Density-functional approach to the three-body dispersion interaction based on the exchange dipole moment

Proynov, Emil; Liu, Fenglai; Gan, Zhengting; Wang, Matthew; Kong, Jing

doi:10.1063/1.4929581

Cited by 12 publications

(16 citation statements)

References 28 publications

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“…As expected, such values are negligible when compared to the predicted differences of the positions of E el ( V ) curve minima computed in VASP and CRYSTAL, not affecting the overall reported trends among the results of individual levels of theory and their interpretation. Such findings are consistent with previous literature reports on many‐body dispersion and its impact on cohesion of molecular crystals, 6,49,50 which state that the three‐body dispersion is the most important for crystals of non‐polar molecules rich in π‐electrons. In the current case of molecular‐ionic crystals, the many‐body interactions are supposed to be governed by the induction component, whereas the three‐body dispersion is expected to be minor.…”

Section: Resultssupporting

confidence: 93%

Tuning the quasi‐harmonic treatment of crystalline ionic liquids within the density functional theory

Červinka

2021

J Comput Chem

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Five ionic liquids are selected for benchmarking the performance of quasi‐harmonic density functional theory (DFT) calculations of structural, phonon, and thermodynamic properties of their crystals. Data predicted by individual computational setups are sorted, establishing a distinct hierarchy among the first‐principles approaches. PBE‐D3 and B3LYP‐D3 functionals are coupled with various plane wave and Gaussian‐type orbital (GTO) basis sets. Propagation of the basis set superposition error and of the imperfections of both functionals into finite‐temperature properties is discussed in detail. PBE‐D3 together with a triple‐zeta GTO basis set often yields the most accurate predictions of predicted molar volume and heat capacity with errors at 1% and 8%, respectively, representing the state‐of‐the‐art for quasi‐harmonic DFT calculations for crystalline ionic liquids. Fortuitous error cancellation between the basis‐set superposition (overbinding) and PBE imperfection (overexpanding) strongly affects the overall accuracy, unlike the case of B3LYP/GTO calculations, impeding systematic convergence of the methodology towards higher accuracy.

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Section: Resultssupporting

confidence: 93%

Tuning the quasi‐harmonic treatment of crystalline ionic liquids within the density functional theory

Červinka

2021

J Comput Chem

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“…An ab initio method to account for this effect within XSAPT+ ai D3 has been introduced, but engenders cost. Alternatively, three-body dispersion corrections of the Axilrod–Teller–Muto (ATM) variety can be introduced: , These corrections were found to be crucial in XSAPT+ ai D3 calculations involving large monomers . In the Tkatchenko–Scheffler (TS) version of this correction, E ATM (TS) , the triatomic C 9 coefficients are derived from the electron density, whereas Grimme’s version ( E ATM (Grimme) ) determines C 9 from the geometric mean of the atomic C 6 coefficients …”

mentioning

confidence: 99%

Accurate and Efficient ab Initio Calculations for Supramolecular Complexes: Symmetry-Adapted Perturbation Theory with Many-Body Dispersion

Carter-Fenk

Lao

Liu

et al. 2019

J. Phys. Chem. Lett.

129

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Symmetry-adapted perturbation theory (SAPT) provides a chemically meaningful energy decomposition scheme for nonbonded interactions that is useful for interpretive purposes. Although formally a dimer theory, we have previously introduced an “extended” version (XSAPT) that incorporates many-body polarization via self-consistent charge embedding. Here, we extend the XSAPT methodology to include nonadditive dispersion, using a modified form of the many-body dispersion (MBD) method of Tkatchenko and co-workers. Dispersion interactions beyond the pairwise atom–atom approximation improve total interaction energies even in small systems, and for large π-stacked complexes these corrections can amount to several kilocalories per mole. The XSAPT+MBD method introduced here achieves errors of ≲1 kcal/mol (as compared to high-level ab initio benchmarks) for the L7 data set of large dispersion-bound complexes and ≲4 kcal/mol (as compared to experiment) for the S30L data set of host–guest complexes. This is superior to the best contemporary density functional methods for noncovalent interactions, at comparable or lower cost. XSAPT+MBD represents a promising method for application to supramolecular assemblies, including protein–ligand binding.

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“…Afterward, wave function DLPNO–CCSD(T) BEs are used for benchmarking the series of DFT functionals for BEs of PEX-M-PEX complexes with selected metal atoms. We also address the use of variants of the D3 correction to dispersion interactions, that is, the D3(0), D3(BJ), and D3(BJ)-ABC methods.…”

Section: Introductionmentioning

confidence: 99%

“…Since some applications show slight differences between CCSD(T) and DLPNO−CCSD(T), 50,69 PEX-M-PEX complexes with selected metal atoms. We also address the use of variants of the D3 correction to dispersion interactions, that is, the D3(0), 31 D3(BJ), 73 and D3(BJ)-ABC 74 methods.…”

Section: ■ Introductionmentioning

confidence: 99%

DFT Functionals for Modeling of Polyethylene Chains Cross-Linked by Metal Atoms. DLPNO–CCSD(T) Benchmark Calculations

2021

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Density functional theory (DFT) functionals for calculations of binding energies (BEs) of the polyethylene (PE) chains cross-linked by selected metal atoms (M) are benchmarked against DLPNO−CCSD(T) and DLPNO−CCSD(T1) data. PEX-M-PEX complexes as compared with plain parallel PEX•••PEX chains with X = 3−9 carbon atoms are model species characterized by a cooperative effect of covalent C-M-C bonds and interchain dispersion interactions. The accuracy of DLPNO−CC methods was assessed by a comparison of BEs with the canonical CCSD(T) results for small PE3-M-PE3 complexes. Functionals for PEX••• PEX and closed-shell PEX-M-PEX complexes (M = Be, Mg, Zn) were benchmarked against DLPNO−CCSD(T) BEs; open-shell complexes (M = Li, Ag, Au) were benchmarked against the DLPNO−CCSD(T1) method with iterative triples. Three dispersion corrections were combined with 25 DFT functionals for calculations of BEs with respect to PEX-M and PEX fragments employing def2-TZVPP and def2-QZVPP basis sets. Accuracy to within 5% for the closed-shell PEX-M-PEX complexes was achieved with five functionals. Less accurate are functionals for the openshell PEX-M-PEX complexes; only two functionals deviate by less than 15% from DLPNO−CCSD(T1). Particularly problematic were PEX-Li-PEX complexes. A reasonable overall performance across all complexes in terms of the mean absolute percentage error is found for the range-separated hybrid functionals ωB97X-D3 and CAM-B3LYP/D3(BJ)-ABC.

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Density-functional approach to the three-body dispersion interaction based on the exchange dipole moment

Cited by 12 publications

References 28 publications

Tuning the quasi‐harmonic treatment of crystalline ionic liquids within the density functional theory

Tuning the quasi‐harmonic treatment of crystalline ionic liquids within the density functional theory

Accurate and Efficient ab Initio Calculations for Supramolecular Complexes: Symmetry-Adapted Perturbation Theory with Many-Body Dispersion

DFT Functionals for Modeling of Polyethylene Chains Cross-Linked by Metal Atoms. DLPNO–CCSD(T) Benchmark Calculations

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