Relativistic band-structure calculations for electronic properties of actinide dioxides

Maehira, Takahiro; Hotta, Takashi

doi:10.1016/j.jmmm.2006.10.127

Cited by 20 publications

(33 citation statements)

References 21 publications

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“…In other words, the LDA calculations fail to produce the 195146-5 CEF ground states in the AnO 2 series as was also previously pointed out, 21,22 whereas the correct CEF behavior for lighter actinide dioxides is reproduced if only the lower 8 states are taken into account.…”

Section: A Nonordered State Calculationsmentioning

confidence: 54%

“…It was actually reported that the LDA approach led to states that are inconsistent with the CEF ground states determined experimentally in the AnO 2 . 21,22 Moreover, the calculations predicted metallic ground states, 21,23 whereas the AnO 2 compounds with light actinides are known to be large gap semiconductors or insulators with energy gaps around 2 eV. [24][25][26] Therefore, first-principles calculations taking into account the strong Coulomb interaction have been applied and have provided insight in the detailed magnetic and electronic character of UO 2 , [27][28][29][30][31][32][33][34] of NpO 2 , 20,31,34 and of PuO 2 , 30,31,[34][35][36][37][38][39][40][41] although the f characters provided in some of these calculations are different from those of the experimental ground states, especially for the ordered states.…”

Section: Introductionmentioning

confidence: 99%

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Microscopic theory of the insulating electronic ground states of the actinide dioxides AnO2(An = U, Np, Pu, Am, and Cm)

2013

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The electronic states of the actinide dioxides AnO 2 (with An = U, Np, Pu, Am, and Cm) are investigated employing first-principles calculations within the framework of the local density approximation +U (LDA + U ) approach, implemented in a full-potential linearized augmented plane-wave scheme. A systematic analysis of the An-5f states is performed which provides intuitive connections between the electronic structures and the local crystalline fields of the f states in the AnO 2 series. Particularly the mechanisms leading to the experimentally observed insulating ground states are investigated. These are found to be caused by the strong spin-orbit and Coulomb interactions of the 5f orbitals; however, as a result of the different configurations, this mechanism works in distinctly different ways for each of the AnO 2 compounds. In agreement with experimental observations, the nonmagnetic states of plutonium and curium dioxide are computed to be insulating, whereas those of uranium, neptunium, and americium dioxides require additional symmetry breaking to reproduce the insulator ground states, a condition which is met with magnetic phase transitions. We show that the occupancy of the An-f orbitals is closely connected to each of the appearing insulating mechanisms. We furthermore investigate the detailed constitution of the noncollinear multipolar moments for transverse 3q magnetic ordered states in UO 2 and longitudinal 3q high-rank multipolar ordered states in NpO 2 and AmO 2 .

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Section: A Nonordered State Calculationsmentioning

confidence: 54%

Section: Introductionmentioning

confidence: 99%

Microscopic theory of the insulating electronic ground states of the actinide dioxides AnO2(An = U, Np, Pu, Am, and Cm)

2013

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“…In this paper, the f-electron level E f is set as the origin of energy, leading to E f = 0. On the other hand, the p-electron level E p is considered to be E p = −4 eV from the comparison of the relativistic band-structure calculation results [21].…”

Section: Parameters Of the Modelmentioning

confidence: 99%

“…In order to clarify the role of f-p hybridization for the appearance of octupole ordering, Maehira and Hotta have performed the band-structure calculations for actinide dioxides by a relativistic linear augmented-plane-wave method with the exchange-correlation potential in a local density approximation [21]. It has been found that the energy bands in the vicinity of the Fermi level are mainly due to the hybridization between actinide 5f and oxygen 2p electrons.…”

Section: Introductionmentioning

confidence: 99%

Key Role of Hybridization between Actinide 5<i>f</i> and Oxygen 2<i>p</i> Orbitals for Electronic Structure of Actinide Dioxides

Hasegawa¹,

Maehira²,

Hotta³

2013

JMP

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In order to promote our understanding on electronic structure of actinide dioxides, we construct a tight-binding model composed of actinide 5f and oxygen 2p electrons, which is called f-p model. After the diagonalization of the f-p model, we compare the eigen-energies in the first Brillouin zone with the results of relativistic band-structure calculations. Here we emphasize a key role of f-p hybridization in order to understand the electronic structure of actinide dioxides. In particular, it is found that the position of energy levels of Г 7 and Г 8 states determined from crystalline electric field (CEF) potentials depends on the f-p hybridization. We investiagte the values of the Slater-Koster integrals for f-p hybridization, (fpσ) and (fpπ), which reproduce simultaneously the local CEF states and the band-structure calculation results. Then, we find that the absolute value of (fpπ) should be small in comparison with (fpσ) = 1 eV. The small value of |(fpπ)| is consistent with the condition to obtain the octupole ordering in the previous analysis of the f-p model.

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“…In addition, conventional density functional theory (DFT) within the LDA or GGA scheme fails to treat the strong correlation of 5f electrons in AmO 2 actinide dioxides [15][16][17]. Therefore, in this work, the structural, phase transition, magnetic and optoelectronic properties of these compounds have been investigated using the full potential linearized augmented plane wave plus local orbital (FP-LAPW+lo) method within GGA+U and spin-orbit coupling (SOC) to properly describe the strong correlation of 5f states.…”

Section: Introductionmentioning

confidence: 99%

GGA+U study on phase transition, optoelectronic and magnetic properties of AmO2 with spin–orbit coupling

Bendjedid

Seddik

Khenata

et al. 2015

Journal of Magnetism and Magnetic Materials

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Relativistic band-structure calculations for electronic properties of actinide dioxides

Cited by 20 publications

References 21 publications

Microscopic theory of the insulating electronic ground states of the actinide dioxides AnO2(An = U, Np, Pu, Am, and Cm)

Microscopic theory of the insulating electronic ground states of the actinide dioxides AnO2(An = U, Np, Pu, Am, and Cm)

Key Role of Hybridization between Actinide 5<i>f</i> and Oxygen 2<i>p</i> Orbitals for Electronic Structure of Actinide Dioxides

GGA+U study on phase transition, optoelectronic and magnetic properties of AmO2 with spin–orbit coupling

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Relativistic band-structure calculations for electronic properties of actinide dioxides

Cited by 20 publications

References 21 publications

Microscopic theory of the insulating electronic ground states of the actinide dioxides AnO2(An = U, Np, Pu, Am, and Cm)

Microscopic theory of the insulating electronic ground states of the actinide dioxides AnO2(An = U, Np, Pu, Am, and Cm)

Key Role of Hybridization between Actinide 5&lt;i&gt;f&lt;/i&gt; and Oxygen 2&lt;i&gt;p&lt;/i&gt; Orbitals for Electronic Structure of Actinide Dioxides

GGA+U study on phase transition, optoelectronic and magnetic properties of AmO2 with spin–orbit coupling

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Key Role of Hybridization between Actinide 5<i>f</i> and Oxygen 2<i>p</i> Orbitals for Electronic Structure of Actinide Dioxides