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Cooperatively enhanced ionic hydrogen bonds in Cl-(CH3OH)(1-3)Ar clusters.

Jordan P Beck1, James M Lisy

  • 1Department of Chemistry, University of Illinois at Urbana−Champaign, Urbana, Illinois 61801, USA.

The Journal of Physical Chemistry. A
|August 21, 2010
PubMed
Summary

Infrared predissociation spectroscopy reveals strong hydrogen bonds in Cl−(CH3OH)nAr clusters. These ionic hydrogen bonds are enhanced by multiple methanol shells, creating unique structures.

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Area of Science:

  • Physical Chemistry
  • Spectroscopy
  • Computational Chemistry

Background:

  • Investigating hydrogen bonding in ionic clusters provides insights into solvation and chemical interactions.
  • Understanding the influence of solvent shells on hydrogen bond strength is crucial for molecular recognition and reaction mechanisms.

Purpose of the Study:

  • To characterize the hydrogen bonding in mass-selected chlorine anion-methanol-argon clusters (Cl−(CH3OH)nAr, n=1-3).
  • To explore the cooperative effects of multiple methanol shells on the Cl−···methanol hydrogen bond strength.
  • To develop and assess computational methods for accurately predicting hydrogen bond frequencies in complex systems.

Main Methods:

  • Infrared predissociation (IRPD) spectroscopy was employed to probe the vibrational modes of Cl−(CH3OH)nAr clusters.
  • The use of methanol-d1 (CH3OD) aided in distinguishing between CH and OH stretching frequencies.
  • A simple computational approach was developed to better approximate hydrogen bond frequencies, as harmonic ab initio methods proved inadequate.

Main Results:

  • IRPD spectra showed intense features at lower frequencies than CH stretches for Cl−(CH3OH)2-3Ar, indicating very strong hydrogen bonds.
  • The Cl−···methanol ionic hydrogen bond strength was found to be cooperatively enhanced by the presence of second and third methanol shells.
  • The strongest hydrogen bond was observed in Cl−(CH3OH)3Ar at 2733 cm−1, a significant red-shift of -948 cm−1 from neutral methanol.

Conclusions:

  • Multiple methanol shells significantly strengthen the ionic hydrogen bond between Cl− and methanol.
  • The experimental method efficiently traps high-energy isomers of Cl− interacting with cold methanol-argon clusters.
  • Advanced computational methods are necessary to accurately model the strong hydrogen bonding observed in these ionic clusters.