A New Look at Homogeneous Ice Nucleation in Supercooled Water Drops

Pruppacher, H. R.

doi:10.1175/1520-0469(1995)052<1924:anlahi>2.0.co;2

Cited by 212 publications

(272 citation statements)

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“…For example, Pruppacher 88 and Zobrist et al 27 produce nucleation rates many orders of magnitude larger than the values observed by Laksmono et al 7 and predicted by our parameterization below 237 K. In particular, Pruppacher 88 predicts that the increase in J hom with decreasing temperature accelerates below 231 K, whereas our parameterization predicts that the nucleation rate should start to decrease with decreasing temperature at around 229 K. The much smaller values of J hom predicted by our parameterization are a result of the strong decrease in translational self-diffusion predicted by the power law fit. We justify the use of a power law on the basis that many thermodynamic and transport properties of supercooled FIG.…”

Section: Discussioncontrasting

confidence: 53%

“…4. The new CNT-based homogeneous ice nucleation rate parameterization J hom (T ) compared to other parameterizations 1,7,27,88 in the literature. While we provide all the individual terms and their parameters of our CNT-based parameterization for J hom in Tables I-VI of the Appendix, it is sometimes necessary to use a more computationally cheaper, i.e., simpler, parameterization.…”

Section: Discussionmentioning

confidence: 99%

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

Koop

Murray

2016

The Journal of Chemical Physics

122

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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Section: Discussioncontrasting

confidence: 53%

Section: Discussionmentioning

confidence: 99%

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

Koop

Murray

2016

The Journal of Chemical Physics

122

155

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“…Here we suggest that using the sulfuric acid viscosity parameters in place of supercooled water in (7) can yield a reasonable value for the diffusion activation energy of single water molecules in solution based on the viscous flow assumption [Pruppacher, 1972]. However, recent studies [Pruppacher, 1995] indicate that the diffusion of water Where m s is the sulfuric acid molality, w s is the sulfuric acid weight percent, and y functions are given in Table 2 The application of the Antonoffs rule of surface tension is another procedure that is commonly used to determine the interface energy between two condensed liquid phases [Adamson, 1990]. This rule states that the interfacial energy between two mutually saturated liquids is given by the absolute difference of their respective surface tensions against vapor (air).…”

Section: B ] X!(t Ws) = A(ws)t • Exp T-to(ws) (6)mentioning

confidence: 99%

A model description for cirrus cloud nucleation from homogeneous freezing of sulfate aerosols

Tabazadeh¹,

Jensen²,

Toon³

1997

J. Geophys. Res.

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Abstract. Classical nucleation theory for homogeneous freezing as well as recent laboratory data are used to formulate an algorithm for ice nucleation from an aqueous sulfuric acid solution droplet. A new pammeterized function is derived from re•nt thermodynamic data to express the variation of stflfiafc acid solution composition with temperature and relative humidity. This function is then used to derive critical ice nucleation parameters from recent laboratory data. The critical nucleation parameters are used in a classical nucleation theory to derive the diffusion activation energy of water molecules in a sulfuric acid solution from the measurements. The derived diffusion activation energy of water molecules in a sulfuric acid solution does not agree with the diffusion activation energy calculated from a viscous flow formulation that is commonly used in classical nucleation rate calculations. Our restfits show that ice nucleation in a stdfate droplet occurs when the interface energy of ice against the stdfate solution is approximately 17 dyn cm 4. We calculate that a supersaturation ratio of about 1.3 to 1.5 is required to nucleate ice from an aqueous stdfuric acid solution droplet in the temperature range of about 185 to 240 K. This supersaturation corresponds to a supercooling of a stdfate solution to about 2 to 3 K below the equilibrium condensation point of ice. Simple functions are given for estimating the nucleation point of ice in the upper troposphere. The differences between previous parameterizations and this work are discussect

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“…13 When, for example, Krämer et al 10 systematically varied the temperature, the measured ice crystal nucleation rate increased by a factor of 70 as the temperature was reduced by just 1 K. Precise control of the thermodynamic state is thus critical to the measurement of nucleation rates. Only able to regulate the relative humidity ͑RH͒ within ±0.5% RH during repeated experiments, Hamza et al 9 reported nucleation rates that varied by a factor of 300.…”

Section: Introductionmentioning

confidence: 99%

Single-particle levitation system for automated study of homogeneous solute nucleation

Olsen

Flagan

Kornfield

2006

Review of Scientific Instruments

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We present an instrument that addresses two critical requirements for quantitative measurements of the homogeneous crystal nucleation rate in supersaturated aqueous solution. First, the need to perform repeated measurements of nucleation incubation times is met by automating experiments to enable programmable cycling of thermodynamic conditions. Second, the need for precise and robust control of the chemical potential in supersaturated aqueous solution is met by implementing a novel technique for regulating relative humidity. The apparatus levitates and weighs micron-sized samples in an electric field, providing access to highly supersaturated states. We report repeated observations of the crystal nucleation incubation time in a supersaturated aqueous sodium chloride droplet, from which we infer the nucleation rate.

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A New Look at Homogeneous Ice Nucleation in Supercooled Water Drops

Cited by 212 publications

References 0 publications

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

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

A model description for cirrus cloud nucleation from homogeneous freezing of sulfate aerosols

Single-particle levitation system for automated study of homogeneous solute nucleation

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