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Insights into Hydration Dynamics and Cooperative Interactions in Glycerol–Water Mixtures by Terahertz Dielectric Spectroscopy

  • Ali Charkhesht
    Ali Charkhesht
    Department of Physics and Center for Soft Matter and Biological Physics, Virginia Tech, Blacksburg, Virginia 24061, United States
  • Djamila Lou
    Djamila Lou
    Department of Physics and Center for Soft Matter and Biological Physics, Virginia Tech, Blacksburg, Virginia 24061, United States
    More by Djamila Lou
  • Ben Sindle
    Ben Sindle
    Department of Physics and Center for Soft Matter and Biological Physics, Virginia Tech, Blacksburg, Virginia 24061, United States
    More by Ben Sindle
  • Chengyuan Wen
    Chengyuan Wen
    Department of Physics and Center for Soft Matter and Biological Physics  and  Macromolecules Innovation Institute, Virginia Tech, Blacksburg, Virginia 24061, United States
  • Shengfeng Cheng
    Shengfeng Cheng
    Department of Physics and Center for Soft Matter and Biological Physics  and  Macromolecules Innovation Institute, Virginia Tech, Blacksburg, Virginia 24061, United States
  • , and 
  • Nguyen Q. Vinh*
    Nguyen Q. Vinh
    Department of Physics and Center for Soft Matter and Biological Physics, Virginia Tech, Blacksburg, Virginia 24061, United States
    *E-mail: [email protected]. Phone: 540-231-3158.
Cite this: J. Phys. Chem. B 2019, 123, 41, 8791–8799
Publication Date (Web):September 20, 2019
https://doi.org/10.1021/acs.jpcb.9b07021
Copyright © 2019 American Chemical Society

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    Abstract

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    We report relaxation dynamics of glycerol–water mixtures as probed by megahertz-to-terahertz dielectric spectroscopy in a frequency range from 50 MHz to 0.5 THz at room temperature. The dielectric relaxation spectra reveal several polarization processes at the molecular level with different time constants and dielectric strengths, providing an understanding of the hydrogen-bonding network in glycerol–water mixtures. We have determined the structure of hydration shells around glycerol molecules and the dynamics of bound water as a function of glycerol concentration in solutions using the Debye relaxation model. The experimental results show the existence of a critical glycerol concentration of ∼7.5 mol %, which is related to the number of water molecules in the hydration layer around a glycerol molecule. At higher glycerol concentrations, water molecules dispersed in a glycerol network become abundant and eventually dominate, and four distinct relaxation processes emerge in the mixtures. The relaxation dynamics and hydration structure in glycerol–water mixtures are further probed with molecular dynamics simulations, which confirm the physical picture revealed by the dielectric spectroscopy.

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