Seeding approach to crystal nucleation

Espinosa, Jorge R.; Vega, Carlos; Valeriani, Chantal; Sanz, Eduardo

doi:10.1063/1.4939641

Cited by 175 publications

(310 citation statements)

References 89 publications

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“…There are also many interests on how ice polymorphs are selected upon ice nucleation [227,228,[230][231][232]. Besides this problem of polymorph selection, the estimation of the barrier height and critical nucleus size is also an important issue and recently there have been many efforts toward this direction [229,[232][233][234][235][236][237]. A link between the so-called Widom line [238], or the thermodynamic anomalies associated with the liquidliquid transition, and the ice nucleation process was also suggested [239].…”

Section: Local Structural Ordering and Homogeneous Crystal Nucleationmentioning

confidence: 99%

Crystal nucleation as the ordering of multiple order parameters

Russo

Tanaka

2016

The Journal of Chemical Physics

100

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Nucleation is an activated process in which the system has to overcome a free energy barrier in order for a first-order phase transition between the metastable and the stable phases to take place. In the liquid-to-solid transition the process occurs between phases of different symmetry, and it is thus inherently a multi-dimensional process, in which all symmetries are broken at the transition. In this Focus Article, we consider some recent studies which highlight the multi-dimensional nature of the nucleation process. Even for a single-component system, the formation of solid crystals from the metastable melt involves fluctuations of two (or more) order parameters, often associated with the decoupling of positional and orientational symmetry breaking. In other words, we need at least two order parameters to describe the free-energy of a system including its liquid and crystalline states. This decoupling occurs naturally for asymmetric particles or directional interactions, focusing here on the case of water, but we will show that it also affects spherically symmetric interacting particles, such as the hard-sphere system. We will show how the treatment of nucleation as a multi-dimensional process has shed new light on the process of polymorph selection, on the effect of external fields on the nucleation process, and on glass-forming ability.

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Section: Local Structural Ordering and Homogeneous Crystal Nucleationmentioning

confidence: 99%

Crystal nucleation as the ordering of multiple order parameters

Russo

Tanaka

2016

The Journal of Chemical Physics

100

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“…1,82 Studies with the TIP4P family of models yield values averaged across several faces ranging between 26.5 ± 0.4 to 29.8 ± 0.8 mJ m −2 , 80,82,83 whereas the mW model of water yields somewhat higher values of 35.5 ± 2.5 mJ m −2 . 84 Estimates of the interfacial energy based on the critical cluster size of hexagonal ice in TIP4P/2005 and TIP4P/ice water models yield an interfacial free energy of 29 ± 3 mJ m −2 . 85 Hence, our estimate of the interfacial energy at melting is at the low end of, but consistent with, the various predictions.…”

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

101

152

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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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“…We compute J hom by plugging parameters obtained by simulations into the expressions given by Classical Nucleation Theory (CNT), 39-42 a combination we call Seeding. 32 The CNT rate is given by:…”

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confidence: 99%

“…The γ iw thus obtained has proven to give correct values for the nucleation rate when combined with Classical Nucleation Theory. 32 Therefore, the γ iw we use for spherical critical clusters at supercooled conditions implicitly includes curvature and temperature corrections to that of a flat interface at coexistence.…”

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Homogeneous Ice Nucleation Rate in Water Droplets

2018

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To predict the radiative forcing of clouds it is necessary to know the rate with which ice homogeneously nucleates in supercooled water. Such rate is often measured in drops to avoid the presence of impurities. At large supercooling small (nanoscopic) drops must be used to prevent simultaneous nucleation events. The pressure inside such drops is larger than the atmospheric one by virtue of the Laplace equation. In this work, we take into account such pressure raise in order to predict the nucleation rate in droplets using the TIP4P/Ice water model. We start from a recent estimate of the maximum drop size that can be used at each supercooling avoiding simultaneous nucleation events [Espinosa et al. J. Chem. Phys., 2016]. We then evaluate the pressure inside the drops with the Laplace equation. Finally, we obtain the rate as a function of the supercooling by interpolating our previous results for 1 and 2000 bar [Espinosa et al. Phys. Rev. Lett. 2016] using the Classical Nucleation Theory expression for the rate.This requires, in turn, interpolating the ice-water interfacial free energy and chemical potential difference. The TIP4P/Ice rate curve thus obtained is in good agreement with most droplet-based experiments. In particular, we find a good agreement with measurements performed using nanoscopic drops, that are currently under debate. The

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Seeding approach to crystal nucleation

Cited by 175 publications

References 89 publications

Crystal nucleation as the ordering of multiple order parameters

Crystal nucleation as the ordering of multiple order parameters

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

Homogeneous Ice Nucleation Rate in Water Droplets

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