Dynamical mean-field theory of photoemission spectra of actinide compounds

Svane, A.

doi:10.1016/j.ssc.2006.08.049

Cited by 39 publications

(38 citation statements)

References 25 publications

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“…Attempts to explain spectra in terms of LS multiplets were not successful, proving the strong spin orbit coupling typical for the actinides. For PuSe, all spectral features observed were recently explained on the basis of DMFT theory constructed to reflect many body effects as multiplet excitations as well as hybridisation with conduction electrons [15]. Similar spectra with such difference in the peak resolution have been observed for the rare earth chalcogenides [14].…”

Section: Pusisupporting

confidence: 62%

Comparative Photoemission Study of Actinide (Am, Pu, Np and U) Metals, Nitrides, and Hydrides

Thomas¹,

Seibert²,

Huber³

et al. 2006

MRS Proc.

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Core-level and valence-band spectra of Pu and the other early actinide compounds show remarkable systematics, which can be understood in the framework of final state screening. We compare the early actinide (U, Np, Pu and Am) metals, nitrides and hydrides and a few other specific compounds (PuSe, PuS, PuC x , PuSi x ) prepared as thin films by sputter deposition. In choosing these systems, we combine inherent 5f band narrowing, due to 5f orbital contraction throughout the actinide series, with variations of the chemical environment in the compounds. Goal of this work was to learn more on the electronic structure of the early actinide systems and to achieve the correct interpretation of their photoemission spectra. The highly correlated nature of the 5f states in systems, which are on the verge to localization, makes this a challenging task, because of the peculiar interplay between ground state DOS and final-state effects. Their influence can be estimated by doing systematic studies on systems with different (5f) bandwidths. We conclude on the basis of such systematic experiments that final-state effects due to strong e-e correlations in narrow 5f-band systems lead to multiplet like structures, analogous to those observed in the case of systems with localized electron states. Such observations in essentially band-like 5f-systems was first surprising, but the astonishing similarity of photoemission spectra of very different chemical systems (e.g. PuSe, Pu 2 C 3 and δ-Pu) points to a common origin, relating them to atomic features rather than material dependent density of states (DOS) features.Mater. Res. Soc. Symp. Proc. Vol. 986

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Section: Pusisupporting

confidence: 62%

Comparative Photoemission Study of Actinide (Am, Pu, Np and U) Metals, Nitrides, and Hydrides

Thomas¹,

Seibert²,

Huber³

et al. 2006

MRS Proc.

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“…In fact, multiplet structure in combination with band-like spectra have employed in a variety of PE studies on actinides (Okada, 1999;Gouder et al, 2005;Svane, 2006;Shick et al, 2007). What is more, this mixture of band-like and atomic-like behavior forces the question when doing calculations whether to start from a band or atomic limit.…”

Section: Kondo Resonancementioning

confidence: 99%

Nature of the5fstates in actinide metals

2009

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Actinide elements produce a plethora of interesting physical behaviors due to the 5f states. This review compiles and analyzes progress in understanding of the electronic and magnetic structure of the 5f states in actinide metals. Particular interest is given to electron energy-loss spectroscopy and many-electron atomic spectral calculations, since there is now an appreciable library of core d → valence f transitions for Th, U, Np, Pu, Am, and Cm. These results are interwoven and discussed against published experimental data, such as x-ray photoemission and absorption spectroscopy, transport measurements, and electron, x-ray, and neutron diffraction, as well as theoretical results, such as density-functional theory and dynamical mean-field theory.

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“…23,32 The recent development of dynamical mean-field theory ͑DMFT͒, 33 combined with the LDA+ U approach, has enriched the field in terms of phenomena accessible to calculations, including both ground state cohesion, 24 phonons, 25 and photoemission. 26,27,34 However, most applications to date invoke the Hubbard Hamiltonian and inherit the uncertainties PHYSICAL REVIEW B 76, 115116 ͑2007͒ …”

mentioning

confidence: 99%

Self-interaction-corrected local spin density theory of5felectron localization in actinides

et al. 2007

Self Cite

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The electronic structures of the actinide elements U, Np, Pu, Am, Cm, and Bk are investigated within the self-interaction-corrected local spin density approximation. This method allows us to describe a dual character of the 5f electrons, some of which occupy localized and corelike states, while the remaining 5f electrons hybridize and form bands. Based on energetics, the calculations predict delocalization and/or paramagnetism in the early actinides and localization and/or antiferromagnetism in the later actinides. The corresponding calculated equilibrium volumes are in agreement with the experimental values. For Pu and Am, the method wrongly predicts magnetic ordering, but we find that the paramagnetic state gives a better description of cohesive properties. Under compression, in the later actinides, a localization-delocalization transition happens gradually as more and more f electrons become bandlike with decreasing volume. Pu is already at this transition point at ambient conditions. Delocalization sets in for Am and Bk at a compression of V ϳ 0.75V 0 , for Cm at V ϳ 0.60V 0 , where V 0 is the equilibrium volume, and the transition is complete for V ϳ͑0.4-0.5͒V 0 in these three elements.Am. 23,32 The recent development of dynamical mean-field theory ͑DMFT͒, 33 combined with the LDA+ U approach, has enriched the field in terms of phenomena accessible to calculations, including both ground state cohesion, 24 phonons, 25 and photoemission. 26,27,34 However, most applications to date invoke the Hubbard Hamiltonian and inherit the uncertainties PHYSICAL REVIEW B 76, 115116 ͑2007͒

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Dynamical mean-field theory of photoemission spectra of actinide compounds

Cited by 39 publications

References 25 publications

Comparative Photoemission Study of Actinide (Am, Pu, Np and U) Metals, Nitrides, and Hydrides

Comparative Photoemission Study of Actinide (Am, Pu, Np and U) Metals, Nitrides, and Hydrides

Nature of the5fstates in actinide metals

Self-interaction-corrected local spin density theory of5felectron localization in actinides

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