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Reactive and Inelastic Channels in the Ca*···FCH3 Transition State: A Simple Branching Mechanism.

M Briant, E Gloaguen, A Beswick1

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The Journal of Physical Chemistry. A
|March 14, 2015
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This summary is machine-generated.

Excited calcium atoms react with fluoromethane (CH3F) via direct dissociation or forming calcium fluoride (CaF*). Both pathways are fast and nearly equal in intensity, driven by excited potential surfaces.

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Area of Science:

  • Chemical Physics
  • Molecular Dynamics
  • Spectroscopy

Background:

  • Understanding excited state dynamics is crucial for controlling chemical reactions.
  • Calcium atom interactions with small molecules are fundamental in astrochemistry and materials science.

Purpose of the Study:

  • Investigate the excited state dynamics of calcium-fluoromethane (Ca···CH3F) complexes.
  • Elucidate the competitive dissociation and reaction pathways following laser excitation.

Main Methods:

  • Preparation of Ca···CH3F complexes using supersonic expansion and laser ablation.
  • Tunable laser excitation to probe specific molecular states.
  • Velocity map imaging and time-of-flight mass spectrometry to analyze fragment recoil and alignment.

Main Results:

  • Observed two competitive channels: direct dissociation and reactive channel forming CaF* + CH3.
  • Both dissociation and reaction processes were found to be quasi-direct and of comparable intensity.
  • Fragment analysis revealed specific excited states leading to these outcomes.

Conclusions:

  • The electronically excited potential surface of Ca*···FCH3 initiates fast predissociation.
  • This predissociation leads to two repulsive surfaces, resulting in either Ca (1P1) + CH3F or CaF((2)Δ) + CH3 products.
  • The study provides insights into the ultrafast dynamics of atom-molecule interactions.