Real-space imaging of the electron-pair density hole in molecular Auger–Meitner decay
Abstract Electrons in matter can rearrange extremely quickly under external perturbations, underpinning subsequent structural and chemical transformations. Coulomb interactions between neighbouring electrons often shape this response, giving rise to correlated motion and strongly affecting the distribution of electrons in the system. Here we show that non-resonant hard X-ray scattering can directly access changes in the radial electron-pair density during the rapid rearrangement of core and valence electrons. We do this by studying sulfur hexafluoride molecules undergoing Auger–Meitner decay. We exploit a second-order interaction between the X-ray photons and the molecules to trigger and probe the decay dynamics with a single pulse, capturing the electron loss and redistribution before the molecules dissociate. The experiment shows that changes in electron-pair densities can be isolated and measured on ultrafast timescales, providing insight into the real-space evolution of highly excited and short-lived electronic states.
Authors
- Brian Stankus (ORCID: https://orcid.org/0000-0002-1351-1286)
- Elke Faßhauer (ORCID: https://orcid.org/0000-0001-8187-6052)
- Asami Odate (ORCID: https://orcid.org/0000-0002-3377-1413)
- Mats Simmermacher (ORCID: https://orcid.org/0000-0001-9848-7010)
- Haiwang Yong (ORCID: https://orcid.org/0000-0002-5860-4259)
- Ruaridh Forbes (ORCID: https://orcid.org/0000-0003-2097-5991)
- Thomas Northey (ORCID: https://orcid.org/0000-0002-6011-454X)
- Daniel Ratner (ORCID: https://orcid.org/0000-0002-5747-7323)
- Xuan Xu (ORCID: https://orcid.org/0000-0001-7804-0369)
- Adam Kirrander (ORCID: https://orcid.org/0000-0002-3347-8137)
- Michael P. Minitti (ORCID: https://orcid.org/0000-0002-9854-9717)
- Peter Weber (ORCID: https://orcid.org/0000-0001-6022-6050)
- Andrés Moreno Carrascosa (ORCID: https://orcid.org/0000-0003-1045-7760)
- Wenpeng Du (ORCID: https://orcid.org/0000-0002-7857-7788)
- Nathan Goff (ORCID: https://orcid.org/0009-0008-3007-0639)
- Mengning Liang (ORCID: https://orcid.org/0009-0003-6711-4555)
- Lingyu Ma (ORCID: https://orcid.org/0000-0002-2300-1132)
- Joseph C. Cooper (ORCID: https://orcid.org/0009-0002-4992-1997)
- Kyle Acheson
Institutions
- Brown University (US)
- SLAC National Accelerator Laboratory (US)
- University of Oxford (GB)
- Linac Coherent Light Source (US)
- University of Tübingen (DE)
Publication Details
- Journal
- Nature Physics
- Published
- 2026-06-30
- DOI
- https://doi.org/10.1038/s41567-026-03363-8
- Primary Topic
- Laser-Matter Interactions and Applications
- Type
- article
- Field-Weighted Citation Impact
- 0.00
Funders
- National Science Foundation
- U.S. Department of Energy
- Oak Ridge Associated Universities
- Leverhulme Trust
- University of Oxford
- Deutsche Forschungsgemeinschaft
- Agence Nationale de la Recherche
- Eberhard Karls Universität Tübingen
- National Institutes of Health
- Office of Science
- Oak Ridge Institute for Science and Education
- Engineering and Physical Sciences Research Council
- Division of Chemistry
- Basic Energy Sciences
- Workforce Development for Teachers and Scientists
- SLAC National Accelerator Laboratory