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Diffusive dynamics during the high-to-low density transition in amorphous ice.

Fivos Perakis1,2, Katrin Amann-Winkel1, Felix Lehmkühler3,4

  • 1Department of Physics, AlbaNova University Center, Stockholm University, S-10691 Stockholm, Sweden.

Proceedings of the National Academy of Sciences of the United States of America
|June 28, 2017
PubMed
Summary

Researchers investigated amorphous ices, exploring the transition between high-density amorphous (HDA) and low-density amorphous (LDA) forms. They observed distinct structural domains and dynamics, suggesting a liquid-liquid transition in ultraviscous water.

Keywords:
X-ray photon-correlation spectroscopyamorphous iceglass transitionliquid–liquid transitionsupercooled water

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Area of Science:

  • Condensed matter physics
  • Physical chemistry
  • Materials science

Background:

  • Water exhibits high-density amorphous (HDA) and low-density amorphous (LDA) forms.
  • These forms may represent glassy states of high-density liquid (HDL) and low-density liquid (LDL).
  • The nature of the glass transition and the HDA-LDA transition in water remain debated.

Purpose of the Study:

  • To investigate the structural and dynamical properties during the high-to-low-density transition in amorphous ice.
  • To provide new experimental evidence for the debated transitions in water's phase diagram.
  • To probe dynamics on the nanometer length scale using X-ray scattering techniques.

Main Methods:

  • Combined wide-angle X-ray scattering (WAXS) and X-ray photon-correlation spectroscopy (XPCS) in small-angle X-ray scattering (SAXS) geometry.
  • Analyzed structure factor and radial distribution function to determine structural properties.
  • Utilized XPCS in SAXS geometry to probe dynamics and structural relaxation on the nanometer length scale.

Main Results:

  • Observed coexistence of two structurally distinct domains at 125 K.
  • Identified a slow dynamical component in HDA related to viscoelastic relaxation and stress release.
  • Detected a faster, temperature-dependent dynamical component above 110 K, indicative of nanoscale diffusion, which persisted after transitioning to the low-density form.

Conclusions:

  • The experimental findings are most consistent with a liquid-liquid transition in the ultraviscous regime of water.
  • The study provides new insights into the complex phase behavior of amorphous water.
  • The observed dynamics support the interpretation of distinct liquid states preceding the amorphous ice transitions.