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Glass Polymorphism in Hyperquenched Aqueous LiCl Solutions.

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Dilute LiCl-H2O solutions exhibit distinct high-density and low-density glass polymorphs below 4.3 mol% LiCl. Lithium chloride (LiCl) primarily impacts the low-density form, influencing its structure and dynamics.

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Area of Science:

  • Physical Chemistry
  • Materials Science
  • Condensed Matter Physics

Background:

  • Understanding glass polymorphism is crucial for materials science.
  • Dilute aqueous solutions, like LiCl-H2O, can exhibit different glass structures.
  • Previous studies suggested structural heterogeneity in LiCl-H2O glasses.

Purpose of the Study:

  • To investigate the glass polymorphism of dilute LiCl-H2O solutions.
  • To characterize the high-density and low-density glass states.
  • To determine the influence of LiCl concentration on glass properties.

Main Methods:

  • Vitrification of LiCl-H2O solutions using hyperquenching (∼10^6 K s^-1).
  • High-pressure annealing to transform glasses to their high-density state.
  • Ex situ characterization via isobaric heating, X-ray diffraction, and differential scanning calorimetry.

Main Results:

  • Distinct high-density and low-density glass polymorphs observed for LiCl concentrations ≤ 4.3 mol%.
  • A polyamorphic transition and two distinct glass transition temperatures (Tg,1 and Tg,2) identified.
  • LiCl significantly impacts the low-density glass, altering structure, lowering Tg,1, and changing relaxation dynamics.

Conclusions:

  • A transition from water-dominated to solute-dominated behavior occurs between 4.3 and 5.8 mol% LiCl.
  • LiCl is homogeneously distributed in the low-density glass, contradicting previous heterogeneity claims.
  • Higher cooling rates in this study likely explain the observed homogeneous distribution compared to prior work.