Bond energy decomposition analysis for subsystem density functional theory

Beyhan, Selami; Götz, Andreas W.; Visscher, Lucas

doi:10.1063/1.4793629

Cited by 15 publications

(25 citation statements)

References 104 publications

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“…A recent energy decomposition analysis of subsystem DFT calculations [44] has shown that the inclusion of empirical van der Waals terms in the interaction energy has the effect of improving the binding energies calculated with GGA functionals. In line with those findings, we show that the FDE binding energies are dramatically improved if the non-additive correlation energy functional is made non-local in character and is evaluated with the Fluctuation-Dissipation Theorem.…”

Section: Discussionmentioning

confidence: 99%

“…First, Visscher and coworkers [44], demonstrated that the FDE coupled with semiempirical dispersion corrections yields accurate interaction energies. Second, Cha lasiński and coworkers [45], used a projector-based partitioning of HF and KS-DFT wavefunctions into fragment wavefunctions to define an interfragment dispersion correction calculated with the GCP formula which yielded excellent interaction energies.…”

Section: Introductionmentioning

confidence: 99%

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FDE-vdW: A van der Waals inclusive subsystem density-functional theory

Kevorkyants

Eshuis

Pavanello

2014

The Journal of Chemical Physics

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We present a formally exact van der Waals inclusive electronic structure theory, called FDE-vdW, based on the Frozen Density Embedding formulation of subsystem Density-Functional Theory. In subsystem DFT, the energy functional is composed of subsystem additive and non-additive terms. We show that an appropriate definition of the long-range correlation energy is given by the value of the nonadditive correlation functional. This functional is evaluated using

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Section: Discussionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

FDE-vdW: A van der Waals inclusive subsystem density-functional theory

Kevorkyants

Eshuis

Pavanello

2014

The Journal of Chemical Physics

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“…But we do note the great promise of density embedding methods, of which there are various flavors. [47][48][49][50][51][52][53] However, we will not cover embedding methods further in this perspective, except to note that density embedding not only can serve as a way to speed up DFT calculations, but also it can serve as a new way to combine WFT with DFT, which is an approach that has great promise but is not fully covered in this article.…”

Section: B What Is Kohn-sham Dft?mentioning

confidence: 99%

The behavior of active diffusiophoretic suspensions: An accelerated Laplacian dynamics study

Yan

Brady

2016

The Journal of Chemical Physics

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This article presents a perspective on Kohn-Sham density functional theory (KS-DFT) for electronic structure calculations in chemical physics. This theory is in widespread use for applications to both molecules and solids. We pay special attention to several aspects where there are both concerns and progress toward solutions. These include: 1. The treatment of open-shell and inherently multiconfigurational systems (the latter are often called multireference systems and are variously classified as having strong correlation, near-degeneracy correlation, or high static correlation; KS-DFT must treat these systems with broken-symmetry determinants). 2. The treatment of noncovalent interactions. 3. The choice between developing new functionals by parametrization, by theoretical constraints, or by a combination. 4. The ingredients of the exchange-correlation functionals used by KS-DFT, including spin densities, the magnitudes of their gradients, spin-specific kinetic energy densities, nonlocal exchange (Hartree-Fock exchange), nonlocal correlation, and subshell-dependent corrections (DFT+U). 5. The quest for a universal functional, where we summarize some of the success of the latest Minnesota functionals, namely MN15-L and MN15, which were obtained by optimization against diverse databases. 6. Time-dependent density functional theory, which is an extension of DFT to treat time-dependent problems and excited states. The review is a snapshot of a rapidly moving field, and-like Marcel Duchamp-we hope to convey progress in a stimulating way. Published by AIP Publishing. [http://dx

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“…This led to as accurate binding energies of weakly bonded molecular dyads as supersystem RPA [e.g., mean unsigned errors of < 0.5 kcal/mol against CCSD(T) on the S22 set [57,58] ]. Beyhan [59] also proposed a Grimme-like long-range correction to the nonadditive correlation energy which led to much improved interaction energies. To account for dispersion interactions between subsystems, eQE can include London dispersion forces as implemented in the main QE code base.…”

Section: Periodic Systemsmentioning

confidence: 99%

eQE: An open‐source density functional embedding theory code for the condensed phase

Genova

Ceresoli

Krishtal

et al. 2017

Int J of Quantum Chemistry

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In this work, we present the main features and algorithmic details of a novel implementation of the frozen density embedding (FDE) formulation of subsystem density functional theory (DFT) that is specifically designed to enable ab initio molecular dynamics (AIMD) simulations of largescale condensed-phase systems containing 1000s of atoms. This code (available at http://eqe. rutgers.edu) has been given the moniker of embedded Quantum ESPRESSO (eQE) as it is a generalization of the open-source Quantum ESPRESSO (QE) suite of programs. The strengths of eQE reside in a hierarchical parallelization scheme that allows for an efficient and fully self-consistent treatment of the electronic structure (via the addition of an additional DIIS extrapolation layer) while simultaneously exploiting the inherent symmetries and periodicities in the system (via sampling of subsystem-specific first Brillouin zones and utilization of subsystem-specific basis sets).While bulk liquids and molecular crystals are two classes of systems that exemplify the utility of the FDE approach (as these systems can be partitioned into weakly interacting subunits), we show that eQE has significantly extended this regime of applicability by outperforming standard semilocal Kohn-Sham DFT (KS-DFT) for large-scale heterogeneous catalysts with quite different layerspecific electronic structure and intrinsic periodicities. eQE features very favorable strong parallel scaling for a model system of bulk liquid water composed of 256 water molecules, which allows for a significant decrease in the overall time to solution when compared to KS-DFT. We show that eQE achieves speedups greater than one order of magnitude (>103) when performing AIMD simulations of such large-scale condensed-phase systems as: (1) | I N T R O D U C T I O NThe Kohn-Sham (KS) formulation of density functional theory (DFT) [1] is currently the most widely employed electronic structure method in the fields of chemistry, physics, and materials science. This is largely due to the fact that KS-DFT employing semilocal exchange-correlation (xc) functionals produces models of remarkable accuracy and predictive capability [2] with a relatively low associated computational cost (that in general Int J Quantum Chem. 2017;117:e25401.

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Bond energy decomposition analysis for subsystem density functional theory

Cited by 15 publications

References 104 publications

FDE-vdW: A van der Waals inclusive subsystem density-functional theory

FDE-vdW: A van der Waals inclusive subsystem density-functional theory

The behavior of active diffusiophoretic suspensions: An accelerated Laplacian dynamics study

eQE: An open‐source density functional embedding theory code for the condensed phase

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