Abstract
Supercooled water may offer clues to the anomalous properties of its normal liquid state1. The supercooled state also shows anomalous thermodynamic and transport properties at low temperatures2,3,4. Although there are several theoretical explanations for this behaviour, no consensus has emerged1,2,5,6,7,8,9,10,11,12. Some theories preclude the existence of the supercooled liquid below an apparent thermodynamic singularity at 228?K (refs 2, 7, 9); others are consistent with a continuous region of metastability from the melting point at 273?K to the glass transition temperature at 136?K (refs 6, 8, 13). But the data needed to distinguish between these possibilities have not yet been forthcoming. Here we determine the diffusivity of amorphous ice by studying isotope intermixing in films less than 500 nanometres thick. The magnitude and temperature dependence of the diffusivity is consistent with the idea that the amorphous solid water melts into a deeply metastable extension of normal liquid water before crystallizing at 160?K. This argues against the idea of a singularity in the supercooled regime at ambient pressure.
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Acknowledgements
We thank C. A. Angell, H. E. Stanley, R. J. Speedy, P. Debenedetti, E. Mayer, S. Sastry, P. Poole, F. Sciortino, F. Starr, H. D. Lüdemann and A. Geiger for discussions. This work was supported by the US Department of Energy, Office of Basic Energy Sciences, Chemical Sciences Division. Pacific Northwest National Laboratory is operated for the US Department of Energy by Battelle.
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Smith, R., Kay, B. The existence of supercooled liquid water at 150?K. Nature 398, 788–791 (1999). https://doi.org/10.1038/19725
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DOI: https://doi.org/10.1038/19725
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