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Photoelectron Imaging of Anions Illustrated by 310 Nm Detachment of F−
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Imaging molecular geometry with electron momentum spectroscopy.

Enliang Wang1,2, Xu Shan1,2, Qiguo Tian1

  • 1Hefei National Laboratory for Physical Sciences at Microscale and Department of Modern Physics, University of Science and Technology of China, Hefei, Anhui, 230026, China.

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Electron momentum spectroscopy now reveals molecular geometry by analyzing orbital interference. This technique precisely measures interatomic distances, offering simultaneous insights into electron density and molecular structure.

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Area of Science:

  • Quantum chemistry
  • Molecular spectroscopy
  • Electron scattering physics

Background:

  • Electron momentum spectroscopy (EMS) images molecular orbital electron densities in momentum space.
  • Molecular geometry information is often obscured in EMS due to the single-centered nature of molecular orbital wavefunctions.

Purpose of the Study:

  • To develop a method for retrieving molecular geometry, specifically interatomic distances, from EMS data.
  • To demonstrate the simultaneous acquisition of electron density distributions and molecular geometry information.

Main Methods:

  • Analyzing multicenter interference effects in the ratios of electron momentum profiles between symmetric and anti-symmetric molecular orbitals.
  • Utilizing the sensitive dependence of oscillation periods on interatomic distances.

Main Results:

  • Successfully retrieved F-F distances in CF4 and O-O distances in CO2 with sub-Ångström precision.
  • Demonstrated simultaneous imaging of molecular orbital electron densities and molecular geometry in a single measurement.

Conclusions:

  • A novel approach using EMS enables precise determination of interatomic distances by exploiting multicenter interference.
  • This method provides a robust tool for molecular imaging, with potential for ultrafast molecular dynamics studies.