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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.
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Submitted on : Tuesday, September 7, 2021 - 3:48:18 PM
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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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