Super-resolution stimulated X-ray Raman spectroscopy

Kai Li (), Christian Ott, Marcus Agåker, Phay J. Ho, Gilles Doumy, Alexander Magunia, Marc Rebholz, Marc Simon, Tommaso Mazza, Alberto Fanis, Thomas M. Baumann, Jacobo Montano, Nils Rennhack, Sergey Usenko, Yevheniy Ovcharenko, Kalyani Chordiya, Lan Cheng, Jan-Erik Rubensson, Michael Meyer, Thomas Pfeifer (), Mette B. Gaarde and Linda Young ()
Additional contact information
Kai Li: The University of Chicago
Christian Ott: Max-Planck-Institut für Kernphysik
Marcus Agåker: Uppsala University
Phay J. Ho: Argonne National Laboratory
Gilles Doumy: Argonne National Laboratory
Alexander Magunia: Max-Planck-Institut für Kernphysik
Marc Rebholz: Max-Planck-Institut für Kernphysik
Marc Simon: Sorbonne Université, CNRS
Tommaso Mazza: European XFEL
Alberto Fanis: European XFEL
Thomas M. Baumann: European XFEL
Jacobo Montano: European XFEL
Nils Rennhack: European XFEL
Sergey Usenko: European XFEL
Yevheniy Ovcharenko: European XFEL
Kalyani Chordiya: University of Hamburg
Lan Cheng: Johns Hopkins University
Jan-Erik Rubensson: Uppsala University
Michael Meyer: European XFEL
Thomas Pfeifer: Max-Planck-Institut für Kernphysik
Mette B. Gaarde: Louisiana State University
Linda Young: The University of Chicago

Nature, 2025, vol. 643, issue 8072, 662-668

Abstract: Abstract Propagation of intense X-ray pulses through dense media has led to the observation of phenomena such as atomic X-ray lasing1,2, self-induced transparency3 and stimulated X-ray Raman scattering (SXRS)4. SXRS has been long predicted as a means to launch and probe valence-electron wavepackets and as a building block for nonlinear X-ray spectroscopies5,6. However, experimental observations of SXRS to date4,7,8 have not provided spectroscopic information, and theoretical modelling has largely implemented hard-to-realize phase-coherent attosecond pulses. Here we demonstrate SXRS with spectroscopic precision, that is, detection of valence-excited states in neon with a near Fourier-limited joint energy–time resolution of 0.1 eV–40 fs. We used a new covariance analysis between statistically spiky broadband incident X-ray and scattered X-ray Raman pulses. Using 18,000 single shots, we beat not only the incident (about 8 eV) bandwidth but also the approximately 0.2 eV instrumental energy resolution, thus creating super-resolution conditions, in analogy to super-resolved fluorescence microscopy9. Our experimental results, supported by ab initio propagation simulations, reveal the competition between lasing in the ion and stimulated Raman scattering in the neutral. We demonstrate enhanced signal collection efficiency and a broad excitation window, surpassing spontaneous Raman efficiencies by orders of magnitude. This stochastic SXRS approach represents a first step towards tracking elementary events that determine chemical outcomes10.

Date: 2025
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DOI: 10.1038/s41586-025-09214-5

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