Combined triple and double bonds to uranium: The N≡U=N-H uranimine nitride molecule prepared in solid argon

Inorganic Chemistry

Volumn 50, Issue 8, 2011, Pages 3826-3831

  Wang, Xuefeng ^a,b   Andrews, Lester ^a,b   Vlaisavljevich, Bess ^c   Gagliardi, Laura ^c  

^a UNIVERSITY OF VIRGINIA   (United States)

^b TONGJI UNIVERSITY   (China)

^c University of Minnesota   (United States)

Author keywords

[No Author keywords available]

Indexed keywords

EID: 79955452635     PISSN: 00201669     EISSN: None     Source Type: Journal    
DOI: 10.1021/ic2003244     Document Type: Article

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60. 28 The terminal NU triple bond contains two σ and four π bonding electrons. The inside UN bond contains four π bonding electrons, and the NH bond involves two σ bonding electrons. B3LYP predicts a larger partial charge on the hydrogen, ca. 0.24. This difference should be attributed to two effects: the basis set employed in the CASSCF/CASPT2 calculations is different compared to the one employed in the B3LYP calculations, and it is well-known that Mulliken population analysis is very sensitive to the basis set. The CASSCF/CASPT2 density is different from the B3LYP density, as expected, and this is reflected in the partial charges. CASSCF theory describes systems in a more "covalent" manner because of the presence of the bonding and antibonding pair of orbitals in the wave functions, and it is thus not unexpected that it predicts the system to be more covalent than a single determinant method like B3LYP.
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