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Ultrafast Molecular Three-Electron Auger Decay.

Raimund Feifel1,2, John H D Eland1,3, Richard J Squibb1,2

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Three-electron Auger decay, a rare process, was observed in CH3F. This ultrafast decay of double inner-valence holes occurs much faster than previously thought possible.

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Area of Science:

  • Atomic and Molecular Physics
  • Quantum Chemistry
  • Ultrafast Spectroscopy

Background:

  • Three-electron Auger decay is a theoretically predicted but experimentally elusive atomic process.
  • This decay involves two outer-shell electrons filling an inner-shell vacancy, emitting one Auger electron.
  • Such transitions are typically forbidden by selection rules, leading to very long decay lifetimes.

Purpose of the Study:

  • To provide theoretical predictions and experimental evidence for three-electron Auger decay.
  • To investigate the decay mechanism of double inner-valence-hole states in molecules.
  • To determine the decay lifetime of this exotic process.

Main Methods:

  • High-resolution photoelectron spectroscopy was used to probe the electronic states.
  • Time-dependent density-functional theory (TD-DFT) was employed for theoretical calculations.
  • Analysis of spectral features to identify and characterize the three-electron Auger decay.

Main Results:

  • Direct experimental evidence for a few-femtosecond three-electron Auger decay of a double inner-valence-hole state in CH3F was obtained.
  • The observed decay lifetime is significantly shorter than expected for forbidden transitions.
  • Theoretical predictions align with the experimental observations.

Conclusions:

  • Double inner-valence vacancies in molecules can decay exclusively via ultrafast three-electron Auger processes.
  • This phenomenon challenges existing selection rules for atomic and molecular decay.
  • The study predicts that this ultrafast decay mechanism is widespread in molecules.