Van der Waals interactions at surfaces by density functional theory using Wannier functions

Silvestrelli, Pier Luigi; Benyahia, Karima; Grubišić, Sonja; Ancilotto, Francesco; Toigo, Flavio

doi:10.1063/1.3077288

Cited by 57 publications

(69 citation statements)

References 40 publications

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“…The atomic vdW radii in g TS in eq 58 are replaced by distances from the centers of the MLWFs at which n A (r) falls below a predetermined threshold; the choice for this distance was the subject of a later modification. 220 The MLWF partitioning used in vdW-WF significantly differs from the atomic partitioning used in the XDM and TS models. Given that the ALL polarizability functional is nonlinear in the input density (α ALL [n 1 + n 2 ] ≠ α ALL [n 1 ] + α ALL [n 2 ]), using it with the individual fragment densities as the input constitutes a different scheme than evaluating the functional integrand with the total density and then partitioning the integral according to the MLWF fragments.…”

Section: Chemical Reviewsmentioning

confidence: 99%

First-Principles Models for van der Waals Interactions in Molecules and Materials: Concepts, Theory, and Applications

2017

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Noncovalent van der Waals (vdW) or dispersion forces are ubiquitous in nature and influence the structure, stability, dynamics, and function of molecules and materials throughout chemistry, biology, physics, and materials science. These forces are quantum mechanical in origin and arise from electrostatic interactions between fluctuations in the electronic charge density. Here, we explore the conceptual and mathematical ingredients required for an exact treatment of vdW interactions, and present a systematic and unified framework for classifying the current first-principles vdW methods based on the adiabatic-connection fluctuation−dissipation (ACFD) theorem (namely the Rutgers−Chalmers vdW-DF, Vydrov−Van Voorhis (VV), exchange-hole dipole moment (XDM), Tkatchenko−Scheffler (TS), many-body dispersion (MBD), and random-phase approximation (RPA) approaches). Particular attention is paid to the intriguing nature of many-body vdW interactions, whose fundamental relevance has recently been highlighted in several landmark experiments. The performance of these models in predicting binding energetics as well as structural, electronic, and thermodynamic properties is connected with the theoretical concepts and provides a numerical summary of the state-of-the-art in the field. We conclude with a roadmap of the conceptual, methodological, practical, and numerical challenges that remain in obtaining a universally applicable and truly predictive vdW method for realistic molecular systems and materials.

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Section: Chemical Reviewsmentioning

confidence: 99%

First-Principles Models for van der Waals Interactions in Molecules and Materials: Concepts, Theory, and Applications

2017

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“…For a better accuracy, as done in previous applications on adsorption processes [24,25,27,28,30], we have also included the interactions of the MLWFs of the physisorbed fragments not only with the MLWFs of the underlying surface, within the reference supercell, but also with a sufficient number of periodically-repeated surface MLWFs (in any case, given the R −6 decay of the vdW interactions, the convergence with the number of repeated images is rapidly achieved). Electron-ion interactions were described using ultrasoft pseudopotentials by explicitly including 11 valence electrons per Ag, Au, and Cu atom.…”

Section: Computational Detailsmentioning

confidence: 99%

“…[19][20][21]). We have developed a family of such methods, all based on the generation of the Maximally Localized Wannier Functions (MLWFs) [22], successfully applied to a variety of systems, including small molecules, water clusters, graphite and graphene, water layers interacting with graphite, interfacial water on semiconducting substrates, hydrogenated carbon nanotubes, molecular solids, and the interaction of rare gases and small molecules with metal surfaces [23][24][25][26][27][28][29][30][31][32][33][34][35]. Of a particular value is the possibility of dealing with metal surfaces; in fact insulating surfaces could be somehow treated even using atom-based semiempirical approaches where an approximately derived R −6 term, multiplied by a suitable short-range damping function, is explicitly introduced.…”

Section: Introductionmentioning

confidence: 99%

Van Der Waals-Corrected Density Functional Theory Simulation of Adsorption Processes on Noble-Metal Surfaces: Xe on Ag(111), Au(111), and Cu(111)

Silvestrelli¹,

Ambrosetti²

2016

J Low Temp Phys

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The DFT/vdW-WF2s1 method based on the generation of localized Wannier functions, recently developed to include the van der Waals interactions in the Density Functional Theory and describe adsorption processes on metal surfaces by taking metal-screening effects into account, is applied to the case of the interaction of Xe with noble-metal surfaces, namely Ag(111), Au(111), and Cu(111).The study is also repeated by adopting the DFT/vdW-QHO-WF variant relying on the Quantum Harmonic Oscillator model which describes well many-body effects. Comparison of the computed equilibrium binding energies and distances, and the C 3 coefficients characterizing the adatomsurface van der Waals interactions, with available experimental and theoretical reference data shows that the methods perform well and elucidate the importance of properly including screening effects. The results are also compared with those obtained by other vdW-corrected DFT schemes, including PBE-D, vdW-DF, vdW-DF2, rVV10, and by the simpler Local Density Approximation (LDA) and semilocal (PBE) Generalized Gradient Approximation (GGA) approaches.

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“…Silvestrelli et al 68 have studied the adsorption of Ar on graphite and of Ar, He (and also H 2 molecule) on the Al(100) surface. A representation of Al(100) and the adsorption sites on this surface are shown in the topmost panel of Fig.…”

Section: Adsorption Of Noble Gas Atomsmentioning

confidence: 99%

Accounting for van der Waals interactions between adsorbates and surfaces in density functional theory based calculations: selected examples

2013

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This article reviews the different density functional theory (DFT) methods available in the literature for dealing with dispersion interactions and recent applications of DFT approaches including van der Waals corrections in the study of the interaction of atoms and molecules with several different surfaces. Focus is given to the interaction of atoms and molecules with metal, metal oxide and graphite surfaces or more complex systems. It will be shown that DFT approaches including van der Waals corrections present significant advances over standard exchange correlation functionals for treating systems dominated by weak interactions.

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Van der Waals interactions at surfaces by density functional theory using Wannier functions

Cited by 57 publications

References 40 publications

First-Principles Models for van der Waals Interactions in Molecules and Materials: Concepts, Theory, and Applications

First-Principles Models for van der Waals Interactions in Molecules and Materials: Concepts, Theory, and Applications

Van Der Waals-Corrected Density Functional Theory Simulation of Adsorption Processes on Noble-Metal Surfaces: Xe on Ag(111), Au(111), and Cu(111)

Accounting for van der Waals interactions between adsorbates and surfaces in density functional theory based calculations: selected examples

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