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Water polyamorphism: reversibility and (dis)continuity.

Katrin Winkel1, Michael S Elsaesser, Erwin Mayer

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Area of Science:

  • Condensed matter physics
  • Physical chemistry
  • Materials science

Background:

  • Understanding water's anomalies is crucial for comprehending its phase diagram.
  • The metastable noncrystalline states of water and their phase transitions remain poorly understood.
  • Puzzles persist regarding supercooled liquid water and its amorphous ice proxies at low temperatures.

Purpose of the Study:

  • To investigate the phase transitions between different amorphous states of ice.
  • To elucidate the nature of amorphous-amorphous transitions under decompression.
  • To provide insights into the liquid-liquid transition hypothesis in water.

Main Methods:

  • Decompression of very high density amorphous ice (VHDA) from 1.1 to 0.02 GPa at 140 K.
  • Dilatometry and powder X-ray diffraction of quench-recovered states.
  • Analysis of pressure-induced transitions between LDA, e-HDA, and VHDA.

Main Results:

  • Demonstrated reversible connections between low-density amorphous ice (LDA), expanded high-density amorphous ice (e-HDA), and VHDA.
  • Identified two distinct amorphous-amorphous transitions: a first-order-like e-HDA to LDA transition and a higher-order VHDA to e-HDA transition.
  • VHDA and e-HDA were found to be the most stable states during decompression.

Conclusions:

  • The observed transitions support a single first-order liquid-liquid transition scenario with a second critical point.
  • Evidence disfavors the hypothesis of multiple first-order liquid-liquid transitions and a third critical point.
  • This study offers new perspectives on the complex phase behavior of water's amorphous states.