On the electronic structure of the UO2 molecule

Laura Gagliardi; Björn O. Roos; Per Åke Malmqvist; John M. Dyke

doi:10.1021/jp012888z

On the electronic structure of the UO₂ molecule

Laura Gagliardi, Björn O. Roos, Per Åke Malmqvist, John M. Dyke

Chemistry (Twin Cities)

Research output: Contribution to journal › Article › peer-review

88 Scopus citations

Abstract

The structure and vibrational frequencies of the UO₂ molecule have been determined using multiconfigurational wave functions (CASSCF/CASPT2), together with a newly developed method to treat spin-orbit coupling. The molecule has been found to have a (5fφ)(7s), ³Φ_u, Ω = 2 ground state with a U-O bond distance of 1.77 Å. The computed antisymmetric stretching σ_u frequency is 923 cm^-1 with a 16/18 isotope ratio of 1.0525 which compares with the experimental values of 915 cm^-1 and 1.0526, respectively. Calculations of the first adiabatic ionization energy gave the value 6.17 eV, which is 0.7 eV larger than the currently accepted experimental result. Reasons for this difference are suggested.

Original language	English (US)
Pages (from-to)	10602-10606
Number of pages	5
Journal	Journal of Physical Chemistry A
Volume	105
Issue number	46
DOIs	https://doi.org/10.1021/jp012888z
State	Published - Nov 22 2001

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10.1021/jp012888z

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abstract = "The structure and vibrational frequencies of the UO2 molecule have been determined using multiconfigurational wave functions (CASSCF/CASPT2), together with a newly developed method to treat spin-orbit coupling. The molecule has been found to have a (5fφ)(7s), 3Φu, Ω = 2 ground state with a U-O bond distance of 1.77 {\AA}. The computed antisymmetric stretching σu frequency is 923 cm-1 with a 16/18 isotope ratio of 1.0525 which compares with the experimental values of 915 cm-1 and 1.0526, respectively. Calculations of the first adiabatic ionization energy gave the value 6.17 eV, which is 0.7 eV larger than the currently accepted experimental result. Reasons for this difference are suggested.",

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AU - Gagliardi, Laura

AU - Roos, Björn O.

AU - Malmqvist, Per Åke

AU - Dyke, John M.

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AB - The structure and vibrational frequencies of the UO2 molecule have been determined using multiconfigurational wave functions (CASSCF/CASPT2), together with a newly developed method to treat spin-orbit coupling. The molecule has been found to have a (5fφ)(7s), 3Φu, Ω = 2 ground state with a U-O bond distance of 1.77 Å. The computed antisymmetric stretching σu frequency is 923 cm-1 with a 16/18 isotope ratio of 1.0525 which compares with the experimental values of 915 cm-1 and 1.0526, respectively. Calculations of the first adiabatic ionization energy gave the value 6.17 eV, which is 0.7 eV larger than the currently accepted experimental result. Reasons for this difference are suggested.

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On the electronic structure of the UO₂ molecule

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