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Title: X-ray Emission Spectroscopy at X-ray Free Electron Lasers: Limits to Observation of the Classical Spectroscopic Response for Electronic Structure Analysis

Abstract

X-ray free electron lasers (XFELs) provide ultrashort intense X-ray pulses suitable to probe electron dynamics but can also induce a multitude of nonlinear excitation processes. These affect spectroscopic measurements and interpretation, particularly for upcoming brighter XFELs. Here we identify and discuss the limits to observing classical spectroscopy, where only one photon is absorbed per atom for a Mn2+ in a light element (O, C, H) environment. X-ray emission spectroscopy (XES) with different incident photon energies, pulse intensities, and pulse durations is presented. A rate equation model based on sequential ionization and relaxation events is used to calculate populations of multiply ionized states during a single pulse and to explain the observed X-ray induced spectral lines shifts. Furthermore this model provides easy estimation of spectral shifts, which is essential for experimental designs at XFELs and illustrates that shorter X-ray pulses will not overcome sequential ionization but can reduce electron cascade effects.

Authors:
ORCiD logo [1]; ORCiD logo [2];  [3];  [4];  [5];  [6];  [7];  [8]; ORCiD logo [5];  [9];  [10];  [11];  [11];  [12];  [5];  [13];  [11];  [6];  [14];  [15] more »;  [13];  [11];  [6];  [6];  [16];  [11];  [11];  [6];  [17];  [13];  [11];  [11];  [5];  [18];  [11];  [6];  [11];  [13];  [11];  [13]; ORCiD logo [19]; ORCiD logo [1];  [11] « less
+ Show Author Affiliations
  1. Purdue Univ., West Lafayette, IN (United States)
  2. Purdue Univ., West Lafayette, IN (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  3. Purdue Univ., West Lafayette, IN (United States); Battelle, Pittsburgh, PA (United States)
  4. Arizona State Univ., Tempe, AZ (United States); European XFEL GmbH, Hamburg (Germany)
  5. Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany); Univ. Hamburg, Hamburg (Germany)
  6. Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany)
  7. Paul Scherrer Inst. (PSI), Villigen (Switzerland)
  8. European XFEL GmbH, Hamburg (Germany)
  9. Arizona State Univ., Tempe, AZ (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)
  10. Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
  11. Arizona State Univ., Tempe, AZ (United States)
  12. SUNY Univ. at Buffalo, Buffalo, NY (United States); BioXFEL Science and Technology Center, Buffalo, NY (United States)
  13. SLAC National Accelerator Lab., Menlo Park, CA (United States)
  14. Univ. of Wisconsin—Milwaukee, Milwaukee, WI (United States)
  15. Beijing Computational Science Research Center, Beijing (China)
  16. BioXFEL Science and Technology Center, Buffalo, NY (United States)
  17. Univ. of California Davis, Davis (United States)
  18. Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany); SLAC National Accelerator Lab., Menlo Park, CA (United States); Max-Planck Institute for the Structure and Dynamics of Matter, Hamburg (Germany)
  19. Univ. of Washington, Seattle, WA (United States)
Publication Date:
Research Org.:
SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1503076
Grant/Contract Number:  
AC02-76SF00515; CHE-1350909; DBI-1231306; 1R01GM095583; 1R01GM117342-01
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry Letters
Additional Journal Information:
Journal Volume: 10; Journal Issue: 3; Journal ID: ISSN 1948-7185
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
47 OTHER INSTRUMENTATION

Citation Formats

Jensen, Scott C., Sullivan, Brendan, Hartzler, Daniel A., Aguilar, Jose Meza, Awel, Salah, Bajt, Saša, Basu, Shibom, Bean, Richard, Chapman, Henry N., Conrad, Chelsie, Frank, Matthias, Fromme, Raimund, Martin-Garcia, Jose M., Grant, Thomas D., Heymann, Michael, Hunter, Mark S., Kirian, Richard A., Knoska, Juraj, Kupitz, Christopher, Li, Xuanxuan, Liang, Mengning, Lisova, Stella, Mariani, Valerio, Mazalova, Victoria, Messerschmidt, Marc, Moran, Michael, Nelson, Garrett, Oberthür, Dominik, Schaffer, Alex, Sierra, Raymond G., Vaughn, Natalie, Weierstall, Uwe, Wiedorn, Max O., Xavier, P. Lourdu, Yang, Jay -How, Yefanov, Oleksandr, Zatsepin, Nadia A., Aquila, Andrew, Fromme, Petra, Boutet, Sébastien, Seidler, Gerald T., Pushkar, Yulia, and Ketawala, Gihan. X-ray Emission Spectroscopy at X-ray Free Electron Lasers: Limits to Observation of the Classical Spectroscopic Response for Electronic Structure Analysis. United States: N. p., 2018. Web. doi:10.1021/acs.jpclett.8b03595.
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Jensen, Scott C., Sullivan, Brendan, Hartzler, Daniel A., Aguilar, Jose Meza, Awel, Salah, Bajt, Saša, Basu, Shibom, Bean, Richard, Chapman, Henry N., Conrad, Chelsie, Frank, Matthias, Fromme, Raimund, Martin-Garcia, Jose M., Grant, Thomas D., Heymann, Michael, Hunter, Mark S., Kirian, Richard A., Knoska, Juraj, Kupitz, Christopher, Li, Xuanxuan, Liang, Mengning, Lisova, Stella, Mariani, Valerio, Mazalova, Victoria, Messerschmidt, Marc, Moran, Michael, Nelson, Garrett, Oberthür, Dominik, Schaffer, Alex, Sierra, Raymond G., Vaughn, Natalie, Weierstall, Uwe, Wiedorn, Max O., Xavier, P. Lourdu, Yang, Jay -How, Yefanov, Oleksandr, Zatsepin, Nadia A., Aquila, Andrew, Fromme, Petra, Boutet, Sébastien, Seidler, Gerald T., Pushkar, Yulia, & Ketawala, Gihan. X-ray Emission Spectroscopy at X-ray Free Electron Lasers: Limits to Observation of the Classical Spectroscopic Response for Electronic Structure Analysis. United States. https://doi.org/10.1021/acs.jpclett.8b03595
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Jensen, Scott C., Sullivan, Brendan, Hartzler, Daniel A., Aguilar, Jose Meza, Awel, Salah, Bajt, Saša, Basu, Shibom, Bean, Richard, Chapman, Henry N., Conrad, Chelsie, Frank, Matthias, Fromme, Raimund, Martin-Garcia, Jose M., Grant, Thomas D., Heymann, Michael, Hunter, Mark S., Kirian, Richard A., Knoska, Juraj, Kupitz, Christopher, Li, Xuanxuan, Liang, Mengning, Lisova, Stella, Mariani, Valerio, Mazalova, Victoria, Messerschmidt, Marc, Moran, Michael, Nelson, Garrett, Oberthür, Dominik, Schaffer, Alex, Sierra, Raymond G., Vaughn, Natalie, Weierstall, Uwe, Wiedorn, Max O., Xavier, P. Lourdu, Yang, Jay -How, Yefanov, Oleksandr, Zatsepin, Nadia A., Aquila, Andrew, Fromme, Petra, Boutet, Sébastien, Seidler, Gerald T., Pushkar, Yulia, and Ketawala, Gihan. Wed . "X-ray Emission Spectroscopy at X-ray Free Electron Lasers: Limits to Observation of the Classical Spectroscopic Response for Electronic Structure Analysis". United States. https://doi.org/10.1021/acs.jpclett.8b03595. https://www.osti.gov/servlets/purl/1503076.
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@article{osti_1503076,
title = {X-ray Emission Spectroscopy at X-ray Free Electron Lasers: Limits to Observation of the Classical Spectroscopic Response for Electronic Structure Analysis},
author = {Jensen, Scott C. and Sullivan, Brendan and Hartzler, Daniel A. and Aguilar, Jose Meza and Awel, Salah and Bajt, Saša and Basu, Shibom and Bean, Richard and Chapman, Henry N. and Conrad, Chelsie and Frank, Matthias and Fromme, Raimund and Martin-Garcia, Jose M. and Grant, Thomas D. and Heymann, Michael and Hunter, Mark S. and Kirian, Richard A. and Knoska, Juraj and Kupitz, Christopher and Li, Xuanxuan and Liang, Mengning and Lisova, Stella and Mariani, Valerio and Mazalova, Victoria and Messerschmidt, Marc and Moran, Michael and Nelson, Garrett and Oberthür, Dominik and Schaffer, Alex and Sierra, Raymond G. and Vaughn, Natalie and Weierstall, Uwe and Wiedorn, Max O. and Xavier, P. Lourdu and Yang, Jay -How and Yefanov, Oleksandr and Zatsepin, Nadia A. and Aquila, Andrew and Fromme, Petra and Boutet, Sébastien and Seidler, Gerald T. and Pushkar, Yulia and Ketawala, Gihan},
abstractNote = {X-ray free electron lasers (XFELs) provide ultrashort intense X-ray pulses suitable to probe electron dynamics but can also induce a multitude of nonlinear excitation processes. These affect spectroscopic measurements and interpretation, particularly for upcoming brighter XFELs. Here we identify and discuss the limits to observing classical spectroscopy, where only one photon is absorbed per atom for a Mn2+ in a light element (O, C, H) environment. X-ray emission spectroscopy (XES) with different incident photon energies, pulse intensities, and pulse durations is presented. A rate equation model based on sequential ionization and relaxation events is used to calculate populations of multiply ionized states during a single pulse and to explain the observed X-ray induced spectral lines shifts. Furthermore this model provides easy estimation of spectral shifts, which is essential for experimental designs at XFELs and illustrates that shorter X-ray pulses will not overcome sequential ionization but can reduce electron cascade effects.},
doi = {10.1021/acs.jpclett.8b03595},
journal = {Journal of Physical Chemistry Letters},
number = 3,
volume = 10,
place = {United States},
year = {Wed Dec 19 00:00:00 EST 2018},
month = {Wed Dec 19 00:00:00 EST 2018}
}
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    Works referencing / citing this record:

    Inception of electronic damage of matter by photon-driven post-ionization mechanisms
    journal, March 2019

    • Błachucki, W.; Kayser, Y.; Czapla-Masztafiak, J.
    • Structural Dynamics, Vol. 6, Issue 2
    • DOI: 10.1063/1.5090332

    Inception of electronic damage of matter by photon-driven post-ionization mechanisms
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    • Structural Dynamics, Vol. 6, Issue 2
    • DOI: 10.1063/1.5090332
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