Multi-channel electronic and vibrational dynamics in polyatomic resonant high-order harmonic generation
Year: 2015
Type: article
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.
Source: Nature Communications
DOI: 10.1038/ncomms6952
Institutions: Centre National de la Recherche Scientifique, Université de Bordeaux, Commissariat à l'Énergie Atomique et aux Énergies Alternatives, Centre Lasers Intenses et Applications, University of Ottawa, National Research Council Canada, Weizmann Institute of Science, Institut Rayonnement-Matière de Saclay, CEA Paris-Saclay, Laboratoire Interactions, Dynamiques et Lasers, Institut de Recherche sur les Systèmes Atomiques et Moléculaires Complexes, Laboratoire Collisions Agrégats Réactivité, Université de Toulouse
Language: English
Subfield: Atomic and Molecular Physics, and Optics
Field: Physics and Astronomy
Domain: Physical Sciences
Open Access status: gold
Estimated APC paid: $6,990
OpenAlex ID: W2001479368