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Recovery of High-Energy Photoelectron Circular Dichroism through Fano Interference.

G Hartmann1, M Ilchen1,2, Ph Schmidt1

  • 1Institut für Physik und CINSaT, Universität Kassel, Heinrich-Plett-Strasse 40, 34132 Kassel, Germany.

Physical Review Letters
|September 7, 2019
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Summary

Photoelectron circular dichroism (PECD) was observed for fast electrons, challenging the notion that only low-energy electrons probe molecular chirality. This study reveals PECD in high-energy photoelectrons due to resonant Auger decay and Fano interference.

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Area of Science:

  • Atomic and Molecular Physics
  • Quantum Chemistry
  • Spectroscopy

Background:

  • Photoelectron Circular Dichroism (PECD) typically requires low kinetic energy electrons to probe molecular chirality.
  • The magnitude of PECD is generally linked to the photoelectron's ability to interact with the molecule's chiral structure.

Purpose of the Study:

  • To investigate the occurrence of substantial PECD for high-energy photoelectrons.
  • To explore the underlying mechanisms responsible for PECD in fast photoelectrons.

Main Methods:

  • Utilizing participator resonant Auger decay following O 1s excitation of methyloxirane.
  • Analyzing Fano interference between direct and resonant photoionization pathways for high-energy photoelectrons (>500 eV).

Main Results:

  • Demonstrated significant PECD for very fast photoelectrons (above 500 eV).
  • Observed anomalous dispersion in the dichroic parameter, including a sign change across the resonance.
  • Attributed the effect to Fano interference between direct and resonant photoionization pathways.

Conclusions:

  • High-energy photoelectrons can exhibit substantial PECD, expanding the applicability of this technique.
  • Fano interference plays a crucial role in generating PECD even when individual pathways are weak.
  • The observed anomalous dispersion is analogous to the Cotton effect in X-ray spectroscopy.