Quantum-Path-Resolved Attosecond High-Harmonic Spectroscopy

Camper, Antoine; Ferré, Amélie; Blanchet, Valérie; Descamps, Dominique; Lin, Nan; Petit, Stéphane; Lucchese, Robert; Salières, Pascal; Ruchon, Thierry; Mairesse, Yann

doi:10.1103/physrevlett.130.083201

Title: Quantum-Path-Resolved Attosecond High-Harmonic Spectroscopy

Journal Article · Tue Feb 21 00:00:00 EST 2023 · Physical Review Letters

DOI:https://doi.org/10.1103/physrevlett.130.083201· OSTI ID:1974769

^[1]; Ferré, Amélie ^[2];

^[3];

^[3]; Lin, Nan ^[4]; Petit, Stéphane ^[3];

^[5];

^[6];

^[3]

University Paris-Saclay, Gif-sur-Yvette (France); University of Oslo (Norway)
Aix-Marseille University, Marseille (France)
University of Bordeaux, Talence (France)
University Paris-Saclay, Gif-sur-Yvette (France); Chinese Academy of Sciences (CAS), Sahnghai (China)
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
University Paris-Saclay, Gif-sur-Yvette (France)

Strong-field ionization of molecules releases electrons which can be accelerated and driven back to recombine with their parent ion, emitting high-order harmonics. This ionization also initiates attosecond electronic and vibrational dynamics in the ion, evolving during the electron travel in the continuum. Revealing this subcycle dynamics from the emitted radiation usually requires advanced theoretical modeling. Here we show that this can be avoided by resolving the emission from two families of electronic quantum paths in the generation process. The corresponding electrons have the same kinetic energy, and thus the same structural sensitivity, but differ by the travel time between ionization and recombination-the pump-probe delay in this attosecond self-probing scheme. We measure the harmonic amplitude and phase in aligned CO₂ and N₂ molecules and observe a strong influence of laser-induced dynamics on two characteristic spectroscopic features: a shape resonance and multichannel interference. This quantum-path-resolved spectroscopy thus opens wide prospects for the investigation of ultrafast ionic dynamics, such as charge migration.

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Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB); European Research Council (ERC); USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-05CH11231

OSTI ID:: 1974769

Alternate ID(s):: OSTI ID: 1958623

Journal Information:: Physical Review Letters, Vol. 130, Issue 8; ISSN 0031-9007

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

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