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Selective Bond Breaking in CO_{2}^{2+} Induced by Photoelectron Recoil.

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Photoelectron momentum dictates bond breaking in carbon dioxide (CO2) after ionization. This leads to asymmetric molecular dissociation and a significant nondipole effect in fragment emission, impacting molecular dynamics research.

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Area of Science:

  • Atomic and Molecular Physics
  • Chemical Physics
  • Quantum Chemistry

Background:

  • Core ionization of carbon dioxide (CO2) often results in Auger-Meitner decay, forming a dication that can dissociate.
  • Understanding the fragmentation pathways of molecules after photoionization is crucial for various fields.

Purpose of the Study:

  • To experimentally investigate the role of photoelectron recoil momentum in CO2 dication dissociation.
  • To quantify the bond cleavage asymmetry and its dependence on photoelectron emission direction.
  • To explore the resulting nondipole effects in molecular fragmentation.

Main Methods:

  • High-energy (20 keV) photon impact on CO2 molecules.
  • Coincidence measurements of photoelectrons and fragment ions (CO+ and O+).
  • Analysis of fragment momentum correlation to determine bond dissociation pathways.

Main Results:

  • Demonstrated that photoelectron recoil momentum directs which CO2 bond breaks.
  • Observed up to 25% asymmetry in bond cleavage, correlated with photoelectron emission direction.
  • Identified a significant nondipole effect in the laboratory frame, with O+ fragments preferentially emitted opposite to light propagation.

Conclusions:

  • The photoelectron's momentum is a key factor controlling dissociation pathways in ionized CO2.
  • This momentum-dependent dissociation leads to observable asymmetries and nondipole effects in fragment emission.
  • Findings provide new insights into electron-ion-ion coincidence spectroscopy and molecular fragmentation dynamics.