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Gallo, P., Amann-Winkel, K., Angell, C.A., Anisimov, M.A., Caupin, F., Chakravarty, C., Lascaris, E., Loerting, T., Panagiotopoulos, A.Z., Russo, J., Sellberg, J.A., Stanley, H.E., Tanaka, H., Vega, C., Xu, L. and Pettersson, L.G.M. (2016) Water: A Tale of Two Liquids. Chemical Reviews, 116, 7463-7500.
https://doi.org/10.1021/acs.chemrev.5b00750
has been cited by the following article:
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TITLE:
Liquid Pre-Freezing Percolation Transition to Equilibrium Crystal-in-Liquid Mesophase
AUTHORS:
Leslie V. Woodcock
KEYWORDS:
Liquid State, Percolation, Phase Transition, Pre-Freezing Mesophase
JOURNAL NAME:
Natural Science,
Vol.10 No.7,
July
23,
2018
ABSTRACT: Pre-freezing anomalies are explained by a percolation transition that delineates the existence of a pure equilibrium liquid state above the temperature of 1st-order freezing to the stable crystal phase. The precursor to percolation transitions are hetero-phase fluctuations that give rise to molecular clusters of an otherwise unstable state in the stable host phase. In-keeping with the Ostwald’s step rule, clusters of a crystalline state, closest in stability to the liquid, are the predominant structures in pre-freezing hetero-phase fluctuations. Evidence from changes in properties that depend upon density and energy fluctuations suggests embryonic nano-crystallites diverge in size and space at a percolation threshold, whence a colloidal-like equilibrium is stabilized by negative surface tension. Below this transition temperature, both crystal and liquid states percolate the phase volume in an equilibrium state of dispersed coexistence. We obtain a preliminary estimate of the prefreezing percolation line for water determined from higher-order discontinuities in Gibbs energy that derivatives the isothermal rigidity [(dp/dρ)T] and isochoric heat capacity [(dU/dT)v] respectively. The percolation temperature varies only slightly with pressure from 51.5°C at 0.1 MPa to around 60°C at 100 MPa. We conjecture that the predominant dispersed crystal structure is a tetrahedral ice, which is the closest of the higher-density ices (II to XV) to liquid water in configurational energy. Inspection of thermodynamic and transport properties of liquid argon also indicate the existence of a similar prefreezing percolation transition at ambient pressures (0.1 MPa) around 90 K, ~6% above the triple point (84 K). These findings account for many anomalous properties of equilibrium and supercooled liquids generally, and also explain Kauzmann’s “paradox” at a “glass” transition.
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