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

Abstract

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 20 W cm -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-raymore » 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 in this paper, 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.« less

Authors:
 [1];  [2];  [3];  [4];  [5];  [6];  [7]; ORCiD logo [8];  [8];  [9];  [10];  [10];  [11];  [12];  [13];  [7];  [14];  [14]; ORCiD logo [15];  [15] more »; ORCiD logo [16]; ORCiD logo [17];  [17];  [17];  [17]; ORCiD logo [18];  [19] « less
  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
Publication Date:
Research Org.:
SLAC National Accelerator Lab., Menlo Park, CA (United States); Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1419966
Alternate Identifier(s):
OSTI ID: 1477978
Grant/Contract Number:  
AC02-76SF00515; SC0016494; AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Physics. B, Atomic, Molecular and Optical Physics
Additional Journal Information:
Journal Volume: 51; Journal Issue: 3; Journal ID: ISSN 0953-4075
Publisher:
IOP Publishing
Country of Publication:
United States
Language:
English
Subject:
74 ATOMIC AND MOLECULAR PHYSICS; ultrafast molecular dynamics; x-ray spectroscopies and phenomena; table-top sources; x-ray free-electron lasers; attosecond phenomena

Citation Formats

Young, Linda, Ueda, Kiyoshi, Gühr, Markus, Bucksbaum, Philip H., Simon, Marc, Mukamel, Shaul, Rohringer, Nina, Prince, Kevin C., Masciovecchio, Claudio, Meyer, Michael, Rudenko, Artem, Rolles, Daniel, Bostedt, Christoph, Fuchs, Matthias, Reis, David A., Santra, Robin, Kapteyn, Henry, Murnane, Margaret, Ibrahim, Heide, Légaré, François, Vrakking, Marc, Isinger, Marcus, Kroon, David, Gisselbrecht, Mathieu, L’Huillier, Anne, Wörner, Hans Jakob, and Leone, Stephen R. Roadmap of ultrafast x-ray atomic and molecular physics. United States: N. p., 2018. Web. doi:10.1088/1361-6455/aa9735.
Young, Linda, Ueda, Kiyoshi, Gühr, Markus, Bucksbaum, Philip H., Simon, Marc, Mukamel, Shaul, Rohringer, Nina, Prince, Kevin C., Masciovecchio, Claudio, Meyer, Michael, Rudenko, Artem, Rolles, Daniel, Bostedt, Christoph, Fuchs, Matthias, Reis, David A., Santra, Robin, Kapteyn, Henry, Murnane, Margaret, Ibrahim, Heide, Légaré, François, Vrakking, Marc, Isinger, Marcus, Kroon, David, Gisselbrecht, Mathieu, L’Huillier, Anne, Wörner, Hans Jakob, & Leone, Stephen R. Roadmap of ultrafast x-ray atomic and molecular physics. United States. doi:10.1088/1361-6455/aa9735.
Young, Linda, Ueda, Kiyoshi, Gühr, Markus, Bucksbaum, Philip H., Simon, Marc, Mukamel, Shaul, Rohringer, Nina, Prince, Kevin C., Masciovecchio, Claudio, Meyer, Michael, Rudenko, Artem, Rolles, Daniel, Bostedt, Christoph, Fuchs, Matthias, Reis, David A., Santra, Robin, Kapteyn, Henry, Murnane, Margaret, Ibrahim, Heide, Légaré, François, Vrakking, Marc, Isinger, Marcus, Kroon, David, Gisselbrecht, Mathieu, L’Huillier, Anne, Wörner, Hans Jakob, and Leone, Stephen R. Tue . "Roadmap of ultrafast x-ray atomic and molecular physics". United States. doi:10.1088/1361-6455/aa9735. https://www.osti.gov/servlets/purl/1419966.
@article{osti_1419966,
title = {Roadmap of ultrafast x-ray atomic and molecular physics},
author = {Young, Linda and Ueda, Kiyoshi and Gühr, Markus and Bucksbaum, Philip H. and Simon, Marc and Mukamel, Shaul and Rohringer, Nina and Prince, Kevin C. and Masciovecchio, Claudio and Meyer, Michael and Rudenko, Artem and Rolles, Daniel and Bostedt, Christoph and Fuchs, Matthias and Reis, David A. and Santra, Robin and Kapteyn, Henry and Murnane, Margaret and Ibrahim, Heide and Légaré, François and Vrakking, Marc and Isinger, Marcus and Kroon, David and Gisselbrecht, Mathieu and L’Huillier, Anne and Wörner, Hans Jakob and Leone, Stephen R.},
abstractNote = {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 (1020 W cm-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 in this paper, 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.},
doi = {10.1088/1361-6455/aa9735},
journal = {Journal of Physics. B, Atomic, Molecular and Optical Physics},
number = 3,
volume = 51,
place = {United States},
year = {2018},
month = {1}
}

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Figures / Tables:

Figure 1 Figure 1: Phase space covered by the XFEL and HHG sources discussed in this roadmap. For XFELs, the pulse duration represents that of a single pulse, whereas for HHG, the range spans both single pulses and pulse trains spaced by the period of the driver laser. The numbers in eachmore » island indicate the number of photons/pulse/1% bandwidth. Research to extend the limits of all represented quantities, photon energy, time scale and photon number per pulse, is pursued for both XFEL and HHG sources. The emphasis for XFELs is to extend the time scale to the attosecond regime and photon energy above 20 keV; the emphasis for HHG is to extend the photon energy range to hard x-ray and photon number per pulse. For properties not represented by these basic quantities, XFELs seek enhanced temporal coherence and synchronization with external sources, and both sources seek increased average power and controlled polarization.« less

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