Non-linear enhancement of ultrafast X-ray diffraction through transient resonances

Stephan Kuschel (), Phay J. Ho (), Andre Al Haddad, Felix F. Zimmermann, Leonie Flueckiger, Matthew R. Ware, Joseph Duris, James P. MacArthur, Alberto Lutman, Ming-Fu Lin, Xiang Li, Kazutaka Nakahara, Jeff W. Aldrich, Peter Walter, Linda Young, Christoph Bostedt, Agostino Marinelli () and Tais Gorkhover ()
Additional contact information
Stephan Kuschel: Stanford PULSE Institute
Phay J. Ho: Argonne National Laboratory
Andre Al Haddad: Argonne National Laboratory
Felix F. Zimmermann: Stanford PULSE Institute
Leonie Flueckiger: La Trobe University
Matthew R. Ware: Stanford PULSE Institute
Joseph Duris: SLAC National Accelerator Laboratory
James P. MacArthur: SLAC National Accelerator Laboratory
Alberto Lutman: SLAC National Accelerator Laboratory
Ming-Fu Lin: SLAC National Accelerator Laboratory
Xiang Li: SLAC National Accelerator Laboratory
Kazutaka Nakahara: SLAC National Accelerator Laboratory
Jeff W. Aldrich: SLAC National Accelerator Laboratory
Peter Walter: SLAC National Accelerator Laboratory
Linda Young: Argonne National Laboratory
Christoph Bostedt: Argonne National Laboratory
Agostino Marinelli: SLAC National Accelerator Laboratory
Tais Gorkhover: Stanford PULSE Institute

Nature Communications, 2025, vol. 16, issue 1, 1-8

Abstract: Abstract Diffraction-before-destruction imaging with ultrashort X-ray pulses can visualize non-equilibrium processes, such as chemical reactions, with sub-femtosecond precision in the native environment. Here, a nanospecimen diffracts a single X-ray flash before it disintegrates. The sample structure can be reconstructed from the coherent diffraction image (CDI). State-of-the-art X-ray snapshots lack high spatial resolution because of weak diffraction signal. Bleaching effects from photo-ionization significantly restrain image brightness scaling. We find that non-linear transient ion resonances can overcome this barrier if X-ray laser pulses are shorter than in most experiments. We compared snapshots from individual ≈ 100 nm Xe nanoparticles as a function of pulse duration and incoming X-ray fluence. Our experimental results and Monte Carlo simulations suggest that transient resonances can increase ionic scattering cross sections significantly beyond literature values. This provides a novel avenue towards substantial improvement of the spatial resolution in CDI in combination with sub-femtosecond temporal precision at the nanoscale.

Date: 2025
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DOI: 10.1038/s41467-025-56046-y

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