Multiple-core-hole resonance spectroscopy with ultraintense X-ray pulses

Aljoscha Rörig, Sang-Kil Son (), Tommaso Mazza, Philipp Schmidt, Thomas M. Baumann, Benjamin Erk, Markus Ilchen, Joakim Laksman, Valerija Music, Shashank Pathak, Daniel E. Rivas, Daniel Rolles, Svitozar Serkez, Sergey Usenko, Robin Santra, Michael Meyer and Rebecca Boll ()
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Aljoscha Rörig: European XFEL
Sang-Kil Son: Deutsches Elektronen-Synchrotron DESY
Tommaso Mazza: European XFEL
Philipp Schmidt: European XFEL
Thomas M. Baumann: European XFEL
Benjamin Erk: Deutsches Elektronen-Synchrotron DESY
Markus Ilchen: European XFEL
Joakim Laksman: European XFEL
Valerija Music: European XFEL
Shashank Pathak: Kansas State University
Daniel E. Rivas: European XFEL
Daniel Rolles: Kansas State University
Svitozar Serkez: European XFEL
Sergey Usenko: European XFEL
Robin Santra: Universität Hamburg
Michael Meyer: European XFEL
Rebecca Boll: European XFEL

Nature Communications, 2023, vol. 14, issue 1, 1-10

Abstract: Abstract Understanding the interaction of intense, femtosecond X-ray pulses with heavy atoms is crucial for gaining insights into the structure and dynamics of matter. One key aspect of nonlinear light–matter interaction was, so far, not studied systematically at free-electron lasers—its dependence on the photon energy. Here, we use resonant ion spectroscopy to map out the transient electronic structures occurring during the complex charge-up pathways of xenon. Massively hollow atoms featuring up to six simultaneous core holes determine the spectra at specific photon energies and charge states. We also illustrate how different X-ray pulse parameters, which are usually intertwined, can be partially disentangled. The extraction of resonance spectra is facilitated by the possibility of working with a constant number of photons per X-ray pulse at all photon energies and the fact that the ion yields become independent of the peak fluence beyond a saturation point. Our study lays the groundwork for spectroscopic investigations of transient atomic species in exotic, multiple-core-hole states that have not been explored previously.

Date: 2023
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DOI: 10.1038/s41467-023-41505-1

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