Bulk Properties of Transition Metals: A Challenge for the Design of Universal Density Functionals

Janthon, Patanachai; Luo, Sijie; Kozlov, Sergey M.; Viñes, Francesc; Limtrakul, Jumras; Truhlar, Donald G.

doi:10.1021/ct500532v

Cited by 265 publications

(302 citation statements)

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“…This is also the case when using meta-GGA functionals, yet to a lesser extent [21]. Hybrid functionals, providing excellent description of the thermochemistry of main group molecules, are unadvised, because of their failure in treating largely delocalized systems, such as transition metals and graphene [22]. Calculations within the Random Phase Approximation (RPA) were suggested as a good choice [23] to model graphene-metal systems.…”

Section: Introductionmentioning

confidence: 99%

The contact of graphene with Ni(111) surface: description by modern dispersive forces approaches

et al. 2016

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Here we present a Density Functional Theory (DFT) study on the suitability of modern corrections for the inclusion of dispersion related terms (DFT-D) in treating the interaction of graphene and metal surfaces, exemplified by the graphene/Ni(111) system. The Perdew-Burke-Ernzerhof (PBE) exchange-correlation functional is used as basis, on top of which we tested the family of Grimme corrections (D2 and D3, including Becke-Jonson damping and Andersson approach) as well as different flavors of the approach by Tkatchenko and Scheffler (TS). Two experimentally observed chemisorbed states, top-fcc and bridge-top conformations, were examined, as well as one physisorbed situation, the hcp-fcc state. Geometric, energetic, and electronic properties were compared to sets of experimental data for our model system of graphene/Ni(111), but also for available data of bulk Ni, graphite, and free-standing graphene. Results show that two of the most recent approximations, the fully ab initio TS-MBD, and the semi-empirical Grimme D3 correction are best suited to describe graphene↔metal contacts, yet, comparing to earlier studies, the Rev-vdW-DF2 functional is also a good option, whereas optB86-vdW and optB88b-vdW functionals are fairly close to experimental values to be harmless used. The present results highlight how different approaches for the approximate treatment of dispersive forces yield different results, and so finetuning and testing of the envisioned approach for every specific system is advisable. The present survey clears the path for future accurate and affordable theoretical studies of nanotechnologic devices based on graphene-metal contacts.

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Section: Introductionmentioning

confidence: 99%

The contact of graphene with Ni(111) surface: description by modern dispersive forces approaches

et al. 2016

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“…69,[71][72][73][74] A princípio, estes sólidos foram investigados para validar a metodologia empregada nesse estudo ao confrontar os resultados com dados da literatura. Em segundo passo, estes resultados foram usados como parâmetros de referência para a investigação das partículas em nanoescala.…”

Section: Sólidos Cristalinosunclassified

“…Mais especificamente, observou-se que metais de transição dos grupos 3, 4, 7, 8 e 12 têm preferência pela estrutura hcp, metais de transição dos grupos 5 e 6 têm preferência pela estrutura bcc e metais de transição dos grupos 9, 10 e 11 têm preferência pela estrutura fcc; as duas exceções são Fe e Co, que adotam, respectivamente, bcc e hcp. Todas as estruturas de menor energia calculadas coincidem com dados encontrados na literatura, tanto experimental 69 quanto teórica, 74 exceto para Mn e Hg, cujas estruturas de menor energia (i.e., uma estrutura denominada α-Mn, 75 …”

Section: Estabilidade Relativaunclassified

“…74 Na Figura 5.b, observa-se um comportamento parabólico para as curvas de energia de coesão ao longo dos períodos de transição para as estruturas cristalinas mais estáveis. Podese verificar que o comportamento parabólico está de acordo com dados da literatura 69,82 e a explicação para a parabolicidade da curva tem relação com o deslocamento da banda de Fermi sobre a banda-d dos metais de transição, o que será discutida de forma mais abrangente na próxima subseção uma vez que se trata de um efeito de origem eletrônica.…”

Section: Propriedades Energéticasunclassified

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Investigação ab initio dos mecanismos de formação de nanoligas core-shell com platina e metais de transição dos períodos 3d, 4d e 5d

Justo¹

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“…[306] However, for properties of bulk solids, revTPSS usually improves over TPSS. [30,[307][308][309][310][311][312][313] For further details about the revTPSS performance see Section 4.…”

Section: The Revtpss Exchange-correlation Functional (2009)mentioning

confidence: 99%

Kinetic‐energy‐density dependent semilocal exchange‐correlation functionals

Sala

Fabiano

Constantin

2016

Int J of Quantum Chemistry

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We present the theory of semilocal exchange-correlation (XC) energy functionals which depend on the Kohn-Sham kinetic energy density (KED), including the relevant class of meta-generalized gradient approximation (meta-GGA) functionals. Thanks to the KED ingredient, meta-GGA functionals can satisfy different exact constraints for XC energy and can be made one-electron selfcorrelation free. This leads to a better accuracy over a wider range of properties with respect to GGAs, often reaching the accuracy of hybrid functionals, but at much reduced computational cost.An extensive survey of the relevant literature on existing KED dependent XC functionals is provided, considering nonempirical, semi-empirical, and fully empirical ones. A deeper analysis and a wide benchmark are presented for functionals derived considering only exact constraints and parameters obtained from model and/or atomic systems. K E Y W O R D Sdensity functional theory, kinetic energy, meta-GGA | I N T R O D U C T I O NKohn-Sham (KS)-density functional theory (DFT) [1][2][3][4][5] is nowadays one of the most popular computational approaches in quantum chemistry, solid-state physics, and materials science. [6][7][8][9][10][11] While the ground-state description of a real system of interacting electrons requires a complicate N-electron wavefunction, in KS-DFT this is mapped onto an auxiliary system of noninteracting electrons having the same ground-state density, which can be easily described using N single-particle KS orbitals. [1,2] The correspondence between the many-electron problem and the KS system is in principle exact [1,3] and it is based on the so called exchange-correlation (XC) energy functional, which collects all the quantum electron-electron interaction terms beyond the Hartree one. [12] Within the constrained-search formalism, [13] the XC energy functional is:E xc ½q 5 min W!q hWjT 1V ee jWi2T s ½q 2J½q 5E x ½q 1U c ½q 1T c ½q ;(1) where W is an N-electron ground-state wavefunction yielding the electron density q,T is the kinetic energy (KE) operator,V ee is the electron-electron interaction operator, T s is the KE of the noninteracting system, J is the Coulomb energy, E x is the exact exchange energy, and U c and T c represent, respectively, the potential and the kinetic contributions to the DFT correlation energy E c 5U c 1T c . The important point of Equation1 is that it is an universal functional of the electron density. However, its explicit functional form is not known, and any practical realization of KS-DFT is based on an approximated XC functional. The latter determines in practice the overall accuracy of the KS-DFT calculation.The study of the exact properties of the XC energy functional as well as the development of new and improved approximations have been hot research topics in DFT for more than three decades, and a large number of XC approximations has been proposed. [12,14,15] The different XC functionals are usually classified, according to their complexity, on the so called Jacob's ladder of DFT [14,16] whic...

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Bulk Properties of Transition Metals: A Challenge for the Design of Universal Density Functionals

Cited by 265 publications

References 65 publications

The contact of graphene with Ni(111) surface: description by modern dispersive forces approaches

The contact of graphene with Ni(111) surface: description by modern dispersive forces approaches

Investigação <i>ab initio</i> dos mecanismos de formação de nanoligas <i>core-shell</i> com platina e metais de transição dos períodos 3<i>d</i>, 4<i>d</i> e 5<i>d</i>

Kinetic‐energy‐density dependent semilocal exchange‐correlation functionals

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