Year: 2026
Type: article
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.
Source: Nature Physics
Authors: Mats Simmermacher, Nathan Goff, Andres Moreno Carrascosa, Elke Fasshauer, Thomas Northey, Lingyu Ma, Haiwang Yong, Brian Stankus, Asami Odate, Xuan Xu, Wenpeng Du, Kyle Acheson, Joseph C. Cooper, Daniel Ratner, Mengning Liang, Ruaridh Forbes, Michael P. Minitti, Adam Kirrander, Peter M. Weber
Institutions: University of Oxford, Brown University, University of Tübingen, University of California San Diego, Western Connecticut State University, University of Southampton, National Research Council Canada, SLAC National Accelerator Laboratory, Thomas Jefferson National Accelerator Facility, Linac Coherent Light Source, Old Dominion University, University of California, Davis
Language: English
Subfield: Radiation
Field: Physics and Astronomy
Domain: Physical Sciences
Open Access status: hybrid
Estimated APC paid: $12,690
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
Awards: G1229526393, G1286251239, G1384715801, Vollständige Quantendynamik des interPartikel CoulombElektroneneinfangs, G1538770391, G1568668747, G17040919, A New Effect in Ultrafast X-ray Scattering, G2371548206, G262532246, G2824785710, G2917895714, G303061748, Electron Densities and Electron Correlations by X-Ray Scattering, G389884619, G4037216677, G4101533273, G4235786860, A Joined-up Approach to New Molecular Simulation Technologies to Harness Ultrafast Photochemistry, G4654690619, G4711507462, G473396326, G4775162344, G495301720, G498139845, High-Repetition Rate X-ray Detector for the Coherent X-ray Imaging Instrument at LCLS, A Universal Approach for Solving Real-World Problems Using Quantum Dynamics: Coherent States for Molecular Simulations (COSMOS), G515206079, G5570207115, G601061201, G6017181652, G6550344761, G7283024673, G7619220232, G7719906390, STRUCTURAL MOLECULAR DYNAMICS USING ULTRAFAST GAS X-RAY SCATTERING, Next Generation Experiment and Theory for Photoelectron Spectroscopy, G8382000481, G8570346810, G8925327636, G911061179, G916731797, G969889393
OpenAlex ID: W7166689329