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Intermolecular Interactions at the Silica-Liquid Interface Modulate the Fermi Resonance Coupling in Surface Methanol.

Thomas T Bui1, Luis A Colón1, Luis Velarde1

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Vibrational sum-frequency generation spectroscopy revealed how acetonitrile influences methanol's Fermi resonance at the silica-liquid interface. Diluting methanol with acetonitrile significantly enhances this Fermi resonance, indicating tunable molecular interactions.

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Area of Science:

  • Surface science
  • Spectroscopy
  • Physical chemistry

Background:

  • Understanding solid/liquid interfaces is crucial in various chemical and physical processes.
  • Vibrational sum-frequency generation (vSFG) spectroscopy is a powerful technique for probing interfacial molecular structures and dynamics.

Purpose of the Study:

  • To investigate the effect of binary solvent mixtures on the vibrational properties of molecules at a buried interface.
  • To quantify the influence of acetonitrile on the Fermi resonance of methanol at the hydrophilic fused silica/liquid interface.

Main Methods:

  • Utilized vibrational sum-frequency generation (vSFG) spectroscopy to study the fused silica/binary solvent interface.
  • Analyzed the Fermi resonance peak suppression and intensity changes in vSFG spectra with varying acetonitrile (MeCN) and methanol (MeOH) concentrations.
  • Quantified Fermi resonance coupling using the Fermi resonance coupling coefficient (W) and the intensity ratio (R).

Main Results:

  • High methanol concentrations suppressed the Fermi resonance peak in vSFG spectra.
  • As methanol was diluted with perdeuterated acetonitrile, the Fermi resonance intensity progressively increased.
  • Calculated Fermi resonance coupling coefficient (W) increased from 10 ± 10 cm⁻¹ to 46 ± 4 cm⁻¹ as MeOH mole fraction decreased from 1.0 to 0.1.
  • Intensity ratio (R) increased from 0.01 ± 0.02 to 0.43 ± 0.16 over the same concentration range.

Conclusions:

  • Solvation by acetonitrile effectively tunes the Fermi coupling of methanol vibrations at the silica/liquid interface.
  • The study demonstrates a method for controlling and quantifying interfacial molecular vibrational behavior through solvent composition.
  • Findings provide insights into molecular interactions at buried interfaces, relevant for catalysis, materials science, and nanotechnology.