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

Sander Woutersen, Bernd Ensing, Michiel Hilbers, Zuofeng Zhao, Charles Angell

Research output: Contribution to journalArticle

22 Citations (Scopus)

Abstract

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.

Original languageEnglish (US)
Pages (from-to)1127-1131
Number of pages5
JournalScience
Volume359
Issue number6380
DOIs
StatePublished - Mar 9 2018

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aqueous solutions
liquids
water
pressure ice
crystallization
hydrogen bonds
ice
heat measurement
simulation
infrared spectroscopy
anomalies
molecular dynamics
cooling
thermodynamics
molecules

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Cite this

A liquid-liquid transition in supercooled aqueous solution related to the HDA-LDA transition. / Woutersen, Sander; Ensing, Bernd; Hilbers, Michiel; Zhao, Zuofeng; Angell, Charles.

In: Science, Vol. 359, No. 6380, 09.03.2018, p. 1127-1131.

Research output: Contribution to journalArticle

Woutersen, Sander ; Ensing, Bernd ; Hilbers, Michiel ; Zhao, Zuofeng ; Angell, Charles. / A liquid-liquid transition in supercooled aqueous solution related to the HDA-LDA transition. In: Science. 2018 ; Vol. 359, No. 6380. pp. 1127-1131.
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