Interaction of Hydrogen Chloride with Ice Surfaces:  The Effects of Grain Size, Surface Roughness, and Surface Disorder

McNeill, V. Faye; Geiger, Franz M.; Loerting, Thomas; Trout, Bernhardt L.; Molina, Luisa T.; Molina, Mario J.

doi:10.1021/jp068914g

Cited by 55 publications

(111 citation statements)

References 111 publications

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“…Recently, direct laboratory evidence showed that HCl-and HNO 3 -ice interactions are highly dependent on the surface state of the ice substrate (McNeill et al, 2006(McNeill et al, , 2007Moussa et al, 2013). This pioneering work overcomes the main limitation of the above studies, by providing a link between Atmos.…”

Section: Uptake To the Disordered Interfacementioning

confidence: 93%

“…3.1 and 3.2), and experimentally verified by optical reflectance (Elbaum et al, 1993), by ellipsometry (McNeill et al, 2006(McNeill et al, , 2007, and directly by partial electron yield near-edge X-ray absorption fine structure (NEXAFS) (Bluhm et al, 2002). Observations of impurity-amplified or -induced disorder at ice surfaces depend on experimental conditions, the method of experimental probing, and on the type of impurity.…”

Section: The Thickness and Effect Of Impuritiesmentioning

confidence: 96%

“…We refer the reader to Huthwelker et al (2006) for a detailed discussion on experimental methods. In those experiments probing surface reactions is usually achieved by using ice samples with a high surface-to-volume ratio (e. g. Abbatt et al, 1992;McNeill et al, 2007;BartelsRausch et al, 2010;Kurková et al, 2011). However, these studies give no direct evidence for the surface reactions, as discussed in Bartels-Rausch et al (2011).…”

Section: Physical Environmentsmentioning

confidence: 99%

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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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Section: Uptake To the Disordered Interfacementioning

confidence: 93%

Section: The Thickness and Effect Of Impuritiesmentioning

confidence: 96%

Section: Physical Environmentsmentioning

confidence: 99%

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

et al. 2014

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“…On the contrary, McNeill et al (McNeill et al 2007) concluded that the HCl adsorption and surface-to-bulk flux on polar stratospheric cloud ice particles is slightly influenced by the QLL thickness, which is allowed to vary between 1 nm and 300 nm.…”

Section: Resultsmentioning

confidence: 99%

“…As an example, Molina and coworkers (McNeill et al 2007) studied the interaction of HCl with polar stratospheric cloud ice particles and found that the solute can induce the formation of a QLL at the characteristic temperatures of these clouds.…”

mentioning

confidence: 99%

The Quasi-Liquid Layer of ice revisited: the role of temperature gradients and tip chemistry in AFM studies

Constantin¹,

Gianetti²,

Longinotti³

et al. 2018

Preprint

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Abstract. In this work, we present new results of Atomic Force Microscopy (AFM) force curves over pure ice at different temperatures, performed with two different environmental chambers and different kind of AFM tips. Our results provide insight to resolve the controversy on the interpretation of experimental AFM curves on the ice-air interface for determining the thickness of the quasi-liquid layer (QLL). The use of a mini environmental chamber, that provides an accurate control of the temperature and humidity of the gases in contact with the sample, allowed us for the first time to get force curves over 15 the ice-air interface without jump-in (jumps of the tip onto the ice surface, widely observed in previous studies). These results suggest a QLL thickness below 1 nm within the explored temperature range (-7 ºC to -2 ºC). This upper bound is significantly lower than most of the previous AFM results, which suggests that previous authors overestimate the equilibrium QLL thickness, due to temperature gradients, or indentation of ice during the jump-in. Additionally, we proved that the hydrophobicity of AFM tips affects significantly the results of the experiments. Overall, this work shows that, if one 20 chooses properly the experimental conditions, the QLL thicknesses obtained by AFM lay over the lower bound of the highly disperse results reported in the literature. This allows estimating upper boundaries for the QLL thicknesses, which is relevant to validate QLL theories, and to improve multiphase atmospheric chemistry models.

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Effects of injected ice particles in the lower stratosphere on the Antarctic ozone hole

et al. 2015

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The Antarctic ozone hole will continue to be observed in the next 35-50 years, although the emissions of chlorofluorocarbons (CFCs) have gradually been phased out during the last two decades. In this paper, we suggest a geo-engineering approach that will remove substantial amounts of hydrogen chloride (HCl) from the lower stratosphere in fall, and hence limit the formation of the Antarctic ozone hole in late winter and early spring. HCl will be removed by ice from the atmosphere at temperatures higher than the threshold under which polar stratospheric clouds (PSCs) are formed if sufficiently large amounts of ice are supplied to produce water saturation. A detailed chemical-climate numerical model is used to assess the expected efficiency of the proposed geo-engineering method, and specifically to calculate the removal of HCl by ice particles. The size of ice particles appears to be a key parameter: larger particles (with a radius between 10 and 100 μm) appear to be most efficient for removing HCl. Sensitivity studies lead to the conclusions that the ozone recovery is effective when ice particles are supplied during May and June in the latitude band ranging from 70 ∘ S to 90 ∘ S and in the altitude layer ranging from 10 to 26 km. It appears, therefore, that supplying ice particles to the Antarctic lower stratosphere could be effective in reducing the depth of the ozone hole. In addition, photodegradation of CFCs might be accelerated when ice is supplied due to enhanced vertical transport of this efficient greenhouse gas.

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Interaction of Hydrogen Chloride with Ice Surfaces: The Effects of Grain Size, Surface Roughness, and Surface Disorder

Cited by 55 publications

References 111 publications

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

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

The Quasi-Liquid Layer of ice revisited: the role of temperature gradients and tip chemistry in AFM studies

Effects of injected ice particles in the lower stratosphere on the Antarctic ozone hole

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