Limits of metastability in amorphous ices: the neutron scattering Debye–Waller factor

Amann‐Winkel, Katrin; Löw, Florian; Handle, Philip H.; Knoll, Wiebke; Peters, Judith; Geil, Burkhard; Fujara, F.; Loerting, Thomas

doi:10.1039/c2cp42797d

Cited by 13 publications

(18 citation statements)

References 40 publications

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“…The thermal stability of eHDA compared with the other states was shown in the literature in many different ways. Although different experimental methods, such as neutron scattering [27,54], calorimetric measurements [10] and dielectric spectroscopy [40] show the same trend, the absolute values differ slightly due to every method using not only a different observable but also different heating rate, due to experimental restrictions. In the current study, we now compared different heating rates within the same experimental method and found that when using a 10× faster heating rate of 4 K min −1 , the conversion appears distinct both for the HDA-like state starting from VHDA and eHDA 0.07 (figure 3).…”

Section: Discussionmentioning

confidence: 99%

X-ray studies of the transformation from high- to low-density amorphous water

Mariedahl

Perakis

Späh

et al. 2019

Phil. Trans. R. Soc. A.

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Here we report about the structural evolution during the conversion from high-density amorphous ices at ambient pressure to the low-density state. Using high-energy X-ray diffraction, we have monitored the transformation by following in reciprocal space the structure factor S OO ( Q ) and derived in real space the pair distribution function g OO ( r ). Heating equilibrated high-density amorphous ice (eHDA) at a fast rate (4 K min –1 ), the transition to the low-density form occurs very rapidly, while domains of both high- and low-density coexist. On the other hand, the transition in the case of unannealed HDA (uHDA) and very-high-density amorphous ice is more complex and of continuous nature. The direct comparison of eHDA and uHDA indicates that the molecular structure of uHDA contains a larger amount of tetrahedral motives. The different crystallization behaviour of the derived low-density amorphous states is interpreted as emanating from increased tetrahedral coordination present in uHDA. This article is part of the theme issue ‘The physics and chemistry of ice: scaffolding across scales, from the viability of life to the formation of planets'.

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Section: Discussionmentioning

confidence: 99%

X-ray studies of the transformation from high- to low-density amorphous water

Mariedahl

Perakis

Späh

et al. 2019

Phil. Trans. R. Soc. A.

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“…Quasielastic neutron scattering measurements on LDA-I and uHDA previously showed the absence of such fast precursor processes 100 . Recently these experiments were repeated using LDA-II and eHDA 89 . The Debye-Waller factor shows a very weak sub-T g anomaly in some of the samples, which might be the signature of fast precursor dynamics and hence a signature for a glass transition.…”

Section: Structure Of Water In the Liquid Statementioning

confidence: 99%

X-ray and Neutron Scattering of Water

et al. 2016

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International audienceThis review article focuses on the most recent advances in X-ray and neutron scattering studies of water structure, from ambient temperature to the deeply supercooled and amorphous states, and of water diffusive and collective dynamics, in disparate thermodynamic conditions and environments. In particular, the ability to measure X-ray and neutron diffraction of water with unprecedented high accuracy in an extended range of momentum transfers has allowed the derivation of detailed O–O pair correlation functions. A panorama of the diffusive dynamics of water in a wide range of temperatures (from 400 K down to supercooled water) and pressures (from ambient up to multiple gigapascals) is presented. The recent results obtained by quasi-elastic neutron scattering under high pressure are compared with the existing data from nuclear magnetic resonance, dielectric and infrared measurements, and modeling. A detailed description of the vibrational dynamics of water as measured by inelastic neutron scattering is presented. The dependence of the water vibrational density of states on temperature and pressure, and in the presence of biological molecules, is discussed. Results about the collective dynamics of water and its dispersion curves as measured by coherent inelastic neutron scattering and inelastic X-ray scattering in different thermodynamic conditions are reported

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“…This has been out of reach in research on amorphous ices so far even though calorimetry methods reaching heating rates on the order of 10 5 K/s were employed to study them [31,32] . However, it has been possible to study whether or not a glass transition can be observed upon heating amorphous ice prior to crystallization and/or prior to the transformation to other amorphous ices [20,31–44] . This glass transition would lead to an ultraviscous liquid state which is also called deeply supercooled liquid water.…”

Section: Introductionmentioning

confidence: 99%

The glass transition in high-density amorphous ice

Loerting

Fuentes-Landete

Handle

et al. 2015

Journal of Non-Crystalline Solids

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There has been a long controversy regarding the glass transition in low-density amorphous ice (LDA). The central question is whether or not it transforms to an ultraviscous liquid state above 136 K at ambient pressure prior to crystallization. Currently, the most widespread interpretation of the experimental findings is in terms of a transformation to a superstrong liquid above 136 K. In the last decade some work has also been devoted to the study of the glass transition in high-density amorphous ice (HDA) which is in the focus of the present review. At ambient pressure HDA is metastable against both ice I and LDA, whereas at > 0.2 GPa HDA is no longer metastable against LDA, but merely against high-pressure forms of crystalline ice. The first experimental observation interpreted as the glass transition of HDA was made using in situ methods by Mishima, who reported a glass transition temperature Tg of 160 K at 0.40 GPa. Soon thereafter Andersson and Inaba reported a much lower glass transition temperature of 122 K at 1.0 GPa. Based on the pressure dependence of HDA's Tg measured in Innsbruck, we suggest that they were in fact probing the distinct glass transition of very high-density amorphous ice (VHDA). Very recently the glass transition in HDA was also observed at ambient pressure at 116 K. That is, LDA and HDA show two distinct glass transitions, clearly separated by about 20 K at ambient pressure. In summary, this suggests that three glass transition lines can be defined in the p–T plane for LDA, HDA, and VHDA.

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Limits of metastability in amorphous ices: the neutron scattering Debye–Waller factor

Cited by 13 publications

References 40 publications

X-ray studies of the transformation from high- to low-density amorphous water

X-ray studies of the transformation from high- to low-density amorphous water

X-ray and Neutron Scattering of Water

The glass transition in high-density amorphous ice

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