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Structural differences between unannealed and expanded high-density amorphous ice based on isotope substitution neutron diffraction
Stockholm University, Faculty of Science, Department of Physics. University of Innsbruck, Austria.
Number of Authors: 32019 (English)In: Molecular Physics, ISSN 0026-8976, E-ISSN 1362-3028, Vol. 117, no 22, p. 3207-3216Article in journal (Refereed) Published
Abstract [en]

We here report isotope substitution neutron diffraction experiments on two variants of high-density amorphous ice (HDA): its unannealed form prepared via pressure-induced amorphization of hexagonal ice at 77 K, and its expanded form prepared via decompression of very-high density amorphous ice at 140 K. The latter is about 17 K more stable thermally, so that it can be heated beyond its glass-to-liquid transition to the ultraviscous liquid form at ambient pressure. The structural origin for this large thermal difference and the possibility to reach the deeply supercooled liquid state has not yet been understood. Here we reveal that the origin for this difference is found in the intermediate range structure, beyond about 3.6 angstrom. The hydration shell markedly differs at about 6 angstrom. The local order, by contrast, including the first as well as the interstitial space between first and second shell is very similar for both. 'eHDA' that is decompressed to 0.20 GPa instead of 0.07 GPa is here revealed to be rather far away from well-relaxed eHDA. Instead it turns out to be roughly halfway between VHDA and eHDA - stressing the importance for decompressing VHDA to at least 0.10 GPa to make an eHDA sample of good quality.

Place, publisher, year, edition, pages
2019. Vol. 117, no 22, p. 3207-3216
Keywords [en]
Amorphous ice, water, neutron diffraction
National Category
Chemical Sciences Physical Sciences
Identifiers
URN: urn:nbn:se:su:diva-173177DOI: 10.1080/00268976.2019.1649487ISI: 000480109700001OAI: oai:DiVA.org:su-173177DiVA, id: diva2:1352090
Available from: 2019-09-17 Created: 2019-09-17 Last updated: 2019-12-07Bibliographically approved

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