Emergence of pseudoresonance in high-intensity resonant inelastic x-ray scattering

Sang Kil Son; Thomas M. Baumann; Jacob Pedersen; Laura Budewig; Kai Li; Hans Ågren; Olle Björneholm; Rebecca Boll; John Bozek; Carl Caleman; Sebastian Cardoch; Lucas M. Cornetta; Alberto De Fanis; Emiliano De Santis; Simon Dold; Gilles Doumy; Ulrich Eichmann; Xiaochun Gong; Johan Gråsjö; Alice E. Green; Iyas Ismail; Ludvig Kjellsson; Eva Lindroth; Tommaso Mazza; Jacobo Montalvo; Terry Mullins; Christian Ott; Yevheniy Ovcharenko; Thomas Pfeifer; Maria Novella Piancastelli; Ralph Püttner; Nils Rennhack; Nina Rohringer; Cecilia Sánchez-Hanke; Conny Säthe; Philipp Schmidt; Björn Senffleben; Marc Simon; Nicusor Timneanu; Moto Togawa; Kiyoshi Ueda; Sergey Usenko; Hans Jakob Wörner; Weiqing Xu; Zhong Yin; Linda Young; Joseph Nordgren; Marcus Agåker; John Söderström; Sonia Coriani; Michael Meyer; Robin Santra; Jan Erik Rubensson

doi:10.1103/drmh-vmgk

Emergence of pseudoresonance in high-intensity resonant inelastic x-ray scattering

Sang Kil Son^*
, Thomas M. Baumann
, Jacob Pedersen
, Laura Budewig
, Kai Li
, Hans Ågren
, Olle Björneholm
, Rebecca Boll
, John Bozek
, Carl Caleman
, Sebastian Cardoch
, Lucas M. Cornetta
, Alberto De Fanis
, Emiliano De Santis
, Simon Dold
, Gilles Doumy
, Ulrich Eichmann
, Xiaochun Gong
, Johan Gråsjö
, Alice E. Green

Iyas Ismail, Ludvig Kjellsson, Eva Lindroth, Tommaso Mazza, Jacobo Montalvo, Terry Mullins, Christian Ott, Yevheniy Ovcharenko, Thomas Pfeifer^*, Maria Novella Piancastelli, Ralph Püttner, Nils Rennhack, Nina Rohringer, Cecilia Sánchez-Hanke, Conny Säthe, Philipp Schmidt, Björn Senffleben, Marc Simon, Nicusor Timneanu, Moto Togawa, Kiyoshi Ueda, Sergey Usenko, Hans Jakob Wörner, Weiqing Xu, Zhong Yin, Linda Young, Joseph Nordgren, Marcus Agåker, John Söderström, Sonia Coriani, Michael Meyer, Robin Santra, Jan Erik Rubensson^*

^*Corresponding author for this work

Center for Free-Electron Laser Science CFEL
German Electron Synchrotron
European XFEL
Department of Chemistry
Technical University of Denmark
Norwegian University of Science and Technology
Department of Physics
University of Hamburg
The University of Chicago
Chemical Sciences and Engineering Division
Argonne National Laboratory
Department of Physics and Astronomy
Uppsala University
l'Orme des Merisiers
Universidade de São Paulo
University of Rome Tor Vergata
Lund University
Max-Born-Institute for Nonlinear Optics and Short Pulse Spectroscopy
Zhejiang University
Department of Chemistry
Stanford University
University of Edinburgh
Sorbonne Université
Department of Physics
Stockholm University
Max Planck Institute for Nuclear Physics
Fachbereich Physik
Free University of Berlin
Diamond Light Source
Department of Chemistry
Tohoku University
School Physical Science and Technology
ShanghaiTech University
Laboratory of Physical Chemistry
Swiss Federal Institute of Technology Zurich
Center for Transformative Science
International Center for Synchrotron Radiation Innovation Smart

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

Abstract

We report resonant inelastic x-ray scattering (RIXS) spectra of neon atoms interacting with intense x-ray pulses generated using an x-ray free-electron laser (XFEL). We find that an unexpected peak emerges near the Ka line of Ne, which does not coincide with any physical resonances of neon ions. We perform theoretical calculations based on a quantum-state-resolved rate-equation approach with x-ray-induced processes including possible resonant excitations. Our dynamics simulations demonstrate that a sequence of multiple resonant photoabsorption events are involved and the interplay of those multiple resonances in combination with the relatively large spectral bandwidth of XFEL radiation leads to the emergent resonance-like structure at a position where no resonances exist. Our finding offers critical guidance for future applications of high-intensity RIXS at XFEL facilities.

Original language	English
Article number	L051101
Journal	Physical Review A
Volume	112
Issue number	5
DOIs	https://doi.org/10.1103/drmh-vmgk
State	Published - 7 Nov 2025
Externally published	Yes

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Son, S. K., Baumann, T. M., Pedersen, J., Budewig, L., Li, K., Ågren, H., Björneholm, O., Boll, R., Bozek, J., Caleman, C., Cardoch, S., Cornetta, L. M., De Fanis, A., De Santis, E., Dold, S., Doumy, G., Eichmann, U., Gong, X., Gråsjö, J., ... Rubensson, J. E. (2025). Emergence of pseudoresonance in high-intensity resonant inelastic x-ray scattering. Physical Review A, 112(5), Article L051101. https://doi.org/10.1103/drmh-vmgk

@article{6b83ad51e3ca4e5db7de8eb445399280,

title = "Emergence of pseudoresonance in high-intensity resonant inelastic x-ray scattering",

abstract = "We report resonant inelastic x-ray scattering (RIXS) spectra of neon atoms interacting with intense x-ray pulses generated using an x-ray free-electron laser (XFEL). We find that an unexpected peak emerges near the Ka line of Ne, which does not coincide with any physical resonances of neon ions. We perform theoretical calculations based on a quantum-state-resolved rate-equation approach with x-ray-induced processes including possible resonant excitations. Our dynamics simulations demonstrate that a sequence of multiple resonant photoabsorption events are involved and the interplay of those multiple resonances in combination with the relatively large spectral bandwidth of XFEL radiation leads to the emergent resonance-like structure at a position where no resonances exist. Our finding offers critical guidance for future applications of high-intensity RIXS at XFEL facilities.",

author = "Son, \{Sang Kil\} and Baumann, \{Thomas M.\} and Jacob Pedersen and Laura Budewig and Kai Li and Hans {\AA}gren and Olle Bj{\"o}rneholm and Rebecca Boll and John Bozek and Carl Caleman and Sebastian Cardoch and Cornetta, \{Lucas M.\} and \{De Fanis\}, Alberto and \{De Santis\}, Emiliano and Simon Dold and Gilles Doumy and Ulrich Eichmann and Xiaochun Gong and Johan Gr{\aa}sj{\"o} and Green, \{Alice E.\} and Iyas Ismail and Ludvig Kjellsson and Eva Lindroth and Tommaso Mazza and Jacobo Montalvo and Terry Mullins and Christian Ott and Yevheniy Ovcharenko and Thomas Pfeifer and Piancastelli, \{Maria Novella\} and Ralph P{\"u}ttner and Nils Rennhack and Nina Rohringer and Cecilia S{\'a}nchez-Hanke and Conny S{\"a}the and Philipp Schmidt and Bj{\"o}rn Senffleben and Marc Simon and Nicusor Timneanu and Moto Togawa and Kiyoshi Ueda and Sergey Usenko and W{\"o}rner, \{Hans Jakob\} and Weiqing Xu and Zhong Yin and Linda Young and Joseph Nordgren and Marcus Ag{\aa}ker and John S{\"o}derstr{\"o}m and Sonia Coriani and Michael Meyer and Robin Santra and Rubensson, \{Jan Erik\}",

note = "Publisher Copyright: {\textcopyright} (2025), (Published by the American Physical Society under the terms of the Creative Commons Attribution 4.0 International license.), All Rights Reserved.",

year = "2025",

month = nov,

day = "7",

doi = "10.1103/drmh-vmgk",

language = "英语",

volume = "112",

journal = "Physical Review A",

issn = "2469-9926",

publisher = "American Physical Society",

number = "5",

}

Son, SK, Baumann, TM, Pedersen, J, Budewig, L, Li, K, Ågren, H, Björneholm, O, Boll, R, Bozek, J, Caleman, C, Cardoch, S, Cornetta, LM, De Fanis, A, De Santis, E, Dold, S, Doumy, G, Eichmann, U, Gong, X, Gråsjö, J, Green, AE, Ismail, I, Kjellsson, L, Lindroth, E, Mazza, T, Montalvo, J, Mullins, T, Ott, C, Ovcharenko, Y, Pfeifer, T, Piancastelli, MN, Püttner, R, Rennhack, N, Rohringer, N, Sánchez-Hanke, C, Säthe, C, Schmidt, P, Senffleben, B, Simon, M, Timneanu, N, Togawa, M, Ueda, K, Usenko, S, Wörner, HJ, Xu, W, Yin, Z, Young, L, Nordgren, J, Agåker, M, Söderström, J, Coriani, S, Meyer, M, Santra, R & Rubensson, JE 2025, 'Emergence of pseudoresonance in high-intensity resonant inelastic x-ray scattering', Physical Review A, vol. 112, no. 5, L051101. https://doi.org/10.1103/drmh-vmgk

TY - JOUR

T1 - Emergence of pseudoresonance in high-intensity resonant inelastic x-ray scattering

AU - Son, Sang Kil

AU - Baumann, Thomas M.

AU - Pedersen, Jacob

AU - Budewig, Laura

AU - Li, Kai

AU - Ågren, Hans

AU - Björneholm, Olle

AU - Boll, Rebecca

AU - Bozek, John

AU - Caleman, Carl

AU - Cardoch, Sebastian

AU - Cornetta, Lucas M.

AU - De Fanis, Alberto

AU - De Santis, Emiliano

AU - Dold, Simon

AU - Doumy, Gilles

AU - Eichmann, Ulrich

AU - Gong, Xiaochun

AU - Gråsjö, Johan

AU - Green, Alice E.

AU - Ismail, Iyas

AU - Kjellsson, Ludvig

AU - Lindroth, Eva

AU - Mazza, Tommaso

AU - Montalvo, Jacobo

AU - Mullins, Terry

AU - Ott, Christian

AU - Ovcharenko, Yevheniy

AU - Pfeifer, Thomas

AU - Piancastelli, Maria Novella

AU - Püttner, Ralph

AU - Rennhack, Nils

AU - Rohringer, Nina

AU - Sánchez-Hanke, Cecilia

AU - Säthe, Conny

AU - Schmidt, Philipp

AU - Senffleben, Björn

AU - Simon, Marc

AU - Timneanu, Nicusor

AU - Togawa, Moto

AU - Ueda, Kiyoshi

AU - Usenko, Sergey

AU - Wörner, Hans Jakob

AU - Xu, Weiqing

AU - Yin, Zhong

AU - Young, Linda

AU - Nordgren, Joseph

AU - Agåker, Marcus

AU - Söderström, John

AU - Coriani, Sonia

AU - Meyer, Michael

AU - Santra, Robin

AU - Rubensson, Jan Erik

PY - 2025/11/7

Y1 - 2025/11/7

N2 - We report resonant inelastic x-ray scattering (RIXS) spectra of neon atoms interacting with intense x-ray pulses generated using an x-ray free-electron laser (XFEL). We find that an unexpected peak emerges near the Ka line of Ne, which does not coincide with any physical resonances of neon ions. We perform theoretical calculations based on a quantum-state-resolved rate-equation approach with x-ray-induced processes including possible resonant excitations. Our dynamics simulations demonstrate that a sequence of multiple resonant photoabsorption events are involved and the interplay of those multiple resonances in combination with the relatively large spectral bandwidth of XFEL radiation leads to the emergent resonance-like structure at a position where no resonances exist. Our finding offers critical guidance for future applications of high-intensity RIXS at XFEL facilities.

AB - We report resonant inelastic x-ray scattering (RIXS) spectra of neon atoms interacting with intense x-ray pulses generated using an x-ray free-electron laser (XFEL). We find that an unexpected peak emerges near the Ka line of Ne, which does not coincide with any physical resonances of neon ions. We perform theoretical calculations based on a quantum-state-resolved rate-equation approach with x-ray-induced processes including possible resonant excitations. Our dynamics simulations demonstrate that a sequence of multiple resonant photoabsorption events are involved and the interplay of those multiple resonances in combination with the relatively large spectral bandwidth of XFEL radiation leads to the emergent resonance-like structure at a position where no resonances exist. Our finding offers critical guidance for future applications of high-intensity RIXS at XFEL facilities.

UR - https://www.scopus.com/pages/publications/105027140457

U2 - 10.1103/drmh-vmgk

DO - 10.1103/drmh-vmgk

M3 - 快报

AN - SCOPUS:105027140457

SN - 2469-9926

VL - 112

JO - Physical Review A

JF - Physical Review A

IS - 5

M1 - L051101

ER -

Emergence of pseudoresonance in high-intensity resonant inelastic x-ray scattering

Abstract

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