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 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 Zatsepin, Andrew Aquila, Petra Fromme, Sébastien Boutet, Gerald T. Seidler, Yulia Pushkar

Research output: Contribution to journalArticle

1 Citation (Scopus)

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

Fingerprint

X ray lasers
Free electron lasers
free electron lasers
Electronic structure
electronic structure
X rays
Ionization
Photons
spectroscopy
x rays
Electrons
Design of experiments
pulses
Laser pulses
Spectroscopy
Atoms
ionization
shift
light elements
photons

ASJC Scopus subject areas

  • Materials Science(all)
  • Physical and Theoretical Chemistry

Cite this

X-ray Emission Spectroscopy at X-ray Free Electron Lasers : Limits to Observation of the Classical Spectroscopic Response for Electronic Structure Analysis. / 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.; Ketawala, Gihan; Kirian, Richard; 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; Aquila, Andrew; Fromme, Petra; Boutet, Sébastien; Seidler, Gerald T.; Pushkar, Yulia.

In: Journal of Physical Chemistry Letters, Vol. 10, No. 3, 07.02.2019, p. 441-446.

Research output: Contribution to journalArticle

Jensen, SC, Sullivan, B, Hartzler, DA, Aguilar, JM, Awel, S, Bajt, S, Basu, S, Bean, R, Chapman, HN, Conrad, C, Frank, M, Fromme, R, Martin-Garcia, JM, Grant, TD, Heymann, M, Hunter, MS, Ketawala, G, Kirian, R, Knoska, J, Kupitz, C, Li, X, Liang, M, Lisova, S, Mariani, V, Mazalova, V, Messerschmidt, M, Moran, M, Nelson, G, Oberthür, D, Schaffer, A, Sierra, RG, Vaughn, N, Weierstall, U, Wiedorn, MO, Xavier, PL, Yang, JH, Yefanov, O, Zatsepin, N, Aquila, A, Fromme, P, Boutet, S, Seidler, GT & 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, vol. 10, no. 3, pp. 441-446. https://doi.org/10.1021/acs.jpclett.8b03595
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. ; Ketawala, Gihan ; Kirian, Richard ; 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 ; Aquila, Andrew ; Fromme, Petra ; Boutet, Sébastien ; Seidler, Gerald T. ; Pushkar, Yulia. / X-ray Emission Spectroscopy at X-ray Free Electron Lasers : Limits to Observation of the Classical Spectroscopic Response for Electronic Structure Analysis. In: Journal of Physical Chemistry Letters. 2019 ; Vol. 10, No. 3. pp. 441-446.
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AU - Jensen, Scott C.

AU - Sullivan, Brendan

AU - Hartzler, Daniel A.

AU - Aguilar, Jose Meza

AU - Awel, Salah

AU - Bajt, Saša

AU - Basu, Shibom

AU - Bean, Richard

AU - Chapman, Henry N.

AU - Conrad, Chelsie

AU - Frank, Matthias

AU - Fromme, Raimund

AU - Martin-Garcia, Jose M.

AU - Grant, Thomas D.

AU - Heymann, Michael

AU - Hunter, Mark S.

AU - Ketawala, Gihan

AU - Kirian, Richard

AU - Knoska, Juraj

AU - Kupitz, Christopher

AU - Li, Xuanxuan

AU - Liang, Mengning

AU - Lisova, Stella

AU - Mariani, Valerio

AU - Mazalova, Victoria

AU - Messerschmidt, Marc

AU - Moran, Michael

AU - Nelson, Garrett

AU - Oberthür, Dominik

AU - Schaffer, Alex

AU - Sierra, Raymond G.

AU - Vaughn, Natalie

AU - Weierstall, Uwe

AU - Wiedorn, Max O.

AU - Xavier, P. Lourdu

AU - Yang, Jay How

AU - Yefanov, Oleksandr

AU - Zatsepin, Nadia

AU - Aquila, Andrew

AU - Fromme, Petra

AU - Boutet, Sébastien

AU - Seidler, Gerald T.

AU - Pushkar, Yulia

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