A study of the ice–water interface using the TIP4P/2005 water model

Benet, Jorge; MacDowell, Luis G.; Sanz, Eduardo

doi:10.1039/c4cp03398a

Cited by 44 publications

(62 citation statements)

References 49 publications

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“…The error bars are calculated taking into consideration the uncertainties on the estimated melting temperature (∼10 K) and the fitting procedure. As compared to previous studies on molecular compounds using the capillary fluctuation method, 48,112 the linear domain is more limited and the data are much noisier. It might indicate that some interfaces are not completely rough or a possible size effect.…”

Section: Simulation Detailsmentioning

confidence: 91%

Predictive Calculation of the Crystallization Tendency of Model Pharmaceuticals in the Supercooled State from Molecular Dynamics Simulations

Gerges

Affouard

2015

J. Phys. Chem. B

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Molecular dynamics (MD) simulations were used to perform a comparative study of the crystallization tendency from the melt of two model pharmaceutical compounds: felodipine and nifedipine. Two crystalline polymorphs of nifedipine (N(α), N(β)) and felodipine (FI, FII) have been studied. Calculations were performed on liquid and crystal systems separately in order to determine their main physical properties (diffusivity, density, and enthalpy). A fair agreement was found between the simulation and the known experimental data confirming the ability of the force field GAFF to reproduce accurately the experimental data for both compounds. Simulations of the crystal-liquid interface enabled the determination of the melting temperature and the interfacial free energy of the different polymorphs. Guided by the classical nucleation theory (CNT) predictions and different growth mechanism models (normal, two-dimensional, and screw dislocation), the nucleation and growth rates have been determined. The present investigation particularly raises the very important role of the solid-liquid interfacial free energy and its interplay with the driving force during the crystallization. The origin of the higher crystallization tendency of nifedipine with respect to felodipine is discussed from the present computed kinetic and thermodynamical factors.

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Section: Simulation Detailsmentioning

confidence: 91%

Predictive Calculation of the Crystallization Tendency of Model Pharmaceuticals in the Supercooled State from Molecular Dynamics Simulations

Gerges

Affouard

2015

J. Phys. Chem. B

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“…It is not obvious that we should compare these values for stacking-disordered ice to literature values of interfacial energy of hexagonal ice, but computational studies suggest there is only a small difference in interfacial energy between the different forms of ice I, 78,79 and that the basal face of hexagonal ice at equilibrium may be stacking disordered. 80 Hence, we cautiously compare our values of σ sd,l at the melting temperature with values determined for hexagonal ice also at the melting temperature. From experiments, there is a substantial spread of the reported interfacial energy at 273.15 K, 1 but it has been suggested that the value of Hardy 81 of 29.1 ± 0.8 mJ m −2 may be the most reliable.…”

Section: Fitting the Cnt-based Model To Experimental Datamentioning

confidence: 99%

A physically constrained classical description of the homogeneous nucleation of ice in water

Koop

Murray

2016

The Journal of Chemical Physics

119

155

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Liquid water can persist in a supercooled state to below 238 K in the Earth's atmosphere, a temperature range where homogeneous nucleation becomes increasingly probable. However, the rate of homogeneous ice nucleation in supercooled water is poorly constrained, in part, because supercooled water eludes experimental scrutiny in the region of the homogeneous nucleation regime where it can exist only fleetingly. Here we present a new parameterization of the rate of homogeneous ice nucleation based on classical nucleation theory. In our approach, we constrain the key terms in classical theory, i.e., the diffusion activation energy and the ice-liquid interfacial energy, with physically consistent parameterizations of the pertinent quantities. The diffusion activation energy is related to the translational self-diffusion coefficient of water for which we assess a range of descriptions and conclude that the most physically consistent fit is provided by a power law. The other key term is the interfacial energy between the ice embryo and supercooled water whose temperature dependence we constrain using the Turnbull correlation, which relates the interfacial energy to the difference in enthalpy between the solid and liquid phases. The only adjustable parameter in our model is the absolute value of the interfacial energy at one reference temperature. That value is determined by fitting this classical model to a selection of laboratory homogeneous ice nucleation data sets between 233.6 K and 238.5 K. On extrapolation to temperatures below 233 K, into a range not accessible to standard techniques, we predict that the homogeneous nucleation rate peaks between about 227 and 231 K at a maximum nucleation rate many orders of magnitude lower than previous parameterizations suggest. This extrapolation to temperatures below 233 K is consistent with the most recent measurement of the ice nucleation rate in micrometer-sized droplets at temperatures of 227-232 K on very short time scales using an X-ray laser technique. In summary, we present a new physically constrained parameterization for homogeneous ice nucleation which is consistent with the latest literature nucleation data and our physical understanding of the properties of supercooled water. C 2016 Author(s). All article content, except where otherwise noted, is licensed under a Creative Commons Attribution (CC BY) license

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“…1). Comparing our results for the ice-vapor interface with our previous study of the ice-water interface will prove insightful [44]. Since we aim at studying large wavelength fluctuations, we prepare the exposed faces with an elongated geometry, with box side L x ≫ L y .…”

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confidence: 99%

Premelting-Induced Smoothening of the Ice-Vapor Interface

et al. 2016

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We perform computer simulations of the quasiliquid layer of ice formed at the ice-vapor interface close to the ice Ih-liquid-vapor triple point of water. Our study shows that the two distinct surfaces bounding the film behave at small wavelengths as atomically rough and independent ice-water and water-vapor interfaces. For long wavelengths, however, the two surfaces couple, large scale parallel fluctuations are inhibited, and the ice-vapor interface becomes smooth. Our results could help explain the complex morphology of ice crystallites. DOI: 10.1103/PhysRevLett.117.096101 Nakaya summarized his research on snow flakes in a famous haiku: "They are letters sent to us from the sky" [1]. Indeed, the habit of ice crystals grown from bulk vapor change from plates, to columns, to plates, and yet back to columns as the temperature is cooled down below the triple point, with the well known dendritic patterns appearing at sufficiently high supersaturations [2]. Accordingly, the final growth form of a tiny ice crystal conveys detailed information on the atmosphere where it grew [3].At a macroscopic level, it is well known that changes in ice crystal habits result from a crossover in the growth rates of the basal and prismatic faces, but exactly what structural transformations occur on the surface to drive this crossover is far from being understood [1,2,4,5]. Kuroda and Lacmann explained the crossover in crystal growth rates as a result of the formation of a thin quasiliquid layer on the ice surface that could set up at different temperatures depending on the crystal facet [6].The hypothesis that ice could exhibit a quasiliquid layer dates back to Faraday, and the formation of such a layer on solid surfaces is now well characterized theoretically as a premelting surface phase transition [7]. Experimentally, the advent of modern optical and surface scattering techniques has allowed us to gather ample evidence as regards the existence of a premelting liquid film on the surface of ice [8][9][10][11][12][13][14]. Unfortunately, the relatively high vapor pressure of ice makes it very difficult to achieve sizable equilibrium crystals [2], while the presence of impurities has a very large impact on the surface structure [12,15]. Accordingly, many other relevant properties, such as the premelting temperature, the thickness of the quasiliquid layer, or the presence of surface melting remain a matter of debate [8].One particularly important structural property with a large impact on crystal growth rates is the surface roughness [6,16,17]. Contrary to smooth or singular facets, which have a limited number of defects and serve as the basis for most crystal growth models, rough surfaces present diverging height fluctuations, which do not differ macroscopically from those found in a fluid interface. As a result, rough crystal planes with correlation lengths that are larger than the crystallite disappear and become round [18][19][20]. More importantly, as far as the crystal habits and growth forms are concerned, the roughening of a s...

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A study of the ice–water interface using the TIP4P/2005 water model

Cited by 44 publications

References 49 publications

Predictive Calculation of the Crystallization Tendency of Model Pharmaceuticals in the Supercooled State from Molecular Dynamics Simulations

Predictive Calculation of the Crystallization Tendency of Model Pharmaceuticals in the Supercooled State from Molecular Dynamics Simulations

A physically constrained classical description of the homogeneous nucleation of ice in water

Premelting-Induced Smoothening of the Ice-Vapor Interface

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