Water Accommodation and Desorption Kinetics on Ice

Kong, Xiangrui; Papagiannakopoulos, Panos; Thomson, Erik S.; Markovíc, Nikola; Pettersson, Jan B. C.

doi:10.1021/jp503504e

Cited by 42 publications

(78 citation statements)

References 50 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…Figure 6 summarizes the water accommodation coefficients determined for HxOH-, AcOH-, and HNO 3 -coated ice surfaces together with the bare ice results. 4 Adsorption of nitric acid and AcOH results in α obs values close to unity, and thus, the acids significantly enhance accommodation compared to pure ice. The observed α obs values are comparable for HxOH-covered ice and bare ice, but as illustrated in Figure 5, the underlying kinetics are completely altered by the adsorption of the alcohol, which functions as a relatively inefficient barrier for accommodation as well as desorption of water.…”

Section: Resultsmentioning

confidence: 99%

“…For example, water molecules will, on average, spend approximately 5 ms on an ice surface at 200 K before either desorbing or diffusing into the bulk. 4 Here, we focus on water accommodation on ice and organic surfaces that serve as proxies for the more complex systems expected to be found in the atmosphere. Several studies confirm that α s for water molecules on ice is close to unity due to efficient energy transfer to phonons at surface impact and a relatively high binding energy for water to the ice surface.…”

Section: Introductionmentioning

confidence: 99%

See 1 more Smart Citation

Water Accommodation on Ice and Organic Surfaces: Insights from Environmental Molecular Beam Experiments

et al. 2014

Self Cite

View full text Add to dashboard Cite

Water uptake on aerosol and cloud particles in the atmosphere modifies their chemistry and microphysics with important implications for climate on Earth. Here, we apply an environmental molecular beam (EMB) method to characterize water accommodation on ice and organic surfaces. The adsorption of surface-active compounds including short-chain alcohols, nitric acid, and acetic acid significantly affects accommodation of D2O on ice. n-Hexanol and n-butanol adlayers reduce water uptake by facilitating rapid desorption and function as inefficient barriers for accommodation as well as desorption of water, while the effect of adsorbed methanol is small. Water accommodation is close to unity on nitric-acid- and acetic-acid-covered ice, and accommodation is significantly more efficient than that on the bare ice surface. Water uptake is inefficient on solid alcohols and acetic acid but strongly enhanced on liquid phases including a quasi-liquid layer on solid n-butanol. The EMB method provides unique information on accommodation and rapid kinetics on volatile surfaces, and these studies suggest that adsorbed organic and acidic compounds need to be taken into account when describing water at environmental interfaces.

show abstract

Section: Resultsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Water Accommodation on Ice and Organic Surfaces: Insights from Environmental Molecular Beam Experiments

et al. 2014

Self Cite

View full text Add to dashboard Cite

show abstract

“…This has the beneficial effect that sublimation from the electrodes is at least 10 3 times less than from the sample surfaces and can be neglected, which simplifies the calculation of the deposition rate. Under the well-supported assumption of a sticking probability of unity for water molecules on water ice under the experimental conditions employed here (Batista et al, 2005;Brown et al, 1996;Gibson et al, 2011;Kong et al, 2014), Eq. (A1) can be expressed in terms of the saturation vapor pressure p sat,s over the ice sample surfaces, yielding for the particle mass growth rate…”

Section: Appendix A: Nanoparticle Growth Modelmentioning

confidence: 98%

“…These measurements typically employed a quadrupole mass spectrometer (QMS) and/or a quartz crystal microbalance to measure desorption rates. Desorption rates can be used to infer saturation vapor pressures under the well-supported assumption that the sticking coefficient for water molecules on water ice is unity at these temperatures (Batista et al, 2005;Brown et al, 1996;Gibson et al, 2011;Kong et al, 2014). Measuring water vapor desorption rates at the temperatures under investigation is a challenging task and previous experiments were influenced by contamination issues, showed a very large degree of scattering in the data or yielded unphysically low vapor pressures below that of ice I h (Bryson et al, 1974;Fraser et al, 2001;La Spisa et al, 2001).…”

Section: Comparison To Literature Datamentioning

confidence: 99%

The vapor pressure over nano-crystalline ice

2018

View full text Add to dashboard Cite

Abstract. The crystallization of amorphous solid water (ASW) is known to form nano-crystalline ice. The influence of the nanoscale crystallite size on physical properties like the vapor pressure is relevant for processes in which the crystallization of amorphous ices occurs, e.g., in interstellar ices or cold ice cloud formation in planetary atmospheres, but up to now is not well understood. Here, we present laboratory measurements on the saturation vapor pressure over ice crystallized from ASW between 135 and 190 K. Below 160 K, where the crystallization of ASW is known to form nano-crystalline ice, we obtain a saturation vapor pressure that is 100 to 200 % higher compared to stable hexagonal ice. This elevated vapor pressure is in striking contrast to the vapor pressure of stacking disordered ice which is expected to be the prevailing ice polymorph at these temperatures with a vapor pressure at most 18 % higher than that of hexagonal ice. This apparent discrepancy can be reconciled by assuming that nanoscale crystallites form in the crystallization process of ASW. The high curvature of the nano-crystallites results in a vapor pressure increase that can be described by the Kelvin equation. Our measurements are consistent with the assumption that ASW is the first solid form of ice deposited from the vapor phase at temperatures up to 160 K. Nano-crystalline ice with a mean diameter between 7 and 19 nm forms thereafter by crystallization within the ASW matrix. The estimated crystal sizes are in agreement with reported crystal size measurements and remain stable for hours below 160 K. Thus, this ice polymorph may be regarded as an independent phase for many atmospheric processes below 160 K and we parameterize its vapor pressure using a constant Gibbs free energy difference of (982 ± 182) J mol −1 relative to hexagonal ice.

show abstract

“…These observations suggest that control of bulk accommodation lies not at the interface between the QLL and vapor but at the ice‐like/quasi‐liquid interface. Indeed, a two‐stage kinetic scheme embodying these ideas has been demonstrated to successfully account for accommodation measurements across a wide range of temperatures [ Kong , ; Kong et al , ]. Bolstering this view is evidence that the development and propagation of steps is facet‐specific; i.e., they are processes that are sensitive to the symmetry of the underlying facet [ Libbrecht , , , ; Libbrecht and Rickerby , ]; this implies microscopic influence over those processes.…”

Section: Introductionmentioning

confidence: 99%

A quasi‐liquid mediated continuum model of faceted ice dynamics

et al. 2016

View full text Add to dashboard Cite

We present a quasi‐liquid mediated continuum model for ice growth consisting of partial differential equations informed by molecular dynamics simulations. The main insight from molecular dynamics is the appearance of periodic variations in the equilibrium vapor pressure and quasi‐liquid thickness of the ice/vapor interface. These variations are incorporated in the continuum model as subgrid scale microsurfaces. We show that persistent faceted ice growth in the presence of inhomogeneities in the ambient vapor field is due to a spontaneous narrowing of terraces at facet corners, which compensates for higher ambient water vapor density via feedback between surface supersaturation and quasi‐liquid thickness. We argue that this emergent behavior has the mathematical structure of a stable limit cycle and characterize its robustness in terms of ranges of parameters that support it. Because the model is relevant in the high‐surface‐coverage regime, it serves as a useful complement to the Burton‐Cabrera‐Frank framework. Quantitative aspects and limitations of the model are also discussed.

show abstract

Water Accommodation and Desorption Kinetics on Ice

Cited by 42 publications

References 50 publications

Water Accommodation on Ice and Organic Surfaces: Insights from Environmental Molecular Beam Experiments

Water Accommodation on Ice and Organic Surfaces: Insights from Environmental Molecular Beam Experiments

The vapor pressure over nano-crystalline ice

A quasi‐liquid mediated continuum model of faceted ice dynamics

Contact Info

Product

Resources

About