Communication: Relativistic Fock-space coupled cluster study of small building blocks of larger uranium complexes

Journal Article · Mon Jul 28 00:00:00 EDT 2014 · Journal of Chemical Physics

DOI:https://doi.org/10.1063/1.4891801· OSTI ID:22419908

Tecmer, Paweł; Visscher, Lucas ^[1]; Severo Pereira Gomes, André ^[2]; Knecht, Stefan ^[3]

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1. Amsterdam Center for Multiscale Modeling (ACMM), VU University Amsterdam, De Boelelaan 1083, 1081 HV Amsterdam (Netherlands)
2. Laboratoire PhLAM, CNRS, UMR 8523, Université de Lille 1, Bât P5, F-59655 Villeneuve d’Ascq Cedex (France)
3. ETH Zürich, Laboratory of Physical Chemistry, Vladimir-Prelog-Weg 2, CH-8093 Zürich (Switzerland)

We present a study of the electronic structure of the [UO{sub 2}]{sup +}, [UO{sub 2}]{sup 2} {sup +}, [UO{sub 2}]{sup 3} {sup +}, NUO, [NUO]{sup +}, [NUO]{sup 2} {sup +}, [NUN]{sup −}, NUN, and [NUN]{sup +} molecules with the intermediate Hamiltonian Fock-space coupled cluster method. The accuracy of mean-field approaches based on the eXact-2-Component Hamiltonian to incorporate spin–orbit coupling and Gaunt interactions are compared to results obtained with the Dirac–Coulomb Hamiltonian. Furthermore, we assess the reliability of calculations employing approximate density functionals in describing electronic spectra and quantities useful in rationalizing Uranium (VI) species reactivity (hardness, electronegativity, and electrophilicity)

• OSTI ID: 22419908
• Journal Information: Journal of Chemical Physics, Vol. 141, Issue 4; Other Information: (c) 2014 AIP Publishing LLC; Country of input: International Atomic Energy Agency (IAEA); ISSN 0021-9606
• Country of Publication: United States
• Language: English

Related Subjects

74 ATOMIC AND MOLECULAR PHYSICS
ACCURACY
APPROXIMATIONS
ELECTRONIC STRUCTURE
HAMILTONIANS
HARDNESS
INTERACTIONS
MOLECULES
SPECTRA
URANIUM
URANIUM COMPLEXES
URANIUM DIOXIDE