Melting the ice one layer at a time

Michaelides, Angelos; Slater, Ben

doi:10.1073/pnas.1619259114

Cited by 21 publications

(21 citation statements)

References 20 publications

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“…Bizarrely, some of the water molecules in the outermost two bilayers are more strongly bound to the crystal than molecules in the crystal bulk. These computational results were corroborated in a separate study by Moreira et al 103 Recent SFG measurements 104,105 that showed that the surface of ice has properties resembling supercooled water argue that there are two key temperatures in the premelting regime: ~245 K, which signals the melting of the outermost bilayer, and ~270 K, which signals the melting of the second bilayer. The interpretation is supported by the insight from the work of Sanchez et al 16 , which showed, using molecular dynamics with a polarizable water model, that the first bilayer melts around 235 K and the second around 270 K. Studies by Smit et al and Sanchez et al suggest that around 270 K only the outer two layers are melted and form a film of around 1 nm in thickness.…”

Section: [H1] High Vacuum and Modelling Studiessupporting

confidence: 54%

“…The defect-free crystalline ice surface has an amorphous like quality, which may be related to the evolution of the quasiliquid layer (QLL). Intriguingly, a sum frequency generation (SFG) and molecular dynamic (MD) study by Sanchez et al 16 showed a clear melting of the first two bilayers but no clear melting of the third bilayer, which may be expected to be a consequence of the distinct polarisation character of the outer two layers of ice 105 . Part a, b and c adapted from ref.…”

Section: Figurementioning

confidence: 99%

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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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Section: [H1] High Vacuum and Modelling Studiessupporting

confidence: 54%

Section: Figurementioning

confidence: 99%

Surface premelting of water ice

2019

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“…[35] Secondly, there is also no consensus on the thickness of the premelting layer, which varies between 10 to several hundred Angstroms close to the triple point. [35,49] Thirdly, the nature of the transition itself, which appear likely to be a continuous process as reported recently. [23,25] Finally, It had been apparently unresolved for a long time whether the premelting layer remains finite, [36][37][38] or diverges (surface melting), [27,39] at the triple point.…”

Section: Introductionmentioning

confidence: 75%

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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“…As the controversy regarding the film thickness could start to clarify with agreement between widely different experimental techniques [11,12,[18][19][20], new and exciting observations have been made regarding the properties of the premelting film, both at [15,21,22], and off ice/vapor coexistence [13]. Sanchez et al performed a Sum Frequency Generation experiment (SFG) of the ice surface along the sublimation line and found evidence of a discrete bilayer melting transition [15,17]. Off coexistence, experiments [13] have found a discontinuous transition from a thin to a thick premelting film occurring at watervapor supersaturation that is often known as frustrated complete wetting [23][24][25][26].…”

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confidence: 99%

Rounded Layering Transitions on the Surface of Ice

et al. 2020

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Understanding the wetting properties of premelting films requires knowledge of the film's equation of state, which is not usually available. Here we calculate the disjoining pressure curve of premelting films, and perform a detailed thermodynamic characterization of premelting behavior on ice. Analysis of the density profiles reveals the signature of weak layering phenomena, from one to two and from two to three water molecular layers. However, disjoining pressure curves, which closely follow expectations from a renormalized mean field liquid state theory, show that there are no layering phase transitions in the thermodynamic sense along the sublimation line. Instead, we find that transitions at mean field level are rounded due to capillary wave fluctuations. We see signatures that true first order layering transitions could arise at low temperatures, for pressures between the metastable line of water/vapor coexistence and the sublimation line. The extrapolation of the disjoining pressure curve above water vapor saturation displays a true first order phase transition from a thin to a thick film consistent with experimental observations. arXiv:2003.02945v1 [cond-mat.soft]

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Melting the ice one layer at a time

Cited by 21 publications

References 20 publications

Surface premelting of water ice

Surface premelting of water ice

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

Rounded Layering Transitions on the Surface of Ice

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