Core-level nonlinear spectroscopy triggered by stochastic X-ray pulses

Yves Kayser (), Chris Milne, Pavle Juranić, Leonardo Sala, Joanna Czapla-Masztafiak, Rolf Follath, Matjaž Kavčič, Gregor Knopp, Jens Rehanek, Wojciech Błachucki, Mickaël G. Delcey, Marcus Lundberg, Krzysztof Tyrała, Diling Zhu, Roberto Alonso-Mori, Rafael Abela, Jacinto Sá () and Jakub Szlachetko ()
Additional contact information
Yves Kayser: Physikalisch-Technische Bundesanstalt
Chris Milne: Paul Scherrer Institut
Pavle Juranić: Paul Scherrer Institut
Leonardo Sala: Paul Scherrer Institut
Joanna Czapla-Masztafiak: Institute of Nuclear Physics Polish Academy of Sciences
Rolf Follath: Paul Scherrer Institut
Matjaž Kavčič: Institut Jožef Stefan
Gregor Knopp: Paul Scherrer Institut
Jens Rehanek: Paul Scherrer Institut
Wojciech Błachucki: Institute of Physical Chemistry, Polish Academy of Sciences
Mickaël G. Delcey: Department of Chemistry- Ångström, Uppsala University
Marcus Lundberg: Department of Chemistry- Ångström, Uppsala University
Krzysztof Tyrała: Institute of Nuclear Physics Polish Academy of Sciences
Diling Zhu: Linac Coherent Light Source (LCLS), SLAC National Accelerator Laboratory
Roberto Alonso-Mori: Linac Coherent Light Source (LCLS), SLAC National Accelerator Laboratory
Rafael Abela: Paul Scherrer Institut
Jacinto Sá: Institute of Physical Chemistry, Polish Academy of Sciences
Jakub Szlachetko: Institute of Nuclear Physics Polish Academy of Sciences

Nature Communications, 2019, vol. 10, issue 1, 1-10

Abstract: Abstract Stochastic processes are highly relevant in research fields as different as neuroscience, economy, ecology, chemistry, and fundamental physics. However, due to their intrinsic unpredictability, stochastic mechanisms are very challenging for any kind of investigations and practical applications. Here we report the deliberate use of stochastic X-ray pulses in two-dimensional spectroscopy to the simultaneous mapping of unoccupied and occupied electronic states of atoms in a regime where the opacity and transparency properties of matter are subject to the incident intensity and photon energy. A readily transferable matrix formalism is presented to extract the electronic states from a dataset measured with the monitored input from a stochastic excitation source. The presented formalism enables investigations of the response of the electronic structure to irradiation with intense X-ray pulses while the time structure of the incident pulses is preserved.

Date: 2019
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DOI: 10.1038/s41467-019-12717-1

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