Experiments indicating a second hydrogen ordered phase of ice VI

Chemical Science
Tobias M GasserThomas Loerting

Abstract

In the last twelve years five new ice phases were experimentally prepared. Two of them are empty clathrate hydrates and three of them represent hydrogen ordered counterparts of previously known disordered ice phases. Here, we report on hydrogen ordering in ice VI samples produced by cooling at pressures up to 2.00 GPa. Based on results from calorimetry, dielectric relaxation spectroscopy, Raman spectroscopy, and powder X-ray diffraction the existence of a second hydrogen ordered polymorph related to ice VI is suggested. Powder X-ray data show the oxygen network to be the one of ice VI. For the 1.80 GPa sample the activation energy from dielectric spectroscopy is 45 kJ mol-1, which is much larger than for the known hydrogen ordered proxy of ice VI, ice XV. Raman spectroscopy indicates the 1.80 GPa sample to be more ordered than ice XV. It is further distinct from ice XV in that it experiences hydrogen disordering above ≈103 K which is 26 K below the ice XV to ice VI disordering transition. Consequently, below 103 K it is thermodynamically more stable than ice XV, adding a stability region to the phase diagram of water. For the time being we suggest to call this new phase ice β-XV and to relabel it ice XVIII once its crystal stru...Continue Reading

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Citations

Jul 2, 2019·Physical Chemistry Chemical Physics : PCCP·Alexander V ThoenyThomas Loerting
Aug 30, 2019·Molecules : a Journal of Synthetic Chemistry and Natural Product Chemistry·Xiao-Ling QinPeng Zhang
Jan 3, 2019·The Review of Scientific Instruments·A BaumgartnerS Fella
Jul 1, 2019·The Journal of Chemical Physics·L J PlagaR Böhmer
Feb 17, 2019·The Journal of Chemical Physics·Christoph G Salzmann
Sep 16, 2019·The Journal of Chemical Physics·B MassaniJ Loveday
Mar 13, 2020·Proceedings of the National Academy of Sciences of the United States of America·Kazuki KomatsuHiroyuki Kagi
Feb 20, 2021·Nature Communications·Ryo YamaneHiroyuki Kagi
Feb 20, 2021·Nature Communications·Tobias M GasserThomas Loerting
Apr 10, 2021·The Journal of Chemical Physics·Christoph G SalzmannJohn L Finney
May 6, 2021·Polymers·Kacper DrużbickiFelix Fernandez-Alonso
May 28, 2021·Nature Communications·Christoph G SalzmannCraig L Bull
May 28, 2021·Nature Communications·Thomas C Hansen
Jun 15, 2021·ACS Omega·Xue-Chun WangPeng Zhang
Jan 24, 2020·The Journal of Physical Chemistry Letters·Alexander Rosu-FinsenChristoph G Salzmann
Oct 26, 2018·The Journal of Physical Chemistry. B·Daniel R MobergFrancesco Paesani
Oct 15, 2021·The Journal of Physical Chemistry. B·Tobias M GasserThomas Loerting

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Methods Mentioned

BETA
X-ray
neutron diffraction

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