We here study pressure-induced amorphization and polyamorphic transitions in frozen bulk glycerol–water solutions experimentally.

Water is an intriguing substance. It shows sharp and reversible transitions between amorphous ices and, possibly, a liquid–liquid phase transition. Here, we discuss how this behavior is altered by the addition of solutes, such as salts and alcohols.

Computer simulations of glassy water–glycerol mixtures: molecular structure and density during the pressure-induced amorphous–amorphous (LDA–HDA) transformation.

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The nature of amorphous ices has been debated for more than 35 years. In essence, the question is whether they are related to ice polymorphs or to liquids. The fact that amorphous ices are traditionally prepared from crystalline ice via pressure-induced amorphization has made a clear distinction tricky. In this work, we vitrify liquid droplets through cooling at ≥106 K ⋅ s−1 and pressurize the glassy deposit. We observe a first order–like densification upon pressurization and recover a high-density glass. The two glasses resemble low- and high-density amorphous ice in terms of both structure and thermal properties. Vitrified water shows all features that have been reported for amorphous ices made from crystalline ice. The only difference is that the hyperquenched and pressurized deposit shows slightly different crystallization kinetics to ice I upon heating at ambient pressure. This implies a thermodynamically continuous connection of amorphous ices with liquids, not crystals.