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Photoelectron Imaging of Anions Illustrated by 310 Nm Detachment of F−
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Published on: July 27, 2018

Intramolecular photoelectron diffraction in the gas phase.

K Ueda1, C Miron, E Plésiat

  • 1Institute of Multidisciplinary Research for Advanced Materials, Tohoku University, Sendai 980-8577, Japan.

The Journal of Chemical Physics
|October 5, 2013
PubMed
Summary

We observed intramolecular photoelectron diffraction during molecular photoionization, evidenced by oscillating cross-section ratios. This phenomenon reveals structural information about neutral and ionic molecules.

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Area of Science:

  • Quantum Chemistry
  • Molecular Spectroscopy
  • Atomic Physics

Background:

  • Photoionization is a fundamental process where a photon ejects an electron from an atom or molecule.
  • Vibrational excitation accompanying photoionization can provide insights into molecular dynamics and structure.
  • Intramolecular photoelectron diffraction has not been unambiguously observed in collective vibrational excitation.

Purpose of the Study:

  • To provide experimental and theoretical evidence of intramolecular photoelectron diffraction.
  • To investigate the role of collective vibrational excitation in photoionization.
  • To explore the potential of this phenomenon for determining molecular structure.

Main Methods:

  • High-resolution photoionization measurements of CF4, BF3, and CH4.
  • First-principles calculations using static-exchange and time-dependent density functional theory.
  • Analysis of vibrationally resolved photoionization cross-section ratios (v-ratios).

Main Results:

  • Pronounced oscillations in v-ratios were observed as a function of photon energy.
  • These oscillations serve as a fingerprint of electron diffraction by surrounding atoms.
  • Excellent agreement was found between theoretical calculations and experimental measurements.

Conclusions:

  • Intramolecular photoelectron diffraction is unambiguously demonstrated in collective vibrational excitation.
  • The observed v-ratios contain structural information about neutral molecules and their cations.
  • This method shows potential for structural determination of molecular species.