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Time-resolved nuclear dynamics in bound and dissociating acetylene.

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Structural Dynamics (Melville, N.Y.)
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Summary

Investigating acetylene molecular ions using ultrafast laser pulses revealed vibrations in bound acetylene cations and enhanced ionization in dissociating dications. This study sheds light on molecular dynamics and ionization mechanisms.

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Area of Science:

  • Molecular Physics
  • Quantum Chemistry
  • Ultrafast Spectroscopy

Background:

  • Understanding molecular dynamics is crucial for controlling chemical reactions.
  • Acetylene molecular ions are fundamental systems for studying bond breaking and formation.
  • Time-resolved experiments provide insights into ultrafast processes.

Purpose of the Study:

  • To investigate nuclear dynamics in bound and dissociating acetylene molecular ions.
  • To probe molecular vibrations and ionization mechanisms using time-resolved reaction microscopy.
  • To elucidate the role of electron dynamics in molecular fragmentation.

Main Methods:

  • Time-resolved reaction microscopy with a pair of few-cycle laser pulses.
  • Production of vibrating bound acetylene cations and dissociating dications.
  • Probing nuclear dynamics via ionization to higher charge states and Coulomb explosion.
  • Semi-classical on-the-fly dynamics simulations for time-dependent ionization processes.

Main Results:

  • Observed CC-bond vibrations in acetylene (HCCH) and vinylidene (CCHH) cations with ~26 fs periodicity.
  • Found enhanced ionization along CH- and CC-bonds in dissociating dications between 10 fs and 40 fs.
  • Simulations revealed underlying mechanisms of time-dependent ionization.

Conclusions:

  • Acetylene molecular ions exhibit distinct dynamical behaviors in bound and dissociating states.
  • Ultrafast laser pulses can precisely control and probe molecular ion dynamics.
  • The study provides a detailed understanding of ionization processes in molecular fragmentation.