Role of van der Waals interactions in adsorption of Xe on Cu(111) and Pt(111)

Lazić, Predrag; Crljen, Željko; Brako, R.; Gumhalter, B.

doi:10.1103/physrevb.72.245407

Cited by 55 publications

(67 citation statements)

References 33 publications

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“…Another test that LDA gives right numbers for wrong reasons can be easily done by shifting the graphene layer away from the Ir surface and noticing that the standard asymptotic dependence of the van der Waals layer-surface attraction energy is not reproduced. Also, by inspecting the curvature of the adsorption energy minimum and comparing it with experimental values shows that LDA does not give the correct result [28,29].…”

Section: Resultsmentioning

confidence: 99%

Rationale for switching to nonlocal functionals in density functional theory

Lazić

Atodiresei

Caciuc

et al. 2012

J. Phys.: Condens. Matter

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Abstract. The Density Functional Theory (DFT) has been steadily improving over the past few decades, becoming the standard tool for electronic structure calculations. The early local functionals (LDA) were eventually replaced by more accurate semi-local functionals (GGA) which are in use today. A major persisting drawback is the lack of the nonlocal correlation which is at the core of dispersive (van der Waals) forces, so that a large and important class of systems remains outside the scope of DFT. The vdW-DF correlation functional of Langreth and Lundqvist published in 2004 was the first nonlocal functional which could be easily implemented. Beyond expectations, the nonlocal functional have brought significant improvement to systems that were believed not to be sensitive to nonlocal correlations. In this paper we use the example of graphene nanodomes growing on Ir(111) surface, where with the increase of the size of the graphene islands the character of the bonding changes from strong chemisorption towards almost pure physisorption. We demonstrate how the seamless character of the vdW-DF functionals makes it possible to treat all regimes selfconsistently, proving to be a systematic and consistent improvement of DFT regardless of the nature of bonding. We also discuss the typical surface science example of CO adsorption on (111) surfaces of metals, which shows that the nonlocal correlation may also be crucial for strongly chemisorbed systems. We briefly discuss open questions, in particular the choice of the most appropriate exchange part of the functional. As the vdW-DF begins to appear implemented selfconsistently in a number of popular DFT codes, with numerical cost close to the GGA calculations, we draw the attention of the DFT community to the advantages and benefits of adoption of this new class of functionals.

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Section: Resultsmentioning

confidence: 99%

Rationale for switching to nonlocal functionals in density functional theory

Lazić

Atodiresei

Caciuc

et al. 2012

J. Phys.: Condens. Matter

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“…in particular, for Xe a general tendency is found [6,[8][9][10][11] for adsorption on metallic surfaces in the low-coordination top sites (this behavior is attributed [6,16] to the delocalization of charge density that increases the Pauli repulsion effect at the hollow sites relative to the top site and lifts the potential well upwards both in energy and height).…”

Section: Introductionmentioning

confidence: 99%

“…We chose the PBE [44] reference DFT functional, which is probably the most popular GGA functional. The problem of choosing the optimal DFT functional, particularly in its exchange component, to be combined with long-range vdW interactions and the related problem of completely eliminating double counting of correlation effects still remain open [19]; however they are expected to be more crucial for adsorption systems characterized by relatively strong adparticle-substrate bonds ("chemisorption") and, for instance, for the determination of the perpendicular vibration frequency [11] than for the equilibrium properties of the physisorbed systems we focus on in our paper.…”

Section: Computational Detailsmentioning

confidence: 99%

“…Rare-gas adsorption on many close-packed metal surfaces, such as Ag(111), Al(111), Cu(111), Pd(111), Pt(111),.. have been extensively studied both experimentally [3][4][5][6] and theoretically [6][7][8][9][10][11][12][13][14][15]. Due to the non-directional character of the vdW interactions that should be dominant in physisorption processes, surface sites that maximize the coordination of the rare-gas adsorbate atom are expected to be the preferred ones, thus favoring the hollow adsorption site.…”

Section: Introductionmentioning

confidence: 99%

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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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“…These authors attributed the on-top site preference to charge polarization of both the Xe atom and underlying noble or transition metal (TM) atom as a consequence of the Pauli repulsion. Lazić et al [20] reported the results of potentials between a Xe and the substrate using the GGA with an intra-fragment treatment of the vdW interaction for models with one monolayer of Xe on the Cu(111) and Pt(111) surfaces, respectively. With the vdW interaction, the minimum separation between the Xe and the on-top Cu (Pt) atom is 3.20 (3.10) Å, compared to the experimental minimum of 3.60 (3.40) Å.…”

Section: Introductionmentioning

confidence: 99%

First principles studies of a Xe atom adsorbed on Nb(110) surface

Dağ

Shaughnessy

Fong

et al. 2012

Physica B: Condensed Matter

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We study adsorption sites of a single Xe adatom on Nb(110) surface using a density functional theory approach: The on-top site is the most favorable position for the adsorption. We compare the binding features of the present study to earlier studies of a Xe adatom on close-packed (111) surface of face-centered cubic metals. The different features are attributed through a microscopic picture to the less than half filled d-states in Nb.

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Role of van der Waals interactions in adsorption of Xe on Cu(111) and Pt(111)

Cited by 55 publications

References 33 publications

Rationale for switching to nonlocal functionals in density functional theory

Rationale for switching to nonlocal functionals in density functional theory

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

First principles studies of a Xe atom adsorbed on Nb(110) surface

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