Magneto-optic Kerr effect in a spin-polarized zero-moment ferrimagnet

The magneto-optical Kerr effect (MOKE) is often assumed to be proportional to the magnetisation of a magnetically ordered metallic sample; in metallic ferrimagnets with chemically distinct sublattices, such as rare-earth transition-metal alloys, it depends on the difference between the sublattice contributions. Here we show that in a highly spin polarized, fully compensated ferrimagnet, where the sublattices are chemically similar, MOKE is observed even when the net moment is strictly zero. We analyse the spectral ellipsometry and MOKE of Mn 2 Ru x Ga, and show that this behaviour is due to a highly spin-polarized conduction band dominated by one of the two manganese sublattices which creates helicity-dependent reflectivity determined by a broad Drude tail. Our findings open new prospects for studying spin dynamics in the infra-red.Comment: 7 pages, 7 figure

Reconciling the theoretical and experimental electronic structure of NbO2

Metal-insulator transition materials such as NbO2 have generated much excitement in recent years for their potential applications in computing and sensing. NbO2 has generated considerable debate over the nature of the phase transition, and the values for the band gap/band widths in the insulating phase. We present a combined theoretical and experimental study of the band gap and electronic structure of the insulating phase of NbO2. We carry out ab-initio density functional theory plus U calculations, directly determining U and J parameters for both the Nb 4d and O 2p subspaces through the recently introduced minimum-tracking linear response method. We find a fundamental bulk band gap of 0.80 eV for the full DFT+U+J theory. We also perform calculations and measurements for a (100) oriented thin film. Scanning tunnelling spectroscopy measurements show that the surface band gap varies from 0.75 eV to 1.35 eV due to an excess of oxygen in and near the surface region of the film. Slab calculations indicate metallicity localised at the surface region caused by an energy level shift consistent with a reduction in Coulomb repulsion. We demonstrate that this effect in combination with the simple, low cost DFT+U+J method can account for the band widths and p-d gap observed in X-ray photoelectron spectroscopy experiments. Overall, our results indicate the possible presence of a 2D anisotropic metallic layer at the (100) surface of NbO2.Comment: 11 pages, 5 figures, plus 3 pages of Supporting Informatio

Crystallographic characterisation of ultra-thin, or amorphous transparent conducting oxides:the case for raman spectroscopy.

The electronic and optical properties of transparent conducting oxides (TCOs) are closely linked to their crystallographic structure on a macroscopic (grain sizes) and microscopic (bond structure) level. With the increasing drive towards using reduced film thicknesses in devices and growing interest in amorphous TCOs such as n-type InGaZnO 4 (IGZO), ZnSnO 3 (ZTO), p-type Cu x CrO 2 , or ZnRh 2 O 4 , the task of gaining in-depth knowledge on their crystal structure by conventional X-ray diffraction-based measurements are becoming increasingly difficult. We demonstrate the use of a focal shift based background subtraction technique for Raman spectroscopy specifically developed for the case of transparent thin films on amorphous substrates. Using this technique we demonstrate, for a variety of TCOs CuO, a-ZTO, ZnO:Al), how changes in local vibrational modes reflect changes in the composition of the TCO and consequently their electronic properties

Unravelling the atomic and electronic structure of nanocrystals on superconducting Nb(110): Impact of the oxygen monolayer

The Niobium surface is almost always covered by a native oxide layer which greatly influences the performance of superconducting devices. Here we investigate the highly stable Niobium oxide overlayer of Nb(110), which is characterised by its distinctive nanocrystal structure as observed by scanning tunnelling microscopy (STM). Our ab-initio density functional theory (DFT) calculations show that a subtle reconstruction in the surface Niobium atoms gives rise to rows of 4-fold coordinated oxygen separated by regions of 3-fold coordinated oxygen. The 4-fold oxygen rows are determined to be the source of the nanocrystal pattern observed in STM, and the two chemical states of oxygen observed in core-level X-ray photoelectron spectroscopy (XPS) are ascribed to the 3-fold and 4-fold oxygens. Furthermore, we find excellent agreement between the DFT calculated electronic structure with scanning tunnelling spectroscopy and valence XPS measurements.Comment: 8 pages, 4 figures, plus 3 pages of Supporting Informatio

Oxidation of Nb(110): atomic structure of the NbO layer and its influence on further oxidation.

NbO terminated Nb(110) and its oxidation are examined by scanning tunneling microscopy and spectroscopy (STS). The oxide structures are strongly influenced by the structural and electronic properties of the underlying NbO substrate. The NbO is terminated by one-dimensional few-nanometer nanocrystals, which form an ordered pattern. High-resolution STS measurements reveal that the nanocrystals and the regions between the nanocrystals exhibit different electronic characters. Low-dosage oxidation, sufficient for sub-monolayer coverage of the NbO, with subsequent UHV annealing results in the formation of resolved sub-nanometer clusters, positioned in-between the nanocrystals. Higher dosage oxidation results in the formation of a closed Nb2O5-y layer, which is confirmed by X-ray photoelectron spectroscopy measurements. The pentoxide is amorphous at the atomic-scale. However, large scale (tens of nanometers) structures are observed with their symmetry matching that of the underlying nanocrystals

On the floating of the topological surface state on top of a thick lead layer: The case of the Pb/Bi2Se3 interface

The puzzling question about the floating of the topological surface state on top of a thick Pb layer, has now possibly been answered. A study of the interface made by Pb on Bi2Se3 for different temperature and adsorbate coverage condition, allowed us to demonstrate that the evidence reported in the literature can be related to the surface diffusion phenomenon exhibited by the Pb atoms, which leaves the substrate partially uncovered. Comprehensive density functional theory calculations show that despite the specific arrangement of the atoms at the interface, the topological surface state cannot float on top of the adlayer but rather tends to move inward within the substrate.Comment: 9 pages, 5 figure

Electrically-driven phase transition in magnetite nanostructures

Magnetite (Fe$_{3}$O$_{4}$), an archetypal transition metal oxide, has been used for thousands of years, from lodestones in primitive compasses[1] to a candidate material for magnetoelectronic devices.[2] In 1939 Verwey[3] found that bulk magnetite undergoes a transition at T$_{V}$ $\approx$ 120 K from a high temperature "bad metal" conducting phase to a low-temperature insulating phase. He suggested[4] that high temperature conduction is via the fluctuating and correlated valences of the octahedral iron atoms, and that the transition is the onset of charge ordering upon cooling. The Verwey transition mechanism and the question of charge ordering remain highly controversial.[5-11] Here we show that magnetite nanocrystals and single-crystal thin films exhibit an electrically driven phase transition below the Verwey temperature. The signature of this transition is the onset of sharp conductance switching in high electric fields, hysteretic in voltage. We demonstrate that this transition is not due to local heating, but instead is due to the breakdown of the correlated insulating state when driven out of equilibrium by electrical bias. We anticipate that further studies of this newly observed transition and its low-temperature conducting phase will shed light on how charge ordering and vibrational degrees of freedom determine the ground state of this important compound.Comment: 17 pages, 4 figure

Valence band modification of Cr2O3 by Ni-doping: creating a high figure of merit p-type TCO

p-Type transparent conductors and semiconductors still suffer from remarkably low performance compared to their more widespread n-type counterparts, despite extensive investigation into their development. In this contribution, we present a comparative study on the defect chemistry of potential p-type transparent conducting oxides Mg-doped and Ni-doped Cr 2 O 3 . Conductivities as high as 28 S cm -1 were achieved by Ni-doping. By benchmarking crystallography and spectroscopy characterization against density functional theory calculations, we show that the incorporation of Ni into Cr 2 O 3 contributes to the composition of the valence band, making the formed holes more delocalized, while Mg states do not interact with the valence band in Mg-doped Cr 2 O 3 . Furthermore, it is experimentally proven that Ni has a higher solubility in Cr 2 O 3 than Mg, at least in the highly non-thermodynamic deposition conditions used for these experiments, which directly translates into a higher acceptor concentration. The combination of these two effects means that Ni is a more effective acceptor in Cr 2 O 3 than Mg and explains the improved conductivity observed for the former

Growth of 1T ' MoTe2 by thermally assisted conversion of electrodeposited tellurium films

Molybdenum ditelluride (MoTe2) is a transition metal dichalcogenide (TMD) which has two phases stable under ambient conditions, a semiconducting (2H) and semimetallic (1T') phase. Despite a host of interesting properties and potential applications, MoTe2 is one of the less-studied TMDs, perhaps due its relatively low abundance in nature or challenges associated with its synthesis, such as the toxicity of most precursors. In this report, we describe the fabrication of thin films of phase-pure IT' MoTe2 using predeposited molybdenum and electrodeposited tellurium layers, at the relatively low temperature of 450 C. This method allows control over film geometry and over the tellurium concentration during the conversion. The MoTe2 films are characterized by Raman spectroscopy, X-ray photoelectron spectroscopy, X-ray diffraction, atomic force microscopy, and electron microscopies. When applied as a catalyst for the hydrogen evolution reaction, the films display promising initial results. The MoTe2 films have a Tafel slope of below 70 mV dec(-1) and compare favorably with other MoTe2 catalysts reported in the literature, especially considering the inherently scalable fabrication method. The variation in electrocatalytic behavior with thickness and morphology of the films is also investigated