Dual 5f character in two allotropes of uranium trihydride studied via a first principles calculation

Li, Rusong; Wan, Yi-dan; Lü, Xing; Wang, Jintao; Xin, Duqiang; Jianxiang, Zhang

doi:10.1016/j.chemphys.2020.110876

Cited by 8 publications

(8 citation statements)

References 36 publications

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“…Previous experimental observation and theoretical calculations both suggest that the spin–orbit coupling (SOC) interaction is responsible for the characteristic f-derived features in f-electron-based materials, , in particular, the multiplet structures in the vicinity of the Fermi level. The SOC interaction would split f orbitals into two manifolds with the total angular momenta of j = 5/2 and j = 7/2, respectively; this picture also holds true for CeAs addressed in this work. In fact, the spin–orbit strength is computed within DFT cycles and needs to be updated during self-consistent DFT + DMFT calculations .…”

Section: Computational Detailssupporting

confidence: 56%

Structure-Dependent Phase Diagram of the Occupation Number of 4f Electrons in Cerium Monoarsenide

Xie

Xin

et al. 2022

J. Phys. Chem. C

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In order to investigate the structure-dependent correlation strength and occupation number of 4f electrons in cerium monoarsenide (CeAs) with the NaCl-type (B1-type) and CsCl-type (B2-type) structures, respectively, we perform a first principles calculation based on a many-body method merging density functional theory with dynamical mean-field theory (DMFT). Calculation results suggest that with the increase of the lattice constants, the Ce 4f j = 7/2 manifold maintains the insulating behavior, while the j = 5/2 component undergoes the insulating → metallic → insulating and the insulating → metallic transitions, respectively, for B1-type and B2-type structures. Quasi-particle weights demonstrate that the j = 7/2 manifold is in the weakly correlated regime, and the j = 5/2 component transforms from the weakly to moderately correlated state, irrespective of the crystal structure. Ce 4f electrons transform from a slight itinerant state into a localized state for the B1-type structure. A structure-dependent phase diagram of the occupation number suggests that the occupation numbers of individual 4f n (n = 0, 1, 2, 3) configurations and Ce 4f electrons (n f) could be modulated in terms of the crystal structure and/or the lattice constant.

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Section: Computational Detailssupporting

confidence: 56%

Structure-Dependent Phase Diagram of the Occupation Number of 4f Electrons in Cerium Monoarsenide

Xie

Xin

et al. 2022

J. Phys. Chem. C

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“…1(b)) of U( i ) and U( ii ) in intact β-UH 3 are different, and specifically they exhibit the localized and itinerant characters, respectively. 25 The H atoms reside in the U-tetrahedral sites of β-UH 3 with a distance of 2.26 Å from the four caged U atoms, and the volume of each U-tetrahedron is 6.23 Å 3 .…”

Section: Resultsmentioning

confidence: 99%

“…S1 (ESI †), the density of states shows that b-UH 3 is metallic and the 5f states of U are positioned at the Fermi level, which are consistent with the experimental result. 25 But, the localization of 5f electrons increases with U eff increasing, which is more obvious in spin density. In Fig.…”

Section: Methodsmentioning

confidence: 94%

“…The decomposition mechanism of b-UH 3As shown in Fig.1(a), the b-UH 3 is depicted by four separated UH 12 cages labelled as cages 1-4, and twelve uncaged/interstitial U atoms; especially, U atoms in b-UH 3 can be divided into two types: caged U in UH 12 and uncaged/interstitial U corresponding to sites ''I'' and ''II'' named by Taylor 28. The spin densities (Fig.1(b)) of U(I) and U(II) in intact b-UH 3 are different, and specifically they exhibit the localized and itinerant characters, respectively 25. The H atoms reside in the U-tetrahedral sites of b-UH 3 with a distance of 2.26 Å from the four caged U atoms, and the volume of each U-tetrahedron is 6.23 Å 3 .…”

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confidence: 99%

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Initial decomposition mechanisms and the inverse effects of temperature and P_H₂ on the thermodynamic stability of UH₃

Zhang

Zhao

Song

et al. 2023

Phys. Chem. Chem. Phys.

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“…Furthermore, either DFT + U with the inherent static treatment of the electronic correlation or the hybrid functionals might fail to capture the spectra feature of the moderately correlated systems. For example, abovementioned techniques could not appropriately capture the complicated electronic structures of Pu-based materials, which simultaneously exhibit the quasi-particle peaks in the vicinity of Fermi energy, the lower Hubbard band (LHB) and the upper Hubbard band (UHB) due to coexistence of itinerant and localized 5f electrons [19,33]. More recently, a unified many-body scheme (DFT + DMFT) could be employed to the weakly, moderately and strongly correlated systems on the same footing and, simultaneously captures the band-like and atomic-like features of electronic states [34].…”

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confidence: 99%

Site‐dependent correlation strength and occupation number of 5f electrons in alpha phase plutonium metal

Lü

Xin

et al. 2023

Int J of Quantum Chemistry

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In order to quantify the site‐dependent correlation strengths in terms of the quasi‐particle weights and the occupation numbers of 5f electrons in alpha phase plutonium metal with eight crystallographically nonequivalent atomic sites Pun (n = 1–8), we perform a first principles calculation by using a many‐body method merging density functional theory with dynamical mean‐field theory plus the relativistic and correlation effects. The quasi‐particle weight, the electronic spectrum function, the hybridization function, as well as the occupation number of Pu 5f electrons all suggest that Pu1 and Pu8 atoms have the most itinerant and the most localized 5f electrons, respectively, while the other atoms Pun (n = 2–7) exhibit an intermediate correlation strength. The quasi‐particle weights demonstrate that only the jj or intermediate coupling scheme is more appropriate for Pu 5f electrons in comparison with the Russel–Saunders (LS) scheme. The electronic spectrum function and the occupation analysis establish that Pu 5f electrons simultaneously have dual itinerant and localized regimes with average 5f occupation numbers of n5f between 4.8994 and 4.9628, which are mainly composed of 5f4, 5f5, and 5f6 configurations, irrespective of different atomic sites. Finally, we also estimate the so‐called quasi‐particle band structure to directly compare with angle‐resolved photoemission spectrum.

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Dual 5f character in two allotropes of uranium trihydride studied via a first principles calculation

Cited by 8 publications

References 36 publications

Structure-Dependent Phase Diagram of the Occupation Number of 4f Electrons in Cerium Monoarsenide

Structure-Dependent Phase Diagram of the Occupation Number of 4f Electrons in Cerium Monoarsenide

Initial decomposition mechanisms and the inverse effects of temperature and P_H₂ on the thermodynamic stability of UH₃

Site‐dependent correlation strength and occupation number of 5f electrons in alpha phase plutonium metal

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Dual 5f character in two allotropes of uranium trihydride studied via a first principles calculation

Cited by 8 publications

References 36 publications

Structure-Dependent Phase Diagram of the Occupation Number of 4f Electrons in Cerium Monoarsenide

Structure-Dependent Phase Diagram of the Occupation Number of 4f Electrons in Cerium Monoarsenide

Initial decomposition mechanisms and the inverse effects of temperature and PH2 on the thermodynamic stability of UH3

Site‐dependent correlation strength and occupation number of 5f electrons in alpha phase plutonium metal

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Initial decomposition mechanisms and the inverse effects of temperature and P_H₂ on the thermodynamic stability of UH₃