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

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)
Authors:
;  [1] ;  [2] ;  [3]
  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)
Publication Date:
OSTI Identifier:
22419908
Resource Type:
Journal Article
Resource Relation:
Journal Name: Journal of Chemical Physics; Journal Volume: 141; Journal Issue: 4; Other Information: (c) 2014 AIP Publishing LLC; Country of input: International Atomic Energy Agency (IAEA)
Country of Publication:
United States
Language:
English
Subject:
74 ATOMIC AND MOLECULAR PHYSICS; ACCURACY; APPROXIMATIONS; ELECTRONIC STRUCTURE; HAMILTONIANS; HARDNESS; INTERACTIONS; MOLECULES; SPECTRA; URANIUM; URANIUM COMPLEXES; URANIUM DIOXIDE