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<p>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.</p>

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Real-space imaging of the electron-pair density hole in molecular Auger–Meitner decay

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年6月30日

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  • 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

摘要

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.