skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Establishing nonlinearity thresholds with ultraintense X-ray pulses

Abstract

X-ray techniques have evolved over decades to become highly refined tools for a broad range of investigations. Importantly, these approaches rely on X-ray measurements that depend linearly on the number of incident X-ray photons. The advent of X-ray free electron lasers (XFELs) is opening the ability to reach extremely high photon numbers within ultrashort X-ray pulse durations and is leading to a paradigm shift in our ability to explore nonlinear X-ray signals. However, the enormous increase in X-ray peak power is a double-edged sword with new and exciting methods being developed but at the same time well-established techniques proving unreliable. Consequently, accurate knowledge about the threshold for nonlinear X-ray signals is essential. Here in this paper we report an X-ray spectroscopic study that reveals important details on the thresholds for nonlinear X-ray interactions. By varying both the incident X-ray intensity and photon energy, we establish the regimes at which the simplest nonlinear process, two-photon X-ray absorption (TPA), can be observed. From these measurements we can extract the probability of this process as a function of photon energy and confirm both the nature and sub-femtosecond lifetime of the virtual intermediate electronic state.

Authors:
 [1];  [2];  [2];  [3];  [2];  [3];  [4];  [5];  [6];  [7];  [3];  [3];  [8];  [3];  [3];  [3];  [9];  [3];  [3]
  1. Paul Scherrer Inst. (PSI), Villigen (Switzerland); Jan Kochanowski Univ., Kielce (Poland). Inst. of Physics
  2. Univ. of Fribourg, Fribourg (Switzerland)
  3. Paul Scherrer Inst. (PSI), Villigen (Switzerland)
  4. Uppsala Univ. (Sweden). Dept. of Chemistry; Polish Academy of Sciences (PAS), Warsaw (Poland). Inst. of Physical Chemistry
  5. SLAC National Accelerator Lab., Menlo Park, CA (United States). Linac Coherent Light Source (LCLS); National Science Foundation BioXFEL Science and Technology Center (STC), Buffalo, NY (United States)
  6. SLAC National Accelerator Lab., Menlo Park, CA (United States). Linac Coherent Light Source (LCLS)
  7. SLAC National Accelerator Lab., Menlo Park, CA (United States). Linac Coherent Light Source (LCLS); Brookhaven National Lab. (BNL), Upton, NY (United States)
  8. Paul Scherrer Inst. (PSI), Villigen (Switzerland); Federal Inst. of Technology, Zurich (Switzerland). Inst. for Chemical and Bioengineering
  9. Jan Kochanowski Univ., Kielce (Poland). Inst. of Physics
Publication Date:
Research Org.:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); Swiss National Science Foundation (SNSF); National Science Centre, Poland
OSTI Identifier:
1340403
Report Number(s):
BNL-113187-2016-JA
Journal ID: ISSN 2045-2322
Grant/Contract Number:
SC00112704; AC02-76SF00515; 135040; 2015/19/B/ST2/00931
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Scientific Reports
Additional Journal Information:
Journal Volume: 6; Journal ID: ISSN 2045-2322
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND TECHNOLOGY

Citation Formats

Szlachetko, Jakub, Hoszowska, Joanna, Dousse, Jean-Claude, Nachtegaal, Maarten, Błachucki, Wojciech, Kayser, Yves, Sà, Jacinto, Messerschmidt, Marc, Boutet, Sebastien, Williams, Garth J., David, Christian, Smolentsev, Grigory, van Bokhoven, Jeroen A., Patterson, Bruce D., Penfold, Thomas J., Knopp, Gregor, Pajek, Marek, Abela, Rafael, and Milne, Christopher J. Establishing nonlinearity thresholds with ultraintense X-ray pulses. United States: N. p., 2016. Web. doi:10.1038/srep33292.
Szlachetko, Jakub, Hoszowska, Joanna, Dousse, Jean-Claude, Nachtegaal, Maarten, Błachucki, Wojciech, Kayser, Yves, Sà, Jacinto, Messerschmidt, Marc, Boutet, Sebastien, Williams, Garth J., David, Christian, Smolentsev, Grigory, van Bokhoven, Jeroen A., Patterson, Bruce D., Penfold, Thomas J., Knopp, Gregor, Pajek, Marek, Abela, Rafael, & Milne, Christopher J. Establishing nonlinearity thresholds with ultraintense X-ray pulses. United States. doi:10.1038/srep33292.
Szlachetko, Jakub, Hoszowska, Joanna, Dousse, Jean-Claude, Nachtegaal, Maarten, Błachucki, Wojciech, Kayser, Yves, Sà, Jacinto, Messerschmidt, Marc, Boutet, Sebastien, Williams, Garth J., David, Christian, Smolentsev, Grigory, van Bokhoven, Jeroen A., Patterson, Bruce D., Penfold, Thomas J., Knopp, Gregor, Pajek, Marek, Abela, Rafael, and Milne, Christopher J. Tue . "Establishing nonlinearity thresholds with ultraintense X-ray pulses". United States. doi:10.1038/srep33292. https://www.osti.gov/servlets/purl/1340403.
@article{osti_1340403,
title = {Establishing nonlinearity thresholds with ultraintense X-ray pulses},
author = {Szlachetko, Jakub and Hoszowska, Joanna and Dousse, Jean-Claude and Nachtegaal, Maarten and Błachucki, Wojciech and Kayser, Yves and Sà, Jacinto and Messerschmidt, Marc and Boutet, Sebastien and Williams, Garth J. and David, Christian and Smolentsev, Grigory and van Bokhoven, Jeroen A. and Patterson, Bruce D. and Penfold, Thomas J. and Knopp, Gregor and Pajek, Marek and Abela, Rafael and Milne, Christopher J.},
abstractNote = {X-ray techniques have evolved over decades to become highly refined tools for a broad range of investigations. Importantly, these approaches rely on X-ray measurements that depend linearly on the number of incident X-ray photons. The advent of X-ray free electron lasers (XFELs) is opening the ability to reach extremely high photon numbers within ultrashort X-ray pulse durations and is leading to a paradigm shift in our ability to explore nonlinear X-ray signals. However, the enormous increase in X-ray peak power is a double-edged sword with new and exciting methods being developed but at the same time well-established techniques proving unreliable. Consequently, accurate knowledge about the threshold for nonlinear X-ray signals is essential. Here in this paper we report an X-ray spectroscopic study that reveals important details on the thresholds for nonlinear X-ray interactions. By varying both the incident X-ray intensity and photon energy, we establish the regimes at which the simplest nonlinear process, two-photon X-ray absorption (TPA), can be observed. From these measurements we can extract the probability of this process as a function of photon energy and confirm both the nature and sub-femtosecond lifetime of the virtual intermediate electronic state.},
doi = {10.1038/srep33292},
journal = {Scientific Reports},
number = ,
volume = 6,
place = {United States},
year = {Tue Sep 13 00:00:00 EDT 2016},
month = {Tue Sep 13 00:00:00 EDT 2016}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Citation Metrics:
Cited by: 12works
Citation information provided by
Web of Science

Save / Share:
  • We describe the methodology of our recently developed Monte Carlo rate equation (MCRE) approach, which systematically incorporates bound-bound resonances to model multiphoton ionization dynamics induced by high-fluence, high-intensity x-ray free-electron laser (XFEL) pulses. These resonances are responsible for ionization far beyond that predicted by the sequential single photon absorption model and are central to a quantitative understanding of atomic ionization dynamics in XFEL pulses. We also present calculated multiphoton ionization dynamics for Kr and Xe atoms in XFEL pulses for a variety of conditions, to compare the effects of bandwidth, pulse duration, pulse fluence, and photon energy. This comprehensive computationalmore » investigation reveals areas in the photon energy–pulse fluence landscape where resonances are critically important. We also uncover a mechanism, preservation of inner-shell vacancies (PIVS), whereby radiation damage is enhanced at higher XFEL intensities and identify the sequence of core-outer–Rydberg, core-valence, and core-core resonances encountered during multiphoton x-ray ionization.« less
  • Simulations show that intense plasma-amplified pulses of 100 fs duration and below are feasible by seeding specifically tailored plasma with an ultrashort pulse of high harmonic radiation. Seeding overcomes gain narrowing by driving amplifying media into saturation earlier, and compensates for reduced gain resulting from boosting the lasing transition linewidth. We conclude that ultrahigh intensities (above 10{sup 16} W cm{sup -2}) could be reached.
  • Irradiation of porous (with porosity in excess of 70%) silicon target with femtosecond laser pulses of 10{sup 16} W cm{sup -2} intensity increased by a factor of 3.5 the efficiency of generation of hard x-ray radiation with photon energies E > 8 keV. The increase was 30-fold for E > 2.5 keV. The relationship between this effect and the parameters of the luminescence emitted by porous silicon was investigated. (letters to the editor)