The mechanisms for pressure-induced amorphization of ice Ih

J. S. Tse (), D. D. Klug, C. A. Tulk, I. Swainson, E. C. Svensson, C.-K. Loong, V. Shpakov, V. R. Belosludov, R. V. Belosludov and Y. Kawazoe
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J. S. Tse: Steacie Institute for Molecular Sciences, National Research Council of Canada
D. D. Klug: Steacie Institute for Molecular Sciences, National Research Council of Canada
C. A. Tulk: Steacie Institute for Molecular Sciences, National Research Council of Canada
I. Swainson: Steacie Institute for Molecular Sciences, National Research Council of Canada
E. C. Svensson: Steacie Institute for Molecular Sciences, National Research Council of Canada
C.-K. Loong: Argonne National Laboratory
V. Shpakov: Inorganic Chemistry Institute, Russian Academy of Sciences
V. R. Belosludov: Inorganic Chemistry Institute, Russian Academy of Sciences
R. V. Belosludov: Institute for Materials Research, Tokoku University
Y. Kawazoe: Institute for Materials Research, Tokoku University

Nature, 1999, vol. 400, issue 6745, 647-649

Abstract: Abstract There has been considerable interest in the structure of liquid water at low temperatures and high pressure following the discovery of the high-density amorphous (HDA) phase of ice Ih (ref. 1). HDA ice forms at a pressure close to the extrapolated melting curve of ice, leading to the suggestion that it may have structure similar to that of dense water. On annealing, HDA ice transforms into a low-density amorphous (LDA) phase with a distinct phase boundary2,3. Extrapolation of thermodynamic data along the HDA–LDA coexistence line into the liquid region has led to the hypothesis that there might exist a second critical point for water and the speculation that liquid water is mixture of two distinct structures with different densities4,5. Here we critically examine this hypothesis. We use quasi-harmonic lattice-dynamics calculations to show that the amorphization mechanism in ice Ih changes from thermodynamic melting for T > 162 K to mechanical melting at lower temperatures. The vibrational spectra of ice Ih, LDA ice and quenched water also indicate a structure for LDA ice that differs from that of the liquid. These results call into question the validity of there being a thermodynamic connection between the amorphous and liquid phases of water.

Date: 1999
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DOI: 10.1038/23216

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