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Abstract: A detailed magnetic phase diagram of FeGe membranes with fields applied out-of-plane is determined using small-angle soft x-ray elastic scattering. In addition to the well-established skyrmion and helical phase, we identify an additional ordered phase which partly coexists with the helical phase in a pocket beneath the skyrmion phase. Furthermore, an evolution of the modulation wave vector, q , is observed when traversing the magnetic phase pocket. For the ordinary and the additional helical phase, q only varies with normalized field but not with temperature—in sharp contrast to the skyrmion phase, for which q is both field and temperature dependent. This study of the helical phases in thin FeGe membranes lays the foundation for their use in future magnetic storage and logic devices.

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Abstract: B2-ordered FeRh undergoes a first-order metamagnetic transition from an antiferromagnet (AF) to a ferromagnet (FM) upon heating. Thin films of B2-ordered FeRh are grown using DC magnetron sputtering and characterized for their behaviour at GHz frequencies and their dynamic behaviour over hour timescales. Ferromagnetic resonance investigations reveal a change in the spectroscopic splitting factor, g, through the range of the transition probed here. By introducing a model that describes the development of the two magnetic phases through the transition, this change in g is shown to be consistent with the development of an exchange coupling across the magnetic phase boundary that induces a non-zero magnetic moment in the AF phase as the result of a thickness dependent phase transition in the AF layer. The influence of such a phase transition is also seen in the extracted value of the Gilbert damping parameter in this experiment. Spin-wave resonance measurements are then performed to try and conclusively measure the exchange coupling between the two magnetic states in FeRh. Measuring the exchange stiffness through the transition reveals that the AF phase has a non-zero exchange energy that varies through the measurement range probed here. The behaviour of the exchange stiffness in the AF layer is attributed to a combination of both the onset of the exchange coupling and the presence of evanescent spin-waves, both of which are consequences of the thickness dependent phase transition in the AF layer. It was then shown that the structure of both magnetic phases could be measured directly with X-Ray Magnetic Dichroism using both linearly and circularly polarized light. The objects measured in these experiments are then characterized for their dynamic properties using X-Ray Photon Correlation Spectroscopy. These studies reveal reveal that the dynamic behaviour of the system is dependent on the type of magnetic dichroism used to probe it. This study also shows it is possible use x-ray magnetic linear dichroism to directly measure the structural and dynamic behaviour of AF materials.

Open Access

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Abstract: The design of active and durable catalysts for the H2O/O2 interconversion is one of the major challenges of electrocatalysis for renewable energy. The oxygen evolution reaction (OER) is catalyzed by SrRuO3 with low potentials (ca. 1.35 VRHE), but the catalyst’s durability is insufficient. Here we show that Na doping enhances both activity and durability in acid media. DFT reveals that whereas SrRuO3 binds reaction intermediates too strongly, Na doping of ~0.125 leads to nearly optimal OER activity. Na doping increases the oxidation state of Ru, thereby displacing positively O p-band and Ru d-band centers, weakening Ru-adsorbate bonds. The enhanced durability of Na-doped perovskites is concomitant with the stabilization of Ru centers with slightly higher oxidation states, higher dissolution potentials, lower surface energy and less distorted RuO6 octahedra. These results illustrate how high OER activity and durability can be simultaneously engineered by chemical doping of perovskites.

Open Access

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Abstract: We present the results of x-ray scattering and muon-spin relaxation (μ+SR) measurements on the iron-pnictide compound FeCrAs. Polarized non-resonant magnetic x-ray scattering results reveal the 120 periodicity expected from the suggested three-fold symmetric, non-collinear antiferromagnetic structure. μ+SR measurements indicate a magnetically ordered phase throughout the bulk of the material below T N=105(5) K. There are signs of fluctuating magnetism in a narrow range of temperatures above T N involving low-energy excitations, while at temperatures well below T N behaviour characteristic of freezing of dynamics is observed, likely reflecting the effect of disorder in our polycrystalline sample. Using density functional theory we propose a distinct muon stopping site in this compound and assess the degree of distortion induced by the implanted muon.

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Abstract: The ground-state orbital occupancy of the Ru4+ ion in Ca2−xLaxRuO4[x=0, 0.05(1), 0.07(1), and 0.12(1)] was investigated by performing x-ray absorption spectroscopy (XAS) in the vicinity of the O K edge as a function of the angle between the incident beam and the surface of the single-crystal samples. A minimal model of the hybridization between the O 2p states probed at the K edge and the Ru 4d orbitals was used to analyze the XAS data, allowing the ratio of hole occupancies nxy/nyz,zx to be determined as a function of doping and temperature. For the samples displaying a low-temperature insulating ground state (x≤0.07), nxy/nyz,zx is found to increase significantly with increasing doping, with increasing temperature acting to further enhance nxy/nyz,zx. For the x=0.12 sample, which has a metallic ground state, the XAS spectra are found to be independent of temperature and not to be describable by the minimal hybridization model, while being qualitatively similar to the spectra displayed by the x≤0.07 samples above their insulating to metallic transitions. To understand the origin of the evolution of the electronic structure of Ca2−xLaxRuO4 across its phase diagram, we have performed theoretical calculations based on a model Hamiltonian, comprising electron-electron correlations, crystal field Δ, and spin-orbit coupling λ, of a Ru-O-Ru cluster, with realistic values used to parametrize the various interactions taken from the literature. Our calculations of the Ru hole occupancy as a function of Δ/λ provide an excellent description of the general trends displayed by the data. In particular they establish that the enhancement of nxy/nyz,zx is driven by significant modifications to the crystal field as the tetragonal distortion of the RuO6 octahedral changes from compressive to tensile with La doping. We have also used our model to show that the hole occupancy of the O 2p and Ru 4d orbitals displays the same general trend as a function of Δ/λ, thus validating the minimal hybridization model used to analyze the data. In essence, our results suggest that the predominant mechanism driving the emergence of the low-temperature metallic phase in La-doped Ca2RuO4 is the structurally induced redistribution of holes within the t2g orbitals, rather than the injection of free carriers.