Relaxation dynamics and transformation kinetics of deeply supercooled water: Temperature, pressure, doping, and proton/deuteron isotope effects

Sonja Lemke, Philip H. Handle, Lucie J. Plaga, Josef N. Stern, Markus Seidl, Violeta Fuentes-Landete, Katrin Amann-Winkel, Karsten W. Köster, Catalin Gainaru, Thomas Loerting, Roland Böhmer

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27 Scopus citations

Abstract

Above its glass transition, the equilibrated high-density amorphous ice (HDA) transforms to the low-density pendant (LDA). The temperature dependence of the transformation is monitored at ambient pressure using dielectric spectroscopy and at elevated pressures using dilatometry. It is found that near the glass transition temperature of deuterated samples, the transformation kinetics is 300 times slower than the structural relaxation, while for protonated samples, the time scale separation is at least 30 000 and insensitive to doping. The kinetics of the HDA to LDA transformation lacks a proton/deuteron isotope effect, revealing that this process is dominated by the restructuring of the oxygen network. The x-ray diffraction experiments performed on samples at intermediate transition stages reflect a linear combination of the LDA and HDA patterns implying a macroscopic phase separation, instead of a local intermixing of the two amorphous states.

Original languageEnglish
Article number034506
JournalJournal of Chemical Physics
Volume147
Issue number3
DOIs
StatePublished - Jul 21 2017
Externally publishedYes

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