Arrhenius analysis of anisotropic surface self-diffusion on the prismatic facet of ice

Gladich, Ivan; Pfalzgraff, William; Maršálek, Ondřej; Jungwirth, Pavel; Roeselová, Martina; Neshyba, Steven

doi:10.1039/c1cp22238d

Cited by 32 publications

(62 citation statements)

References 36 publications

(64 reference statements)

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“…The onset temperature of disorder is found to depend on the crystal facet exposed to the vapour phase, for example on the basal plane, the first sign of interfacial disorder occurs about 100 K below the melting point, whereas on the prism plane disorder was observed around T m -80 K (Conde et al, 2008). The thickness of the disorder also shows systematic differences between the different crystal facets (Conde et al, 2008;Pfalzgraff et al, 2011) in agreement with 15 experimental observations (Sect. 2.3.2).…”

Section: Simulations Of Disorder On Pure Icesupporting

confidence: 86%

“…Molecular dynamics simulations show that a disordered layer develops spontaneously 5 at the free surface of ice at temperatures below the melting point (Bolton and Petterson, 2000;Picaud, 2006;Vega et al, 2006;Bishop et al, 2009;Neshyba et al, 2009;Pereyra and Carignano, 2009;Pfalzgraff et al, 2011). This has been observed regardless of the water model and the crystallographic plane exposed to the vapour phase ( Fig.…”

Section: Simulations Of Disorder On Pure Icementioning

confidence: 92%

“…2.3.2). Simulations reveal that the surface disorder begins with a small fraction of water molecules leaving the outermost crystalline layer of ice and becoming mobile as adsorbed molecules on the crystal lattice (Bishop et al, 2009;Pfalzgraff et al, 2011). With increasing temperature, the number of vacancies in the outermost crystalline layer increases, giving rise to aggregates of (increasingly Figures…”

Section: Simulations Of Disorder On Pure Icementioning

confidence: 99%

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Relationship between snow microstructure and physical and chemical processes

Bartels-Rausch¹,

Jacobi²,

Kahan³

et al. 2012

Preprint

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Ice and snow in the environment are important because they not only act as a host to rich chemistry but also provide a matrix for physical exchanges of contaminants within the ecosystem. This review discusses how the structure of snow influences both chemical reactivity and physical processes, which thereby makes snow a unique medium for study. The focus is placed on impacts of the presence of liquid and surface disorder using many experimental studies, simulations, and field observations from the molecular to the micro-scale

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Section: Simulations Of Disorder On Pure Icesupporting

confidence: 86%

Section: Simulations Of Disorder On Pure Icementioning

confidence: 92%

Section: Simulations Of Disorder On Pure Icementioning

confidence: 99%

See 1 more Smart Citation

Relationship between snow microstructure and physical and chemical processes

Bartels-Rausch¹,

Jacobi²,

Kahan³

et al. 2012

Preprint

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show abstract

“…Consequently, techniques sensitive to the outermost surface layers will always get a higher water mobility than methods looking at the bulk of the disordered interface or at grain boundaries; the differences may well span orders of magnitude. Molecular dynamics work by Pfalzgraff et al (2010Pfalzgraff et al ( , 2011 and Gladich et al (2011) confirmed the enhanced mobility of water molecules on free ice surfaces in the temperature range from 230 K to the melting point and provided more details Atmos. Chem.…”

Section: Diffusion Of Water At the Ice Surfacementioning

confidence: 88%

A review of air–ice chemical and physical interactions (AICI): liquids, quasi-liquids, and solids in snow

et al. 2014

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Abstract. Snow in the environment acts as a host to rich chemistry and provides a matrix for physical exchange of contaminants within the ecosystem. The goal of this review is to summarise the current state of knowledge of physical processes and chemical reactivity in surface snow with relevance to polar regions. It focuses on a description of impurities in distinct compartments present in surface snow, such as snow crystals, grain boundaries, crystal surfaces, and liquid parts. It emphasises the microscopic description of the ice surface and its link with the environment. Distinct differences between the disordered air–ice interface, often termed quasi-liquid layer, and a liquid phase are highlighted. The reactivity in these different compartments of surface snow is discussed using many experimental studies, simulations, and selected snow models from the molecular to the macro-scale. Although new experimental techniques have extended our knowledge of the surface properties of ice and their impact on some single reactions and processes, others occurring on, at or within snow grains remain unquantified. The presence of liquid or liquid-like compartments either due to the formation of brine or disorder at surfaces of snow crystals below the freezing point may strongly modify reaction rates. Therefore, future experiments should include a detailed characterisation of the surface properties of the ice matrices. A further point that remains largely unresolved is the distribution of impurities between the different domains of the condensed phase inside the snowpack, i.e. in the bulk solid, in liquid at the surface or trapped in confined pockets within or between grains, or at the surface. While surface-sensitive laboratory techniques may in the future help to resolve this point for equilibrium conditions, additional uncertainty for the environmental snowpack may be caused by the highly dynamic nature of the snowpack due to the fast metamorphism occurring under certain environmental conditions. Due to these gaps in knowledge the first snow chemistry models have attempted to reproduce certain processes like the long-term incorporation of volatile compounds in snow and firn or the release of reactive species from the snowpack. Although so far none of the models offers a coupled approach of physical and chemical processes or a detailed representation of the different compartments, they have successfully been used to reproduce some field experiments. A fully coupled snow chemistry and physics model remains to be developed.

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“…Two types of mechanisms take place in the QLL: in-plane diffusion and hopping among different layers. 17,49 A detailed characterization of the interlayer molecule exchange mechanism can be found in Pfalzgraff et al 17 :…”

Section: Dynamicsmentioning

confidence: 99%

Structure and Dynamics of the Quasi-Liquid Layer at the Surface of Ice from Molecular Simulations

Kling

Donadio

2018

J. Phys. Chem. C

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We characterized the structural and dynamical properties of the quasi-liquid layer (QLL) at the surface of ice by molecular dynamics simulations with a thermodynamically consistent water model. Our simulations show that for three low-index ice surfaces only the outermost molecular layer presents short-range and mid-range disorder and is diffusive. The onset temperature for normal diffusion is much higher than the glass temperature of supercooled water, although the diffusivity of the QLL is higher than that of bulk water at the corresponding temperature. The underlying subsurface layers impose an ordered template, which produces a regular patterning of the ice/water interface at any temperature, and is responsible for the major differences between QLL and bulk water, especially for what concern the dynamics and the mid-range structure of the hydrogen-bonded network. Our work highlights the need of a holistic approach to the characterization of QLL, as a single experimental technique may probe only one specific feature, missing part of the complexity of this fascinating system.

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Arrhenius analysis of anisotropic surface self-diffusion on the prismatic facet of ice

Cited by 32 publications

References 36 publications

Relationship between snow microstructure and physical and chemical processes

Relationship between snow microstructure and physical and chemical processes

A review of air–ice chemical and physical interactions (AICI): liquids, quasi-liquids, and solids in snow

Structure and Dynamics of the Quasi-Liquid Layer at the Surface of Ice from Molecular Simulations

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