Role of Spin-Orbit Coupling in High-Order Harmonic Generation Revealed by Supercycle Rydberg Trajectories

N. Mayer, S. Beaulieu, Á. Jiménez-Galán, S. Patchkovskii, O. Kornilov, D. Descamps, S. Petit, O. Smirnova, Y. Mairesse, and M. Y. Ivanov
Phys. Rev. Lett. 129, 173202 – Published 18 October 2022
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Abstract

High-harmonic generation is typically thought of as a sub-laser-cycle process, with the electron’s excursion in the continuum lasting a fraction of the optical cycle. However, it was recently suggested that long-lived Rydberg states can play a particularly important role in high harmonic generation by atoms driven by the combination of the counterrotating circularly polarized fundamental light field and its second harmonic. Here we report direct experimental evidence of very long and stable Rydberg trajectories contributing to high-harmonic generation in such fields. We track their dynamics inside the laser pulse using the spin-orbit evolution in the ionic core, utilizing the spin-orbit Larmor clock. We confirm their effect on harmonic emission both via microscopic simulations and by showing how this radiation can lead to a well-collimated macroscopic far-field signal. Our observations contrast sharply with the general view that long-lived Rydberg orbits should generate negligible contribution to the macroscopic far-field high harmonic response of the medium.

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  • Received 7 December 2021
  • Revised 26 July 2022
  • Accepted 8 September 2022

DOI:https://doi.org/10.1103/PhysRevLett.129.173202

© 2022 American Physical Society

Physics Subject Headings (PhySH)

Atomic, Molecular & Optical

Authors & Affiliations

N. Mayer1, S. Beaulieu2, Á. Jiménez-Galán1,3, S. Patchkovskii1, O. Kornilov1, D. Descamps2, S. Petit2, O. Smirnova1, Y. Mairesse2, and M. Y. Ivanov1,4,5

  • 1Max-Born-Institute, Max-Born Straße 2A, 12489 Berlin, Germany
  • 2Université de Bordeaux—CNRS—CEA, Centre Lasers Intenses et Applications (CELIA), UMR5107, F33405 Talence, France
  • 3Joint Attosecond Science Laboratory, National Research Council of Canada and University of Ottawa, Ottawa, Canada
  • 4Department of Physics, Humboldt University, Newtonstraße 15, D-12489 Berlin, Germany
  • 5Blackett Laboratory, Imperial College London, SW7 2AZ London, United Kingdom

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Issue

Vol. 129, Iss. 17 — 21 October 2022

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