Resonant inelastic x-ray scattering from UOand UN.

Resonant inelastic x-ray scattering (RIXS) using an incident energy tuned to the uraniumN4,5absorption edges is reported from epitaxial films of-UOand UN. Theory shows that for UOthe multiplets associated with a 5configuration with a ground state of2F5/2and the excited state of2F7/2are observed. However, the strong transition predicted at a transfer energy of 1.

Temperature-dependent anisotropy in the bond lengths of UOas a result of phonon-induced atomic correlations.

Previous experiments on cubic UOhave suggested that the temperature dependences of the nearest-neighbour U-O and U-U distances are. We have acquired total-scattering neutron diffraction patterns out to = 23.5 Åfor50 View Article and Find Full Text PDF

Thermal Energy Transport in Oxide Nuclear Fuel.

To efficiently capture the energy of the nuclear bond, advanced nuclear reactor concepts seek solid fuels that must withstand unprecedented temperature and radiation extremes. In these advanced fuels, thermal energy transport under irradiation is directly related to reactor performance as well as reactor safety. The science of thermal transport in nuclear fuel is a grand challenge as a result of both computational and experimental complexities.

X-ray synchrotron radiation studies of actinide materials.

By reviewing a selection of X-ray diffraction (XRD), resonant X-ray scattering (RXS), X-ray magnetic circular dichroism (XMCD), resonant and non-resonant inelastic scattering (RIXS, NIXS), and dispersive inelastic scattering (IXS) experiments, the potential of synchrotron radiation techniques in studying lattice and electronic structure, hybridization effects, multipolar order and lattice dynamics in actinide materials is demonstrated.

Resonant inelastic x-ray spectroscopy on UO as a test case for actinide materials.

Resonant inelastic x-ray spectroscopy at the uranium N absorption edge at 778 eV has been used to reveal the excitations in UO up to 1 eV. The earlier (1989) studies by neutron inelastic scattering of the crystal-field states within the H multiplet are confirmed. In addition, the first excited state of the F multiplet at ∼520 meV has been established, and there is a weak signal corresponding to the next excited state at ∼920 meV.

The fifty years it has taken to understand the dynamics of UOin its ordered state.

In 1966 Roger Cowley (together with Gerald Dolling) reported the first neutron inelastic scattering from the magnetic excitations from UObelow its antiferromagnetic ordering temperature of 30 K. They showed the strong magnon-phonon coupling in this material and that the excitations appeared to contain an additional mode that was not anticipated. Cowley never returned to UO, but showed a keen interest in the developments.

Probing Magnetism in the Vortex Phase of PuCoGa_{5} by X-Ray Magnetic Circular Dichroism.

We measure x-ray magnetic circular dichroism (XMCD) spectra at the Pu M_{4,5} absorption edges from a newly prepared high-quality single crystal of the heavy-fermion superconductor ^{242}PuCoGa_{5}, exhibiting a critical temperature T_{c}=18.7  K. The experiment probes the vortex phase below T_{c} and shows that an external magnetic field induces a Pu 5f magnetic moment at 2 K equal to the temperature-independent moment measured in the normal phase up to 300 K by a superconducting quantum interference device.

Magnetic polarization of the americium J=0 ground state in AmFe(2).

Trivalent americium has a nonmagnetic (J=0) ground state arising from the cancellation of the orbital and spin moments. However, magnetism can be induced by a large molecular field if Am^{3+} is embedded in a ferromagnetic matrix. Using the technique of x-ray magnetic circular dichroism, we show that this is the case in AmFe_{2}.

Distinct magnetic phase transition at the surface of an antiferromagnet.

In the majority of magnetic systems the surface is required to order at the same temperature as the bulk. In the present Letter, we report a distinct and unexpected surface magnetic phase transition at a lower temperature than the Néel temperature. Employing grazing incidence x-ray resonant magnetic scattering, we have observed the near-surface behavior of uranium dioxide.

Understanding the complex phase diagram of uranium: the role of electron-phonon coupling.

We report an experimental determination of the dispersion of the soft phonon mode along [100] in uranium as a function of pressure. The energies of these phonons increase rapidly, with conventional behavior found by 20 GPa, as predicted by recent theory. New calculations demonstrate the strong pressure (and momentum) dependence of the electron-phonon coupling, whereas the Fermi-surface nesting is surprisingly independent of pressure.

Resonant x-ray scattering investigation of magnetic ordering in NpAs(1 - x)Se(x) (x = 0.05, 0.10).

A resonant x-ray scattering investigation of the NpAs(1 - x)Se(x) system with single crystals of 5 and 10% Se content is reported. The main features of the magnetic phase diagram previously studied by neutron scattering were confirmed. The coexistence within a single domain of ferro- and antiferro-components in the low-T ferrimagnetic phase was established, as well as the single-k character of the incommensurate phase and of the antiferromagnetic component of the ferrimagnetic phase.

Polarized-neutron-scattering study of the spin-wave excitations in the 3-k ordered phase of uranium antimonide.

The anisotropy of magnetic fluctuations propagating along the [1 1 0] direction in the ordered phase of uranium antimonide has been studied using polarized inelastic neutron scattering. The observed polarization behavior of the spin waves is a natural consequence of the longitudinal 3-k magnetic structure; together with recent results on the 3-k-transverse uranium dioxide, these findings establish this technique as an important tool to study complex magnetic arrangements. Selected details of the magnon excitation spectra of USb have also been reinvestigated, indicating the need to revise the currently accepted theoretical picture for this material.

Anomalous shift of magnetic diffuse scattering studied by neutron diffraction.

Neutron diffraction results, in the vicinity of the magnetic phase transition of USb and MnF(2), are reported. The thermal evolution of the magnetic diffuse signal and nuclear Bragg reflections demonstrate that the centre of gravity of the magnetic signals does not lie at the predicted position as calculated from nuclear reflections. This phenomenon, called the q-shift, was first found using resonance x-ray scattering (RXS).

Electronic state of PuCoGa5 and NpCoGa5 as probed by polarized neutrons.

By using single crystals and polarized neutrons, we have measured the orbital and spin components of the microscopic magnetization in the paramagnetic state of NpCoGa(5) and PuCoGa(5). The microscopic magnetization of NpCoGa(5) agrees with that observed in bulk susceptibility measurements and the magnetic moment has spin and orbital contributions as expected for intermediate coupling. In contrast, for PuCoGa(5), which is a superconductor with a high transition temperature, the microscopic magnetization in the paramagnetic state is small, temperature-independent, and significantly below the value found with bulk techniques at low temperatures.

Fermi surface topology and the superconducting gap function in UPd2Al3: a neutron spin-echo study.

We report on a single crystal neutron spin-echo investigation of the low-energy dynamic response in the heavy-fermion superconductor UPd2Al3 in the vicinity of the antiferromagnetic wave vector Q(0)=(0 0 0.5). Well inside the superconducting phase, antiferromagnetic quasielastic scattering, which is present in the normal state, is absent for relaxation times up to 10 ns, equivalent to an energy resolution of approximately 1 microeV.

Magnetization dynamics in the normal and superconducting phases of UPd(2)Al(3): II. Inferences on the nodal gap symmetry.

This paper provides an analysis of neutron inelastic scattering experiments on single crystals of UPd(2)Al(3). The emphasis is on establishing robust general inferences on the joint antiferromagnetic-superconducting state that characterizes UPd(2)Al(3) at low temperatures. A distinction is drawn between these conclusions and various theoretical perspectives of a more model-sensitive nature that have been raised in the literature.

Formation of a new dynamical mode in -uranium observed by inelastic x-ray and neutron scattering.

Phonon dispersion curves were obtained from inelastic x-ray and neutron scattering measurements on alpha-uranium single crystals at temperatures from 298 to 573 K. Both measurements showed a softening and an abrupt loss of intensity in the longitudinal optic branch along [00zeta] above 450 K. Above the same temperature a new dynamical mode of comparable intensity emerges along the [01zeta] zone boundary with energy near the top of the phonon spectrum.

A high-pressure structure in curium linked to magnetism.

Curium lies at the center of the actinide series and has a half-filled shell with seven 5f electrons spatially residing inside its radon core. As a function of pressure, curium exhibits five different crystallographic phases up to 100 gigapascals, of which all but one are also found in the preceding element, americium. We describe here a structure in curium, Cm III, with monoclinic symmetry, space group C2/c, found at intermediate pressures (between 37 and 56 gigapascals).

Superconductivity in the americium metal as a function of pressure: probing the Mott transition.

High-pressure measurements of the resistivity of americium metal are reported to 27 GPa and down to temperatures of 0.4 K. The unusual dependence of the superconducting temperature (T(c)) on pressure is deduced.

Direct observation of itinerant magnetism in the 5f-electron system UTe.

Our electron photoemission experiments demonstrate that the magnetization of the ferromagnetic state of UTe is proportional to the binding energy of the hybridized band centered around 50 meV below EF. This proportionality is direct evidence that the ferromagnetism of UTe is itinerant; i.e.

Structural tuning of unconventional superconductivity in PuMGa5 (M=Co,Rh).

The superconducting properties of the recently discovered PuMGa5 (M=Co,Rh) superconductors, including the power law behavior of the specific heat, the evolution of the superconducting transition T(c) temperature with pressure, and the linear relation between T(c) and ratio of tetragonal lattice parameters c/a, are compared to those of the heavy fermion CeMIn5 (M=Co,Rh,Ir) unconventional superconductors. The striking similarity of the properties between the two families of superconductors suggests a common physics and a common (magnetically mediated) mechanism of superconductivity.

Local structure and charge distribution in the UO(2)-U(4)O(9) system.

Analysis of X-ray absorption fine structure spectra of UO(2+x) for x = 0-0.20 (UO(2)--U(4)O(9)) reveals that the adventitious O atoms are incorporated as oxo groups with U--O distances of 1.74 A, most likely associated with U(VI), that occur in clusters so that the UO(2) fraction of the material largely remains intact.

Higher order speciation effects on plutonium L(3) X-ray absorption near edge spectra.

Pu L(3) X-ray near edge absorption spectra for Pu(0-VII) are reported for more than 60 chalcogenides, chlorides, hydrates, hydroxides, nitrates, carbonates, oxy-hydroxides, and other compounds both as solids and in solution, and substituted in zirconolite, perovskite, and borosilicate glass. This large database extends the known correlations between the energy and shape of these spectra from the usual association of the XANES with valence and site symmetry to higher order chemical effects. Because of the large number of compounds of these different types, a number of novel and unexpected behaviors are observed, such as effects resulting from the medium and disorder that can be as large as those from valence.