Coexistence of Superconductivity and Charge Density Waves in Tantalum Disulfide: Experiment and Theory.

The coexistence of charge density wave (CDW) and superconductivity in tantalum disulfide (2H-TaS_{2}) at low temperature is boosted by applying hydrostatic pressures to study both vibrational and magnetic transport properties. Around P_{c}, we observe a superconducting dome with a maximum superconducting transition temperature T_{c}=9.1 K. First-principles calculations of the electronic structure predict that, under ambient conditions, the undistorted structure is characterized by a phonon instability at finite momentum close to the experimental CDW wave vector. Upon compression, this instability is found to disappear, indicating the suppression of CDW order. The calculations reveal an electronic topological transition (ETT), which occurs before the suppression of the phonon instability, suggesting that the ETT alone is not directly causing the structural change in the system. The temperature dependence of the first vortex penetration field has been experimentally obtained by two independent methods. While a d wave and single-gap BCS prediction cannot describe the lower critical field H_{c1} data, the temperature dependence of the H_{c1} can be well described by a single-gap anisotropic s-wave order parameter.

Photoinduced reduction of surface states in Fe:ZnO.

We report on the electronic structure of nano-crystalline Fe:ZnO, which has recently been found to be an efficient photocatalyst. Using resonant photoemission spectroscopy, we determine the binding energy of Fe 3d states corresponding to different valencies and coordination of the Fe atoms. The photo-activity of ZnO reduces Fe from 3+ to 2+ in the surface region of the nano-crystalline material due to the formation of oxygen vacancies. Electronic states corresponding to low-spin Fe(2+) are observed and attributed to crystal field modification at the surface. These states are potentially important for the photocatalytic sensitivity to visible light due to their location deep in the ZnO bandgap. X-ray absorption and x-ray photoemission spectroscopy suggest that Fe is only homogeneously distributed for concentrations up to 3%. Increased concentrations does not result in a higher concentration of Fe ions in the surface region. This is limiting the photocatalytic functionality of ZnO, where the most efficient Fe doping concentration has been shown to be 1%-4%.

Near-room-temperature colossal magnetodielectricity and multiglass properties in partially disordered La2NiMnO6.

We report magnetic, dielectric, and magnetodielectric responses of the pure monoclinic bulk phase of partially disordered La2NiMnO6, exhibiting a spectrum of unusual properties and establish that this compound is an intrinsically multiglass system with a large magnetodielectric coupling (8%-20%) over a wide range of temperatures (150-300 K). Specifically, our results establish a unique way to obtain colossal magnetodielectricity, independent of any striction effects, by engineering the asymmetric hopping contribution to the dielectric constant via the tuning of the relative-spin orientations between neighboring magnetic ions in a transition-metal oxide system. We discuss the role of antisite (Ni-Mn) disorder in emergence of these unusual properties.

Perpendicular and in-plane hole asymmetry in a strained NiFe2O4film.

Strained materials can exhibit drastically modified physical properties in comparison to their fully relaxed analogues. We report on the x-ray absorption spectra (XAS) and magnetic circular dichroism (XMCD) of a strained NiFe2O4inverse spinel film grown on a symmetry matched single crystal MgGa2O4substrate. The Ni XAS spectra exhibit a sizable difference in the white line intensity for measurements with the x-ray electric field parallel to the film plane (normal incidence) vs when the electric field is at an angle (off-normal). A considerable difference is also observed in the FeL2,3XMCD spectrum. Modeling of the XAS and XMCD spectra indicate that the modified energy ordering of the cation 3dstates in the strained film leads to a preferential filling of 3dstates with out-of-plane character. In addition, the results point to the utility of x-ray spectroscopy in identifying orbital populations even with elliptically polarized x-rays.

On the interface magnetism of thin oxidized Co films: orbital and spin moments.

An x-ray magnetic circular dichroism study of a polycrystalline Co/CoO bilayer is presented. Using both the chemical specificity and surface sensitivity in the core level techniques, we find that uncompensated Co(2+) spin moments participate in the remanent ferromagnetic response of the bilayer that has oxygen nearest neighbors. These are likely located at the Co/CoO interface. As intermixing of magnetic species is not present in Co/CoO, it is concluded that the observed interface moments are due to interface roughness. Given their direction, these moments appear to not directly correlate to the exchange bias in these bilayers.

A setup for element specific magnetization dynamics using the transverse magneto-optic Kerr effect in the energy range of 30-72 eV.

In this paper, we present a spectrometer that is designed for element-specific and time-resolved transverse magneto-optic Kerr effect experiments at the high-harmonic generation pump-probe facility High Energy Laser Induced Overtone Source (HELIOS) laboratory. HELIOS delivers photons with energies between 30 eV and 72 eV with an overall time resolution of less than 40 fs. The spectrometer is based on a Rowland-circle geometry and allows for simultaneous measurements of all magnetic transition-metal elements. The setup also features easy sample transfer and alignment, and it combines high photon throughput, optimized data acquisition, and a fast switching of the magnetic field at the sample. The spectrometer performance is demonstrated by measuring the ultrafast demagnetization of permalloy. Our data are, for all practical purposes, identical to what have been reported in the earlier high-order harmonic generation work of a similar sample by Mathias et al. [Proc. Natl. Acad. Sci. U. S. A. 109, 4792-4797 (2012)], however, obtained within 15% of the acquisition time compared to their study. Furthermore, our data show a shift of the demagnetization curve of Ni relative to Fe, which has previously been interpreted as a delay of the Ni demagnetization to that of Fe [S. Mathias et al., Proc. Natl. Acad. Sci. U. S. A. 109, 4792-4797 (2012)].

Detection of microwave phase variation in nanometre-scale magnetic heterostructures.

The internal phase profile of electromagnetic radiation determines many functional properties of metal, oxide or semiconductor heterostructures. In magnetic heterostructures, emerging spin electronic phenomena depend strongly upon the phase profile of the magnetic field H at gigahertz frequencies. Here we demonstrate nanometre-scale, layer-resolved detection of electromagnetic phase through the radio frequency magnetic field H(rf) in magnetic heterostructures. Time-resolved X-ray magnetic circular dichroism reveals the local phase of the radio frequency magnetic field acting on individual magnetizations M(i) through the susceptibility as M = χH(rf). An unexpectedly large phase variation, ~40°, is detected across spin-valve trilayers driven at 3 GHz. The results have implications for the identification of novel effects in spintronics and suggest general possibilities for electromagnetic-phase profile measurement in heterostructures.

Influence of ligand states on the relationship between orbital moment and magnetocrystalline anisotropy.

The spin and orbital moments of Au/Co/Au trilayers grown on a W(110) single crystal substrate have been investigated by means of x-ray magnetic circular dichroism. Our findings suggest that the orbital moment of Co does not obtain a maximum value along the easy axis, in contrast with previous experience. This is attributed to the large spin-orbit interaction within the Au caps. Both second order perturbation theory and first principles calculations show how the magnetocrystalline anisotropy (MCA) is dramatically influenced by this effect, and how this leads to the fact that the orbital moment anisotropy is not proportional to the MCA.

Sample preserving deep interface characterization technique.

We propose a nondestructive technique based on atomic core-level shifts to characterize the interface quality of thin film nanomaterials. Our method uses the inherent sensitivity of the atomic core-level binding energies to their local surroundings in order to probe the layer-resolved binary alloy composition profiles at deeply embedded interfaces. From an analysis based upon high energy x-ray photoemission spectroscopy and density functional theory of a Ni/Cu fcc (100) model system, we demonstrate that this technique is a sensitive tool to characterize the sharpness of a buried interface. We performed controlled interface tuning by gradually approaching the diffusion temperature of the multilayer, which lead to intermixing. We show that core-level spectroscopy directly reflects the changes in the electronic structure of the buried interfaces, which ultimately determines the functionality of the nanosized material.

Vanishing magnetic interactions in ferromagnetic thin films.

We have used element-specific hysteresis measurements, based on the x-ray magnetic circular dichroism technique, to investigate magnetic trilayer structures composed of Fe and Ni layers. Within a critical regime we have discovered a class of structures in which the exchange interaction, the mechanism responsible for the macroscopic magnetism, can become vanishingly small. The experimental observations are supported by first principles theory and are explained as arising from a cancellation of several competing magnetic interactions. Hence, we have discovered a system with a novel exchange interaction between magnetic layers in direct contact that replaces the conventional exchange interaction in ferromagnets.

How carbon monoxide adsorbs in different sites.

The interplay between the electronic and the geometric structure of adsorbates is of fundamental importance for the understanding of many surface phenomena. Using x-ray emission spectroscopy and ab initio cluster calculations, this issue has been investigated in unprecedented detail for CO adsorption in different adsorption sites. The investigation establishes pi bonding and sigma repulsion, both increasing with the number of coordinated metal atoms. The two contributions partly compensate each other, leading to only small differences in adsorption energies for the different adsorption sites despite very large variations in the electronic structure.

Quantitative analysis of L-edge white line intensities: the influence of saturation and transverse coherence.

We have performed x-ray absorption spectroscopy at the Fe, Ni, and Co L2,3 edges of in situ grown thin magnetic films. We compare electron yield measurements performed at SSRL and BESSY-I. Differences in the L2,3 white line intensities are found for all three elements, comparing data from the two facilities. We propose a correlation between spectral intensities and the degree of spatial coherence of the exciting radiation. The electron yield saturation effects are stronger for light with a higher degree of spatial coherence. Therefore the observed, coherence related, intensity variations are due to an increase in the absorption coefficient, and not to secondary channel related effects.

Auger resonant Raman scattering in itinerant electron systems: continuum excitation in Cu.

The role of electron localization for resonant photoemission and Auger resonant Raman scattering to occur in an extended system was studied by polarization dependent resonant photoemission at the Cu L edges. Auger resonant Raman scattering was observed for continuum excitation into van Hove singularities at the L(1) and X(1) points, 4.2 and 7.7 eV above threshold. These findings show that resonant photoemission and Auger resonant Raman scattering are general features of photoemission independent of the degree of electron localization.

Magnetic X-ray circular dichroism on in situ grown 3d magnetic thin films on surfaces.

Epitaxic thin and ultrathin films on surfaces allow crystallographic phases that do not occur naturally in the bulk to be stabilized. They also offer new possibilities for an improved understanding of soft X-ray photoabsorption in magnetic systems. Data collected using the Elliptically Polarizing Undulator at BL 5.2 of the Stanford Synchrotron Radiation Laboratory are presented herein. Fe, Co and Ni films were prepared on Cu(100) surfaces. L2,3-edge spectra were recorded with circular and linear light. Fresnel diffractometry was used to quantify the degree of transverse beam coherence. A quantitative analysis of the spectral features indicates a correlation of the spectral intensities and the transverse beam coherence. Resonant reflectivity spectra for Co ultrathin films that exhibit strong dichroism are presented. The reflectivity data indicate that interference effects of the reflected beams at the two interfaces are of importance, even for ultrathin films.