Interfacial Excess Free Energies of Solid–Liquid Interfaces by Molecular Dynamics Simulation and Thermodynamic Integration

Leroy, Frédéric; Santos, Daniel J. V. A. dos; Müller‐Plathe, Florian

doi:10.1002/marc.200800746

Cited by 87 publications

(84 citation statements)

References 36 publications

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“…Considering the results obtained in Section 3.1, we will show that this method leads to the determination of the work of adhesion W SL . We also show that it leads to the solid-liquid interfacial tension relative to the solid surface tension rather than the absolute solid-liquid interfacial tension as we previously assumed in the publications where the method was developed 29,36 and employed. 42,[45][46] In the phantom-wall method, a solid-liquid interface of interest is reversibly turned into another interface by the action of a wall (the phantom wall, modeled through the WCA-PL potential) which repels only liquid molecules.…”

Section: The Phantom-wall Approachmentioning

confidence: 81%

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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Section: The Phantom-wall Approachmentioning

confidence: 81%

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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“…To better understand this behavior, we use the thermodynamic integration (TI) technique (37) to calculate the free energy of the system as a function of two orientation angles ðθ; ϕÞ of a rhombic graphene flake when one of the sharp corners of the flake is fixed at a distance of 0.4 nm above the bilayer (the detailed implementation of the TI method is given in SI Text). Here θ is the angle between the long diagonal axis of the flake and the bilayer within the graphene plane and ϕ is the angle between the vectors normal to the graphene plane and the membrane plane (Fig.…”

Section: Resultsmentioning

confidence: 99%

Graphene microsheets enter cells through spontaneous membrane penetration at edge asperities and corner sites

Yuan

Bussche

et al. 2013

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

679

638

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Understanding and controlling the interaction of graphene-based materials with cell membranes is key to the development of graphene-enabled biomedical technologies and to the management of graphene health and safety issues. Very little is known about the fundamental behavior of cell membranes exposed to ultrathin 2D synthetic materials. Here we investigate the interactions of graphene and few-layer graphene (FLG) microsheets with three cell types and with model lipid bilayers by combining coarse-grained molecular dynamics (MD), all-atom MD, analytical modeling, confocal fluorescence imaging, and electron microscopic imaging. The imaging experiments show edge-first uptake and complete internalization for a range of FLG samples of 0.5-to 10-μm lateral dimension. In contrast, the simulations show large energy barriers relative to k B T for membrane penetration by model graphene or FLG microsheets of similar size. More detailed simulations resolve this paradox by showing that entry is initiated at corners or asperities that are abundant along the irregular edges of fabricated graphene materials. Local piercing by these sharp protrusions initiates membrane propagation along the extended graphene edge and thus avoids the high energy barrier calculated in simple idealized MD simulations. We propose that this mechanism allows cellular uptake of even large multilayer sheets of micrometer-scale lateral dimension, which is consistent with our multimodal bioimaging results for primary human keratinocytes, human lung epithelial cells, and murine macrophages. molecular dynamics simulation | graphene-cell interaction | lipid membrane | edge cutting | corner penetration

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“…60 The surface energy of the water-gas interface is obtained from free energy calculations (free energy perturbation-based phantom-wall algorithm 61,62 ) and interaction energy analyses are carried out for comparison. We would mention that the energy terms in Eq.…”

Section: B Surface Energy Calculation Between Water Monolayer and Sumentioning

confidence: 99%

Linear relationship between water wetting behavior and microscopic interactions of super-hydrophilic surfaces

Liu

Wang

Guo

et al. 2013

The Journal of Chemical Physics

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Using molecular dynamics simulations, we show a fine linear relationship between surface energies and microscopic Lennard-Jones parameters of super-hydrophilic surfaces. The linear slope of the super-hydrophilic surfaces is consistent with the linear slope of the super-hydrophobic, hydrophobic, and hydrophilic surfaces where stable water droplets can stand, indicating that there is a universal linear behavior of the surface energies with the water-surface van der Waals interaction that extends from the super-hydrophobic to super-hydrophilic surfaces. Moreover, we find that the linear relationship exists for various substrate types, and the linear slopes of these different types of substrates are dependent on the surface atom density, i.e., higher surface atom densities correspond to larger linear slopes. These results enrich our understanding of water behavior on solid surfaces, especially the water wetting behaviors on uncharged super-hydrophilic metal surfaces.

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Interfacial Excess Free Energies of Solid–Liquid Interfaces by Molecular Dynamics Simulation and Thermodynamic Integration

Cited by 87 publications

References 36 publications

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

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

Graphene microsheets enter cells through spontaneous membrane penetration at edge asperities and corner sites

Linear relationship between water wetting behavior and microscopic interactions of super-hydrophilic surfaces

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