Assessment of Different Quantum Mechanical Methods for the Prediction of Structure and Cohesive Energy of Molecular Crystals

Cutini, Michele; Civalleri, Bartolomeo; Corno, Marta; Orlando, Roberto; Brandenburg, Jan Gerit; Maschio, Lorenzo; Ugliengo, Piero

doi:10.1021/acs.jctc.6b00304

Cited by 96 publications

(155 citation statements)

References 75 publications

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“…112 The C21 and X23 sets have been used in a certain number of studies for testing functionals. 22,95,108,[112][113][114][115][116][117][118][119][120][121][122][123][124][125][126] From our results, we can see that most dispersion-corrected functionals except vdW-DF lead to reasonably small errors for the equilibrium lattice constant a 0 . Compared to the other dispersion-corrected functionals, SCAN+rVV10 has a more pronounced tendency to underestimate a 0 (−3% for NH 3 and −2% CO 2 ), while SCAN (and TM) without NL-vdW correction was already pretty good and compete with the best dispersion-corrected functionals.…”

Section: Methodsmentioning

confidence: 93%

Nonlocal van der Waals functionals for solids: Choosing an appropriate one

Tran

Kalantari

Traoré

et al. 2019

Phys. Rev. Materials

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The nonlocal van der Waals (NL-vdW) functionals [Dion et al., Phys. Rev. Lett. 92, 246401 (2004)] are being applied more and more frequently in solid-state physics, since they have shown to be much more reliable than the traditional semilocal functionals for systems where weak interactions play a major role. However, a certain number of NL-vdW functionals have been proposed during the last few years, such that it is not always clear which one should be used. In this work, an assessment of NL-vdW functionals is presented. Our test set consists of weakly bound solids, namely rare gases, layered systems like graphite, and molecular solids, but also strongly bound solids in order to provide a more general conclusion about the accuracy of NL-vdW functionals for extended systems. We found that among the tested functionals, rev-vdW-DF2 [Hamada, Phys. Rev. B 89, 121103(R) (2014)] is very accurate for weakly bound solids, but also quite reliable for strongly bound solids.SL/hybrid xc alone should not already lead to an overbinding, otherwise adding E NL c,disp can only make the results worse. Thus, the combination E SL/hybrid xc + E NL c,disp has to be well-balanced in order to provide accurate geometry and binding energy. 23,25,36,40 Among the NL-vdW functionals that are available in the literature, a certain number of them were selected for the present work. However, we did not consider NL-vdW functionals based on hybrid functionals, 37,38,41,42 since they lead to calculations that are much more expensive, especially for solids. They are therefore less interesting from a practical point of view as long as the electronic structure is of no particular interest. Thus, only semilocal-based NL-vdW functionals are considered and now listed.vdW-DF from Dion et al. (DRSLL), 2 the first proposed NL-vdW functional that can be applied to systems with arbitrary geometry, consists of the GGA exchange revPBE 43 (a reoptimization of PBE 14 ) and LDA correlation 44,45 for the semilocal part. The nonlocal term, Eq. (2), of the vdW-DF functional (DRSLL kernel Φ) has subsequently been used in combination with other semilocal components, and among them, those that are considered in the present work are the following four. C09-vdW from Cooper, 46 which uses a GGA (C09x) for exchange and LDA for correlation. optB88-vdW and optB86b-vdW, which are two of the functionals developed by Klimeš et al.,21,23 and use for the semilocal component, the GGAs optB88 and optB86b for exchange and LDA for correlation. Note that optB88 and optB86b are reoptimizations of B88 47 and B86b, 48 respectively. vdW-DF-cx from Berland and Hyldgaard, 25 which consists of a GGA exchange component, LV-PW86r, that is combined with LDA correlation and was constructed to be more consistent with the DRSLL kernel. vdW-DF2 from Lee et al. (LMKLL) 36 uses the GGA exchange PW86R 36 (a reoptimization of PW86 49 ) and LDA for correlation, while the kernel Φ (called LMKLL) in E NL c,disp has the same analytical form as the original DRSLL kernel, but with a reoptimized parameter Z ...

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Section: Methodsmentioning

confidence: 93%

Nonlocal van der Waals functionals for solids: Choosing an appropriate one

Tran

Kalantari

Traoré

et al. 2019

Phys. Rev. Materials

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“…The D3 and gCP corrections as well as both HF-3c and PBEh-3c approaches, originally proposed for molecular calculations, have been extended to periodic systems and implemented in the CRYSTAL17 code (Brandenburg et al, 2013;Brandenburg & Grimme, 2013aCutini et al, 2016). The two composite methods are particularly targeted to model molecular crystals.…”

Section: Dispersion-corrected Functionals and Composite Methods Formentioning

confidence: 99%

“…When a finite pre-stress σ pre is applied in the form of a hydrostatic pressure P, within the frame of finite Eulerian strain, the elastic stiffness constants become ( B3LYP-D*/TZP 3.0 AE 1.9 (6.0) 4.6 AE 6.0 (17.9) Cutini et al (2016) SP-B3LYP-D* 5.2 AE 5.8 (15.6) Cutini et al (2016)…”

Section: Elastic Constants Under Pressurementioning

confidence: 99%

Quantum‐mechanical condensed matter simulations with CRYSTAL

Dovesi

Erba

Orlando

et al. 2018

WIREs Comput Mol Sci

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“…The noncovalent interaction of H 2 O and H 2 O 2 is determined by intermolecular H‐bonds of different strength . The B3LYP functional produces reasonable geometries, harmonic frequencies, and IR intensities of the molecular crystals with H‐bonds of different strength and does not require the use of different empirical corrections . The slab parameters are fixed, and structural relaxations are limited to the positional parameters of atoms.…”

Section: Methodsmentioning

confidence: 99%

Effect of aluminum vacancies on the H₂O₂ or H₂O interaction with a gamma‐AlOOH surface. A solid‐state DFT study

Medvedev

Mikhaylov

Chernyshov

et al. 2019

Int J of Quantum Chemistry

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The adsorption of a single H 2 O 2 or H 2 O molecule on a family of periodic slab models of γ-AlOOH is studied by solid-state DFT. The single H 2 O 2 or Н 2 О molecule interacts with the perfect (010) slab by intermolecular hydrogen bonds (H-bonds). In the models of γ-AlOOH with oxygen and aluminum vacancies, H 2 O 2 or Н 2 О also forms covalent OÁÁÁAl bonds. The energies of covalent OÁÁÁAl and H-bonds are estimated by a combined approach based on simultaneous consideration of the total binding energies with BSSE correction and empirical schemes of the Н-bond energy evaluation. The OÁÁÁAl bond energy ranges from~75 to~156 kJ mol −1 . The total energy of H-bond interactions in the case of H 2 O 2 exceeds that of Н 2 О by~30 kJ mol −1 for all considered slab models. In contrast to Н 2 О, a H 2 O 2 molecule always forms two H-bonds as the proton donor. The energy of these bonds noticeably increase on defect γ-AlOOH surfaces in comparison with the perfect slab due to formation of short (strong) H-bonds by adsorbed H 2 O 2 . K E Y W O R D S catalytic center, intermolecular H-bond energy/enthalpy, oxygen and aluminum vacancies, perfect and defect slab models, the Bader analysis of periodic electron density

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Assessment of Different Quantum Mechanical Methods for the Prediction of Structure and Cohesive Energy of Molecular Crystals

Cited by 96 publications

References 75 publications

Nonlocal van der Waals functionals for solids: Choosing an appropriate one

Nonlocal van der Waals functionals for solids: Choosing an appropriate one

Quantum‐mechanical condensed matter simulations with CRYSTAL

Effect of aluminum vacancies on the H₂O₂ or H₂O interaction with a gamma‐AlOOH surface. A solid‐state DFT study

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Assessment of Different Quantum Mechanical Methods for the Prediction of Structure and Cohesive Energy of Molecular Crystals

Cited by 96 publications

References 75 publications

Nonlocal van der Waals functionals for solids: Choosing an appropriate one

Nonlocal van der Waals functionals for solids: Choosing an appropriate one

Quantum‐mechanical condensed matter simulations with CRYSTAL

Effect of aluminum vacancies on the H2O2 or H2O interaction with a gamma‐AlOOH surface. A solid‐state DFT study

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Product

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Effect of aluminum vacancies on the H₂O₂ or H₂O interaction with a gamma‐AlOOH surface. A solid‐state DFT study