Real-Space Imaging of the Electron-Pair Density Hole in Molecular Auger-Meitner Decay

Authors

• Mats Simmermacher, University of Oxford
• Nathan Goff, Brown University
• Andres Moreno Carrascosa, University of Oxford
• Elke Fasshauer, University of Tübingen
• Thomas Northey, University of Oxford
• Lingyu Ma, Brown University
• Haiwang Yong, University of California San Diego
• Brian Stankus, Western Connecticut State University
• Asami Odate, Brown University
• Xuan Xu, Brown University
• Wenping Du, Brown University
• Kyle Acheson, University of Oxford
• Joseph C. Cooper, University of Oxford
• Daniel Ratner, Old Dominion UniversityFollow
• Mengning Liang, SLAC National Accelerator Laboratory
• Ruaridh Forbes, University of California, Davis
• Michael P. Minitti, SLAC National Accelerator Laboratory
• Adam Kirrander, University of Oxford
• Peter M. Weber, Brown University

Document Type

Article

Publication Date

2026

DOI

10.1038/s41567-026-03363-8

Publication Title

Nature Physics

Volume

Advance online publication

Pages

10 pp.

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.

Rights

© 2026 The Authors.

This article is licensed under a Creative Commons Attribution 4.0 International (CC BY 4.0) License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original authors and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder.

Data Availability

Article states: "The source data for Figs. 2 and 3 and Extended Data Figs. 1–3 are available via figshare at https://doi.org/10.6084/m9.figshare.32316573 (ref. 51). The repository also provides MOLPRO input and output files, as well as the calculated scattering signals of the individuals states that enter the kinetic model of the Auger–Meitner decay. Further data are available from the corresponding authors upon reasonable request."

Original Publication Citation

Simmermacher, M., Goff, N., Carrascosa, A. M., Fasshauer, E., Northey, T., Ma, L. Y., Yong, H. W., Stankus, B., Odate, A., Xu, X., Du, W. P., Acheson, K., Cooper, J. C., Ratner, D., Liang, M. N., Forbes, R., Minitti, M. P., Kirrander, A., & Weber, P. M. (2026). Real-space imaging of the electron-pair density hole in molecular Auger-Meitner decay. Nature Physics. Advance online publication. https://doi.org/10.1038/s41567-026-03363-8

ORCID

0000-0002-5747-7323 (Ratner)

Repository Citation

Simmermacher, Mats; Goff, Nathan; Moreno Carrascosa, Andres; Fasshauer, Elke; Northey, Thomas; Ma, Lingyu; Yong, Haiwang; Stankus, Brian; Odate, Asami; Xu, Xuan; Du, Wenping; Acheson, Kyle; Cooper, Joseph C.; Ratner, Daniel; Liang, Mengning; Forbes, Ruaridh; Minitti, Michael P.; Kirrander, Adam; and Weber, Peter M., "Real-Space Imaging of the Electron-Pair Density Hole in Molecular Auger-Meitner Decay" (2026). Physics Faculty Publications. 1060.
https://digitalcommons.odu.edu/physics_fac_pubs/1060