Van Der Waals Density Functionals for Graphene Layers and Graphite

Birowska, Magdalena; Milowska, Karolina Z.; Majewski, J. A.

doi:10.12693/aphyspola.120.845

Cited by 90 publications

(62 citation statements)

References 21 publications

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“…In particular, the S‐ab site is more favorable than the S‐aa site by nearly 0.05 eV. This type of configuration corresponds to the Bernal's AB stacking for two adjacent graphene sheets in graphite . Therefore, the adsorption of DA on regular graphene shows behavior resembling that of nucleobases, that is, the stacking configurations are favoring over the perpendicular or “T” configurations; the former being related to the presence of π–π interactions, the latter to CH⋅⋅⋅π interactions .…”

Section: Resultsmentioning

confidence: 95%

Noncovalent Interactions between Dopamine and Regular and Defective Graphene

Fernández

Castellani

2017

ChemPhysChem

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The role of noncovalent interactions in the adsorption of biological molecules on graphene is a subject of fundamental interest regarding the use of graphene as a material for sensing and drug delivery. The adsorption of dopamine on regular graphene and graphene with monovacancies (GV) is theoretically studied within the framework of density functional theory. Several adsorption modes are considered, and notably those in which the dopamine molecule is oriented parallel or quasi-parallel to the surface are the more stable. The adsorption of dopamine on graphene implies an attractive interaction of a dispersive nature that competes with Pauli repulsion between the occupied π orbitals of the dopamine ring and the π orbitals of graphene. If dopamine adsorbs at the monovacancy in the A-B stacking mode, a hydrogen bond is produced between one of the dopamine hydroxy groups and one carbon atom around the vacancy. The electronic charge redistribution due to adsorption is consistent with an electronic drift from the graphene or GV surface to the dopamine molecule.

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Section: Resultsmentioning

confidence: 95%

Noncovalent Interactions between Dopamine and Regular and Defective Graphene

Fernández

Castellani

2017

ChemPhysChem

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“…The SIESTA code and the implemented VDW functional (denoted as DF2, LMKLL in the code) have been tested in many articles for gr (see. e.g., recent refs …”

Section: Methodsmentioning

confidence: 99%

“…e.g., recent refs. [26,27] ). We have used Troullier Martin, norm conserving, relativistic pseudopotentials in fully separable Kleinman and Bylander form for both Carbon and Ru.…”

Section: Ab Initio Dft Calculationsmentioning

confidence: 99%

The classical molecular dynamics simulation of graphene on Ru(0001) using a fitted Tersoff interface potential

Süle

Szendrő

2013

Surface & Interface Analysis

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The accurate molecular dynamics simulation of weakly bound adhesive complexes, such as supported graphene, is challenging due to the lack of an adequate interface potential. Instead of the widely used Lennard-Jones potential for weak and long-range interactions we use a newly parameterized Tersoff-potential for graphene/Ru(0001) system. The new interfacial force field provides adequate moiré superstructures in accordance with scanning tunnelling microscopy images and with DFT results. In particular, the corrugation of ξ ≈ 1.0 ± 0.2Å is found which is somewhat smaller than found by DFT approaches (ξ ≈ 1.2Å) and is close to STM measurements (ξ ≈ 0.8 ± 0.3Å). The new potential could open the way towards large scale simulations of supported graphene with adequate moiré supercells in many fields of graphene research. Moreover, the new interface potential might provide a new strategy in general for getting accurate interaction potentials for weakly bound adhesion in large scale systems in which atomic dynamics is inaccessible yet by accurate DFT calculations. keywords: atomistic and nanoscale simulations, molecular dynamics simulations, corrugation of graphene, moire superstructures INTRODUCTIONSince the reliable ab initio density functional theory (DFT) methods with various van der Waals (VDW) functionals can be used only up to ∼ 1000 atoms [1] the development of an adequate classical interfacial force-field for supported graphene (gr) is crucial. Although, classical molecular dynamics (CMD) simulations can not be used for the study of electronic structure, however, many important properties of graphene, such as surface topography, moire supercells and interfacial binding characteristics, adhesion as well as defects and many other features can in principle be studied by CMD simulations [2, 3] without the explicit consideration of the electron density or orbitals.The size-limit of DFT is especially serious if accurate geometry optimization or molecular dynamics simulations should be carried out. Moreover, various VDW DFT functionals provide diverging results [1, 4]. In particular, accurate DFT potential energy curves for the interface of gr-substrate systems has been obtained only by the extremely expensive random phase approximation (RPA) for small modell systems which fail, however, to include the full moire-superstructure [4][5][6]. Using CMD simulations no size-limit problem occurs. An important limitation here, however, is the limited availability of accurate interface potential for weak interactions. The widely accepted choice is the simple pairwise Lennard-Jones (LJ) potential. In the present paper we point out that this potential is inadequate, however, for gr/Ru(0001) due to the improper prediction of the binding sites (registry). Therefore, the development of reliable interatomic potentials for gr-support systems is inevitable.First principles calculations (such as density functional theory, DFT) have widely been used in the last few years to understand corrugation of nanoscale gr sheets on various substra...

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“…Among the number of computational simulations related to this topic, and in the context of our study, it is worth mentioning the early works of di Vincenzo et al 17 (with explicit reference to anharmonicity in the E 2g (1) mode) and Gonze et al, 25 where the lack of an accurate computational methodology was discussed. More recently, vdW contributions were specifically taken into account in the calculations, 15,16,[26][27][28][29] and the particular energetic barrier involved in the transition from the stable ABA to the AAA stacking of graphene sheets in graphite was calculated. 15,16,26,27 From the energetic profiles connecting both stackings, the vibrational frequency of the E 2g (1) mode can be straightforwardly calculated.…”

mentioning

confidence: 99%

“…More recently, vdW contributions were specifically taken into account in the calculations, 15,16,[26][27][28][29] and the particular energetic barrier involved in the transition from the stable ABA to the AAA stacking of graphene sheets in graphite was calculated. 15,16,26,27 From the energetic profiles connecting both stackings, the vibrational frequency of the E 2g (1) mode can be straightforwardly calculated. 16 Anharmonicity of phonons in carbon-based materials has also been the subject of rigorous theoretical studies by Bonini et al 22 and Paulatto et al 30 (and references therein).…”

mentioning

confidence: 99%

Anharmonicity effects in the frictionlike mode of graphite

et al. 2016

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Graphite is a prototypical solid lubricant demanding a thorough understanding of its low-friction behavior. The E 2g (1) Raman active vibrational mode of graphite is associated with the rigid-layer relative movement of its graphene sheets. Thus, this mode can provide a good means of exploring the low resistance of graphene layers to slip with respect to each other. To take advantage of this fact, the anharmonicity of the E 2g (1) mode has to be carefully characterized and evaluated since the atomic arrangement of carbon atoms in the ambient condition ABA stacking of graphite evidences potential asymmetry. The calculated one dimensional energetic profile of the E 2g (1) mode reveals this local anisotropy around the energy minima and can be microscopically interpreted in terms of electron density interactions. Morse-like potentials accurately fit the energetic profiles at different inter-layer separations, and provide simple analytical expressions for evaluating harmonic and anharmonic contributions to the Γ-point E 2g (1) frequency, ω E 2g (1) , under a perturbative algebraic treatment. We quantify how the anharmonic contribution increases with the available energy (E) at zero pressure, and how this contribution decreases as hydrostatic pressure (p) or uniaxial stress is applied for a given available energy. The calculated ω E 2g (1) − p and ω E 2g (1) − E trends indicate an increasing (decreasing) of frictional forces in graphite with pressure (temperature).Our conclusions are supported by the good agreement of the calculated frequencies with existing Raman experiments under hydrostatic pressure conditions.

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Van Der Waals Density Functionals for Graphene Layers and Graphite

Cited by 90 publications

References 21 publications

Noncovalent Interactions between Dopamine and Regular and Defective Graphene

Noncovalent Interactions between Dopamine and Regular and Defective Graphene

The classical molecular dynamics simulation of graphene on Ru(0001) using a fitted Tersoff interface potential

Anharmonicity effects in the frictionlike mode of graphite

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