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Adding a length scale to the polyamorphic ice debate.

C A Tulk1, R Hart, D D Klug

  • 1Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, USA.

Physical Review Letters
|October 10, 2006
PubMed
Summary
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Annealing very high density amorphous ice reveals a continuous breakdown and abrupt local structural change, leading to a new network. This differs from typical phase transitions, reconciling prior experimental data.

Area of Science:

  • Condensed matter physics
  • Materials science
  • Physical chemistry

Background:

  • Amorphous ices, particularly very high-density amorphous ice (HDA), exhibit complex structural ordering.
  • Understanding the relationship between short-range and intermediate-range ordering (IRO) is crucial for characterizing amorphous materials.
  • Previous studies have presented conflicting data regarding structural transitions in amorphous ice.

Purpose of the Study:

  • To investigate the correlation between short-range oxygen-oxygen structure and intermediate-range ordering (IRO) in very high-density amorphous ice during annealing.
  • To elucidate the nature of structural changes and transitions occurring in HDA ice.
  • To reconcile discrepancies in previous experimental findings on amorphous ice structure.

Main Methods:

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  • X-ray scattering techniques were employed to probe the structural properties.
  • Molecular dynamics simulations were utilized to model the atomic arrangements and dynamics.
  • Correlating scattering data with simulation results provided insights into structural evolution.

Main Results:

  • Intermediate-range ordering (IRO) in HDA ice continuously breaks down upon annealing, with correlations weakening beyond 7 Angstrom.
  • A distinct, abrupt change in local structure (O-O-O angles) occurs at a critical point.
  • Following this abrupt local change, a new IRO network continuously reemerges.

Conclusions:

  • The structural transition in HDA ice is not a classic first-order phase transition.
  • The observed mechanism involves continuous IRO breakdown followed by abrupt local structural rearrangement.
  • This finding provides a unified explanation for previously disparate experimental observations on amorphous ice.