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Area of Science:

  • Materials Science
  • Condensed Matter Physics
  • Physical Chemistry

Background:

  • High-density amorphous ice (HDA) exists in various forms with differing thermal stabilities.
  • The structural origins of these stability differences and the potential to access the deeply supercooled liquid state remain unclear.

Purpose of the Study:

  • To investigate the structural differences between unannealed HDA and expanded HDA (eHDA).
  • To elucidate the structural basis for the enhanced thermal stability of eHDA.
  • To understand the conditions necessary for preparing high-quality eHDA samples.

Main Methods:

  • Isotope substitution neutron diffraction experiments were performed on two HDA variants.
  • Unannealed HDA was prepared by pressure-induced amorphization of hexagonal ice at 77 K.
  • Expanded HDA (eHDA) was prepared by decompression of very-high density amorphous ice (VHDA) at 140 K.

Main Results:

  • Significant differences in the intermediate-range structure (beyond 3.6 Å) and hydration shells (around 6 Å) were observed between the HDA variants.
  • Local order, including the first and interstitial shells, showed high similarity.
  • eHDA decompressed at 0.20 GPa was found to be structurally distinct from well-relaxed eHDA, resembling a state between VHDA and eHDA.

Conclusions:

  • The enhanced thermal stability of eHDA is attributed to differences in its intermediate-range structure.
  • Proper decompression of VHDA to at least 0.10 GPa is crucial for obtaining high-quality eHDA.
  • These findings provide insight into the structural landscape of amorphous ices and their supercooled states.