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

A. Ferré 1 A. E. Boguslavskiy 2 M. Dagan 3 Valérie Blanchet 1 B. D. Bruner 3 F. Burgy 1 A. Camper 4 D. Descamps 1 B. Fabre 1 N. Fedorov 1 J. Gaudin 1 G. Geoffroy 1 J. Mikosch 2, 5 S. Patchkovskii 2, 5 S. Petit 1 T. Ruchon 4, 6 H. Soifer 3 David Staedter 7 I. Wilkinson 2 A. Stolow 2, 8 N. Dudovich 3 Y. Mairesse 1
1 CELIA - Centre d'Etudes Lasers Intenses et Applications
2 NRC - National Research Council of Canada
3 Department of Physics of Complex System
4 LIDyl - Laboratoire Interactions, Dynamiques et Lasers (ex SPAM)
5 MBI - Max-Born-Institut für Nichtlineare Optik und Kurzzeitspektroskopie
6 ATTO - Attophysique
IRAMIS - Institut Rayonnement Matière de Saclay, LIDyl - Laboratoire Interactions, Dynamiques et Lasers (ex SPAM)
7 Femto (LCAR)
LCAR - Laboratoire Collisions Agrégats Réactivité
8 Department of Chemistry, University of Ottawa, 10 Marie Curie, Ottawa, Ontario, Canada KIN 6N5
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.
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https://hal-cea.archives-ouvertes.fr/cea-01244391
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Last modification on : Tuesday, April 5, 2022 - 3:16:19 AM
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CEA | CEA-UPSAY | INSTITUT-SCIENCES-LUMIERE | GS-CHIMIE | GS-ENGINEERING | IRAMIS | DAM | UNIV-TLSE3 | UNIV-PARIS-SACLAY | IRAMIS-LIDYL | CNRS | LCAR_FEM | ANR | IRSAMC | LCAR

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A. Ferré, A. E. Boguslavskiy, M. Dagan, Valérie Blanchet, B. D. Bruner, et al.. Multi-channel electronic and vibrational dynamics in polyatomic resonant high-order harmonic generation. Nature Communications, Nature Publishing Group, 2015, 6, pp.5952. ⟨10.1038/ncomms6952⟩. ⟨cea-01244391⟩

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