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Ligand exchange dynamics in aqueous solution studied with 2DIR spectroscopy.

Sungnam Park1, Minbiao Ji, Kelly J Gaffney

  • 1PULSE Institute for Ultrafast Energy Science, SLAC National Accelerator Laboratory, Stanford University, Stanford, California 94305, USA.

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We observed anion exchange in magnesium ion solutions using 2DIR spectroscopy. This study reveals the MgNCS(+) contact ion pair dissociation time constant is 52 ps.

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Area of Science:

  • Physical Chemistry
  • Solution Chemistry
  • Spectroscopy

Background:

  • Magnesium ions in concentrated solutions are coordinated by water, perchlorate, and thiocyanate.
  • Previous studies noted microsecond water ligand residence times for Mg(2+).
  • Anion exchange in the Mg(2+) first solvation shell was not experimentally observed before.

Purpose of the Study:

  • To investigate ligand exchange dynamics in concentrated Mg(2+) solutions.
  • To resolve interconversion between free thiocyanate and MgNCS(+) contact ion pairs.
  • To quantify dynamical distinctions between free and ion-paired anions.

Main Methods:

  • Time-resolved multidimensional vibrational spectroscopy (2DIR spectroscopy).
  • Utilizing the CN stretching frequency sensitivity of thiocyanate (SCN(-)) to ion pairing.
  • Analyzing orientational relaxation and spectral diffusion dynamics.

Main Results:

  • Successfully resolved interconversion between free SCN(-) and MgNCS(+) contact ion pairs.
  • Measured the MgNCS(+) contact ion pair dissociation time constant at 52 ± 10 ps.
  • Observed perchlorate-thiocyanate anion exchange in the Mg(2+) first solvation shell.

Conclusions:

  • This study provides the first experimental observation of anion exchange in the Mg(2+) cation's first solvent shell.
  • The observed dynamics are attributed to anion exchange within the solvation shell.
  • 2DIR spectroscopy effectively quantifies dynamical differences between free and ion-paired anions.