Molecular structure and thermodynamic properties of the gaseous ThC2 and ThC4 species

Kovács, Attila; Konings, R.J.M.

doi:10.1016/j.jnucmat.2007.04.049

Cited by 15 publications

(10 citation statements)

References 18 publications

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“…The present multireference calculations confirm the planar fan‐type structure ( I ; see Figure 1) to be the global minimum for both tetracarbides, thus supporting the previous single‐reference MP2 results on ThC 4 16. Moreover, structure I has the lowest energy for all the spin multiplicities covered in the present study for ThC 4 and UC 4 .…”

Section: Resultssupporting

confidence: 90%

“…The electronic ground states of UC and some actinide dicarbides have been computed very recently by using relativistic multireference methods: (UC, UC 2 ),10,11 (ThC 2 , UC 2 ),17 (PuC 2 , AmC 2 ) 18. We note that the main properties of ThC 2 were in good agreement with the above‐mentioned MP2 study 16…”

Section: Introductionsupporting

confidence: 77%

“…The early discrete variational Xα calculations on UC 2 13 and the first DFT calculations using relativistic effective core potentials (RECP) on UC 2 14 and PuC and PuC 2 15 had some deficiencies. The recently obtained MP2 data on ThC 2 and ThC 4 16 are more reliable, as shown by later studies (see below). Yet, the multiconfigurational character of these thorium molecules has remained an open question as well as the structural isomerism, as only two structures of each carbide have been investigated 16.…”

Section: Introductionsupporting

confidence: 62%

“…The recently obtained MP2 data on ThC 2 and ThC 4 16 are more reliable, as shown by later studies (see below). Yet, the multiconfigurational character of these thorium molecules has remained an open question as well as the structural isomerism, as only two structures of each carbide have been investigated 16. The electronic ground states of UC and some actinide dicarbides have been computed very recently by using relativistic multireference methods: (UC, UC 2 ),10,11 (ThC 2 , UC 2 ),17 (PuC 2 , AmC 2 ) 18.…”

Section: Introductionsupporting

confidence: 62%

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Theoretical Study of Thorium and Uranium Tetracarbide Molecules

2014

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Keywords: Actinides / Thorium / Uranium / Density functional calculations / Bond theoryThe electronic structure and ground-state molecular properties of neutral Th and U tetracarbides were investigated by relativistic multireference calculations using complete active space self-consistent field/multiconfiguration second-order perturbation theory (CASSCF/CASPT2) with an all-electron basis set as well as by density functional theory (B3LYP) in conjunction with relativistic pseudopotentials. The former calculations were extended with complete active space state interaction (CASSI) calculations accounting for spin-orbit coupling. The four carbon atoms can be arranged in various forms around the actinide atom to result in ten structural isomers found altogether in our study. The electronic ground state in both molecules corresponds to a planar fan-type

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Section: Resultssupporting

confidence: 90%

Section: Introductionsupporting

confidence: 77%

Section: Introductionsupporting

confidence: 62%

Section: Introductionsupporting

confidence: 62%

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Theoretical Study of Thorium and Uranium Tetracarbide Molecules

2014

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“…The correct electronic ground states of some actinide carbides have been elucidated only recently by means of advanced relativistic multireference calculations (UC, UC 2 , ThC 2 , UC 2 , PuC 2 , AmC 2 , UC 2 , UC 3 ). We note that these recent calculations on ThC 2 confirmed the main properties predicted previously using the MP2/RECP method …”

Section: Introductionsupporting

confidence: 87%

Theoretical study of Pu and Am tetracarbide molecules

Pogány

Kovács

Konings

2014

Int J of Quantum Chemistry

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The electronic structure and ground‐state molecular properties of Pu and Am tetracarbides have been investigated by relativistic multireference calculations using CASSCF/CASPT2 theory as well as by density functional theory in conjunction with relativistic pseudopotentials. The CASSCF/CASPT2 treatment has been extended by spin–orbit coupling effects for selected species using the CAS state‐interaction method. The five atoms can form various structural isomers, from which 12 ones have been identified in our study. The electronic ground state in both molecules corresponds to a planar fan‐type structure of C2v symmetry, in which the actinide atom is connected to a bent C4 moiety. The other structures are much higher in energy, the ones computed in this study appear between 250 and 1050 kJ/mol. The bonding characteristics in the most relevant structures have been analyzed on the basis of the valence molecular orbitals and natural bond orbital analysis. The most stable structures have been characterized by their spectroscopic (vibrational and electron) properties. © 2014 Wiley Periodicals, Inc.

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