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Diffusive dynamics during the high-to-low density transition in amorphous ice
Stockholm University, Faculty of Science, Department of Physics. SLAC National Accelerator Laboratory, USA.
Stockholm University, Faculty of Science, Department of Physics.
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Number of Authors: 19
2017 (English)In: Proceedings of the National Academy of Sciences of the United States of America, ISSN 0027-8424, E-ISSN 1091-6490, Vol. 114, no 31, 8193-8198 p.Article in journal (Refereed) Published
Abstract [en]

Water exists in high- and low-density amorphous ice forms (HDA and LDA), which could correspond to the glassy states of high(HDL) and low-density liquid (LDL) in the metastable part of the phase diagram. However, the nature of both the glass transition and the high-to-low-density transition are debated and new experimental evidence is needed. Here we combine wide-angle X-ray scattering (WAXS) with X-ray photon-correlation spectroscopy (XPCS) in the small-angle X-ray scattering (SAXS) geometry to probe both the structural and dynamical properties during the high-to-low-density transition in amorphous ice at 1 bar. By analyzing the structure factor and the radial distribution function, the coexistence of two structurally distinct domains is observed at T = 125 K. XPCS probes the dynamics in momentum space, which in the SAXS geometry reflects structural relaxation on the nanometer length scale. The dynamics of HDA are characterized by a slow component with a large time constant, arising from viscoelastic relaxation and stress release from nanometer-sized heterogeneities. Above 110 K a faster, strongly temperature-dependent component appears, with momentum transfer dependence pointing toward nanoscale diffusion. This dynamical component slows down after transition into the low-density form at 130 K, but remains diffusive. The diffusive character of both the high- and low-density forms is discussed among different interpretations and the results are most consistent with the hypothesis of a liquid-liquid transition in the ultraviscous regime.

Place, publisher, year, edition, pages
2017. Vol. 114, no 31, 8193-8198 p.
Keyword [en]
liquid-liquid transition, glass transition, amorphous ice, X-ray photon-correlation spectroscopy, supercooled water
National Category
Physical Sciences
Identifiers
URN: urn:nbn:se:su:diva-147135DOI: 10.1073/pnas.1705303114ISI: 000406653300040PubMedID: 28652327OAI: oai:DiVA.org:su-147135DiVA: diva2:1145286
Available from: 2017-09-28 Created: 2017-09-28 Last updated: 2017-09-28Bibliographically approved

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