Molecular Simulations of the Transport of Molecules across the Liquid/Vapor Interface of Water

Garrett, Bruce C.; Schenter, Gregory K.; Morita, Akihiro

doi:10.1021/cr040370w

Cited by 138 publications

(178 citation statements)

References 148 publications

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“…(Note: We presented a similar argument in (Smith et al, 2006) but incorrectly reported a 10 nm square instead of a 1 nm square.) Molecular simulations suggest that the timescale for reorganization of the liquid water surface is on the order of a few picoseconds (Garrett et al, 2006). Therefore, evaporation events are too rare to perturb the liquid surface structure, and the surface should be the same under vacuum as it is in equilibrium.…”

Section: Results and Analysismentioning

confidence: 99%

Determination of the evaporation coefficient of D<sub>2</sub>O

et al. 2008

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Abstract. The evaporation rate of D 2 O has been determined by Raman thermometry of a droplet train (12-15 µm diameter) injected into vacuum (∼10 −5 torr). The cooling rate measured as a function of time in vacuum was fit to a model that accounts for temperature gradients between the surface and the core of the droplets, yielding an evaporation coefficient (γ e ) of 0.57±0.06. This is nearly identical to that found for H 2 O (0.62±0.09) using the same experimental method and model, and indicates the existence of a kinetic barrier to evaporation. The application of a recently developed transition-state theory (TST) model suggests that the kinetic barrier is due to librational and hindered translational motions at the liquid surface, and that the lack of an isotope effect is due to competing energetic and entropic factors. The implications of these results for cloud and aerosol particles in the atmosphere are discussed.

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Section: Results and Analysismentioning

confidence: 99%

Determination of the evaporation coefficient of D<sub>2</sub>O

et al. 2008

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“…We recommend use of the term "surface accommodation coefficient", α s , for the probability of adsorption on a clean surface. Note that the symbol S and terms such as sticking probability or adsorption coefficient are used in the literature Carslaw and Peter, 1997;Davidovits et al, 1995;Garrett et al, 2006;Jayne et al, 1990;Pöschl et al, 2007;Tabazadeh and Turco, 1993;Vieceli et al, 2005), however these terms often lack an unequivocal definition. The term thermal accommodation coefficient, α t , has been used to describe the probability that a molecule accommodates to the thermal energy of the substrate upon adsorption in a single collision model, when a molecule collides with the surface (Li et al, 2001;Vieceli et al, 2005;.…”

Section: Surface Accommodation and Kinetics Of Adsorptionmentioning

confidence: 99%

Evaluated kinetic and photochemical data for atmospheric chemistry: Volume VI – heterogeneous reactions with liquid substrates

et al. 2013

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Abstract. This article, the sixth in the ACP journal series, presents data evaluated by the IUPAC Task Group on Atmospheric Chemical Kinetic Data Evaluation. It covers the heterogeneous processes involving liquid particles present in the atmosphere with an emphasis on those relevant for the upper troposphere/lower stratosphere and the marine boundary layer, for which uptake coefficients and adsorption parameters have been presented on the IUPAC website since 2009. The article consists of an introduction and guide to the evaluation, giving a unifying framework for parameterisation of atmospheric heterogeneous processes. We provide summary sheets containing the recommended uptake parameters for the evaluated processes. The experimental data on which the recommendations are based are provided in data sheets in separate appendices for the four surfaces considered: liquid water, deliquesced halide salts, other aqueous electrolytes and sulfuric acid.

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“…The determination of the surface tension of water by computer simulation has been the subject of several studies. [22][23][24][25][26][27][28][29][30][31][32][33][34][35][36][37][38] In the majority of these studies, a slab of liquid is placed in contact with vapor and the surface tension is computed from a mechanical route which requires the calculation of the pressure tensor. 39 A survey of the literature reveals that values of the surface tension from different authors differ in some cases considerably.…”

Section: Introductionmentioning

confidence: 99%

Surface tension of the most popular models of water by using the test-area simulation method

Vega

Miguel²

2007

The Journal of Chemical Physics

676

105

695

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We consider the calculation of the surface tension from simulations of several models of water, such as the traditional TIP3P, SPC, SPC/E, and TIP4P models, and the new generation of TIP4P-like models including the TIP4P/Ew, TIP4P/Ice, and TIP4P/2005. We employ a thermodynamic route proposed by Gloor et al. ͓J. Chem. Phys. 123, 134703 ͑2005͔͒ to determine the surface tension that involves the estimate of the change in free energy associated with a small change in the interfacial area at constant volume. The values of the surface tension computed from this test-area method are found to be fully consistent with those obtained from the standard mechanical route, which is based on the evaluation of the components of the pressure tensor. We find that most models do not reproduce quantitatively the experimental values of the surface tension of water. The best description of the surface tension is given by those models that provide a better description of the vapor-liquid coexistence curve. The values of the surface tension for the SPC/E and TIP4P/Ew models are found to be in reasonably good agreement with the experimental values. From the present investigation, we conclude that the TIP4P/2005 model is able to accurately describe the surface tension of water over the whole range of temperatures from the triple point to the critical temperature. We also conclude that the test area is an appropriate methodological choice for the calculation of the surface tension not only for simple fluids, but also for complex molecular polar fluids, as is the case of water.

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Molecular Simulations of the Transport of Molecules across the Liquid/Vapor Interface of Water

Cited by 138 publications

References 148 publications

Determination of the evaporation coefficient of D<sub>2</sub>O

Determination of the evaporation coefficient of D<sub>2</sub>O

Evaluated kinetic and photochemical data for atmospheric chemistry: Volume VI – heterogeneous reactions with liquid substrates

Surface tension of the most popular models of water by using the test-area simulation method

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Molecular Simulations of the Transport of Molecules across the Liquid/Vapor Interface of Water

Cited by 138 publications

References 148 publications

Determination of the evaporation coefficient of D&lt;sub&gt;2&lt;/sub&gt;O

Determination of the evaporation coefficient of D&lt;sub&gt;2&lt;/sub&gt;O

Evaluated kinetic and photochemical data for atmospheric chemistry: Volume VI – heterogeneous reactions with liquid substrates

Surface tension of the most popular models of water by using the test-area simulation method

Contact Info

Product

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Determination of the evaporation coefficient of D<sub>2</sub>O

Determination of the evaporation coefficient of D<sub>2</sub>O