The malleability of uranium: manipulating the charge-density wave in epitaxial films

We report x-ray synchrotron experiments on epitaxial films of uranium, deposited on niobium and tungsten seed layers. Despite similar lattice parameters for these refractory metals, the uranium epitaxial arrangements are different and the strains propagated along the a-axis of the uranium layers are of opposite sign. At low temperatures these changes in epitaxy result in dramatic modifications to the behavior of the charge-density wave in uranium. The differences are explained with the current theory for the electron-phonon coupling in the uranium lattice. Our results emphasize the intriguing possibilities of producing epitaxial films of elements that have complex structures like the light actinides uranium to plutonium.

Bulk properties and electronic structure of PuFeAsO

Here we present bulk property measurements and electronic structure calculations for PuFeAsO, an actinide analogue of the iron-based rare-earth superconductors RFeAsO. Magnetic susceptibility and heat capacity data suggest the occurrence of an antiferromagnetic transition at TN=50 K. No further anomalies have been observed down to 2 K, the minimum temperature that we have been able to achieve. Structural measurements indicate that PuFeAsO, with its more localized 5f electrons, bears a stronger resemblance to the RFeAsO compounds with larger R ions, than NpFeAsO does.

Negative thermal expansion and antiferromagnetism in the actinide oxypnictide NpFeAsO

A neptunium analogue of the LaFeAsO tetragonal layered compound has been synthesized and characterized by a variety of experimental techniques. The occurrence of long-range magnetic order below a critical temperature T_N = 57 K is suggested by anomalies in the temperature-dependent magnetic susceptibility, electrical resistivity, Hall coefficient, and specific heat curves. Below T_N, powder neutron diffraction measurements reveal an antiferromagnetic structure of the Np sublattice, with an ordered magnetic moment of 1.70(0.07) mu_B aligned along the crystallographic c-axis. No magnetic order has been observed on the Fe sublattice, setting an upper limit of about 0.3 mu_B for the ordered magnetic moment on the iron. High resolution x-ray powder diffraction measurements exclude the occurrence of lattice transformations down to 5 K, in sharp contrast to the observation of a tetragonal-to-orthorhombic distortion in the rare-earth analogues, which has been associated with the stabilization of a spin density wave on the iron sublattice. Instead, a significant expansion of the NpFeAsO lattice parameters is observed with decreasing temperature below T_N, corresponding to a relative volume change of about 0.2% and to an invar behavior between 5 and 20 K. First-principle electronic structure calculations based on the local-spin density plus Coulomb interaction and the local density plus Hubbard-I approximations provide results in good agreement with the experimental findings.

Antiferromagnetic order and domains in Sr3Ir2O7 probed by x-ray resonant scattering

This article reports a detailed x-ray resonant scattering study of the bilayer iridate compound, Sr3Ir2O7, at the Ir L2 and L3 edges. Resonant scattering at the Ir L3 edge has been used to determine that Sr3Ir2O7 is a long-range ordered antiferromagnet below TN 230K with an ordering wavevector, q=(1/2,1/2,0). The energy resonance at the L3 edge was found to be a factor of ~30 times larger than that at the L2. This remarkable effect has been seen in the single layer compound Sr2IrO4 and has been linked to the observation of a Jeff=1/2 spin-orbit insulator. Our result shows that despite the modified electronic structure of the bilayer compound, caused by the larger bandwidth, the effect of strong spin-orbit coupling on the resonant magnetic scattering persists. Using the programme SARAh, we have determined that the magnetic order consists of two domains with propagation vectors k1=(1/2,1/2,0) and k2=(1/2,-1/2,0), respectively. A raster measurement of a focussed x-ray beam across the surface of the sample yielded images of domains of the order of 100 microns size, with odd and even L components, respectively. Fully relativistic, monoelectronic calculations (FDMNES), using the Greens function technique for a muffin-tin potential have been employed to calculate the relative intensities of the L2,3 edge resonances, comparing the effects of including spin-orbit coupling and the Hubbard, U, term. A large L3 to L2 edge intensity ratio (~5) was found for calculations including spin-orbit coupling. Adding the Hubbard, U, term resulted in changes to the intensity ratio <5%.

A study of uranium-based multilayers: II. Magnetic properties

SQUID magnetometry and polarised neutron reflectivity measurements have been employed to characterise the magnetic properties of U/Fe, U/Co and U/Gd multilayers. The field dependence of the magnetisation was measured at 10K in magnetic fields from -70kOe to 70kOe. A temperature dependent study of the magnetisation evolution was undertaken for a selection of U/Gd samples. PNR was carried out in a field of 4.4kOe for U/Fe and U/Co samples (at room temperature) and for U/Gd samples (at 10K). Magnetic dead layers of about 15 Angstrom were observed for U/Fe and U/Co samples, consistent with a picture of interdiffused interfaces. A large reduction in the magnetic moment, constant over a wide range of Gd layer thicknesses, was found for the U/Gd system (about 4 Bohr magnetons compared with 7.63 for the bulk metal). This could be understood on the basis of a pinning of Gd moments arising from a column-like growth mechanism of the Gd layers. A study of the effective anisotropy suggests that perpendicular magnetic anisotropy could occur in multilayers consisting of thick U and thin Gd layers. A reduction in the Curie temperature was observed as a function of Gd layer thickness, consistent with a finite-size scaling behaviour.

A study of uranium-based multilayers: I. Fabrication and structural characterisation

This paper addresses the structural characterisation of a series of U/Fe, U/Co and U/Gd multilayers. X-ray reflectivity has been employed to investigate the layer thickness and roughness parameters along the growth direction and high-angle diffraction measurements have been used to determine the crystal structure and orientation of the layers. For the case of uranium/transition metal systems, the interfaces are diffuse and the transition metals are present in a polycrystalline form of their common bulk phases with a preferred orientation along the closest packed planes; Fe, bcc (110) and Co, hcp (001), respectively. The uranium is present in a poorly crystalline orthorhombic, alpha-U state. In contrast, the U/Gd multilayers have sharp interfaces with negligible intermixing of atomic species, and have a roughness, which is strongly dependent on the gadolinium layer thickness. Diffraction spectra indicate a high degree of crystallinity in both U and Gd layers with intensities consistent with the growth of a novel hcp U phase, stabilised by the hcp gadolinium layers.