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A relativistic density functional study on the uranium hexafluoride and plutonium hexafluoride monomer and dimer species

A relativistic density functional study on the uranium hexafluoride and plutonium hexafluoride monomer and dimer species
A relativistic density functional study on the uranium hexafluoride and plutonium hexafluoride monomer and dimer species
A study on the UF6 monomer and dimer was carried out within the density functional method. The U-F distance in the UF6 monomer was optimized at different levels of theory, pointwise, assuming octahedral geometry, (1) by using an all-electron basis for both U and F in a nonrelativistic calculation; (2) by using a relativistic effective core potential (RECP) on U and nonrelativistic effective core potential (ECP) on the fluorines; and (3) by using RECP on the U atom and an all-electron basis on the F atoms. Atomization energies of 23.11, 33.92, and 35.66 eV were obtained at the three levels, respectively. Relativistic effects lead to about a 50% increase in the atomization energy. For the UF6 dimer, the potential energy curve, as a function of the intermolecular U-U distance, was computed at level 2, and the rotational barrier between the two monomers was determined. Similar calculations were performed on the corresponding PuF6 species. Comparisons are made with experiment and other theoretical studies, where available.
0002-7863
11727-11731
Gagliardi, L.
7289d411-f5b8-4b27-ae02-4eac1ee375b3
Willetts, A.
d24306c3-24c6-42ec-8317-ab5b006357f2
Skylaris, C.-K.
8f593d13-3ace-4558-ba08-04e48211af61
Handy, N. C.
989ad94d-4c70-4f00-94f1-d7c3e341d326
Spencer, S.
ad30ed7a-86f1-40dc-a09d-e1aeb74ba562
Ioannou, A. G.
6056113c-886d-4f46-b2f9-169fb764c4f7
Simper, A. M.
f2c83221-a0f8-4625-84e5-0d7b6fdcbf46
Gagliardi, L.
7289d411-f5b8-4b27-ae02-4eac1ee375b3
Willetts, A.
d24306c3-24c6-42ec-8317-ab5b006357f2
Skylaris, C.-K.
8f593d13-3ace-4558-ba08-04e48211af61
Handy, N. C.
989ad94d-4c70-4f00-94f1-d7c3e341d326
Spencer, S.
ad30ed7a-86f1-40dc-a09d-e1aeb74ba562
Ioannou, A. G.
6056113c-886d-4f46-b2f9-169fb764c4f7
Simper, A. M.
f2c83221-a0f8-4625-84e5-0d7b6fdcbf46

Gagliardi, L., Willetts, A., Skylaris, C.-K., Handy, N. C., Spencer, S., Ioannou, A. G. and Simper, A. M. (1998) A relativistic density functional study on the uranium hexafluoride and plutonium hexafluoride monomer and dimer species. Journal of the American Chemical Society, 120 (45), 11727-11731. (doi:10.1021/ja9811492).

Record type: Article

Abstract

A study on the UF6 monomer and dimer was carried out within the density functional method. The U-F distance in the UF6 monomer was optimized at different levels of theory, pointwise, assuming octahedral geometry, (1) by using an all-electron basis for both U and F in a nonrelativistic calculation; (2) by using a relativistic effective core potential (RECP) on U and nonrelativistic effective core potential (ECP) on the fluorines; and (3) by using RECP on the U atom and an all-electron basis on the F atoms. Atomization energies of 23.11, 33.92, and 35.66 eV were obtained at the three levels, respectively. Relativistic effects lead to about a 50% increase in the atomization energy. For the UF6 dimer, the potential energy curve, as a function of the intermolecular U-U distance, was computed at level 2, and the rotational barrier between the two monomers was determined. Similar calculations were performed on the corresponding PuF6 species. Comparisons are made with experiment and other theoretical studies, where available.

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Published date: 1998

Identifiers

Local EPrints ID: 38413
URI: https://eprints.soton.ac.uk/id/eprint/38413
ISSN: 0002-7863
PURE UUID: a4582c6b-18fd-4632-b9fc-ecf54435b5dc
ORCID for C.-K. Skylaris: ORCID iD orcid.org/0000-0003-0258-3433

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Date deposited: 08 Jun 2006
Last modified: 17 Jul 2018 00:32

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Contributors

Author: L. Gagliardi
Author: A. Willetts
Author: C.-K. Skylaris ORCID iD
Author: N. C. Handy
Author: S. Spencer
Author: A. G. Ioannou
Author: A. M. Simper

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