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 Kupitz; Xuanxuan 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

doi:10.1021/acs.jpclett.8b03595

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 journal › Article › peer-review

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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 language	English (US)
Pages (from-to)	441-446
Number of pages	6
Journal	Journal of Physical Chemistry Letters
Volume	10
Issue number	3
DOIs	https://doi.org/10.1021/acs.jpclett.8b03595
State	Published - Feb 7 2019

ASJC Scopus subject areas

General Materials Science
Physical and Theoretical Chemistry

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10.1021/acs.jpclett.8b03595

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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

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

Research output: Contribution to journal › Article › peer-review

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, RA, 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, NA, 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

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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 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.",

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T2 - Limits to Observation of the Classical Spectroscopic Response for Electronic Structure Analysis

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 A.

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 A.

AU - Aquila, Andrew

AU - Fromme, Petra

AU - Boutet, Sébastien

AU - Seidler, Gerald T.

AU - Pushkar, Yulia

PY - 2019/2/7

Y1 - 2019/2/7

N2 - 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.

AB - 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.

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JO - Journal of Physical Chemistry Letters

JF - Journal of Physical Chemistry Letters

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ER -

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

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