Crystallisation of the amorphous ices in the intermediate pressure regime

Abstract The crystallisation behaviour of very high-density amorphous ice (VHDA) and unannealed high-density amorphous ice (uHDA) has been studied in situ by volumetry and ex situ by powder x-ray diffraction in the intermediate pressure range 0.7–1.8 GPa employing different heating rates (0.5, 5 and...

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Main Authors: J. Stern, T. Loerting
Format: Article
Language:English
Published: Nature Portfolio 2017-06-01
Series:Scientific Reports
Online Access:https://doi.org/10.1038/s41598-017-03583-2
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author J. Stern
T. Loerting
author_facet J. Stern
T. Loerting
author_sort J. Stern
collection DOAJ
description Abstract The crystallisation behaviour of very high-density amorphous ice (VHDA) and unannealed high-density amorphous ice (uHDA) has been studied in situ by volumetry and ex situ by powder x-ray diffraction in the intermediate pressure range 0.7–1.8 GPa employing different heating rates (0.5, 5 and 30 K min−1). This study shows that at pressures >1 GPa the crystallisation behaviour of VHDA and uHDA is basically the same for all heating rates. That is, parallel crystallisation is almost entirely suppressed with mainly ice XII forming. This contrasts former results reporting parallel crystallisation to approximately levelled phase mixtures of ice IV and ice XII even at higher pressures for uHDA. We speculate this to be due to formation of microcracks upon decompression in earlier works, but not in the present one. Crystallisation temperatures T x are up to 16 K higher than previously reported, raising the low-temperature border to no man’s land and opening a considerably larger window for future studies on non-crystalline water. The results indicate uHDA to contain heterogeneities on the nanoscale, but VHDA to be rather homogeneous with nano-crystallites being largely absent. Upon transforming uHDA to VHDA, the nano-scale heterogeneities disappear for >1 GPa whereas microcracks do not.
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spelling doaj.art-5894b83d69064a2783e8bccb042573d82022-12-21T23:00:41ZengNature PortfolioScientific Reports2045-23222017-06-017111010.1038/s41598-017-03583-2Crystallisation of the amorphous ices in the intermediate pressure regimeJ. Stern0T. Loerting1Institute of Physical Chemistry, University of InnsbruckInstitute of Physical Chemistry, University of InnsbruckAbstract The crystallisation behaviour of very high-density amorphous ice (VHDA) and unannealed high-density amorphous ice (uHDA) has been studied in situ by volumetry and ex situ by powder x-ray diffraction in the intermediate pressure range 0.7–1.8 GPa employing different heating rates (0.5, 5 and 30 K min−1). This study shows that at pressures >1 GPa the crystallisation behaviour of VHDA and uHDA is basically the same for all heating rates. That is, parallel crystallisation is almost entirely suppressed with mainly ice XII forming. This contrasts former results reporting parallel crystallisation to approximately levelled phase mixtures of ice IV and ice XII even at higher pressures for uHDA. We speculate this to be due to formation of microcracks upon decompression in earlier works, but not in the present one. Crystallisation temperatures T x are up to 16 K higher than previously reported, raising the low-temperature border to no man’s land and opening a considerably larger window for future studies on non-crystalline water. The results indicate uHDA to contain heterogeneities on the nanoscale, but VHDA to be rather homogeneous with nano-crystallites being largely absent. Upon transforming uHDA to VHDA, the nano-scale heterogeneities disappear for >1 GPa whereas microcracks do not.https://doi.org/10.1038/s41598-017-03583-2
spellingShingle J. Stern
T. Loerting
Crystallisation of the amorphous ices in the intermediate pressure regime
Scientific Reports
title Crystallisation of the amorphous ices in the intermediate pressure regime
title_full Crystallisation of the amorphous ices in the intermediate pressure regime
title_fullStr Crystallisation of the amorphous ices in the intermediate pressure regime
title_full_unstemmed Crystallisation of the amorphous ices in the intermediate pressure regime
title_short Crystallisation of the amorphous ices in the intermediate pressure regime
title_sort crystallisation of the amorphous ices in the intermediate pressure regime
url https://doi.org/10.1038/s41598-017-03583-2
work_keys_str_mv AT jstern crystallisationoftheamorphousicesintheintermediatepressureregime
AT tloerting crystallisationoftheamorphousicesintheintermediatepressureregime