Theoretical study of the Pu and Am dicarbide molecules

Peter Pogány, Attila Kovács, D. Szieberth, Rudy J M Konings

Research output: Contribution to journalArticle

12 Citations (Scopus)

Abstract

The electronic structure and ground-state molecular properties of Pu and Am dicarbides were investigated in this study by relativistic multireference calculations using CASSCF/CASPT2 theory. The electronic ground states in both the molecules correspond to a symmetrical triangular structure, in which the actinide atom is connected to a C 2 moiety. The other experimentally relevant structure, the symmetrical linear arrangement, is higher than 100 kJ/mol in energy. The bonding characteristics in the two structures were analysed on the basis of the valence molecular orbitals. Besides the usual two-electron bonds, a few one-electron bonding orbitals were also identified. We evaluated the electronic spectra with complete active space state interaction (CASSI) calculations taking into account spin-orbit coupling. The infrared and Raman spectral characteristics were obtained using DFT calculations. Assessment of the present results with the previously reported data on Th and U dicarbides provides information on the change of various molecular parameters in the actinide row.

Original languageEnglish
Pages (from-to)1281-1289
Number of pages9
JournalStructural Chemistry
Volume23
Issue number4
DOIs
Publication statusPublished - Aug 2012

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Actinoid Series Elements
Ground state
Molecules
molecules
ground state
Electrons
molecular properties
Molecular orbitals
Discrete Fourier transforms
electronic spectra
Electronic structure
molecular orbitals
Orbits
electrons
electronic structure
Infrared radiation
valence
orbits
orbitals
Atoms

Keywords

  • Actinide dicarbides
  • Bonding
  • DFT
  • Electronic spectra
  • Multireference calculations

ASJC Scopus subject areas

  • Condensed Matter Physics
  • Physical and Theoretical Chemistry

Cite this

Theoretical study of the Pu and Am dicarbide molecules. / Pogány, Peter; Kovács, Attila; Szieberth, D.; Konings, Rudy J M.

In: Structural Chemistry, Vol. 23, No. 4, 08.2012, p. 1281-1289.

Research output: Contribution to journalArticle

Pogány, Peter ; Kovács, Attila ; Szieberth, D. ; Konings, Rudy J M. / Theoretical study of the Pu and Am dicarbide molecules. In: Structural Chemistry. 2012 ; Vol. 23, No. 4. pp. 1281-1289.
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