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; Tais Gorkhover

doi:10.1038/s41467-025-56046-y

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

Nat Commun. 2025 Jan 20;16(1):847. doi: 10.1038/s41467-025-56046-y.

Authors

Stephan Kuschel^{1

2

3

4}, Phay J Ho⁵, Andre Al Haddad^{6

7}, Felix F Zimmermann^{8

9

10}, Leonie Flueckiger¹¹, Matthew R Ware^{8

9}, Joseph Duris⁹, James P MacArthur⁹, Alberto Lutman⁹, Ming-Fu Lin⁹, Xiang Li^{9

12}, Kazutaka Nakahara⁹, Jeff W Aldrich⁹, Peter Walter⁹, Linda Young^{6

13}, Christoph Bostedt^{6

7

14}, Agostino Marinelli¹⁵, Tais Gorkhover^{16

17

18}

Affiliations

¹ SLAC National Accelerator Laboratory, Stanford PULSE Institute, Menlo Park, CA, USA. stephan.kuschel@tu-darmstadt.de.
² SLAC National Accelerator Laboratory, Menlo Park, CA, USA. stephan.kuschel@tu-darmstadt.de.
³ Institute for Experimental Physics/CFEL, University of Hamburg, Hamburg, Germany. stephan.kuschel@tu-darmstadt.de.
⁴ Technical University Darmstadt, Institute of nuclear physics, Darmstadt, Germany. stephan.kuschel@tu-darmstadt.de.
⁵ Chemical Sciences and Engineering Division, Argonne National Laboratory, Lemont, IL, USA. pho@anl.gov.
⁶ Chemical Sciences and Engineering Division, Argonne National Laboratory, Lemont, IL, USA.
⁷ Paul Scherrer Institute, Villigen, Switzerland.
⁸ SLAC National Accelerator Laboratory, Stanford PULSE Institute, Menlo Park, CA, USA.
⁹ SLAC National Accelerator Laboratory, Menlo Park, CA, USA.
¹⁰ IOAP, Technical University of Berlin, Berlin, Germany.
¹¹ La Trobe University, Latrobe, Australia.
¹² Department of Physics, Kansas State University, J.R. Macdonald Laboratory, Manhattan, KS, USA.
¹³ Department of Physics and James Franck Institute, The University of Chicago, Chicago, IL, USA.
¹⁴ LUXS Laboratory for Ultrafast X-ray Sciences, Institute of Chemical Sciences and Engineering, Lausanne, Switzerland.
¹⁵ SLAC National Accelerator Laboratory, Menlo Park, CA, USA. marinelli@slac.stanford.edu.
¹⁶ SLAC National Accelerator Laboratory, Stanford PULSE Institute, Menlo Park, CA, USA. tais.gorkhover@cfel.de.
¹⁷ SLAC National Accelerator Laboratory, Menlo Park, CA, USA. tais.gorkhover@cfel.de.
¹⁸ Institute for Experimental Physics/CFEL, University of Hamburg, Hamburg, Germany. tais.gorkhover@cfel.de.

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.