The density-functional-theory model for plutonium metal is shown to be consistent with recent magnetic measurements that suggest anti-ferromagnetism in Pu-Ga alloys at low temperatures. The theoretical model predicts a stabilization of the face-centered-cubic (fcc, δ) form of plutonium in an anti-ferromagnetic configuration when alloyed with gallium. The ordered magnetic phase occurs because Ga removes the mechanical instability that exists for unalloyed δ-Pu. The cause of the Ga-induced stabilization is a combination of a lowering of the band (kinetic) and electrostatic (Coulomb) energies for the cubic relative to the tetragonal phase.

The intermetallic Pu6Fe is a precipitate commonly found in standard-purity Pu alloys. We are interested in measuring thermophysical properties of this intermetallic, so we are developing methods for producing Pu6Fe with potential for being scaled up. We had success using a powder-based method, where finely divided PuH2 powder was mechanically mixed with Fe powder and reacted in vacuum. Differential scanning calorimetry was used to analyze the phase content of the product. We estimate ∼90% yield of Pu6Fe by weight, with the remainder being Pu. Enthalpy of melting for Pu6Fe was measured to be 31.2 J/g, and the onset temperature was 411.5°C. The product was melted 3 times and appeared to become more homogeneous after each cycle.

γ-U alloys with Mo or Zr are more resistant to hydrogen than U metal. High pressures of H are needed to produce hydrides. Amorphous structure of UH3Mox can be represented as the cubic structure of β-UH3 type with grain size around 1 nm. UH3Zrx are formed in the cubic α-UH3 type of structure. All the hydrides are ferromagnets, with magnetic parameters (magnetic moments, Curie temperature) exceeding those of β-UH3 (0.9 μB/U, 165-170 K). It is deduced that α-UH3 has magnetic properties very similar to β-UH3, despite rather different U-U spacing.

Zirconolite (CaZrTi2O7) is one of the components of Synroc materials, which are regarded throughout the world nuclear as the second generation of high-level nuclear waste forms. The zirconolite phase was synthesized by a sol-gel method, with one variant of the method making use of ascorbic acid as a strong complexing agent. Into the structure of the zirconolite was incorporated 10 mol% Sr. Undoped and doped samples were examined by thermal analyses and X-ray diffraction. Addition of ascorbic acid to the sols lowered the firing temperature and promoted formation of the zirconolite phase.

The combination of density functional theory in local density approximation and dynamical mean field theory (LDA+DMFT) was employed in a preliminary study of the strong electron correlation effects in a promising nuclear fuel—uranium mononitride (UN). For the ferromagnetic phase, the effective impurity problem arising in the LDA+DMFT [1-3] cycle is solved with the spin-polarized T-matrix fluctuation exchange (SPTF) solver, which includes spin–orbit interactions. Concerning the paramagnetic phase, the disordered local moment (DLM) approach was used, based on both standard local density approximation (LDA) and LDA+U. Basic spectral properties and material properties, such as the spin, orbital and total magnetic moments on U atom were calculated for various values of the Hubbard parameter U with a fixed exchange parameter J. Our main focus was to compare the calculated spectral functions (density of states) for different magnetic phases and different methods to the experimental XPS data [4]. On top of that, the total moments of the paramagnetic and ferromagnetic phases are compared with the measured values by neutron spectroscopy [4, 5].

Surprisingly little is known about the mechanism and symmetry of superconducting pairing in PuCoGa5. A common thread with other unconventional superconductors is the presence of spin fluctuations in the normal state, which in this particular case is controlled by strong spin–orbit coupling split bands. The many and anisotropic Fermi surfaces make the guessing of the potential spin-fluctuation nesting vector and resulting symmetry of the pairing function a nontrivial task. To provide much needed guidance for the identification of the pairing symmetry in this multiband superconductor, we perform first-principles based magnetic spin susceptibility calculations to identify the dominant nesting vectors that potentially give rise to interband pairing with nodal d- or s±-wave gap functions.

We examine a novel phase of the underscreened Anderson lattice Model that might pertain to the ”Hidden Ordered” phase of URu2Si2. We show that the system breaks spin-rotational invariance below the critical temperature and spontaneously selects a preferred axis of spin quantization. As a result, the low temperature phase exhibits a magnetic anisotropy, where the electronic properties depend not only on the magnitude of the magnetic field but also on the orientation of the applied field relative to the axis of quantization. The results are discussed in the context of recent experimental findings on URu2Si2.

Density-functional theory (DFT) simulations are applied to obtain elastic, strength, and EOS properties of actinide metals under extreme conditions. In this presentation, we will show our recent study on temperature effects of the properties of solids of actinide metals. For example of low temperature uranium (U) solids, elastic constants are calculated directly from the DFT total energy for the ground-state phase in a wide pressure range. For higher temperature U solids, we are applying a recent scheme to calculate temperature-dependent phonon dispersions through the self-consistent ab initio lattice dynamics (SCAILD) technique. This scheme is particular important for the higher temperature phases that the elasticity cannot be analogously obtained because of its mechanical instability at lower temperatures. From these SCAILD phonon dispersions we then extract the elastic constants from the slopes approaching the Γ point. In addition, the phonon density of states of U obtained from SCAILD/DFT calculations have been used to parameterize a double Debye model for its ion-thermal free energy. We will discuss the ramification of this new Debye model on our development of multi-phase uranium EOS.

We present a computational density functional theory study of UF6 adsorption on ideal as well as hydrogenated and fluorinated graphene. We show that (i) the isotopic splitting in the vibrational spectrum of UF6 observed in vacuum is largely preserved in the adsorbed molecules. The existence of several adsorption configurations with competing Eads leads to overlaps in the vibrational spectra of isotopomers, but isotopomer-unique modes exist on all three surfaces. (ii) The adsorption energy of UF6 is of the order of 1.2 eV on ideal graphene, 1 eV on graphane, and 0.1 eV on fluorographene, i.e. the adsorption strength is moderate and can be controlled by surface modification. (i) and (ii) mean that it may be possible to cause desorption of a selected isotopomer by laser radiation, leading to isotopic separation between the surface and the gas.

Uranium dioxide (UO2) microspheres were fabricated by two sol-gel processes. First used was a classical process variant, as developed at Oak Ridge National Laboratory, consisting of (1) reduction of commercial uranyl to U(IV) nitrate; (2) preparation of a sol by precipitation of uranium hydroxide, its peptization, and solvent extraction of nitrates; and (3) gelation to microspheres by extraction of water through addition of a dewatered 2-ethyl-1-hexanol emulsion. Substantial improvement in microsphere production was achieved by application of a sol-gel process in which ascorbic acid was used as strong complexing agent. In this method, the reduction step was omitted and uranyl (VI) ascorbate sols/hydroxyl sols were formed from a suspension of either a uranium trioxide or a uranyl nitrate solution. Gelation through water extraction yielded perfect microspheres. Other metals can be easy added to these sols. Thermal treatment of the UO2 microspheres by calcination and reduction in hydrogen atmosphere was designed on the basis of differential thermal analysis and thermogravimetric analysis.

This is a preliminary report of a neutron scattering experiment used to investigate 4f electron behavior in Ce.