Electronic structure and chemical bonding in actinide oxides

Monoxides and dioxides of Np, Pu, Am, Cm and Bk

V. A. Gubanov*, A. Rosén, Donald E Ellis

*Corresponding author for this work

Research output: Contribution to journalArticle

33 Citations (Scopus)

Abstract

First-principles molecular cluster calculations of the electronic structure of actinide monoxides and dioxides have been carried out in the local density formalism. AcO610- clusters representative of monoxides and AcO812- clusters for dioxides (Ac = Np, Pu, Am, Cm and Bk) have been studied in spin-restricted and spinpolarized models, using the discrete variational method with numerical atomic basis functions. One-electron energy level diagrams, atomic configurations, charge and spin densities were obtained. It is found that significant covalent mixing of O 2ρ and Ac 5f atomic orbitais occurs for heavy actinide compounds, contrary to the assumption of free-ion models. X-ray photoelectron line shape calculations agree rather well with experimental data on the dioxides. Analogies between systematics of the energy levels of actinide and rare-earth compounds are discussed.

Original languageEnglish (US)
Pages (from-to)17-28
Number of pages12
JournalJournal of Physics and Chemistry of Solids
Volume40
Issue number1
DOIs
StatePublished - Jan 1 1979

Fingerprint

Actinoid Series Elements
Actinides
dioxides
Oxides
Electronic structure
electronic structure
Electron energy levels
oxides
energy levels
Rare earth compounds
rare earth compounds
molecular clusters
Photoelectrons
line shape
photoelectrons
diagrams
electron energy
Ions
formalism
X rays

ASJC Scopus subject areas

  • Chemistry(all)
  • Materials Science(all)
  • Condensed Matter Physics

Cite this

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title = "Electronic structure and chemical bonding in actinide oxides: Monoxides and dioxides of Np, Pu, Am, Cm and Bk",
abstract = "First-principles molecular cluster calculations of the electronic structure of actinide monoxides and dioxides have been carried out in the local density formalism. AcO610- clusters representative of monoxides and AcO812- clusters for dioxides (Ac = Np, Pu, Am, Cm and Bk) have been studied in spin-restricted and spinpolarized models, using the discrete variational method with numerical atomic basis functions. One-electron energy level diagrams, atomic configurations, charge and spin densities were obtained. It is found that significant covalent mixing of O 2ρ and Ac 5f atomic orbitais occurs for heavy actinide compounds, contrary to the assumption of free-ion models. X-ray photoelectron line shape calculations agree rather well with experimental data on the dioxides. Analogies between systematics of the energy levels of actinide and rare-earth compounds are discussed.",
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Electronic structure and chemical bonding in actinide oxides : Monoxides and dioxides of Np, Pu, Am, Cm and Bk. / Gubanov, V. A.; Rosén, A.; Ellis, Donald E.

In: Journal of Physics and Chemistry of Solids, Vol. 40, No. 1, 01.01.1979, p. 17-28.

Research output: Contribution to journalArticle

TY - JOUR

T1 - Electronic structure and chemical bonding in actinide oxides

T2 - Monoxides and dioxides of Np, Pu, Am, Cm and Bk

AU - Gubanov, V. A.

AU - Rosén, A.

AU - Ellis, Donald E

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AB - First-principles molecular cluster calculations of the electronic structure of actinide monoxides and dioxides have been carried out in the local density formalism. AcO610- clusters representative of monoxides and AcO812- clusters for dioxides (Ac = Np, Pu, Am, Cm and Bk) have been studied in spin-restricted and spinpolarized models, using the discrete variational method with numerical atomic basis functions. One-electron energy level diagrams, atomic configurations, charge and spin densities were obtained. It is found that significant covalent mixing of O 2ρ and Ac 5f atomic orbitais occurs for heavy actinide compounds, contrary to the assumption of free-ion models. X-ray photoelectron line shape calculations agree rather well with experimental data on the dioxides. Analogies between systematics of the energy levels of actinide and rare-earth compounds are discussed.

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