Liquid-liquid equilibrium for monodisperse spherical particles

Jagla, E. A.

doi:10.1103/physreve.63.061501

Cited by 120 publications

(123 citation statements)

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“…Two of the models (the TIP5P [45] and the ST2 [46]) treat water as a multiple site rigid body, interacting via electrostatic site-site interactions complemented by a Lennard-Jones potential. The third model is the spherical ''two-scale'' Jagla potential with attractive and repulsive ramps which has been studied in the context of liquid-liquid phase transitions and liquid anomalies [21,[30][31][32]47,48]. For all three models, Xu et al evaluated the loci of maxima of the relevant response functions, compressibility and specific heat, which coincide close to the critical point and give rise to the Widom line.…”

Section: Results For Bulk Watermentioning

confidence: 99%

“…Unlike other network forming materials [26], water behaves as a non-Arrhenius liquid in the experimentally accessible window [16,27,28]. Based on analogies with other network forming liquids and with the thermodynamic properties of the amorphous forms of water, it has been suggested that, at ambient pressure, liquid water should show a dynamic crossover from non-Arrhenius behavior at high T to Arrhenius behavior at low T [24,[29][30][31][32][33]. Using Adam-Gibbs theory [34], the dynamic crossover in water was related to the C max P line [22,35].…”

Section: The Widom Linementioning

confidence: 99%

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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: Results For Bulk Watermentioning

confidence: 99%

Section: The Widom Linementioning

confidence: 99%

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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“…[32][33][34][35][36] In addition, the possibility of a LLPT has been seen in computer simulations of many other pure fluids. [37][38][39][40][41][42][43][44] More importantly, technical questions regarding equilibration raised in Refs. 30 and 31, have no bearing on the qualitative transformations of the glassy states we examine, which are inherently nonequilibrium.…”

Section: Introductionmentioning

confidence: 99%

Pressure-induced transformations in computer simulations of glassy water

Chiu

Starr

Giovambattista

2013

The Journal of Chemical Physics

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Glassy water occurs in at least two broad categories: low-density amorphous (LDA) and highdensity amorphous (HDA) solid water. We perform out-of-equilibrium molecular dynamics simulations to study the transformations of glassy water using the ST2 model. Specifically, we study the known (i) compression-induced LDA-to-HDA, (ii) decompression-induced HDA-to-LDA, and (iii) compression-induced hexagonal ice-to-HDA transformations. We study each transformation for a broad range of compression/decompression temperatures, enabling us to construct a "P-T phase diagram" for glassy water. The resulting phase diagram shows the same qualitative features reported from experiments. While many simulations have probed the liquid-state phase behavior, comparatively little work has examined the transitions of glassy water. We examine how the glass transformations relate to the (first-order) liquid-liquid phase transition previously reported for this model. Specifically, our results support the hypothesis that the liquid-liquid spinodal lines, between a lowdensity and high-density liquid, are extensions of the LDA-HDA transformation lines in the limit of slow compression. Extending decompression runs to negative pressures, we locate the sublimation lines for both LDA and hyperquenched glassy water (HGW), and find that HGW is relatively more stable to the vapor. Additionally, we observe spontaneous crystallization of HDA at high pressure to ice VII. Experiments have also seen crystallization of HDA, but to ice XII. Finally, we contrast the structure of LDA and HDA for the ST2 model with experiments. We find that while the radial distribution functions (RDFs) of LDA are similar to those observed in experiments, considerable differences exist between the HDA RDFs of ST2 water and experiment. The differences in HDA structure, as well as the formation of ice VII (a tetrahedral crystal), are a consequence of ST2 overemphasizing the tetrahedral character of water. © 2013 AIP Publishing LLC.

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“…Experiments as well as simulations suggest that the anomalous thermodynamic and kinetic properties of water are due to the fluctuating, three-dimensional, locally tetrahedral hydrogen-bonded network. Water-like anomalies are seen in other tetrahedral network-forming liquids, such as silica, as well as in model liquids with isotropic core-softened or two-scale pair potentials [3,4,5,6,7,8,9,10,11].In the case of liquids such as water and silica, a quantitative connection between the structure of the tetrahedral network and the macroscopic density or temperature variables can be made by introducing order metrics to gauge the type as well as the extent of structural order [6,7]. The local tetrahedral order parameter, q tet , associated with an atom i (e.g.…”

mentioning

confidence: 99%

Entropy, diffusivity, and structural order in liquids with waterlike anomalies

Sharma

Chakraborty

Chakravarty

2006

The Journal of Chemical Physics

185

204

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The excess entropy, S e , defined as the difference between the entropies of the liquid and the ideal gas under identical density and temperature conditions, is shown to be the critical quantity connecting the structural, diffusional and density anomalies in water-like liquids. Based on simulations of silica and the two-scale ramp liquids, water-like density and diffusional anomalies can be seen as consequences of a characteristic non-monotonic density dependence of S e . The relationship between excess entropy, the order metrics and the structural anomaly can be understood using a pair correlation approximation to S e . 61.20.Qg,05.20.Jj The behaviour of water is anomalous when compared to simple liquids for which the structure and dynamics is dominated by strong, essentially isotropic, short-range repulsions [1,2].For example, over certain ranges of temperature and pressure,the density of water increases with temperature under isobaric conditions (density anomaly) while the self-diffusivity increases with density under isothermal conditions (diffusional anomaly). Experiments as well as simulations suggest that the anomalous thermodynamic and kinetic properties of water are due to the fluctuating, three-dimensional, locally tetrahedral hydrogen-bonded network. Water-like anomalies are seen in other tetrahedral network-forming liquids, such as silica, as well as in model liquids with isotropic core-softened or two-scale pair potentials [3,4,5,6,7,8,9,10,11].In the case of liquids such as water and silica, a quantitative connection between the structure of the tetrahedral network and the macroscopic density or temperature variables can be made by introducing order metrics to gauge the type as well as the extent of structural order [6,7]. The local tetrahedral order parameter, q tet , associated with an atom i (e.g. Si atom in SiO 2 ) is defined aswhere ψ jk is the angle between the bond vectors r ij and r ik where j and k label the four nearest neighbour atoms of the same type [6]. The translational order parameter, τ , measures the extent of pair correlations present in the system and is defined aswhere ξ = rρ 1/3 , r is the pair separation and ξ c is a suitably chosen cut-off distance [12].Since τ increases as the random close-packing limit is approached, it can be regarded as measuring the degree of density ordering. At a given temperature, q tet will show a maximum and τ will show a minimum as a function of density; the loci of these extrema in the order define a structurally anomalous region in the density-temperature (ρT ) plane. Within this structurally anomalous region, the tetrahedral and translational order parameters are found to be strongly correlated. The region of the density anomaly, where (∂ρ/∂T ) P > 0, is bounded by the structurally anomalous region. The diffusionally anomalous region ((∂D/∂ρ) T > 0) closely follows the boundaries of the structurally anomalous region, specially at low temperatures. In water, the structurally anomalous region encloses the region of anomalous diffusivit...

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Liquid-liquid equilibrium for monodisperse spherical particles

Cited by 120 publications

References 18 publications

The puzzling unsolved mysteries of liquid water: Some recent progress

The puzzling unsolved mysteries of liquid water: Some recent progress

Pressure-induced transformations in computer simulations of glassy water

Entropy, diffusivity, and structural order in liquids with waterlike anomalies

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