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Generation and Control of Electrohydrodynamic Flows in Aqueous Electrolyte Solutions
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Local Electric Fields in Aqueous Electrolytes.

Chad I Drexler, Olivia M Cracchiolo1, Ryan L Myers

  • 1Department of Chemistry and Biochemistry, University of Notre Dame, Notre Dame, Indiana 46556, United States.

The Journal of Physical Chemistry. B
|July 27, 2021
PubMed
Summary
This summary is machine-generated.

Salt ions in aqueous solutions cause unexpected low-frequency shifts in molecular vibrations, contrary to established theories. Ion hydration and type significantly influence these vibrational Stark shifts.

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Area of Science:

  • Physical Chemistry
  • Spectroscopy
  • Solution Chemistry

Background:

  • Vibrational spectroscopy probes molecular structure and dynamics.
  • Onsager's reaction field theory predicts blue-shifts in response to electric fields.
  • The influence of salt ions on vibrational spectra in solution is complex.

Purpose of the Study:

  • To investigate vibrational Stark shifts in organic molecules with carbonyl and nitrile groups in aqueous salt solutions.
  • To understand the impact of ion hydration and type on these shifts.
  • To reconcile experimental observations with theoretical predictions.

Main Methods:

  • Experimental vibrational spectroscopy of organic molecules in aqueous salt solutions.
  • Molecular dynamics simulations to model ion-solvent-solute interactions.
  • Analysis of vibrational resonance frequency shifts.

Main Results:

  • Observed low-frequency (red) shifts in vibrational resonances upon salt addition, contradicting Onsager's theory.
  • Ion-specific effects: well-hydrated cations (Mg2+, Li+) strongly affected carbonyls; poorly hydrated cations (Cs+) affected nitriles.
  • Anion effects: I- induced larger shifts than Cl-.
  • Simulations revealed cation-anion pair formation around the probe, generating an electric field consistent with Hofmeister series trends.

Conclusions:

  • The study demonstrates "anti-Onsager" Stark shifts in vibrational spectroscopy.
  • Ion-pairing and Hofmeister series effects explain the observed spectral shifts.
  • These findings are relevant for both vibrational spectroscopy and fluorescence measurements in ionic solutions.