Ice crystallization in water’s “no-man’s land”

Moore, Emily B.; Molinero, Valeria

doi:doi:10.1063/1.3451112

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Negative and positive ion trapping by isotopic molecules in cryocrystals in case of solid parahydrogen containing electrons and H₆⁺ radical cations

We performed electron spin resonance studies of trapped electrons and H6+ radical cations produced by radiolysis of solid parahydrogen (p-H2), p-H2−ortho-D2 (o-D2), and p-H2−HD mixtures. Yields of trapped electrons, H6+ radical cations, and its isotopic analogs H6−nDn+ (4 ≥ n ≥ 1) increased with increasing o-D2 and HD concentrations in solid p-H2. Electrons were found trapped near an o-D2 or an HD in solid p-H2 due to the long-range charge-induced dipole and quadrupole interactions between elec...

Homogeneous water nucleation in a laminar flow diffusion chamber

Homogeneous nucleation rates of water at temperatures between 240 and 270 K were measured in a laminar flow diffusion chamber at ambient pressure and helium as carrier gas. Being in the range of 102–106 cm−3 s−1, the experimental results extend the nucleation rate data from literature consistently and fill a pre-existing gap. Using the macroscopic vapor pressure, density, and surface tension for water we calculate the nucleation rates predicted by classic nucleation theory (CNT) and by the empi...

The crystallization of water at 180 K is studied through large-scale molecular dynamics simulations with the monatomic water model mW. This temperature is in the middle of water’s “no-man’s land,” where rapid ice crystallization prevents the elucidation of the structure of liquid water and its transformation into ice with state of the art experimental methods. We find that critical ice nuclei (that contain less than ten water molecules) form in a time scale shorter than the time required for the relaxation of the liquid, suggesting that supercooled liquid water cannot be properly equilibrated in this region. We distinguish three stages in the crystallization of water at 180 K: concurrent nucleation and growth of ice, followed by consolidation that decreases the number density of ice nuclei, and finally, slow growth of the crystallites without change in their number density. The kinetics of the transformation along the three stages is well described by a single compacted exponential Avrami equation with n ≈ 1.7. This work confirms the coexistence of ice and liquid after water is crystallized in “no-man’s land”: the formation of ice plateaus when there is still 15%–20% of liquid water in the systems, thinly dispersed between ice I crystals with linear dimensions ranging from 3 to 10 nm. We speculate that the nanoscopic size of the crystallites decreases their melting point and slows their evolution toward the thermodynamically most stable fully crystalline state.

Article Outline

INTRODUCTION
MODEL AND METHODS
1. Water potential
2. Simulation methods
3. Isothermal crystallization of instantaneously quenched liquid water
4. Isothermal crystallization of warmed-up LDA glass
5. Identification of ice
6. Identification of ice nuclei
7. Diffusion
8. Radial distribution function
9. Radius of gyration and nonsphericity
RESULTS AND DISCUSSION
1. Kinetics of ice crystallization
2. Mechanism of crystallization of ice
CONCLUSIONS

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KEYWORDS and PACS

Keywords

crystallisation, crystallites, density, freezing, melting point, molecular dynamics method, nanostructured materials, water

PACS

64.70.D-

Solid-liquid transitions
61.20.Ja

Computer simulation of liquid structure
61.43.Bn

Structural modeling: serial-addition models, computer simulation
81.30.-t

Phase diagrams and microstructures developed by solidification and solid-solid phase transformations
64.70.dj

Melting of specific substances

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http://link.aip.org/link/doi/10.1063/1.3451112

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0021-9606 (print)

1089-7690 (online)

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American Institute of Physics

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