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From Molecules to Materials: Engineering New Ionic Liquid Crystals Through Halogen Bonding
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Electronic predissociation in rare gas-dihalogen complexes.

Nicholas Zeigler1, Camille Makarem1, Jie Wei1

  • 1Department of Chemistry and Institute of Materials Science and Engineering, Washington University in St. Louis, St. Louis, Missouri 63130, USA.

The Journal of Chemical Physics
|January 22, 2021
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Summary

Electronic predissociation (EP) was investigated in rare gas-dihalogen complexes. Definitive evidence for EP was found only in Ar⋯I2 complexes, occurring on short timescales and from asymmetric geometries.

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Area of Science:

  • Chemical Physics
  • Molecular Dynamics
  • Spectroscopy

Background:

  • Rare gas-dihalogen complexes (Rg⋯X2) are model systems for studying energy transfer and dissociation dynamics.
  • Electronic predissociation (EP) is a non-radiative decay process that can compete with other dissociation pathways like vibrational predissociation.
  • Understanding EP is crucial for elucidating the complex dissociation mechanisms in weakly bound molecular systems.

Purpose of the Study:

  • To investigate the role of electronic predissociation (EP) in the dissociation dynamics of rare gas-dihalogen complexes (Rg⋯X2).
  • To determine the specific conditions and geometries under which EP occurs in these complexes.
  • To compare the contribution of EP with vibrational predissociation.

Main Methods:

  • Ion time-of-flight velocity-map imaging was employed to probe the dissociation fragments.
  • Complexes were prepared in the B electronic state with varying vibrational excitation (ν') of the dihalogen molecule.
  • Atomic iodine (I) and bromine (Br) fragments from EP were analyzed.

Main Results:

  • Definitive evidence for EP was observed exclusively in argon⋯iodine (Ar⋯I2) complexes.
  • EP occurred across all investigated T-shaped intermolecular levels of Ar⋯I2 with specific vibrational excitations (ν' = 12-22, 24, 25).
  • EP in Ar⋯I2 occurs on timescales faster than rotational periods and suggests dissociation from asymmetric geometries, indicating prior intramolecular vibrational redistribution.

Conclusions:

  • Electronic predissociation is a significant, albeit specific, dissociation pathway in certain rare gas-dihalogen complexes.
  • The findings highlight the importance of intramolecular vibrational redistribution preceding EP in Ar⋯I2.
  • The study provides detailed insights into the competing dissociation mechanisms in Rg⋯X2 systems.