A liquid-liquid transition in supercooled aqueous solution related to the HDA-LDA transition

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Science  09 Mar 2018:
Vol. 359, Issue 6380, pp. 1127-1131
DOI: 10.1126/science.aao7049

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Unmasking supercooled water transitions

The unusual thermodynamic properties of water suggest that when supercooled, a second critical point should exist between two liquid phases that differ in density. Pure water crystallizes before such conditions can be reached. Woutersen et al. studied hydrazinium trifluoroacetate solutions that have similar hydrogen bonding to that of water. They observed a liquid-liquid transition near 190 K by using infrared spectroscopy and calorimetry. The liquid states were analogous to the predicted high- and low-density amorphous phases of water.

Science, this issue p. 1127


Simulations and theory suggest that the thermodynamic anomalies of water may be related to a phase transition between two supercooled liquid states, but so far this phase transition has not been observed experimentally because of preemptive ice crystallization. We used calorimetry, infrared spectroscopy, and molecular dynamics simulations to investigate a water-rich hydrazinium trifluoroacetate solution in which the local hydrogen bond structure surrounding a water molecule resembles that in neat water at elevated pressure, but which does not crystallize upon cooling. Instead, this solution underwent a sharp, reversible phase transition between two homogeneous liquid states. The hydrogen-bond structures of these two states are similar to those established for high- and low-density amorphous (HDA and LDA) water. Such structural similarity supports theories that predict a similar sharp transition in pure water under pressure if ice crystallization could be suppressed.

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