Liquid-liquid phase transitions in supercooled water studied by computer simulations of various water models

Brovchenko, Ivan; Geiger, Alfons; Oleinikova, Alla

doi:10.1063/1.1992481

Cited by 152 publications

(185 citation statements)

References 77 publications

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“…The coincidence of T Â with T p within the error bars indicates that the behavior of the protein is strongly coupled with the behavior of the surrounding solvent, in agreement with recent experiments [51]. Note that T Â is much higher than the glass transition temperature, estimated for TIP5P as T g ¼ 215 K [72]. Thus this crossover is not likely to be related to the glass transition in water.…”

Section: Article In Presssupporting

confidence: 74%

The puzzling unsolved mysteries of liquid water: Some recent progress

Stanley

Kumar

et al. 2007

Physica A: Statistical Mechanics and its Applications

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Water is perhaps the most ubiquitous, and the most essential, of any molecule on earth. Indeed, it defies the imagination of even the most creative science fiction writer to picture what life would be like without water. Despite decades of research, however, water's puzzling properties are not understood and 63 anomalies that distinguish water from other liquids remain unsolved. We introduce some of these unsolved mysteries, and demonstrate recent progress in solving them. We present evidence from experiments and computer simulations supporting the hypothesis that water displays a special transition point (which is not unlike the ''tipping point'' immortalized by Malcolm Gladwell). The general idea is that when the liquid is near this ''tipping point,'' it suddenly separates into two distinct liquid phases. This concept of a new critical point is finding application to other liquids as well as water, such as silicon and silica. We also discuss related puzzles, such as the mysterious behavior of water near a protein. r

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Section: Article In Presssupporting

confidence: 74%

The puzzling unsolved mysteries of liquid water: Some recent progress

Stanley

Kumar

et al. 2007

Physica A: Statistical Mechanics and its Applications

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“…Indeed, it appears that the hypothesized liquid-liquid phase transition is below, or at least close to, the glass transition temperature. A recent simulation analysis of the orientational dynamics of water at fixed density [47] has shown that the temperature of dynamical arrest of the system, defined by the mode coupling theory, is relatively close in temperature and density to recent estimate of the liquid-liquid critical point [73]. However, as we have shown here, the study of the Widom line at temperatures above the liquid-liquid critical point could represent a useful way to investigate the inaccessible part of the supercooled phase diagram of water.…”

Section: Discussionmentioning

confidence: 99%

The Widom line of supercooled water

Franzese¹,

Stanley²

2007

J. Phys.: Condens. Matter

165

204

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Water can be supercooled to temperatures as low as −92• C, the experimental crystal homogeneous nucleation temperature T H at 2 kbar. Within the supercooled liquid phase its response functions show an anomalous increase consistent with the presence of a liquid-liquid critical point located in a region inaccessible to experiments on bulk water. Recent experiments on the dynamics of confined water show that a possible way to understand the properties of water is to investigate the supercooled phase diagram in the vicinity of the Widom line (locus of maximum correlation length) that emanates from the hypothesized liquid-liquid critical point. Here we explore the Widom line for a Hamiltonian model of water using an analytic approach, and discuss the plausibility of the hypothesized liquid-liquid critical point, as well as its possible consequences, on the basis of the assumptions of the model. The present analysis allows us (i) to find an analytic expression for the spinodal line of the high-density liquid phase, with respect to the low-density liquid phase, showing that this line becomes flat in the P-T phase diagram in the physical limit of a large number of available orientations for the hydrogen bonds, as recently seen in simulations and experiments (Xu et al 2005 Proc. Natl Acad. Sci. 102 16558); (ii) to find an estimate of the values for the hypothesized liquid-liquid critical point coordinates that compare very well with Monte Carlo results; and (iii) to show how the Widom line can be located by studying the derivative of the probability of forming hydrogen bonds with local tetrahedral orientation which can be calculated analytically within this approach.

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“…Direct experimental evidences of this phenomenon have been observed in liquid phosphorous [1,2] and triphenyl phosphite [3], while consistent data exists for water [4,5,6,7,8], silica [9,10], aluminate liquids [11], selenium [12], and cobalt [13], among others [14]. Simulations predict a liquid-liquid critical point for supercooled water [15,16,17,18,19,20,21], phosphorous [22], supercooled silica [9,23,24], and hydrogen [25]. For other substances, such as carbon, literature is contradictory [26,27,28].…”

Section: Introductionmentioning

confidence: 99%

Differences between discontinuous and continuous soft-core attractive potentials: The appearance of density anomaly

Franzese

2007

Journal of Molecular Liquids

105

120

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Soft-core attractive potentials can give rise to a phase diagram with three fluid phases at different densities (gas, low-density liquid and high-density liquid), separated by first order phase transition lines ending in critical points. Experiments show a phase diagram with these features for phosphorous and triphenyl-phosphite. Liquid-liquid phase transition could be relevant for water, silica, liquid metals, colloids and protein solutions, among others. Here we compare two potentials with short-range soft-core repulsion and narrow attraction. One of them is a squared potential that is known to have liquid-liquid phase transition, ending in a critical point, and no anomaly in density. The normal, monotonic, behavior of density for isobaric cooling is surprising if compared with molecular liquids, such as water, where a hypothetical critical point is proposed as rationale for the anomalous behavior of density. The second potential is a continuous version of the first. We show that the phase diagram associated to this new potential has, not only the liquid-liquid phase transition, but also the density anomaly. Our result, therefore, shows that the behavior in density is strongly dependent on the derivative of the potential.

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Liquid-liquid phase transitions in supercooled water studied by computer simulations of various water models

Cited by 152 publications

References 77 publications

The puzzling unsolved mysteries of liquid water: Some recent progress

The puzzling unsolved mysteries of liquid water: Some recent progress

The Widom line of supercooled water

Differences between discontinuous and continuous soft-core attractive potentials: The appearance of density anomaly

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