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

Scott C. Jensen, Brendan Sullivan, Daniel A. Hartzler, Jose Meza Aguilar, Salah Awel, Saša Bajt, Shibom Basu, Richard Bean, Henry N. Chapman, Chelsie Conrad, Matthias Frank, Raimund Fromme, Jose M. Martin-Garcia, Thomas D. Grant, Michael Heymann, Mark S. Hunter, Gihan Ketawala, Richard A. Kirian, Juraj Knoska, Christopher KupitzXuanxuan Li, Mengning Liang, Stella Lisova, Valerio Mariani, Victoria Mazalova, Marc Messerschmidt, Michael Moran, Garrett Nelson, Dominik Oberthür, Alex Schaffer, Raymond G. Sierra, Natalie Vaughn, Uwe Weierstall, Max O. Wiedorn, P. Lourdu Xavier, Jay How Yang, Oleksandr Yefanov, Nadia A. Zatsepin, Andrew Aquila, Petra Fromme, Sébastien Boutet, Gerald T. Seidler, Yulia Pushkar

Research output: Contribution to journalArticle

1 Scopus citations

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 Mn 2+ 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. 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.

Original languageEnglish (US)
Pages (from-to)441-446
Number of pages6
JournalJournal of Physical Chemistry Letters
Volume10
Issue number3
DOIs
StatePublished - Feb 7 2019
Externally publishedYes

ASJC Scopus subject areas

  • Materials Science(all)
  • Physical and Theoretical Chemistry

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    Jensen, S. C., Sullivan, B., Hartzler, D. A., Aguilar, J. M., Awel, S., Bajt, S., Basu, S., Bean, R., Chapman, H. N., Conrad, C., Frank, M., Fromme, R., Martin-Garcia, J. M., Grant, T. D., Heymann, M., Hunter, M. S., Ketawala, G., Kirian, R. A., Knoska, J., ... Pushkar, Y. (2019). X-ray Emission Spectroscopy at X-ray Free Electron Lasers: Limits to Observation of the Classical Spectroscopic Response for Electronic Structure Analysis. Journal of Physical Chemistry Letters, 10(3), 441-446. https://doi.org/10.1021/acs.jpclett.8b03595