Temperature Dependence of the Growth Kinetics of Elementary Spiral Steps on Ice Basal Faces Grown from Water Vapor

Inomata, Masahiro; Murata, Ken‐ichiro; Asakawa, Harutoshi; Nagashima, K.; Nakatsubo, Shunichi; Furukawa, Yoshinori; Sazaki, Gen

doi:10.1021/acs.cgd.7b01251

Cited by 15 publications

(37 citation statements)

References 39 publications

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“…This is very much consistent with experimental observations. Indeed, indications of nucleated or spiral growth on the basal facet have been reported in recent years, [81][82][83] confirming the expectations from crystal growth measurements that the basal face of ice is smooth up to the triple point. [80,84] On the contrary, the absence of pII facets in ice crystallites suggests a roughening transition for this face well below the triple point.…”

Section: B Roughnesssupporting

confidence: 76%

Structure and fluctuations of the premelted liquid film of ice at the triple point

et al. 2019

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In this paper we study the structure of the ice/vapor interface in the neighborhood of the triple point for the TIP4P/2005 model. We probe the fluctuations of the ice/film and film/vapor surfaces that separate the liquid film from the coexisting bulk phases at basal, primary prismatic and secondary prismatic planes. The results are interpreted using a coupled sine Gordon plus Interface Hamiltonian model. At large length-scales, the two bounding surfaces are correlated and behave as a single complex ice/vapor interface. For small length, on the contrary, the ice/film and film/vapor surfaces behave very much like independent ice/water and water/vapor interfaces.The study suggests that the basal facet of the TIP4P/2005 model is smooth, the prismatic facet is close to a roughening transition, and the secondary prismatic facet is rough. For the faceted basal face, our fluctuation analysis allows us to estimate the step free energy in good agreement with experiment. Our results allow for a quantitative characterization of the extent to which the adsorbed quasi-liquid layer behaves as water, and explains experimental observations which reveal similar activation energies for crystals grown in bulk vapor or bulk water.

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Section: B Roughnesssupporting

confidence: 76%

Structure and fluctuations of the premelted liquid film of ice at the triple point

et al. 2019

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“…Similarly, the relationship between macroscopic and microscopic observations is still not well-understood. For example, the speed of the layer-by-layer growth of ice surfaces covered with the disordered layers shows a local maximum at ∼ −16 °C, 42 where the second bilayer has been observed to melt, as is discussed above. Connecting such a microscopic observation on the layer-by-layer melting with the macroscopic observation on the layer-by-layer growth of the disordered layers 29,42 is essential to reveal the nature of the disordered layer.…”

Section: Introductionmentioning

confidence: 69%

“…For example, the speed of the layer-by-layer growth of ice surfaces covered with the disordered layers shows a local maximum at ∼ −16 °C, 42 where the second bilayer has been observed to melt, as is discussed above. Connecting such a microscopic observation on the layer-by-layer melting with the macroscopic observation on the layer-by-layer growth of the disordered layers 29,42 is essential to reveal the nature of the disordered layer. The layer-by-layer growth of ice surfaces beneath the QL-film 43 will also provide a deeper insight into the nature of the QL-films.…”

Section: Introductionmentioning

confidence: 69%

The Surface of Ice under Equilibrium and Nonequilibrium Conditions

et al. 2019

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Conspectus The ice premelt, often called the quasi-liquid layer (QLL), is key for the lubrication of ice, gas uptake by ice, and growth of aerosols. Despite its apparent importance, in-depth understanding of the ice premelt from the microscopic to the macroscopic scale has not been gained. By reviewing data obtained using molecular dynamics (MD) simulations, sum-frequency generation (SFG) spectroscopy, and laser confocal differential interference contrast microscopy (LCM-DIM), we provide a unified view of the experimentally observed variation in quasi-liquid (QL) states. In particular, we disentangle three distinct types of QL states of disordered layers, QL-droplet, and QL-film and discuss their nature. The topmost ice layer is energetically unstable, as the topmost interfacial H 2 O molecules lose a hydrogen bonding partner, generating a disordered layer at the ice–air interface. This disordered layer is homogeneously distributed over the ice surface. The nature of the disordered layer changes over a wide temperature range from −90 °C to the bulk melting point. Combined MD simulations and SFG measurements reveal that the topmost ice surface starts to be disordered around −90 °C through a process that the topmost water molecules with three hydrogen bonds convert to a doubly hydrogen-bonded species. When the temperature is further increased, the second layer starts to become disordered at around −16 °C. This disordering occurs not in a gradual manner, but in a bilayer-by-bilayer manner. When the temperature reaches −2 °C, more complicated structures, QL-droplet and QL-film, emerge on the top of the ice surface. These QL-droplets and QL-films are inhomogeneously distributed, in contrast to the disordered layer. We show that these QL-droplet and QL-film emerge only under supersaturated/undersaturated vapor pressure conditions, as partial and pseudopartial wetting states, respectively. Experiments with precisely controlled pressure show that, near the water vapor pressure at the vapor-ice equilibrium condition, no QL-droplet and QL-film can be observed, implying that the QL-droplet and QL-film emerge exclusively under nonequilibrium conditions, as opposed to the disordered layers formed under equilibrium conditions. These findings are connected with many phenomena related to the ice surface. For example, we explain how the disordering of the topmost ice surface governs the slipperiness of the ice surface, allowing for ice skating. Further focus is on the gas uptake mechanism on the ice surface. Finally, we note the unresolved questions and future challenges regarding the ice premelt.

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“…[H1] Heterogeneity at the surface A major experimental breakthrough has come from the work of Gen Sazaki and co-workers. [108][109][110][111]112 Over the last few years, Sazaki et al have pioneered the use of laser confocal microscopy combined with differential interference contrast microscopy to study the surface of ice. One of the many reasons that this work is particularly important is related to the use of a direct local probe to elucidate structural features providing unprecedented insight into features of ice crystals.…”

Section: [H1] High Vacuum and Modelling Studiesmentioning

confidence: 99%

Surface premelting of water ice

2019

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Frozen water has a quasi-liquid layer at its surface that exists even well below the bulk melting temperature; the formation of this layer is termed premelting. The nature of the premelted surface layer, its structure, thickness and how the layer changes with temperature have been debated for over 160 years, since Faraday first postulated the idea of a quasi-liquid layer on ice. Here we briefly review current opinion and evidence on premelting at ice surfaces, gathering data from experiment and computer simulations. In particular, spectroscopy, microscopy and simulation have recently made important contributions to our current understanding of this field. The identification of premelting inhomogeneities, where portions of the surface are quasi-liquid-like and other parts of the surface are decorated with liquid droplets is an intriguing recent development. Untangling the interplay of surface structure, supersaturation and surface defects is currently a major challenge. Similarly, understanding the coupling of surface structure with reactivity at the surface and crystal growth is a pressing problem in understanding the behaviour and formation of ice on Earth.

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Temperature Dependence of the Growth Kinetics of Elementary Spiral Steps on Ice Basal Faces Grown from Water Vapor

Cited by 15 publications

References 39 publications

Structure and fluctuations of the premelted liquid film of ice at the triple point

Structure and fluctuations of the premelted liquid film of ice at the triple point

The Surface of Ice under Equilibrium and Nonequilibrium Conditions

Surface premelting of water ice

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