Systematic beyond-DFT study of binary transition metal oxides

Mandal, Subhasish; Haule, Kristjan; Rabe, Karin M.; Vanderbilt, David

doi:10.1038/s41524-019-0251-7

Cited by 69 publications

(43 citation statements)

References 71 publications

(95 reference statements)

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“…The calculation performed for bulk MnO also show, at the PBE level, the same effects as reported before in the literature [43,44]: there is a wrong splitting of the density of states for the top valence bands, the band gap is too small, and the bottom of the valence bands shows a double peak, as for NiO, which is also not correct. We found that these features are already corrected very well by the addition on an onsite interaction, which yield a nice agreement with the experimental result.…”

Section: Transition Metal Oxides: Mno and Niosupporting

confidence: 65%

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Parameter-free hybridlike functional based on an extended Hubbard model: DFT+U+V

Tancogne-Dejean

Rubio

2020

Phys. Rev. B

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In this paper, we propose an energy functional at the level of DFT + U + V that allows us to compute selfconsistently the values of the onsite interaction, Hubbard U and Hund J, as well as the intersite interaction V. This functional extends the previously proposed ACBN0 functional [L. A. Agapito et al., Phys. Rev. X 5, 011006 (2015)] including both onsite and intersite interactions. We show that this ab initio self-consistent functional yields improved electronic properties for a wide range of materials, ranging from sp materials to strongly correlated materials. This functional can also be seen as an alternative general and systematic way to construct parameter-free hybrid functionals, based on the extended Hubbard model and a selected set of Coulomb integrals, and might be used to develop novel approximations. By extending the DFT + U method to materials where strong local and nonlocal interactions are relevant, this work opens the door to the ab initio study the electronic, ionic, and optical properties of a larger class of strongly correlated materials in and out of equilibrium.

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Section: Transition Metal Oxides: Mno and Niosupporting

confidence: 65%

“…As many prior studies, see for instance Refs. [43,44], we found that the semilocal Perdew-Burke-Ernzerhof (PBE) [45] functional produces a very small band gap for NiO. Adding a Hubbard U improves the energy band gap compared to the experiment.…”

Section: Transition Metal Oxides: Mno and Niomentioning

confidence: 99%

Parameter-free hybridlike functional based on an extended Hubbard model: DFT+U+V

Tancogne-Dejean

Rubio

2020

Phys. Rev. B

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“…While quantum mechanical methods in single-particle theories such as DFT or DFT+U methods (mainly GGA) are fast and can predict accurate results for most structural parameters, even when relatively strong electron correlations are present, qualitative predictions of excited state properties may require beyond-DFT methods 70 . Beyond-DFT calculations have been applied to many materials systems, including cuprates and Fe-based high-temperature superconductors, Mott insulators, heavy Fermion systems, semiconductors, photovoltaics, and topological Mott insulators 70 . In the last few decades, both perturbative and stochastic approaches have been developed to understand these strongly correlated materials.…”

Section: Jarvis-beyond-dftmentioning

confidence: 99%

“…In the JARVIS-Beyond-DFT 70 database we try to answer a few key questions regarding discoveries through a materials database for quantum materials. First, where is it necessary to use a beyond-DFT method, and which method to be use?…”

Section: Jarvis-beyond-dftmentioning

confidence: 99%

The joint automated repository for various integrated simulations (JARVIS) for data-driven materials design

et al. 2020

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The Joint Automated Repository for Various Integrated Simulations (JARVIS) is an integrated infrastructure to accelerate materials discovery and design using density functional theory (DFT), classical force-fields (FF), and machine learning (ML) techniques. JARVIS is motivated by the Materials Genome Initiative (MGI) principles of developing open-access databases and tools to reduce the cost and development time of materials discovery, optimization, and deployment. The major features of JARVIS are: JARVIS-DFT, JARVIS-FF, JARVIS-ML, and JARVIS-tools. To date, JARVIS consists of ≈40,000 materials and ≈1 million calculated properties in JARVIS-DFT, ≈500 materials and ≈110 force-fields in JARVIS-FF, and ≈25 ML models for material-property predictions in JARVIS-ML, all of which are continuously expanding. JARVIS-tools provides scripts and workflows for running and analyzing various simulations. We compare our computational data to experiments or high-fidelity computational methods wherever applicable to evaluate error/uncertainty in predictions. In addition to the existing workflows, the infrastructure can support a wide variety of other technologically important applications as part of the data-driven materials design paradigm. The JARVIS datasets and tools are publicly available at the website: https://jarvis.nist.gov.

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“…Density-functional theory (DFT) [34,35] with its standard local-density and generalized-gradient approximations (LDA and GGA, respectively) to the exchange-correlation functional is by far the most widely used approach in condensedmatter physics and materials science for simulations of a vast variety of materials' properties. Nevertheless, and notwithstanding its numerous successes, it often fails to provide accurate description of TM oxides, not only quantitatively but often even qualitatively (e.g., it predicts a metallic instead of an insulating ground state in some TM oxides [36]). The failure of "standard DFT" is related first and foremost to very large self-interaction errors [37,38] for localized d and f electrons [39][40][41].…”

Section: Introductionmentioning

confidence: 99%

Electronic structure of pristine and Ni-substituted LaFeO3 from near edge x-ray absorption fine structure experiments and first-principles simulations

Timrov

Agrawal

Zhang

et al. 2020

Phys. Rev. Research

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We present a joint theoretical and experimental study of the oxygen K-edge spectra for LaFeO 3 and homovalent Ni-substituted LaFeO 3 (LaFe 0.75 Ni 0.25 O 3), using first-principles simulations based on density-functional theory with extended Hubbard functionals and x-ray absorption near edge structure (XANES) measurements. Ground-state and excited-state XANES calculations employ Hubbard onsite U and intersite V parameters determined from first principles and the Lanczos recursive method to obtain absorption cross sections, which allows for a reliable description of XANES spectra in transition-metal compounds in a very broad energy range, with an accuracy comparable to that of hybrid functionals but at a substantially lower cost. We show that standard gradient-corrected exchange-correlation functionals fail in capturing accurately the electronic properties of both materials. In particular, for LaFe 0.75 Ni 0.25 O 3 they do not reproduce its semiconducting behavior and provide a poor description of the pre-edge features at the O K edge. The inclusion of Hubbard interactions leads to a drastic improvement, accounting for the semiconducting ground state of LaFe 0.75 Ni 0.25 O 3 and for good agreement between calculated and measured XANES spectra. We show that the partial substitution of Ni for Fe affects the conduction-band bottom by generating a strongly hybridized O(2p)-Ni(3d) minority-spin empty electronic state. The present work, based on a consistent correction of self-interaction errors, outlines the crucial role of extended Hubbard functionals to describe the electronic structure of complex transition-metal oxides such as LaFeO 3 and LaFe 0.75 Ni 0.25 O 3 and paves the way to future studies on similar systems.

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Systematic beyond-DFT study of binary transition metal oxides

Cited by 69 publications

References 71 publications

Parameter-free hybridlike functional based on an extended Hubbard model: DFT+U+V

Parameter-free hybridlike functional based on an extended Hubbard model: DFT+U+V

The joint automated repository for various integrated simulations (JARVIS) for data-driven materials design

Electronic structure of pristine and Ni-substituted LaFeO3 from near edge x-ray absorption fine structure experiments and first-principles simulations

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