation: Université de Bordeaux-CNRS-CEA, CELIA, UMR5107, F33405 Talence, France.
authors.forename: D
authors.initials: D
authors.lastname: Descamps
authors.affiliation: Université de Bordeaux-CNRS-CEA, CELIA, UMR5107, F33405 Talence, France.
authors.forename: B
authors.initials: B
authors.lastname: Fabre
authors.affiliation: Université de Bordeaux-CNRS-CEA, CELIA, UMR5107, F33405 Talence, France.
authors.forename: N
authors.initials: N
authors.lastname: Fedorov
authors.affiliation: Université de Bordeaux-CNRS-CEA, CELIA, UMR5107, F33405 Talence, France.
authors.forename: J
authors.initials: J
authors.lastname: Gaudin
authors.affiliation: Université de Bordeaux-CNRS-CEA, CELIA, UMR5107, F33405 Talence, France.
authors.forename: G
authors.initials: G
authors.lastname: Geoffroy
authors.affiliation: 1] National Research Council Canada, 100 Sussex Drive, Ottawa, K1A 0R6 Ontario, Canada [2] Max-Born-Institute, Max-Born-Strasse 2A, 12489 Berlin, Germany.
authors.forename: J
authors.initials: J
authors.lastname: Mikosch
authors.affiliation: 1] National Research Council Canada, 100 Sussex Drive, Ottawa, K1A 0R6 Ontario, Canada [2] Max-Born-Institute, Max-Born-Strasse 2A, 12489 Berlin, Germany.
authors.forename: S
authors.initials: S
authors.lastname: Patchkovskii
authors.affiliation: Université de Bordeaux-CNRS-CEA, CELIA, UMR5107, F33405 Talence, France.
authors.forename: S
authors.initials: S
authors.lastname: Petit
authors.affiliation: CEA, IRAMIS, Lasers, Interactions and Dynamics Laboratory-LIDyL, CEA-SACLAY, F-91191 Gif-sur-Yvette, France.
authors.forename: T
authors.initials: T
authors.lastname: Ruchon
authors.affiliation: Department of Physics of Complex Systems, Weizmann Institute of Science, Rehovot 76100, Israel.
authors.forename: H
authors.initials: H
authors.lastname: Soifer
authors.affiliation: Université de Toulouse-CNRS, LCAR-IRSAMC, 31062 Toulouse, France.
authors.forename: D
authors.initials: D
authors.lastname: Staedter
authors.affiliation: National Research Council Canada, 100 Sussex Drive, Ottawa, K1A 0R6 Ontario, Canada.
authors.forename: I
authors.initials: I
authors.lastname: Wilkinson
authors.affiliation: 1] National Research Council Canada, 100 Sussex Drive, Ottawa, K1A 0R6 Ontario, Canada [2] Department of Physics, University of Ottawa, 150 Louis Pasteur, Ottawa, K1N 6N5 Ontario, Canada [3] Department of Chemistry, University of Ottawa, 10 Marie Curie, Ottawa K1N 6N5 Ontario, Canada K1N 6N5.
authors.forename: A
authors.initials: A
authors.lastname: Stolow
authors.affiliation: Department of Physics of Complex Systems, Weizmann Institute of Science, Rehovot 76100, Israel.
authors.forename: N
authors.initials: N
authors.lastname: Dudovich
authors.affiliation: Université de Bordeaux-CNRS-CEA, CELIA, UMR5107, F33405 Talence, France.
authors.forename: Y
authors.initials: Y
authors.lastname: Mairesse