Abstract

Water freezes below 0 °C at ambient pressure ordinarily to ice Ih, with hexagonal stacking sequence. Under certain conditions, ice with a cubic stacking sequence can also be formed, but ideal ice Ic without stacking-disorder has never been formed until recently. Here we demonstrate a route to obtain ice Ic without stacking-disorder by degassing hydrogen from the high-pressure form of hydrogen hydrate, C2, which has a host framework isostructural with ice Ic. The stacking-disorder free ice Ic is formed from C2 via an intermediate amorphous or nano-crystalline form under decompression, unlike the direct transformations occurring in ice XVI from neon hydrate, or ice XVII from hydrogen hydrate. The obtained ice Ic shows remarkable thermal stability, until the phase transition to ice Ih at 250 K, originating from the lack of dislocations. This discovery of ideal ice Ic will promote understanding of the role of stacking-disorder on the physical properties of ice as a counter end-member of ice Ih.

Highlights

  • Water freezes below 0 °C at ambient pressure, ordinarily to ice Ih with a hexagonal stacking sequence

  • The highest cubicity was limited to ~80%8,14, but it has been reported that ideal ice Ic with 100% cubicity has been obtained by annealing ice XVII10

  • Ice XVI15 and ice XVII16,17 are obtained by degassing gas molecules from neon and hydrogen hydrates, respectively

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Summary

Introduction

Water freezes below 0 °C at ambient pressure ordinarily to ice Ih, with hexagonal stacking sequence. We present the neutron and X-ray diffraction results showing ice Ic without stacking disorder, obtained from degassing hydrogen hydrate C2.

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