Computation of interfacial properties via grand canonical transition matrix Monte Carlo simulation

Grzelak, Eric M.; Errington, Jeffrey R.

doi:10.1063/1.2812285

Cited by 96 publications

(96 citation statements)

References 62 publications

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“…The film areal number density n A in Fig. 2, Inset (blue squares) grows toward the wetting transition at α ' 0.9 (31,33). Interestingly, the water film reaches a mean thickness of about 0.1 nm (converted from an areal density of n A ∼ 3 nm −2 assuming bulk water density in the film), corresponding roughly to a single layer of water molecules, only very close to the wetting transition at a contact angle of roughly θ ' 30°(see SI Text for snapshots of water films).…”

Section: Water Adsorption On a Single Surfacementioning

confidence: 94%

“…In practice, we simulate two surfaces at a large enough surface-surface distance of D = 4 nm so that they do not interfere. This is an important preliminary step, because we will later find stable water wetting films in the asymmetric case of a hydrophilic surface interacting with a hydrophobic surface (30,31). The wetting coefficient k w measures the surface affinity for water and is defined as…”

Section: Water Adsorption On a Single Surfacementioning

confidence: 99%

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From hydration repulsion to dry adhesion between asymmetric hydrophilic and hydrophobic surfaces

Kanduč

Netz

2015

Proc. Natl. Acad. Sci. U.S.A.

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Using all-atom molecular dynamics (MD) simulations at constant water chemical potential in combination with basic theoretical arguments, we study hydration-induced interactions between two overall chargeneutral yet polar planar surfaces with different wetting properties. Whether the water film between the two surfaces becomes unstable below a threshold separation and cavitation gives rise to long-range attraction, depends on the sum of the two individual surface contact angles. Consequently, cavitation-induced attraction also occurs for a mildly hydrophilic surface interacting with a very hydrophobic surface. If both surfaces are very hydrophilic, hydration repulsion dominates at small separations and direct attractive force contribution can-if strong enough-give rise to wet adhesion in this case. In between the regimes of cavitation-induced attraction and hydration repulsion we find a narrow range of contact angle combinations where the surfaces adhere at contact in the absence of cavitation. This dry adhesion regime is driven by direct surface-surface interactions. We derive simple laws for the cavitation transition as well as for the transition between hydration repulsion and dry adhesion, which favorably compare with simulation results in a generic adhesion state diagram as a function of the two surface contact angles.A ccording to the classical Derjaguin-Landau-Verwey-Overbeek (DLVO) theory, the interaction between hydrated surfaces is given by the sum of van der Waals (vdW) and screened electrostatic interactions (1). Although this approach works well in many situations, subnanometer resolved force measurements between individual surfaces demonstrated that additional watermediated interactions are dominant at small separations and depend crucially on the polarity or wetting properties of the surfaces (2-4). Understanding these solvation-induced interactions is still a central issue in all fields concerned with forces between surfaces, colloids, and macromolecular aggregates in water.As is well known, the water film between two hydrophobic surfaces, characterized by water contact angles θ > 90°, becomes freeenergetically unstable below a critical distance and in equilibrium cavitation leads to vapor bubble-induced long-ranged attraction (5-7). Conversely, polar and overall neutral surfaces, characterized by small or vanishing contact angles, exhibit pronounced shortranged repulsive forces, which decay exponentially with a characteristic length in the subnanometer range (8-11). These so-called hydration forces arise from the complex interplay of surface group configurational degrees of freedom, desorption of hydration water from polar surface groups, and ordering of the intersurface water film (4). The understanding of hydration forces has recently been advanced by computer simulations that include explicit water molecules (12)(13)(14).In the absence of direct surface-surface interactions, the transition between cavitation-induced attraction and hydration repulsion should coincide with the contact angle char...

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Section: Water Adsorption On a Single Surfacementioning

confidence: 94%

Section: Water Adsorption On a Single Surfacementioning

confidence: 99%

From hydration repulsion to dry adhesion between asymmetric hydrophilic and hydrophobic surfaces

Kanduč

Netz

2015

Proc. Natl. Acad. Sci. U.S.A.

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“…From the barrier height we have computed line tension ͑␥ L ͒ for different interface lengths ͑L͒ at a particular temperature. In 2D systems the line tension is dependent on the interface length according to the following relation: 18,19 ␥ L = C 1 1…”

Section: Simulation Detailsmentioning

confidence: 99%

Line tension of a two dimensional gas-liquid interface

Santra

Bagchi

2009

The Journal of Chemical Physics

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In two dimensional (2D) gas-liquid systems, the reported simulation values of line tension are known to disagree with the existing theoretical estimates. We find that while the simulation erred in truncating the range of the interaction potential, and as a result grossly underestimated the actual value, the earlier theoretical calculation was also limited by several approximations. When both the simulation and the theory are improved, we find that the estimate of line tension is in better agreement with each other. The small value of surface tension suggests increased influence of noncircular clusters in 2D gas-liquid nucleation, as indeed observed in a recent simulation.

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“…10,[25][26] The test-area method was introduced to calculate γ LV 27 and was extended to the calculation of γ SL in Lennard-Jones systems. 28 We have introduced the phantom-wall method based on thermodynamic integration to obtain W SL .…”

Section: Introductionmentioning

confidence: 99%

Dry-Surface Simulation Method for the Determination of the Work of Adhesion of Solid–Liquid Interfaces

Leroy

Müller‐Plathe

2015

Langmuir

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We introduce a methodology, referred to as the dry-surface method, to calculate the work of adhesion of heterogeneous solid-liquid interfaces by molecular simulation. This method employs a straightforward thermodynamic integration approach to calculate the work of adhesion as the reversible work to turn off the attractive part of the actual solid-liquid interaction potential. It is formulated in such a way that it may be used either to evaluate the ability of force fields to reproduce reference values of the work of adhesion or to optimize force-field parameters with reference values of the work of adhesion as target quantities. The methodology is tested in the case of water on a generic model of nonpolar substrates with the structure of gold. It is validated through a quantitative comparison to phantom-wall calculations and against a previous characterization of the thermodynamics of the gold-water interface. It is found that the work of adhesion of water on nonpolar substrates is a nonlinear function of the microscopic solid-liquid interaction energy parameter. We also comment on the ability of mean-field approaches to predict the work of adhesion of water on nonpolar substrates. In addition, we discuss in detail the information on the solid-liquid interfacial thermodynamics delivered by the phantom-wall approach. We show that phantom-wall calculations yield the solid-liquid interfacial tension relative to the solid surface tension rather than the absolute solid-liquid interfacial tension as previously believed.

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Computation of interfacial properties via grand canonical transition matrix Monte Carlo simulation

Cited by 96 publications

References 62 publications

From hydration repulsion to dry adhesion between asymmetric hydrophilic and hydrophobic surfaces

From hydration repulsion to dry adhesion between asymmetric hydrophilic and hydrophobic surfaces

Line tension of a two dimensional gas-liquid interface

Dry-Surface Simulation Method for the Determination of the Work of Adhesion of Solid–Liquid Interfaces

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