Springell, R.; (2008) Growth and characterisation of uranium multilayers. Doctoral thesis , University of London.

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Abstract

This thesis investigates the extents of the 5f-3d and 5f-4f electronic interactions in U/Fe, U/Co and U/Gd thin films, where electronic hybridisation effects are expected to influence the magnetism of the U 5f states. The samples were prepared by DC magnetron sputtering and included niobium buffer and capping layers to instigate crystalline growth and prevent oxidation of the multilayer stack. Layer thicknesses were varied between 5A and 90A with up to 30 bilayer repeats. The majority of the samples were grown at room temperature, but selected compositions were grown at elevated substrate temperatures. Many well-defined Bragg peaks were evident in the X-ray reflectivity spectra of multilayers of all three systems, indicating a low impurity contamination and a well-reproduced bilayer structure. High-angle X-ray diffraction spectra of the transition metal multilayers revealed poorly crystalline, oriented transition metal layers with a non-crystalline component of Fe and Co of 17A. U/Gd X-ray diffraction spectra displayed intensities up to two orders of magnitude greater than those observed for U/Fe or U/Co samples of similar composition and contained satellite peaks, indicating some degree of coherency between the two species. An intense peak was observed, arising from a crystalline uranium component at a position close to that expected for an exotic hep U phase, oriented in the 001 direction. Bulk magnetisation measurements revealed magnetically 'dead' Fe and Co layers of 15A and magnetic moments tending towards the bulk values of 2.2/zb and 1.7/iB for thick Fe and Co layers respectively. A study of the bulk magnetic properties of the U/Gd system did not indicate the presence of any significant 'dead' layer, but reported a saturation magnetic moment for thick Gd layers of 4.5//b> considerably reduced from the bulk value of 7.63//B- Calculations of the magnetic anisotropy for U/Gd samples revealed a possible transition from the gadolinium moments aligned within the plane of the film to samples displaying perpendicular magnetic anisotropy (PMA), at a gadolinium layer thickness of 5A. This transition could be achieved for thicker Gd layers if the thickness of the U layers were increased. A finite-size scaling effect was observed in a gadolinium layer thickness dependent study of the Curie temperature, indicating a transition from three to two dimensional behaviour for very thin Gd layers. Polarised neutron reflectivity spectra were taken in the specular geometry at magnetic saturation, and were simulated with separate, reduced moment and bulk moment ferromagnetic layers for U/Fe and U/Co samples and a simple bilayer structure for U/Gd samples. This simultaneous measurement of both the physical composition and bulk magnetisation measurements supported results obtained by X-ray reflectivity and magnetometry. The hybridisation of the electronic states in U/Fe and U/Gd resulted in an induced polarisation, detected using element selective techniques. X-ray magnetic circular dichroism measurements at the U Mrv and My edges were used to investigate the spin and orbital components of the uranium magnetic moment and a total magnetic moment on the U site of 0.1/b for the case of U/Fe multilayers, 0.01/zb in U/Gd samples and a signal only barely detectable above the statistical noise in the U/Co system were revealed. A uranium layer thickness dependent study of the magnetic moment values was used to indirectly deduce the profile of uranium magnetisation within the layers. X-ray resonant magnetic reflectivity measurements provided a depth dependent measure of the induced U 5f moment for selected U/Fe samples, which indicated a more complicated interfacial structure than that deduced by X- ray and neutron reflectivity techniques and showed that the majority of the U 5f moment was located at the interface region.

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