Ultrafast X-ray probing of water structure below the homogeneous ice nucleation temperature

Sellberg, J, Huang, C, McQueen, T and Martin, A 2014, 'Ultrafast X-ray probing of water structure below the homogeneous ice nucleation temperature', Nature, vol. 510, no. 7505, pp. 381-384.


Document type: Journal Article
Collection: Journal Articles

Title Ultrafast X-ray probing of water structure below the homogeneous ice nucleation temperature
Author(s) Sellberg, J
Huang, C
McQueen, T
Martin, A
Year 2014
Journal name Nature
Volume number 510
Issue number 7505
Start page 381
End page 384
Total pages 4
Publisher Nature Publishing Group
Abstract Water has a number of anomalous physical properties, and some of these become drastically enhanced on supercooling below the freezing point. Particular interest has focused on thermodynamic response functions that can be described using a normal component and an anomalous component that seems to diverge at about 228 kelvin (refs 1,2,3 ). This has prompted debate about conflicting theories4,5,6,7,8,9,10,11,12 that aim to explain many of the anomalous thermodynamic properties of water. One popular theory attributes the divergence to a phase transition between two forms of liquid water occurring in the no mans land that lies below the homogeneous ice nucleation temperature (TH) at approximately 232 kelvin13 and above about 160 kelvin14, and where rapid ice crystallization has prevented any measurements of the bulk liquid phase. In fact, the reliable determination of the structure of liquid water typically requires temperatures above about 250 kelvin2,15. Water crystallization has been inhibited by using nanoconfinement16, nanodroplets17 and association with biomolecules16 to give liquid samples at temperatures below TH, but such measurements rely on nanoscopic volumes of water where the interaction with the confining surfaces makes the relevance to bulk water unclear18. Here we demonstrate that femtosecond X-ray laser pulses can be used to probe the structure of liquid water in micrometre-sized droplets that have been evaporatively cooled 19,20,21 below TH. We find experimental evidence for the existence of metastable bulk liquid water down to temperatures of  kelvin in the previously largely unexplored no mans land. We observe a continuous and accelerating increase in structural ordering on supercooling to approximately 229 kelvin, where the number of droplets containing ice crystals increases rapidly. But a few droplets remain liquid for about a millisecond even at this temperature. The hope now is that these observations and our detailed structural data will hel
Subject Condensed Matter Imaging
DOI - identifier 10.1038/nature13266
Copyright notice © 2014 Macmillan Publishers Limited. All rights reserved
ISSN 0028-0836
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