Interaction between U/UO2 bilayers and hydrogen studied by in-situ X-ray diffraction

This paper reports experiments investigating the reaction of H$_{2}$ with uranium metal-oxide bilayers. The bilayers consist of $\leq$ 100 nm of epitaxial $\alpha$-U (grown on a Nb buffer deposited on sapphire) with a UO$_{2}$ overlayer of thicknesses of between 20 and 80 nm. The oxides were made either by depositing via reactive magnetron sputtering, or allowing the uranium metal to oxidise in air at room temperature. The bilayers were exposed to hydrogen, with sample temperatures between 80 and 200 C, and monitored via in-situ x-ray diffraction and complimentary experiments conducted using Scanning Transmission Electron Microscopy - Electron Energy Loss Spectroscopy (STEM-EELS). Small partial pressures of H$_{2}$ caused rapid consumption of the U metal and lead to changes in the intensity and position of the diffraction peaks from both the UO$_{2}$ overlayers and the U metal. There is an orientational dependence in the rate of U consumption. From changes in the lattice parameter we deduce that hydrogen enters both the oxide and metal layers, contracting the oxide and expanding the metal. The air-grown oxide overlayers appear to hinder the H$_{2}$-reaction up to a threshold dose, but then on heating from 80 to 140 C the consumption is more rapid than for the as-deposited overlayers. STEM-EELS establishes that the U-hydride layer lies at the oxide-metal interface, and that the initial formation is at defects or grain boundaries, and involves the formation of amorphous and/or nanocrystalline UH$_{3}$. This explains why no diffraction peaks from UH$_{3}$ are observed. {\textcopyright British Crown Owned Copyright 2017/AWE}Comment: Submitted for peer revie

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.Comment: 6 pages, 6 figure

A field induced modulated state in the ferromagnet PrPtAl

The theory of quantum order-by-disorder (QOBD) explains the formation of modulated magnetic states at the boundary between ferromagnetism and paramagnetism in zero field. PrPtAl has been argued to provide an archetype for this. Here, we report the phase diagram in magnetic field, applied along both the easy a axis and hard b axis. For field aligned to the b axis, we find that the magnetic transition temperatures are suppressed and at low temperature there is a single modulated fan state, separating an easy a axis ferromagnetic state from a field polarized state. This fan state is well explained with the QOBD theory in the presence of anisotropy and field. Experimental evidence supporting the QOBD explanation is provided by the large increase in the T^{2} coefficient of the resistivity and direct detection of enhanced magnetic fluctuations with inelastic neutron scattering, across the field range spanned by the fan state. This shows that the QOBD mechanism can explain field induced modulated states that persist to very low temperature

Field-Induced Modulated State in the Ferromagnet PrPtAl

The theory of quantum order-by-disorder (QOBD) explains the formation of modulated magnetic states at the boundary between ferromagnetism and paramagnetism in zero field. PrPtAl has been argued to provide an archetype for this. Here, we report the phase diagram in magnetic field, applied along both the easy a axis and hard b axis. For field aligned to the b axis, we find that the magnetic transition temperatures are suppressed and at low temperature there is a single modulated fan state, separating an easy a axis ferromagnetic state from a field polarized state. This fan state is well explained with the QOBD theory in the presence of anisotropy and field. Experimental evidence supporting the QOBD explanation is provided by the large increase in the T^{2} coefficient of the resistivity and direct detection of enhanced magnetic fluctuations with inelastic neutron scattering, across the field range spanned by the fan state. This shows that the QOBD mechanism can explain field induced modulated states that persist to very low temperature

Structural and magnetic properties of [\lbrackErTb]\rbrackmultilayers

Abstract.: We have investigated the structural and magnetic properties of $\lbrack$ Er|Tb $\rbrack$ multilayers by different scattering methods. Diffuse X-ray scattering under grazing incidence reveals the interface structure in $\lbrack$ Er|Tb $\rbrack$ bilayers and trilayers, indicating vertically correlated roughness between the Er and Tb interfaces. The magnetic properties of $\lbrack$ ErnEr|TbnTb $\rbrack$ superlattices have been studied as a function of the superlattice composition (indices denote the number of atomic layers). Coupled ferromagnetic structures exist in all investigated samples. The phase transition temperature varies with the Tb layer thickness. Modulated magnetic order is short range for all samples beside the $\lbrack$ Er20|Tb5 $\rbrack$ superlattice, the sample with the smallest Tb layer thickness. We observe dipolar antiferromagnetic coupling between single ferromagnetic Tb layers in all samples, with the onset of this ordering depending on the Tb layer thickness. Due to competing interactions, exchange coupling is limited to the interface near region. Therefore long range modulated magnetic order is observed in the $\lbrack$ Er20|Tb5 $\rbrack$ superlattice only, where the interface regions overlap. The distinct differences to the magnetic structure of an Er0.8Tb0.2 alloy film are explained by a highly anisotropic arrangement of neighbouring atoms due to the correlated roughnes

Distinct order of Gd 4f and Fe 3d moments coexisting in GdFe4Al8

Single crystals of flux-grown tetragonal GdFe4Al8 were characterized by thermodynamic, transport, and x-ray resonant magnetic scattering measurements. In addition to antiferromagnetic order at TN ~ 155 K, two low-temperature transitions at T1 ~ 21 K and T2 ~ 27 K were identified. The Fe moments order at TN with an incommensurate propagation vector (tau,tau,0) with tau varying between 0.06 and 0.14 as a function of temperature, and maintain this order over the entire T<TN range. The Gd 4f moments order below T2 with a ferromagnetic component mainly out of plane. Below T1, the ferromagnetic components are confined to the crystallographic plane. Remarkably, at low temperatures the Fe moments maintain the same modulation as at high temperatures, but the Gd 4f moments apparently do not follow this modulation. The magnetic phase diagrams for fields applied in [110] and [001] direction are presented and possible magnetic structures are discussed.Comment: v2: 14 pages, 12 figures; PRB in prin

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 Green's 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%.Comment: 9 pages, 9 figure

Simultaneous dynamic electrical and structural measurements of functional materials

A new materials characterization system developed at the XMaS beamline, located at the European Synchrotron Radiation Facility in France, is presented. We show that this new capability allows to measure the atomic structural evolution (crystallography) of piezoelectric materials whilst simultaneously measuring the overall strain characteristics and electrical response to dynamically (ac) applied external stimuli