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Glass polymorphism and liquid-liquid phase transition in aqueous solutions: experiments and computer simulations
Johannes Bachler1, Philip H Handle, Nicolas Giovambattista
1Institute of Physical Chemistry, University of Innsbruck, A-6020 Innsbruck, Austria. thomas.loerting@uibk.ac.at.
Physical Chemistry Chemical Physics : PCCP
|September 27, 2019
Summary
Water
Area of Science:
- Physical Chemistry
- Materials Science
- Thermodynamics
Background:
- Water exhibits unique amorphous ice forms, known as glass polymorphism or polyamorphism.
- This phenomenon is linked to a potential first-order liquid-liquid phase transition (LLPT) in supercooled water.
- Amorphous ice is the stable phase during this transition.
Purpose of the Study:
- To review experimental and computational studies investigating LLPT and polyamorphism in aqueous solutions.
- To examine solutions containing salts (NaCl, LiCl) and alcohols (glycerol).
- To explore less-studied systems like protein and hydrophobic solutions.
Main Methods:
- Review of existing experimental data.
- Analysis of computer simulations.
- Presentation of original experimental results.
Main Results:
- All studied solutions exhibit polyamorphism and LLPT in dilute, sub-eutectic mixtures.
- Isocompositional transitions occur in alcohol solutions but not ionic solutions.
- Differences arise from water's interaction with solutes: alcohols allow flexible configurations, while ions enforce high-density hydration shells, hindering transitions near ions.
Conclusions:
- Polyamorphism and LLPT in aqueous solutions are influenced by solute type.
- Reinterpretation of past studies can unify understanding.
- Key challenges remain in comparing experimental and simulation results, with eleven open questions identified.
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