Relativistic density functional theory modeling of plutonium and americium higher oxide molecules
Abstract
The results of electronic structure modeling of plutonium and americium higher oxide molecules (actinide oxidation states VI through VIII) by two-component relativistic density functional theory are presented. Ground-state equilibrium molecular structures, main features of charge distributions, and energetics of AnO3, AnO4, An2On (An=Pu, Am), and PuAmOn, n = 6-8, are determined. In all cases, molecular geometries of americium and mixed plutonium-americium oxides are similar to those of the corresponding plutonium compounds, though chemical bonding in americium oxides is markedly weaker. Relatively high stability of the mixed heptoxide PuAmO7 is noticed; the Pu(VIII) and especially Am(VIII) oxides are expected to be unstable.
- Publication:
-
Journal of Chemical Physics
- Pub Date:
- July 2013
- DOI:
- 10.1063/1.4813284
- Bibcode:
- 2013JChPh.139c4307Z
- Keywords:
-
- americium compounds;
- bonds (chemical);
- density functional theory;
- ground states;
- molecular configurations;
- plutonium compounds;
- relativistic corrections;
- 31.15.E-;
- 31.15.ve;
- 33.15.Bh;
- 31.15.aj;
- Density-functional theory;
- Electron correlation calculations for atoms and ions: ground state;
- General molecular conformation and symmetry;
- stereochemistry;
- Relativistic corrections spin-orbit effects fine structure;
- hyperfine structure