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Register a new userNon-additivity of van der Waals forces on liquid surfaces
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Added by
Prashanth Venkataram
Publication date
2016
fields
Physics
and research's language is
English
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We present an approach for modeling nanoscale wetting and dewetting of liquid surfaces that exploits recently developed, sophisticated techniques for computing van der Waals (vdW) or (more generally) Casimir forces in arbitrary geometries. We solve the variational formulation of the Young--Laplace equation to predict the equilibrium shapes of fluid--vacuum interfaces near solid gratings and show that the non-additivity of vdW interactions can have a significant impact on the shape and wetting properties of the liquid surface, leading to very different surface profiles and wetting transitions compared to predictions based on commonly employed additive approximations, such as Hamaker or Derjaguin approximations.
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A version of the Greens functions theory of the Van der Waals forces which can be conveniently used in the presence of spatial dispersion is presented. The theory is based on the fluctuation-dissipation theorem and is valid for interacting bodies, separated by vacuum. Objections against theories acounting for the spatial dispersion are discussed.
The fundamental ideas for a non-local density functional theory -- capable of reliably capturing van der Waals interaction -- were already conceived in the 1990s. In 2004, a seminal paper introduced the first practical non-local exchange-correlation functional called vdW-DF, which has become widely successful and laid the foundation for much further research. However, since then, the functional form of vdW-DF has remained unchanged. Several successful modifications paired the original functional with different (local) exchange functionals to improve performance and the successor vdW-DF2 also updated one internal parameter. Bringing together different insights from almost two decades of development and testing, we present the next-generation non-local correlation functional called vdW-DF3, in which we change the functional form while staying true to the original design philosophy. Although many popular functionals show good performance around the binding separation of van der Waals complexes, they often result in significant errors at larger separations. With vdW-DF3, we address this problem by taking advantage of a recently uncovered and largely unconstrained degree of freedom within the vdW-DF framework that can be constrained through empirical input, making our functional semi-empirical. For two different parameterizations, we benchmark vdW-DF3 against a large set of well-studied test cases and compare our results with the most popular functionals, finding good performance in general for a wide array of systems and a significant improvement in accuracy at larger separations. Finally, we discuss the achievable performance within the current vdW-DF framework, the flexibility in functional design offered by vdW-DF3, as well as possible future directions for non-local van der Waals density functional theory.
In inhomogeneous dielectric media the divergence of the electromagnetic stress is related to the gradients of varepsilon and mu, which is a consequence of Maxwells equations. Investigating spherically symmetric media we show that this seemingly universal relationship is violated for electromagnetic vacuum forces such as the generalized van der Waals and Casimir forces. The stress needs to acquire an additional anomalous pressure. The anomaly is a result of renormalization, the need to subtract infinities in the stress for getting a finite, physical force. The anomalous pressure appears in the stress in media like dark energy appears in the energy-momentum tensor in general relativity. We propose and analyse an experiment to probe the van der Waals anomaly with ultracold atoms. The experiment may not only test an unusual phenomenon of quantum forces, but also an analogue of dark energy, shedding light where nothing is known empirically.
We analyse van der Waals interactions between a pair of dielectrically anisotropic plane-layered media interacting across a dielectrically isotropic solvent medium. We develop a general formalism based on transfer matrices to investigate the van der Waals torque and force in the limit of weak birefringence and dielectric matching between the ordinary axes of the anisotropic layers and the solvent. We apply this formalism to study the following systems: (i) a pair of single anisotropic layers, (ii) a single anisotropic layer interacting with a multilayered slab consisting of alternating anisotropic and isotropic layers, and (iii) a pair of multilayered slabs each consisting of alternating anisotropic and isotropic layers, looking at the cases where the optic axes lie parallel and/or perpendicular to the plane of the layers. For the first case, the optic axes of the oppositely facing anisotropic layers of the two interacting slabs generally possess an angular mismatch, and within each multilayered slab the optic axes may either be the same, or undergo constant angular increments across the anisotropic layers. In particular, we examine how the behaviors of the van der Waals torque and force can be tuned by adjusting the layer thicknesses, the relative angular increment within each slab, and the angular mismatch between the slabs.
The exfoliation of two naturally occurring van der Waals minerals, graphite and molybdenite, arouse an unprecedented level of interest by the scientific community and shaped a whole new field of research: 2D materials research. Several years later, the family of van der Waals materials that can be exfoliated to isolate 2D materials keeps growing, but most of them are synthetic. Interestingly, in nature plenty of naturally occurring van der Waals minerals can be found with a wide range of chemical compositions and crystal structures whose properties are mostly unexplored so far. This Perspective aims to provide an overview of different families of van der Waals minerals to stimulate their exploration in the 2D limit.
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