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Area of Science:

  • Quantum mechanics
  • Molecular physics
  • Atomic and molecular collisions

Background:

  • Electronic core levels in molecules are typically localized to a single atomic site.
  • The behavior of core holes in symmetric molecules during single-photon ionization, specifically localization versus delocalization, is a long-standing quantum mechanical question.

Purpose of the Study:

  • To experimentally investigate core-hole localization and delocalization in symmetric molecules.
  • To demonstrate control over distinct molecular fragmentation pathways based on core-hole behavior.
  • To probe quantum pathway entanglement in core-ionized carbon disulfide (CS2).

Main Methods:

  • Joint experimental and theoretical study of core-ionized carbon disulfide (CS2).
  • Single-photon ionization experiments.
  • Measurement of photoelectron angular distributions within the molecular frame.
  • Theoretical modeling of quantum pathways.

Main Results:

  • Demonstrated experimental control over core-hole localization versus delocalization in CS2.
  • Identified distinct molecular fragmentation pathways corresponding to localized and delocalized core holes.
  • Probed entanglement and disentanglement of quantum pathways during dissociation.

Conclusions:

  • It is experimentally possible to select pathways where the core hole is localized on one sulfur atom or delocalized over two.
  • Photoelectron angular distribution measurements provide direct insight into quantum pathway entanglement in molecular dissociation.
  • This study offers a new perspective on fundamental quantum mechanical principles in molecular systems.