Glass-to-cryogenic-liquid transitions in aqueous solutions suggested by crack healing

Proceedings of the National Academy of Sciences of the United States of America
Chae Un KimSol M Gruner

Abstract

Observation of theorized glass-to-liquid transitions between low-density amorphous (LDA) and high-density amorphous (HDA) water states had been stymied by rapid crystallization below the homogeneous water nucleation temperature (∼235 K at 0.1 MPa). We report optical and X-ray observations suggestive of glass-to-liquid transitions in these states. Crack healing, indicative of liquid, occurs when LDA ice transforms to cubic ice at 160 K, and when HDA ice transforms to the LDA state at temperatures as low as 120 K. X-ray diffraction study of the HDA to LDA transition clearly shows the characteristics of a first-order transition. Study of the glass-to-liquid transitions in nanoconfined aqueous solutions shows them to be independent of the solute concentrations, suggesting that they represent an intrinsic property of water. These findings support theories that LDA and HDA ice are thermodynamically distinct and that they are continuously connected to two different liquid states of water.

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Citations

Jul 17, 2016·The Journal of Chemical Physics·Yoshiharu Suzuki, Osamu Mishima
Feb 15, 2018·Proceedings of the National Academy of Sciences of the United States of America·Chuanlong LinGuoyin Shen
Sep 27, 2019·Physical Chemistry Chemical Physics : PCCP·Johannes BachlerThomas Loerting
Mar 5, 2016·Journal of Applied Crystallography·Qingqiu HuangDoletha M E Szebenyi
Jun 28, 2017·Proceedings of the National Academy of Sciences of the United States of America·Fivos PerakisAnders Nilsson
Mar 26, 2019·Journal of the American Chemical Society·Rui-Kang HuangXiao-Ming Chen
Feb 6, 2018·The Journal of Physical Chemistry. B·Irem AltanPatrick Charbonneau

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