Nonlinear reversal of photoexcitation on the attosecond time scale improves ultrafast X-ray diffraction images
The complex refractive index of a material governs its light-matter interactions, with intense light fields enabling tailored nonlinear optical responses. In the X-ray regime, rapid photoionization limits the potential of nonlinear techniques by inducing irreversible electronic damage. Here we demonstrate that intense, sub-femtosecond X-ray pulses, shorter than typical Auger decay times, can partially reverse photoexcitation via stimulated emission near atomic resonances. By analyzing thousands of coherent diffraction patterns and ion spectra from neon nanoparticles exposed to sub-fs and 15-fs pulses, we observe enhanced X-ray diffraction alongside reduced energy absorption for sub-fs pulses. Theoretical modeling attributes this to dynamics akin to Rabi flopping that prolong the lifetime of resonant states and suppress electronic bleaching. These findings suggest that ultrashort, intense X-ray pulses enable active control of X-ray refractive index and damage pathways, opening avenues for improved high-resolution imaging and nonlinear spectroscopy in complex nanoscale systems.
Authors
- Bruno Langbehn (ORCID: https://orcid.org/0000-0002-3245-8169)
- Taran Driver (ORCID: https://orcid.org/0000-0002-3761-6883)
- Stephan Kuschel (ORCID: https://orcid.org/0000-0001-5159-525X)
- Agostino Marinelli (ORCID: https://orcid.org/0000-0002-7248-4652)
- David Cesar (ORCID: https://orcid.org/0000-0003-3669-1854)
- Joseph Duris (ORCID: https://orcid.org/0000-0002-9930-1166)
- River Robles (ORCID: https://orcid.org/0000-0002-7152-4675)
- Linda Young (ORCID: https://orcid.org/0000-0002-2251-039X)
- Ming‐Fu Lin (ORCID: https://orcid.org/0000-0001-8086-2484)
- Kirk A. Larsen (ORCID: https://orcid.org/0000-0002-3252-260X)
- Michael R. Meyer (ORCID: https://orcid.org/0000-0003-1227-3084)
- Christoph Bostedt (ORCID: https://orcid.org/0000-0001-8169-8639)
- James Cryan (ORCID: https://orcid.org/0000-0002-7776-0919)
- Philip Hart (ORCID: https://orcid.org/0000-0002-4569-3926)
- Daniela Rupp (ORCID: https://orcid.org/0000-0002-6504-7956)
- Anatoli Ulmer (ORCID: https://orcid.org/0000-0001-7864-3063)
- Linos Hecht (ORCID: https://orcid.org/0000-0003-3342-1218)
- Razib Obaid (ORCID: https://orcid.org/0000-0002-1759-4752)
- Adam M. Summers (ORCID: https://orcid.org/0000-0003-2694-4969)
- Simon Dold (ORCID: https://orcid.org/0000-0001-5332-8251)
- Tais Gorkhover (ORCID: https://orcid.org/0009-0001-8804-1186)
- Robert Radloff
- Phay J. Ho (ORCID: https://orcid.org/0000-0001-5214-2180)
- Paris Franz (ORCID: https://orcid.org/0000-0003-2728-6283)
- Zhaoheng Guo (ORCID: https://orcid.org/0000-0003-3873-8804)
- Xiang Li (ORCID: https://orcid.org/0000-0001-8338-4123)
- Peter Walter (ORCID: https://orcid.org/0000-0001-8745-6593)
- Andrei Kamalov (ORCID: https://orcid.org/0009-0008-6909-0442)
- K. Nakahara
- Nick Sudar
- Lara Rönnebeck
Institutions
- Argonne National Laboratory (US)
- Solid State Physics Laboratory (IN)
- Universität Hamburg (DE)
- Laboratoire de physique des Solides (FR)
- HafenCity University Hamburg (DE)
- SLAC National Accelerator Laboratory (US)
- Paul Scherrer Institute (CH)
- Technische Universität Darmstadt (DE)
- Technische Universität Berlin (DE)
- École Polytechnique Fédérale de Lausanne (CH)
- European X-Ray Free-Electron Laser (DE)
- Stanford University (US)
Publication Details
- Journal
- Nature Communications
- Published
- 2026-07-28
- DOI
- https://doi.org/10.1038/s41467-026-75969-8
- Primary Topic
- Advanced X-ray Imaging Techniques
- Type
- article
- Field-Weighted Citation Impact
- 0.00