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>

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 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 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 Convergence of the many-body expansion of interaction potentials: From van der Waals to covalent and metallic systems

2007 ◽  
Vol 76 (1) ◽  
Author(s):  
Andreas Hermann ◽  
Robert P. Krawczyk ◽  
Matthias Lein ◽  
Peter Schwerdtfeger ◽  
I. P. Hamilton ◽  
...  
Keyword(s):  
Van Der Waals ◽  
Many Body ◽  
Interaction Potentials ◽  
The Many ◽  
Metallic Systems
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