Actinide Ground-State Properties-Theoretical Predictions
Actinide Ground-State Properties Theoretical predictions John M. Wills and Olle Eriksson electron-electron correlations—the electronic energy of the ground state of or nearly fifty years, the actinides interactions among the 5f electrons and solids, molecules, and atoms as a func- defied the efforts of solid-state between them and other electrons—are tional of electron density. The DFT Ftheorists to understand their expected to affect the bonding. prescription has had such a profound properties. These metals are among Low-symmetry crystal structures, impact on basic research in both the most complex of the long-lived relativistic effects, and electron- chemistry and solid-state physics that elements, and in the solid state, they electron correlations are very difficult Walter Kohn, its main inventor, was display some of the most unusual to treat in traditional electronic- one of the recipients of the 1998 behaviors of any series in the periodic structure calculations of metals and, Nobel Prize in Chemistry. table. Very low melting temperatures, until the last decade, were outside the In general, it is not possible to apply large anisotropic thermal-expansion realm of computational ability. And DFT without some approximation. coefficients, very low symmetry crystal yet, it is essential to treat these effects But many man-years of intense research structures, many solid-to-solid phase properly in order to understand the have yielded reliable approximate transitions—the list is daunting. Where physics of the actinides. Electron- expressions for the total energy in does one begin to put together an electron correlations are important in which all terms, except for a single- understanding of these elements? determining the degree to which 5f particle kinetic-energy term, can be In the last 10 years, together with electrons are localized at lattice sites.
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