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Alternative Pathway to Double-Core-Hole States.

Iyas Ismail1, Anthony Ferté1, Francis Penent1

  • 1Sorbonne Université, CNRS, Laboratoire de Chimie Physique-Matière et Rayonnement, LCPMR, F-75005 Paris Cedex 05, France.

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Researchers explored excited double-core-hole states in water molecules using x-ray photons. They identified two distinct formation pathways, revealing a new route involving valence electron shake-up during core ionization.

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Area of Science:

  • Atomic and Molecular Physics
  • Quantum Chemistry
  • X-ray Spectroscopy

Background:

  • Core-hole states in molecules are crucial for understanding electronic structure and chemical dynamics.
  • Sequential photoionization processes can lead to complex excited states.
  • Water molecules are fundamental systems for studying electronic processes.

Purpose of the Study:

  • To investigate the formation pathways of excited double-core-hole states in isolated water molecules.
  • To differentiate between direct core-ionization followed by excitation and a novel pathway involving valence electron shake-up.
  • To leverage the unique capabilities of x-ray free-electron lasers (XFELs) for studying ultrafast electronic dynamics.

Main Methods:

  • Utilizing intense, ultrashort, and tunable x-ray pulses from an x-ray free-electron laser (XFEL).
  • Performing high-resolution spectroscopy to probe the electronic states of water molecules.
  • Analyzing spectral features to distinguish between different ionization and excitation pathways.

Main Results:

  • Experimental evidence for excited double-core-hole states in water molecules was obtained.
  • Two distinct pathways leading to these states were identified and characterized.
  • A previously unconsidered pathway involving simultaneous core ionization and valence electron shake-up was confirmed.
  • The results highlight the sensitivity of XFELs in resolving complex photoionization dynamics.

Conclusions:

  • The study elucidates the competing mechanisms for generating double-core-hole states in water.
  • The discovery of the alternative pathway provides new insights into electron correlation effects in core-excited molecules.
  • This work demonstrates the power of XFELs for advanced molecular spectroscopy and probing fundamental electronic processes.