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  • Title: Structural changes of filled ice Ic hydrogen hydrate under low temperatures and high pressures from 5 to 50 GPa.
    Author: Hirai H, Kagawa S, Tanaka T, Matsuoka T, Yagi T, Ohishi Y, Nakano S, Yamamoto Y, Irifune T.
    Journal: J Chem Phys; 2012 Aug 21; 137(7):074505. PubMed ID: 22920129.
    Abstract:
    Low-temperature and high-pressure experiments were performed on the filled ice Ic structure of hydrogen hydrate at previously unexplored conditions of 5-50 GPa and 30-300 K using diamond anvil cells and a helium-refrigeration cryostat. In situ x-ray diffractometry revealed that the cubic filled ice Ic structure transformed to tetragonal at low temperatures and high pressures; the axis ratio of the tetragonal phase changed depending on the pressure and temperature. These results were consistent with theoretical predictions performed via first principle calculations. The tetragonal phase was determined to be stable above 20 GPa at 300 K, above 15 GPa at 200 K, and above 10 GPa at 100 K. Further changes in the lattice parameters were observed from about 45-50 GPa throughout the temperature region examined, which suggests the transformation to another high-pressure phase above 50 GPa. In our previous x-ray study that was performed up to 80 GPa at room temperature, a similar transformation was observed above 50 GPa. In this study, the observed change in the lattice parameters corresponds to the beginning of that transformation. The reasons for the transformation to the tetragonal structure are briefly discussed: the tetragonal structure might be induced due to changes in the vibrational or rotational modes of the hydrogen molecules under low temperature and high pressure.
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