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Title: State-resolved attosecond reversible and irreversible dynamics in strong optical fields

Journal Article · · Nature Physics
DOI: https://doi.org/10.1038/nphys4027 · OSTI ID:1574318
 [1];  [1];  [2];  [3];  [4];  [5]; ORCiD logo [6];  [2];  [7]
  1. Univ. of California, Berkeley, CA (United States)
  2. Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany). Center for Free-Electron Laser Science; Univ. of Hamburg (Germany)
  3. Eastman Chemical Company, Kingsport, TN (United States)
  4. Nanyang Technological Univ., Singapore (Singapore). Centre for Optical Fibre Technology, The Photonics Inst.
  5. Arizona State Univ., Tempe, AZ (United States). Biodesign Center for Applied Structural Discovery
  6. Harvard-Smithsonian Center for Astrophysics, Cambridge, MA (United States); Harvard Univ., Cambridge, MA (United States)
  7. Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
+ Show Author Affiliations

Strong-field ionization (SFI) is a key process for accessing real-time quantum dynamics of electrons on the attosecond timescale. The theoretical foundation of SFI was pioneered in the 1960s, and later refined by various analytical models. While asymptotic ionization rates predicted by these models have been tested to be in reasonable agreement for a wide range of laser parameters, predictions for SFI on the sub-laser-cycle timescale are either beyond the scope of the models or show strong qualitative deviations from full quantum-mechanical simulations. Here in this paper, using the unprecedented state specificity of attosecond transient absorption spectroscopy, we follow the real-time SFI process of the two valence spin–orbit states of xenon. The results reveal that the irreversible tunnelling contribution is accompanied by a reversible electronic population that exhibits an observable spin–orbit-dependent phase delay. A detailed theoretical analysis attributes this observation to transient ground-state polarization, an unexpected facet of SFI that cannot be captured by existing analytical models that focus exclusively on the production of asymptotic electron/ion yields.

Research Organization:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Organization:
Alexander von Humboldt Foundation; National Science Foundation (NSF); U.S. Army Research Office (ARO); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Grant/Contract Number:
AC02-05CH11231
OSTI ID:
1574318
Journal Information:
Nature Physics, Journal Name: Nature Physics Journal Issue: 5 Vol. 13; ISSN 1745-2473
Publisher:
Nature Publishing Group (NPG)Copyright Statement
Country of Publication:
United States
Language:
English

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Cited By (21)

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Hole dynamics in a photovoltaic donor-acceptor couple revealed by simulated time-resolved X-ray absorption spectroscopy journal July 2019
Resolution-of-the-identity approximation for complex-scaled basis functions journal September 2019
The role of transition dipole phase in atomic attosecond transient absorption from the multi-level model journal September 2019
Roadmap of ultrafast x-ray atomic and molecular physics journal January 2018
Attosecond transient-absorption spectroscopy in one-dimensional periodic crystals journal October 2019
Attosecond transient-absorption dynamics of xenon core-excited states in a strong driving field journal March 2017
Attosecond transient-absorption spectroscopy of polar molecules journal November 2018
Signatures of self-modulation effects during pulse propagation in single-pulse absorption spectra journal May 2019
Selectivity of Electronic Coherence and Attosecond Ionization Delays in Strong-Field Double Ionization journal June 2018
Deformation of Atomic p ± Orbitals in Strong Elliptically Polarized Laser Fields: Ionization Time Drifts and Spatial Photoelectron Separation journal November 2018
Attosecond precision in delay measurements using transient absorption spectroscopy journal January 2019
Real-time observation of electronic, vibrational, and rotational dynamics in nitric oxide with attosecond soft x-ray pulses at 400  eV journal January 2019
Roadmap of ultrafast x-ray atomic and molecular physics text January 2019
Roadmap of ultrafast x-ray atomic and molecular physics text January 2018
Hole dynamics in a photovoltaic donor-acceptor couple revealed by simulated time-resolved X-ray absorption spectroscopy text January 2019
Spatiotemporal imaging of valence electron motion text January 2019

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