Beyond-dipole van der Waals contributions within the Many-Body Dispersion framework

2021 ◽  
Author(s):  
Dario Massa ◽  
Alberto Ambrosetti ◽  
Pier Luigi Silvestrelli
Keyword(s):  
Density Functional ◽  
Large Scale ◽  
Local Density ◽  
Van Der Waals ◽  
Van Der Waals Interactions ◽  
Many Body ◽  
Full Account ◽  
Local Density Functional Theory ◽  
Body Level ◽  
The Many

Abstract By introducing a suitable range-separation of the Coulomb coupling in analogy to [A. Ambrosetti et al. JCP 140, 18A508 (2014)], here we extend the Many-Body Dispersion (MBD) approach to include beyond-dipole van der Waals interactions at a full many-body level, in combination with semi-local density functional theory. A reciprocal-space implementation is further introduced in order to efficiently treat periodic systems. Consistent reliability is found frommolecular dimers to large supramolecular complexes and two-dimensional systems. The large weight of both many-body effects and multipolar terms illustrates how a correct description of vdW forces in large-scale systems requires full account of both contributions, beyond standard pairwise dipolar approaches.

scholarly journals O(N)Stochastic Evaluation of Many-Body van der Waals Energies in Large Complex Systems

2021 ◽  
Author(s):  
Pier Paolo Poier ◽  
Louis Lagardère ◽  
Jean-Philip Piquemal
Keyword(s):  
Density Functional ◽  
Van Der Waals ◽  
Van Der Waals Interactions ◽  
Complex Materials ◽  
Many Body ◽  
Functional Theory ◽  
Molecular Systems ◽  
New Strategy ◽  
The Many ◽  
Van Der Waals Energies

We propose a new strategy to solve the Tkatchenko-Scheffler Many-Body Dispersion (MBD) model’s equations. Our approach overcomes the original O(N**3) computational complexity that limits its applicability to large molecular systems within thecontext of O(N) Density Functional Theory (DFT). First, in order to generate the required frequency-dependent screenedpolarizabilities, we introduce an efficient solution to the Dyson-like self-consistent screening equations. The scheme reducesthe number of variables and, coupled to a DIIS extrapolation, exhibits linear-scaling performances. Second, we apply astochastic Lanczos trace estimator resolution to the equations evaluating the many-body interaction energy of coupled quantumharmonic oscillators. While scaling linearly, it also enables communication-free pleasingly-parallel implementations. As the resulting O(N) stochastic massively parallel MBD approach is found to exhibit minimal memory requirements, it opens up the possibility of computing accurate many-body van der Waals interactions of millions-atoms’ complex materials and solvated biosystems with computational times in the range of minutes.

scholarly journals O(N)Stochastic Evaluation of Many-Body van der Waals Energies in Large Complex Systems

2021 ◽  
Author(s):  
Pier Paolo Poir ◽  
Louis Lagardère ◽  
Jean-Philip Piquemal
Keyword(s):  
Density Functional ◽  
Van Der Waals ◽  
Van Der Waals Interactions ◽  
Complex Materials ◽  
Many Body ◽  
Functional Theory ◽  
Molecular Systems ◽  
New Strategy ◽  
The Many ◽  
Van Der Waals Energies

We propose a new strategy to solve the Tkatchenko-Scheffler Many-Body Dispersion (MBD) model’s equations. Our approach overcomes the original O(N**3) computational complexity that limits its applicability to large molecular systems within thecontext of O(N) Density Functional Theory (DFT). First, in order to generate the required frequency-dependent screenedpolarizabilities, we introduce an efficient solution to the Dyson-like self-consistent screening equations. The scheme reducesthe number of variables and, coupled to a DIIS extrapolation, exhibits linear-scaling performances. Second, we apply astochastic Lanczos trace estimator resolution to the equations evaluating the many-body interaction energy of coupled quantumharmonic oscillators. While scaling linearly, it also enables communication-free pleasingly-parallel implementations. As the resulting O(N) stochastic massively parallel MBD approach is found to exhibit minimal memory requirements, it opens up the possibility of computing accurate many-body van der Waals interactions of millions-atoms’ complex materials and solvated biosystems with computational times in the range of minutes.

scholarly journals Including dispersion in density functional theory for adsorption on flat oxide surfaces, in metal–organic frameworks and in acidic zeolites

2020 ◽  
Vol 22 (14) ◽  
pp. 7577-7585 ◽  
Author(s):  
Florian R. Rehak ◽  
GiovanniMaria Piccini ◽  
Maristella Alessio ◽  
Joachim Sauer
Keyword(s):  
Density Functional Theory ◽  
Density Functional ◽  
Van Der Waals ◽  
Metal Organic Frameworks ◽  
Many Body ◽  
Functional Theory ◽  
Metal Organic ◽  
The Many ◽  
Acidic Zeolites ◽  
Better Than

Contrary to common believe, for eight adsorption cases, neither D3 or TS are an improvement compared to D2 nor van der Waals functionals or dDsC. Only the many body approaches are slightly better than D2(Ne) which uses Ne parameters for Mg2+ ions.

scholarly journals Analytical nuclear gradients for the range-separated many-body dispersion model of noncovalent interactions

2016 ◽  
Vol 7 (3) ◽  
pp. 1712-1728 ◽  
Author(s):  
Martin A. Blood-Forsythe ◽  
Thomas Markovich ◽  
Robert A. DiStasio ◽  
Roberto Car ◽  
Alán Aspuru-Guzik
Keyword(s):  
Noncovalent Interactions ◽  
Dispersion Model ◽  
Van Der Waals ◽  
Van Der Waals Interactions ◽  
Many Body ◽  
The Many

This work develops analytical forces for the many-body dispersion model of collective van der Waals interactions.

scholarly journals Benchmarking Several van der Waals Dispersion Approaches for the Description of Intermolecular Interactions

2018 ◽  
Author(s):  
Julien Claudot ◽  
Won June Kim ◽  
Anant Dixit ◽  
Hyungjun Kim ◽  
Tim Gould ◽  
...  
Keyword(s):  
Van Der Waals ◽  
Chem Phys ◽  
Binding Energies ◽  
Van Der Waals Interactions ◽  
Density Functionals ◽  
Many Body ◽  
Blind Test ◽  
Molecular Systems ◽  
Test Sets ◽  
The Many

Seven methods, including three van der Waals density functionals (vdW-DFs) and four different variants of the Tkatchenko-Scheffler (TS) methods, are tested on the A24, L7, and Taylor <i>et al.</i>'s "blind" test sets. It is found that for these systems, the vdW-DFs perform better that the TS methods. In particular, the vdW-DF-cx functional gives binding energies that are the closest to the reference values, while the many body correction of TS does not always lead to an improvement in the description of molecular systems. In light of these results, several directions for further improvements to describe van der Waals interactions are discussed.<br><br>Published as <i>J. Chem. Phys.</i> <b>148</b>, 064112 (2018)<br>

scholarly journals Benchmarking Several van der Waals Dispersion Approaches for the Description of Intermolecular Interactions

2018 ◽  
Author(s):  
Julien Claudot ◽  
Won June Kim ◽  
Anant Dixit ◽  
Hyungjun Kim ◽  
Tim Gould ◽  
...  
Keyword(s):  
Intermolecular Interactions ◽  
Van Der Waals ◽  
Binding Energies ◽  
Van Der Waals Interactions ◽  
Density Functionals ◽  
Many Body ◽  
Blind Test ◽  
Molecular Systems ◽  
Test Sets ◽  
The Many

Seven methods, including three van der Waals density functionals (vdW-DFs) and four different variants of the Tkatchenko-Scheffler (TS) methods, are tested on the A24, L7, and Taylor <i>et al.</i>'s "blind" test sets. It is found that for these systems, the vdW-DFs perform better that the TS methods. In particular, the vdW-DF-cx functional gives binding energies that are the closest to the reference values, while the many body correction of TS does not always lead to an improvement in the description of molecular systems. In light of these results, several directions for further improvements to describe van der Waals interactions are discussed.<br>

scholarly journals Atomistic Simulation of Ceramic/Metal Interfaces: {222}MgO/Cu

1997 ◽  
Vol 3 (4) ◽  
pp. 333-338 ◽  
Author(s):  
R. Benedek ◽  
D.N. Seidman ◽  
L.H. Yang
Keyword(s):  
Molecular Dynamics ◽  
Atomistic Simulation ◽  
Density Functional ◽  
Large Scale ◽  
Interatomic Potential ◽  
Local Density ◽  
Interface State ◽  
Dislocation Network ◽  
Local Density Functional Theory ◽  
Adhesive Energy

Abstract: Atomistic simulations were performed for the {222}MgO/Cu interface by local density functional theory (LDFT) methods, within the plane-wave-pseudopotential representation, and by (classical) molecular dynamics and statics. The electronic spectra obtained with LDFT calculations showed a localized interface state within the bulk MgO gap, approximately 1 eV above the MgO valence band edge. LDFT adhesive energy calculations, as a function of interface spacing and translations parallel to the interface, were employed to devise an interatomic potential suitable for large-scale atomistic simulation. The interface structure, which was obtained with molecular dynamics (and statics) calculations based on the resultant potential, exhibited a misfit dislocation network with trigonal symmetry, and no standoff dislocations.

scholarly journals Van der Waals interactions in selected allotropes of phosphorus

2015 ◽  
Vol 230 (2) ◽  
Author(s):  
Frederik Bachhuber ◽  
Joerg von Appen ◽  
Richard Dronskowski ◽  
Peer Schmidt ◽  
Tom Nilges ◽  
...  
Keyword(s):  
Density Functional ◽  
Local Density ◽  
Van Der Waals ◽  
Van Der Waals Interactions ◽  
Special Focus ◽  
Generalized Gradient ◽  
Long Range Interactions ◽  
Key Factor ◽  
Low Dimensional ◽  
2D And 3D

AbstractSelected allotropes of phosphorus are investigated by different levels of density functional theory (DFT) calculations to evaluate the relative stability orders with a special focus on the role of van der Waals interactions. Phosphorus is an excellent reference system with a large number of allotropes. Starting from low-dimensional molecular (0D, white P) and polymer structures (1D, P nanorods) to layered (2D, black P) and tubular structures (2D and 3D, crystalline forms of red P), covalent structure motifs are interconnected by van der Waals interactions. They are a key factor for the correct energetic description of all P allotropes. A comparative study is carried out within the local density approximation (LDA) and the generalized gradient approximation (GGA), with and without implementation of a dispersion correction by Grimme (GGA-D2). Our intention is to achieve a reasonable agreement of our calculations with experimental data, the plausibility of energy values, and the treatment of long-range interactions. The effect of van der Waals interactions is exemplified for the interlayer distances of black phosphorous and its electronic structure.

Ab-Initio Determination of the Atomic Structure of Symmetrical Tilt Grain Boundaries in BCC Transition Metals

1997 ◽  
Vol 492 ◽  
Author(s):  
C. Elsässer ◽  
O. Beck ◽  
T. Ochs ◽  
B. Meyer
Keyword(s):  
Transition Metals ◽  
Grain Boundary ◽  
Ab Initio ◽  
Grain Boundaries ◽  
Density Functional ◽  
Local Density ◽  
High Symmetry ◽  
Many Body ◽  
Local Density Functional Theory ◽  
Symmetrical Tilt

ABSTRACTAtomistic simulations of grain-boundary structures in body-centered cubic transition metals have revealed that angle-dependent contributions to interatomic interactions are essential. Unfortunately, the results of presently available empirical many-body potentials are not yet always sufficiently reliable for quantitative theoretical predictions of grain-boundary structures, which are consistent with experimental observations, e.g. by high-resolution transmission electron microscopy.Ab-initio electronic-structure calculations based on the local-density-functional theory offer the possibility to determine accurately the microscopic structures of special, high-symmetry grain boundaries, which can be used as data bases for the improvement of empirical many-body potentials. Such ab-initio calculations, with a mixed-basis pseudopotential method and grain-boundary supercells, are presented for Σ5 (310) [001] 36.87° symmetrical tilt grain boundaries in Niobium and Molybdenum.

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