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Compression kinetics influence amorphous ice formation. Slow compression of ice I at 100 K yields crystalline phases, not high-density amorphous ice (HDA), challenging the two-liquid water model for amorphous ice.

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Area of Science:

  • Materials Science
  • Physical Chemistry
  • Condensed Matter Physics

Background:

  • Amorphous water ice exists in multiple forms lacking crystalline order.
  • High-density amorphous ice (HDA) was previously thought to be a glassy state, influencing the two-liquid water model for supercooled water anomalies.
  • Alternative theories suggested HDA forms due to mechanical instability and sluggish kinetics.

Purpose of the Study:

  • To investigate the role of kinetics in the formation of amorphous ice phases.
  • To challenge existing theories linking amorphous ice to supercooled liquid water.
  • To explore the compression pathways of ice I under varying kinetic conditions.

Main Methods:

  • Compression of ice I at 100 Kelvin under controlled, slow kinetic conditions.
  • Comparison of outcomes from slow versus fast compression protocols.
  • Structural analysis of resulting ice phases, including proton ordering and interpenetration.

Main Results:

  • Slow compression of ice I at 100 K produced crystalline phases: ice IX', ice XV', and ice VIII'.
  • Fast compression at 100 K yielded high-density amorphous ice (HDA) but not ice IX'.
  • Direct transformation of ice I to ice XV' was found to be structurally inhibited.

Conclusions:

  • Amorphous ice formation is a kinetically arrested transformation between low-density ice I and high-density ice XV'.
  • The study challenges the connection between amorphous ice phases and the two-liquid model of supercooled water.
  • Kinetics, not thermodynamic melting, are crucial in determining the formation of amorphous versus crystalline ice structures.