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Title: Roadmap of ultrafast x-ray atomic and molecular physics

Journal Article · · Journal of Physics. B, Atomic, Molecular and Optical Physics
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  1. Argonne National Lab. (ANL), Argonne, IL (United States); Univ. of Chicago, IL (United States). James Franck Inst., Dept. of Physics
  2. Tohoku Univ., Sendai (Japan). Inst. of Multidisciplinary Research for Advanced Materials
  3. Potsdam Univ., Potsdam-Golm (Germany). Inst. for Physics and Astronomy; SLAC National Accelerator Lab., Menlo Park, CA (United States). Photon Ultrafast Laser Science and Engineering Inst. (PULSE)
  4. SLAC National Accelerator Lab., Menlo Park, CA (United States). Photon Ultrafast Laser Science and Engineering Inst. (PULSE); Stanford Univ., CA (United States). Dept. of Physics
  5. Sorbonne Univ., Paris (France). Laboratoire de Chimie Physique- Matiere et Rayonnement
  6. Univ. of California, Irvine, CA (United States). Dept. of Chemistry
  7. Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany). Center for Free-Electron Laser Science; Univ. of Hamburg (Germany). Dept. of Physics
  8. Elettra Sincrotrone Trieste, Trieste (Italy)
  9. European X-ray Free-Electron Laser (XFEL), Hamburg (Germany)
  10. Kansas State Univ., Manhattan, KS (United States). J.R. Macdonald Lab., Dept. of Physics
  11. Argonne National Lab. (ANL), Argonne, IL (United States)
  12. SLAC National Accelerator Lab., Menlo Park, CA (United States). Photon Ultrafast Laser Science and Engineering Inst. (PULSE); Univ. of Nebraska, Lincoln, NE (United States). Dept. of Physics and Astronomy
  13. SLAC National Accelerator Lab., Menlo Park, CA (United States). Photon Ultrafast Laser Science and Engineering Inst. (PULSE)
  14. Joint Inst. for Lab. Astrophysics (JILA), Boulder, CO (United States). Center for Atomic, Molecular & Optical Physics; Univ. of Colorado, Boulder, CO (United States). Dept. of Physics and Electrical and Computer Engineering
  15. Inst. National de la Recherche Scientifique, Centre Energie, Materiaux, et Telecommunications, Varennes, QC (Canada)
  16. Max Born Inst., Berlin (Germany)
  17. Lund Univ. (Sweden). Dept. of Physics, Atomic Physics
  18. Federal Inst. of Technology, Zurich (Switzerland). Laboratorium fur Physikalische Chemie
  19. Univ. of California, Berkeley, CA (United States). Dept. of Chemistry

X-ray free-electron lasers (XFELs) and table-top sources of x-rays based upon high harmonic generation (HHG) have revolutionized the field of ultrafast x-ray atomic and molecular physics, largely due to an explosive growth in capabilities in the past decade. XFELs now provide unprecedented intensity (10^20Wcm^-2) of x-rays at wavelengths down to ~1 Ångstrom, and HHG provides unprecedented time resolution (~50 attoseconds) and a correspondingly large coherent bandwidth at longer wavelengths. For context, timescales can be referenced to the Bohr orbital period in hydrogen atom of 150 attoseconds and the hydrogen-molecule vibrational period of 8 femtoseconds; wavelength scales can be referenced to the chemically significant carbon K-edge at a photon energy of ~280 eV (44 Ångstroms) and the bond length in methane of ~1 Ångstrom. With these modern x-ray sources one now has the ability to focus on individual atoms, even when embedded in a complex molecule, and view electronic and nuclear motion on their intrinsic scales (attoseconds and Ångstroms). These sources have enabled coherent diffractive imaging, where one can image non-crystalline objects in three dimensions on ultrafast timescales, potentially with atomic resolution. The unprecedented intensity available with XFELs has opened new fields of multiphoton and nonlinear x-ray physics where behavior of matter under extreme conditions can be explored. The unprecedented time resolution and pulse synchronization provided by HHG sources has kindled fundamental investigations of time delays in photoionization, charge migration in molecules, and dynamics near conical intersections that are foundational to AMO physics and chemistry. This roadmap coincides with the year when three new XFEL facilities, operating at Ångstrom wavelengths, opened for users (European XFEL, Swiss-FEL and PAL-FEL in Korea) almost doubling the present worldwide number of XFELs, and documents the remarkable progress in HHG capabilities since its discovery roughly 30 years ago, showcasing experiments in AMO physics and other applications. Here we capture the perspectives of 17 leading groups and organize the contributions into four categories: ultrafast molecular dynamics, multidimensional x-ray spectroscopies; high-intensity x-ray phenomena; attosecond x-ray science.

Research Organization:
SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States); Argonne National Laboratory (ANL), Argonne, IL (United States); Univ. of Colorado, Boulder, CO (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division
Grant/Contract Number:
AC02-76SF00515; SC0016494; AC02-06CH11357; FG02-99ER14982
OSTI ID:
1419966
Alternate ID(s):
OSTI ID: 1477978; OSTI ID: 1677516
Journal Information:
Journal of Physics. B, Atomic, Molecular and Optical Physics, Vol. 51, Issue 3; ISSN 0953-4075
Publisher:
IOP PublishingCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 189 works
Citation information provided by
Web of Science

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A comprehensive simulation framework for imaging single particles and biomolecules at the European X-ray Free-Electron Laser text January 2016
Separation of Photoabsorption and Compton Scattering Contributions to He Single and Double Ionization text January 1995
Compression of amplified chirped optical pulses journal October 1985
Transient lattice contraction in the solid-to-plasma transition text January 2016
Stimulated x-ray Raman Scattering – a critical assessment of the building block of nonlinear x-ray spectroscopy text January 2016
Spectral phase measurement of a Fano resonance using tunable attosecond pulses text January 2016
The 3D-architecture of individual free silver nanoparticles captured by X-ray scattering text January 2015
Attosecond delays in molecular photoionization conference June 2017
Auger Electron Angular Distribution of Double Core-Hole States in the Molecular Reference Frame text January 2010
Ultrafast Extreme Ultraviolet Induced Isomerization of Acetylene Cations text January 2010
Coherent diffractive imaging of single helium nanodroplets with a high harmonic generation source text January 2017
Attosecond physics
  • Kienberger, Reinhard; Krausz, Ferenc
  • ICALEO® 2007: 26th International Congress on Laser Materials Processing, Laser Microprocessing and Nanomanufacturing, International Congress on Applications of Lasers & Electro-Optics https://doi.org/10.2351/1.5061046
conference January 2007
Multiwavelength Anomalous Diffraction at High X-Ray Intensity text January 2011
Time-resolved high-harmonic spectroscopy of the photodissociation of CH3I and CF3I text January 2013
Time-resolved X-ray absorption spectroscopy with a water-window high-harmonic source conference June 2017
Generation of Bright Isolated Attosecond Soft X-Ray Pulses Driven by Multi-Cycle Mid-Infrared Lasers conference January 2014
Hetero-site-specific X-ray pump-probe spectroscopy for femtosecond intramolecular dynamics text January 2016
Circular Dichroism in Multiphoton Ionization of Resonantly Excited $He^{+}$ Ions text January 2017
Photoelectron spectrometer for attosecond spectroscopy of liquids and gases text January 2015
Highly stable, 54mJ Yb-InnoSlab laser platform at 0.5kW average power text January 2017
X-ray two-photon photoelectron sectroscopy: a theoretical study of inner-shell spectra of the organic para-aminophenol molecule text January 2009
Nanoplasma Dynamics of Single Large Xenon Clusters Irradiated with Superintense X-Ray Pulses from the Linac Coherent Light Source Free-Electron Laser text January 2012
Single shot phase contrast imaging using laser-produced Betatron x-ray beams text January 2011
Lorentz meets Fano spectral line shapes: A universal phase and its laser control text January 2013
High photon flux table-top coherent extreme ultraviolet source text January 2014
Experimental x-ray ghost imaging text January 2016
Attosecond delays in molecular photoionization text January 2016
Photoinduced molecular chirality probed by ultrafast resonant X-ray spectroscopy text January 2016
Coherent control with a short-wavelength Free Electron Laser text January 2017
Multiple Ionization of Heavy Atoms by Intense X-Ray Free-Electron Laser Pulses text January 2012
Attosecond dynamics through a Fano resonance: Monitoring the birth of a photoelectron text January 2019

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Real-time observation of disintegration processes within argon clusters ionized by a hard-x-ray pulse of moderate fluence journal February 2020
Mapping ultrafast ionization of atoms and clusters with terahertz-streaking delay text January 2019
Tracking attosecond electronic coherences using phase-manipulated extreme ultraviolet pulses text January 2020
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Nonlinear Coherence Effects in Transient-Absorption Ion Spectroscopy with Stochastic Extreme-Ultraviolet Free-Electron Laser Pulses text January 2019
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Effects of core space and excitation levels on ground-state correlation and photoionization dynamics of Be and Ne text January 2018
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Control of resonant ionization as a function of time delay between two XUV few-femtosecond pulses. Quantitative application to helium preprint January 2019
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Figures / Tables (27)