Electronic structure and magnetic properties of epitaxial FeRh(001) ultra-thin films on W(100)

Epitaxial FeRh(100) films (CsCl structure, $\sim 10\ ML\$ thick), prepared {\it in-situ} on a W(100) single crystal substrate, have been investigated via valence band and core level photoemission. The presence of the temperature-induced, first-order, antiferromagnetic to ferromagnetic (AF$\rightarrow$ FM) transition in these films has been verified via linear dichroism in photoemission from the Fe 3$p$ levels. Core level spectra indicate a large moment on the Fe atom, practically unchanged in the FM and AF phases. Judging from the valence band spectra, the metamagnetic transition takes place without substantial modification of the electronic structure. In the FM phase, the spin-resolved spectra compare satisfactorily to the calculated spin-polarized bulk band structure.Comment: 7 pages, 5 figure

Effect of support of Co-Na-Mo catalysts on the direct conversion of CO<inf>2</inf> to hydrocarbons

This study of the effect of support of Co-Na-Mo based catalysts on the direct hydrogenation of CO$_2$ into hydrocarbons (HC) provides guidelines for the design of catalysts for CO$_2$ conversion. We demonstrate that the surface area of the support and the metal-support interaction have a key role determining the cobalt crystallite size and consequently the activity of the system. Cobalt particles with sizes <2 nm supported on MgO present low reverse water gas shift conversion with negligible Fischer-Tropsch activity. Increasing the cobalt particle size to ~15 nm supported on SiO$_2$ and ZSM-5 supports not only substantially increases the CO$_2$ conversion but it also provides high HC selectivities. Further increase of the cobalt particle size to 25–30 nm has a detrimental effect on the global CO$_2$ conversion with HC:CO ratios below 1, however, lower methane selectivity and enhanced formation of unsaturated HC products are achieved. Additionally, the metal-support interaction potentially also has a strong effect on the growth chain probability of the formed hydrocarbons, increasing as the metal-support interaction increases. These evidences demonstrate that CO$_2$ conversion and hydrocarbon distribution can be tuned towards desired products by controlled catalyst design.University of BathThis is the author accepted manuscript. The final version is available from Elsevier via http://dx.doi.org/10.1016/j.jcou.2016.06.00

Room temperature high frequency transport of Dirac fermions in epitaxially grown Sb_2Te_3 based topological insulators

We report on the observation of photogalvanic effects in epitaxially grown Sb_2Te_3 three-dimensional (3D) topological insulators (TI). We show that asymmetric scattering of Dirac electrons driven back and forth by the terahertz electric field results in a dc electric current. Due to the "symmetry filtration" the dc current is generated in the surface electrons only and provides an opto-electronic access to probe the electric transport in TI, surface domains orientation and details of electron scattering even in 3D TI at room temperature where conventional surface electron transport is usually hindered by the high carrier density in the bulk

Kink far below the Fermi level reveals new electron-magnon scattering channel in Fe

Many properties of real materials can be modeled using ab initio methods within a single-particle picture. However, for an accurate theoretical treatment of excited states, it is necessary to describe electron-electron correlations including interactions with bosons: phonons, plasmons, or magnons. In this work, by comparing spin- and momentum-resolved photoemission spectroscopy measurements to many-body calculations carried out with a newly developed first-principles method, we show that a kink in the electronic band dispersion of a ferromagnetic material can occur at much deeper binding energies than expected (E_b=1.5 eV). We demonstrate that the observed spectral signature reflects the formation of a many-body state that includes a photohole bound to a coherent superposition of renormalized spin-flip excitations. The existence of such a many-body state sheds new light on the physics of the electron-magnon interaction which is essential in fields such as spintronics and Fe-based superconductivity.Comment: 6 pages, 2 figure

Multistate current-induced magnetization switching in Au/Fe/MgO(001) epitaxial heterostructures

Magnetization switching using in-plane charge current recently has been widely investigated in heavy metal/ferromagnet bilayers with the switching mechanism usually attributed to the action of the spin-orbit coupling. Here we study in-plane current induced magnetization switching in model epitaxial bilayers that consist of Au(001) and Fe(001) grown on MgO(001). We use the planar Hall effect combined with magnetooptical Kerr effect (MOKE) microscopy to investigate magnetic properties of the bilayers and current-induced switching. We show that a current density beyond 1.4×107 A/cm can be employed for reproducible electrical switching of the magnetization between multiple stable states that correspond to different arrangements of magnetic domains with magnetization direction along one of the in-plane easy magnetization axes of the Fe(001) film. Lower current densities result in stable intermediate transversal resistances which are interpreted based on MOKE-microscopy investigations as resulting from the current-induced magnetic domain structure that is formed in the area of the Hall cross. We find that the physical mechanism of the current-induced magnetization switching of the Au/Fe/MgO(001) system at room temperature can be fully explained by the Oersted field, which is generated by the charge current flowing mostly through the Au layer

Kinetics of CO2 Hydrogenation to Hydrocarbons over Iron-Silica Catalysts

The conversion of CO2 to hydrocarbons is increasingly seen as a potential alternative source of fuel and chemicals, while at the same time contributing to addressing global warming effects. An understanding of kinetics and mass transfer limitations is vital to both optimise catalyst performance and to scale up the whole process. In this work we report on a systematic investigation of the influence of the different process parameters, including pore size, catalyst support particle diameter, reaction temperature, pressure and reactant flow rate on conversion and selectivity of iron nanoparticle ‐silica catalysts. The results provided on activation energy and mass transfer limitations represent the basis to fully design a reactor system for the effective catalytic conversion of CO2 to hydrocarbons

Shedding Light Onto the Nature of Iron Decorated Graphene and Graphite Oxide Nanohybrids for CO₂ Conversion at Atmospheric Pressure

We report on the design and testing of new graphite and graphene oxide‐based extended π‐conjugated synthetic scaffolds for applications in sustainable chemistry transformations. Nanoparticle‐functionalised carbonaceous catalysts for new Fischer Tropsch and Reverse GasWater Shift (RGWS) transformations were prepared: functional graphene oxides emerged from graphite powders via an adapted Hummer's method and subsequently impregnated with uniform‐sized nanoparticles. Then the resulting nanomaterials were imaged by TEM, SEM, EDX, AFM and characterised by IR, XPS and Raman spectroscopies prior to incorporation of Pd(II) promoters and further microscopic and spectroscopic analysis. Newly synthesised 2D and 3D layered nanostructures incorporating carbon‐supported iron oxide nanoparticulate pre‐catalysts were tested, upon hydrogen reduction in situ, for the conversion of CO2 to CO as well as for the selective formation of CH4 and longer chain hydrocarbons. The reduction reaction was also carried out and the catalytic species isolated and fully characterised. The catalytic activity of a graphene oxide‐supported iron oxide pre‐catalyst converted CO2 into hydrocarbons at different temperatures (305, 335, 370 and 405 °C), and its activity compared well with that of the analogues supported on graphite oxide, the 3‐dimensional material precursor to the graphene oxide. Investigation into the use of graphene oxide as a framework for catalysis showed that it has promising activity with respect to reverse gas water shift (RWGS) reaction of CO2 to CO, even at the low levels of catalyst used and under the rather mild conditions employed at atmospheric pressure. Whilst the γ‐Fe2O3 decorated graphene oxide‐based pre‐catalyst displays fairly constant activity up to 405 °C, it was found by GC‐MS analysis to be unstable with respect to decomposition at higher temperatures. The addition of palladium as a promoter increased the activity of the iron functionalised graphite oxide in the RWGS. The activity of graphene oxide supported catalysts was found to be enhanced with respect to that of iron‐functionalised graphite oxide with, or without palladium as a promoter, and comparable to that of Fe@carbon nanotube‐based systems tested under analogous conditions. These results display a significant step forward for the catalytic activity estimations for the iron functionalised and rapidly processable and scalable graphene oxide. The hereby investigated phenomena are of particular relevance for the understanding of the intimate surface morphologies and the potential role of non‐covalent interactions in the iron oxide‐graphene oxide networks, which could inform the design of nano‐materials with performance in future sustainable catalysis applications

Surface and electronic structure of MOCVD-grown Ga(0.92)In(0.08)N investigated by UV and X-ray photoelectron spectroscopies

The surface and electronic structure of MOCVD-grown layers of Ga(0.92)In(0.08)N have been investigated by means of photoemission. An additional feature at the valence band edge, which can be ascribed to the presence of In in the layer, has been revealed. A clean (0001)-(1x1) surface was prepared by argon ion sputtering and annealing. Stability of chemical composition of the investigated surface subjected to similar ion etching was proven by means of X-ray photoemission spectroscopy.Comment: 13 pages, 6 figure