Electron-energy-loss spectra and the structural stability of nickel oxide:  An LSDA+U study

Dudarev, S. L.; Botton, Gianluigi A.; Savrasov, S. Y.; Humphreys, C. J.; Sutton, A. P.

doi:10.1103/physrevb.57.1505

Cited by 12,472 publications

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“…For a cubic/tetrahedral field, these energy levels are reversed and the g label is removed for tetrahedral systems due to the loss of the inversion centre, thus placing the e set lower in energy than the triply-degenerate t 2 set. The magnitude of splitting is also reduced for tetrahedral (tet) and cubic (cub) 4 ] 3+ cluster, the d 2 orbital is seen to be occupied.…”

Section: Methodsmentioning

confidence: 98%

“…As done previously for the d orbitals, the initial investigation of the occupation of f orbitals was achieved using simple cluster models, namely the tetrahedral and octahedral f 1 species [Ce(CO) 4 ] 3+ and [Ce(CO) 6 ] 3+ . The spin density plots and relative energies of the tetrahedral and octahedral clusters are given in Fig.…”

Section: View Article Onlinementioning

confidence: 99%

“…However, instead of corroborating the experimental observation, the simulations either failed to predict an insulating state or, when antiferromagnetic ordering was explicitly considered, predicted a band gap that was an order of magnitude smaller than experiment. [4][5][6] This was primarily due to the SIE inherent within DFT, which is a direct result of the approximations used to determine the exchange and correlation with both the local density (LDA) and the generalised gradient approximations (GGA). These approximations result in the exchange not cancelling the self Coulomb term, as would be the case in Hartree-Fock theory.…”

Section: Introductionmentioning

confidence: 99%

“…Two popular methods are those derived by Liechtenstein 10 and Dudarev. 4 Of these, the latter is the more widely used due to its simplicity. It is described by the following equation:…”

Section: Introductionmentioning

confidence: 99%

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Occupation matrix control of d- and f-electron localisations using DFT + U

Allen

Watson

2014

Phys. Chem. Chem. Phys.

201

200

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The use of a density functional theory methodology with on-site corrections (DFT + U) has been repeatedly shown to give an improved description of localised d and f states over those predicted with a standard DFT approach. However, the localisation of electrons also carries with it the problem of metastability, due to the possible occupation of different orbitals and different locations. This study details the use of an occupation matrix control methodology for simulating localised d and f states with a plane-wave DFT + U approach which allows the user to control both the site and orbital localisation.This approach is tested for orbital occupation using octahedral and tetrahedral Ti(III) and Ce(III) carbonyl clusters and for orbital and site location using the periodic systems anatase-TiO 2 and CeO 2 . The periodic cells are tested by the addition of an electron and through the formation of a neutral oxygen vacancy (leaving two electrons to localise). These test systems allow the successful study of orbital degeneracies, the presence of metastable states and the importance of controlling the site of localisation within the cell, and it highlights the use an occupation matrix control methodology can have in electronic structure calculations.

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Section: Methodsmentioning

confidence: 98%

Section: View Article Onlinementioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

“…Two popular methods are those derived by Liechtenstein 10 and Dudarev. 4 Of these, the latter is the more widely used due to its simplicity. It is described by the following equation:…”

Section: Introductionmentioning

confidence: 99%

See 2 more Smart Citations

Occupation matrix control of d- and f-electron localisations using DFT + U

Allen

Watson

2014

Phys. Chem. Chem. Phys.

201

200

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“…For the GGA+U calculation, we used the standard Dudarev implementation 33 , where the on-site Coulomb interaction for the localized transition metal d orbitals was parametrized by U eff = U − J with the Perdew-Wang-91 functional. Optimized U eff for the metal atoms in LaBO 3 (U eff = 3.5, 4, 4, 3.3, and 6.4 eV for Cr, Mn, Fe, Co, and Ni, respectively) were taken from References 19,34 .…”

Section: B Computational Methods 1 Density Function Theory (Dft) Modementioning

confidence: 99%

Ab initio GGA+U study of oxygen evolution and oxygen reduction electrocatalysis on the (001) surfaces of lanthanum transition metal perovskites LaBO₃(B = Cr, Mn, Fe, Co and Ni)

Lee

Gadre

Shao‐Horn

et al. 2015

Phys. Chem. Chem. Phys.

109

135

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ARTICLEThis journal is © The Royal Society of Chemistry 2013 J. Name., 2013, 00, 1--3 | 1 A IntroductionSearch and design of highly active and less expensive materials for catalyzing the sluggish kinetics of the oxygen reduction reaction (ORR) and the oxygen evolution reaction (OER) is of primary importance in many electrochemical energy device applications such as direct-solar and electrolytic water splitting, metal-air batteries, and fuel cells [1][2][3][4][5][6] . In replacement of noble metal containing catalysts, first row transition-metal perovskites are promising candidate materials for catalyzing OER and ORR in alkaline solution. A number of activity descriptor approaches provide an efficient and practical guidance to facilitate screening of alternate perovskite OER and ORR catalysts 4,5,7 , such as number of d-electrons 1, 8 , oxidation enthalpy 1, 9 , the p-band center relative to the Fermi level 6 , the degree of overlapping between the e g orbitals of the M(3d) band and the O(2p) band relative to the Fermi level 10 , and free energies of formation of the bulk perovskites relative to metal and H 2 O/H 2 11. However, there are still many questions about surfaces and interfaces of the transition-metal perovskite catalyst systems in the aqueous environment under the OER and ORR conditions which have invoked further experimental studies 12,13 . These questions include, e.g., what are the stable surfaces for these perovskites, how different surface orientations/terminations result in different activities, how the bulk electronic structure descriptors can be used to describe activities of various surface terminations, and whether/how surface stability is linked to surface catalytic activities. First principles-based Density Functional Theory (DFT) methods are now able to simulate catalytic reactions at specific metal oxide surfaces and extract surface electronic structure and energetic details, which can provide new insights into structure-activity relationships and strategies for material design and development 7,[14][15][16] . For example, Man et al. 14 have performed

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Ultrahigh‐Pressure Phase Transitions in FeS₂ and FeO₂: Implications for Super‐Earths' Deep Interior

Huang

Qin

2018

JGR Solid Earth

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Iron oxides play an important role in planetary evolution, but little information about the structural properties of AX2‐type iron oxides under extreme conditions limits our understanding of the so‐called “super‐Earth” planets. Here an investigation into the high‐pressure behavior of FeO2 as well as its sulfide counterpart FeS2, has been conducted by first‐principle calculations based on density functional theory. Both FeO2 and FeS2 are predicted to undergo a italicPatrue3¯‐ Rtrue3¯m‐I4/mmm transition sequence at extreme pressure. Differences in high‐pressure behaviors between FeO2 and FeS2 have been discussed in detail, such as effective coordination number and elasticity. This study not only resolves the controversy about the structural stability of FeS2 under high pressure but also suggests the tenfold coordinated I4/mmm‐type FeO2 may contribute to local chemical heterogeneity by accumulation in the deep interior of a large super‐Earth or water‐rich planet, whose pressure at the core‐mantle boundary can reach 2 TPa.

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Electron-energy-loss spectra and the structural stability of nickel oxide: An LSDA+U study

Cited by 12,472 publications

References 20 publications

Occupation matrix control of d- and f-electron localisations using DFT + U

Occupation matrix control of d- and f-electron localisations using DFT + U

Ab initio GGA+U study of oxygen evolution and oxygen reduction electrocatalysis on the (001) surfaces of lanthanum transition metal perovskites LaBO₃(B = Cr, Mn, Fe, Co and Ni)

Ultrahigh‐Pressure Phase Transitions in FeS₂ and FeO₂: Implications for Super‐Earths' Deep Interior

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Electron-energy-loss spectra and the structural stability of nickel oxide: An LSDA+U study

Cited by 12,472 publications

References 20 publications

Occupation matrix control of d- and f-electron localisations using DFT + U

Occupation matrix control of d- and f-electron localisations using DFT + U

Ab initio GGA+U study of oxygen evolution and oxygen reduction electrocatalysis on the (001) surfaces of lanthanum transition metal perovskites LaBO3(B = Cr, Mn, Fe, Co and Ni)

Ultrahigh‐Pressure Phase Transitions in FeS2 and FeO2: Implications for Super‐Earths' Deep Interior

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Ab initio GGA+U study of oxygen evolution and oxygen reduction electrocatalysis on the (001) surfaces of lanthanum transition metal perovskites LaBO₃(B = Cr, Mn, Fe, Co and Ni)

Ultrahigh‐Pressure Phase Transitions in FeS₂ and FeO₂: Implications for Super‐Earths' Deep Interior