We have measured angular-dependent fluorescence-yield x-ray magnetic circular dichroism spectra on single crystals of the heterometallic 3d - 4f 12-metallacrown-4 TbMn4 and DyMn4 complexes. Simulated spectra using crystal-field multiplet calculations reproduce the experimentally observed spectra. The orientation of the molecules causes linear dichroism spectra of the 4f absorption spectra. This natural linear dichroism shows the anisotropic charge distribution of the rare-earth 4f state in the tetragonal crystal field despite the small 4f crystal-field splitting. The magnetic moment of the molecule is dominated by the rare-earth moment revealing a considerably large contribution of orbital moment. From a sum-rule analysis of experimental and simulated x-ray magnetic circular dichroism, we determined corrected spin and orbital Dy moments at low temperature (14 K) within a magnetic field of 7 T. We find a significant angular dependence of the Dy magnetic moments, indicating the presence of fourth-order magnetic anisotropy.

Enhanced magnetism has recently been reported for the topological-insulator/ferromagnet interface Bi2Se3/EuS with Curie temperatures claimed to be raised above room temperature from the bulk EuS value of 16 K. Here we investigate the analogous interface Bi2Se3/EuSe. EuSe is a low-temperature layered ferrimagnet that is particularly sensitive to external perturbations. We find that superconducting quantum interference device (SQUID) magnetometry of Bi2Se3/EuSe heterostructures reveals precisely the magnetic phase diagram known from EuSe, including the ferrimagnetic phase below 5 K, without any apparent changes from the bulk behavior. Choosing a temperature of 10 K to search for magnetic enhancement, we determine an upper limit for a possible magnetic coercive field of 3 mT. Using interface sensitive x-ray absorption spectroscopy we verify the magnetic divalent configuration of the Eu at the interface without contamination by Eu3+, and by x-ray magnetic circular dichroism (XMCD) we confirm at the interface the magnetic hysteresis obtained by SQUID. XMCD data obtained at 10 K in a magnetic field of 6 T indicate a magnetic spin moment of mz,spin = 7 μB/Eu 2+, in good agreement with the SQUID data and the expected theoretical moment of Eu2+. Subsequent XMCD measurements in zero field show, however, that sizable remanent magnetization is absent at the interface for temperatures down to about 10 K.

Chemically ordered $L{1}_{0}$ $({\mathrm{Fe}}_{100\ensuremath{-}x}{\mathrm{Cr}}_{x})\mathrm{Pt}$ thin films were expitaxially grown on MgO(001) substrates by magnetron sputter-deposition at $770{\phantom{\rule{0.16em}{0ex}}}^{\ensuremath{\circ}}\mathrm{C}$. In this sample series, Fe was continuously substituted by Cr over the full composition range. The lattice parameter in the [001] growth direction steadily increases from $L{1}_{0}$-FePt toward $L{1}_{0}$-CrPt, confirming the incorporation of Cr in the lattice occupying Fe sites. With the observed high degree of chemical ordering and (001) orientation, strong perpendicular magnetic anisotropy is associated, which persists up to a Cr content of $x=20$ at. %. Similarly, the coercive field in the easy-axis direction is strongly reduced, which is, however, further attributed to a strong alteration of the film morphology with Cr substitution. The latter changes from a well-separated island microstructure to a more continuous film morphology. In the dilute alloy with low Cr content, isolated Cr magnetic moments couple antiferromagnetically to the ferromagnetic Fe matrix. In this case, all Cr moments are aligned parallel, thus forming a ferrimagnetic FeCrPt system. With increasing Cr concentration, nearest-neighbor Cr-Cr pairs start to appear, thereby increasing magnetic frustration and disorder, which lead to canting of neighboring magnetic moments, as revealed by atomistic spin-model simulations with model parameters based on first principles. At higher Cr concentrations, a frustrated ferrimagnetic order is established. With Cr substitution of up to 20 at. %, no pronounced change in Curie temperature, which is in the range of 700 K, was noticed. But with further addition the Curie temperature drops down substantially even down to room temperature at 47 at. % Cr. Furthermore, x-ray magnetic circular dichroism studies on dilute alloys containing up to 20 at. % of Cr revealed similar spin moments for Fe and Cr in the range between 2.1--2.5 ${\ensuremath{\mu}}_{B}$ but rather large orbital moments of up to 0.50 $\ifmmode\pm\else\textpm\fi{}0.10\phantom{\rule{4pt}{0ex}}{\ensuremath{\mu}}_{B}$ for Cr. These results were also compared to ab initio calculations.

V2O3 doped with 1.1% Cr is investigated at its isostructural correlation‐driven metal–insulator transition near room temperature in its paramagnetic state with X‐ray magnetic circular dichroism (XMCD) spectroscopy in external magnetic fields. A relative XMCD amplitude of about 2 permille is observed at the L2,3 absorption edges of vanadium as expected for magnetic moment per mass values of the order of 1 J T−1 kg−1 from magnetometry and the literature. Across the metal–insulator transition, the vanadium XMCD spectral shape significantly changes. According to atomic multiplet simulations, these changes are due to a changing orbital occupation indicating a changing phase composition. According to estimates used in this study, the dipole moment of the spin density distribution in the bulk increases such that the effective vanadium spin moment increases by a few percent with temperature in the two‐phase region. Thereby, it partially compensates for the decrease in the relative XMCD amplitude due to a decreasing alignment of the paramagnetic moments. After a few minor temperature cycles, the sample is in a two‐phase state in which the XMCD and X‐ray linear dichroism spectra hardly depend on the temperature, and the specific electrical resistance is intermediate, showing only a weak sign of the metal–insulator transition.

The electronic reconstruction occurring at oxide interfaces may be the source of interesting device concepts for future oxide electronics. Among oxide devices, multiferroic tunnel junctions are being actively investigated as they offer the possibility to modulate the junction current by independently controlling the switching of the magnetization of the electrodes and of the ferroelectric polarization of the barrier. In this Letter, we show that the spin reconstruction at the interfaces of a La_{0.7}Sr_{0.3}MnO_{3}/BaTiO_{3}/La_{0.7}Sr_{0.3}MnO_{3} multiferroic tunnel junction is the origin of a spin filtering functionality that can be turned on and off by reversing the ferroelectric polarization. The ferroelectrically controlled interface spin filter enables a giant electrical modulation of the tunneling magnetoresistance between values of 10% and 1000%, which could inspire device concepts in oxides-based low dissipation spintronics.

We have studied structural and magnetic properties of (FePt)(1-x)Tb-x thin films grown at elevated temperatures on MgO(100) substrates. The incorporation of Tb into the chemically ordered L1(0) FePt lattice gives rise to considerable changes in the structural and magnetic properties, depending on the Tb content and the deposition temperature. When grown at 770 degrees C, pronounced L1(0) ordering of the initial FePt phase is present. It vanishes gradually with Tb addition, thereby forming additional crystalline Tb-Pt phases at higher Tb content. These structural changes are accompanied by a strong reduction of the perpendicular magnetic anisotropy with increasing Tb content, finally resulting in a soft magnetic material with in-plane easy-axis magnetization. Extended x-ray absorption fine-structure measurements were performed to examine the possible incorporation of Tb into the FePt lattice. Based on the number of Pt first neighbors, the transformation from the initial tetragonal L1(0) structure to the chemically disordered fcc (A1) phase with increasing Tb content could be firmly concluded. In a further sample series, FePt was grown at a lower temperature of 530 degrees C, which leads to reduced initial L1(0) chemical ordering. Adding Tb results in strong elastic stress in the lattice, eventually causing full amorphization of the film. Interestingly, in this case, a spin-reorientation transition from in-plane to out-of-plane magnetic easy axis is found at low temperatures, which is associated with an anisotropic chemical short-range order present in the amorphous phase. Furthermore, x-ray magnetic circular dichroism studies at the Fe L-3,L-2 and Tb M-5,M-4 edges for all samples reveal strong antiferromagnetic coupling between Fe and Tb, resulting in a reduction of the net magnetization of the film.

Noncollinear antiferromagnets, with either an L1(2) cubic crystal lattice (e.g., Mn3Ir and Mn3Pt) or a D0(19) hexagonal structure (e.g., Mn3Sn and Mn3Ge), exhibit a number of phenomena of interest to topological spintronics. Among the cubic systems, for example, tetragonally distorted Mn3Pt exhibits an intrinsic anomalous Hall effect (AHE). However, Mn3Pt only enters a noncollinear magnetic phase close to the stoichiometric composition and at suitably large thicknesses. Therefore, we turn our attention to Mn3Ir, the material of choice for use in exchange bias heterostructures. In this letter, we investigate the magnetic and electrical transport properties of epitaxially grown, face-centered-cubic gamma-Mn3Ir thin films with (111) crystal orientation. Relaxed films of 10 nm thickness exhibit an ordinary Hall effect, with a hole-type carrier concentration of (1.500 +/- 0.002) x 10(23) cm(-3). On the other hand, TEM characterization demonstrates that ultrathin 3 nm films grow with significant in-plane tensile strain. This may explain a small net magnetic moment, observed at low temperatures, shown by X-ray magnetic circular dichroism spectroscopy to arise from uncompensated Mn spins. Being of the order of 0.02 mu(B)/atom, this dominates electrical transport behavior, leading to a small AHE and negative magnetoresistance. These results are discussed in terms of crystal microstructure and chiral domain behavior, with spatially resolved XML(C)D-PEEM supporting the conclusion that small antiferromagnetic domains, <20nm in size, with differing chirality account for the absence of observed Berry curvature driven magnetotransport effects. Published under license by AIP Publishing.

We present new experimental low-temperature heat capacity and detailed dynamical spin-structure factor data for the quantum spin-liquid candidate material Ca10Cr7O28. The measured heat capacity shows an almost-perfect linear temperature dependence in the range 0.1 K less than or similar to T less than or similar to 0.5 K, reminiscent of fermionic spinon degrees of freedom. The spin-structure factor exhibits two energy regimes of strong signal which display rather different but solely diffuse scattering features. We theoretically describe these findings by an effective spinon-hopping model which crucially relies on the existence of strong ferromagnetically coupled triangles in the system. Our spinon theory is shown to naturally reproduce the overall weight distribution of the measured spin-structure factor. Particularly, we argue that various different observed characteristic properties of the spin-structure factor and the heat capacity consistently indicate the existence of a spinon Fermi surface. A closer analysis of the heat capacity at the lowest accessible temperatures hints toward the presence of weak f-wave spinon-pairing terms inducing a small partial gap along the Fermi surface (except for discrete nodal Dirac points) and suggesting an overall Z(2) quantum spin-liquid scenario for Ca10Cr7O28.

Ferrimagnetic alloys are extensively studied for their unique magnetic properties leading to possible applications in perpendicular magnetic recording, due to their deterministic ultrafast switching and heat assisted magnetic recording capabilities. On a prototype ferrimagnetic alloy we demonstrate fascinating properties that occur close to a critical temperature where the magnetization is vanishing, just as in an antiferromagnet. From the X-ray magnetic circular dichroism measurements, an anomalous 'wing shape' hysteresis loop is observed slightly above the compensation temperature. This bears the characteristics of an intrinsic exchange bias effect, referred to as atomic exchange bias. We further exploit the X-ray magnetic linear dichroism (XMLD) contrast for probing non-collinear states which allows us to discriminate between two main reversal mechanisms, namely perpendicular domain wall formation versus spin-flop transition. Ultimately, we analyze the elemental magnetic moments for the surface and the bulk parts, separately, which allows to identify in the phase diagram the temperature window where this effect takes place. Moreover, we suggests that this effect is a general phenomenon in ferrimagnetic thin films which may also contribute to the understanding of the mechanism behind the all optical switching effect.

Cubic chiral magnets, such as Cu2OSeO3, exhibit a variety of noncollinear spin textures, including a trigonal lattice of spin whirls, the so-called skyrmions. Using magnetic resonant elastic x-ray scattering (REXS) on a crystalline Bragg peak and its magnetic satellites while exciting the sample with magnetic fields at gigahertz frequencies, we probe the ferromagnetic resonance (FMR) modes of these spin textures by means of the scattered intensity. Most notably, the three eigenmodes of the skyrmion lattice are detected with large sensitivity. As this novel technique, which we label REXS FMR, is carried out at distinct positions in reciprocal space, it allows us to distinguish contributions originating from different magnetic states, providing information on the precise character, weight, and mode mixing as a prerequisite of tailored excitations for applications.

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Single molecule magnets comprising rare earth metals are of high interest due to the unquenched orbital moments of the rare earth ions that result in a large energy barrier for magnetization reversal. We investigate the magnetic properties of polynuclear 3d-4f 15-MC-5 metallacrowns using x-ray magnetic circular dichroism of powder samples at a temperature of 7 K in a magnetic field of 7 T. The sum rule analysis reveals element-specific spin and orbital moments. The magnetic moments of the 3d transition metal Ni(II) ions are coupled antiferromagnetically to each other and contribute only little to the total molecular moment. The spin and orbital moments of the rare earth ions are unexpectedly smaller than the ionic values resulting from Hund's rules. We explain the reduction of the orbital magnetic moment by a finite magnetic anisotropy. Considering an energy functional including magnetic anisotropy and Zeeman energy the powder average reveals a magnetic anisotropy of 28 meV (340 K) in the case of Dy(III) and 7 meV (85 K) in the case of Tb(III). The spin moments agree with the ionic value, too, when the expectation values of the dipole operator are considered.

Mn$_2$Au is an important antiferromagnetic (AF) material for spintronics applications. Due to its very high N\'eel temperature of about 1500 K, some of the basic properties are difficult to explore, such as the AF susceptibility and the exchange constants. Experimental determination of these properties is further complicated in thin films by unavoidable presence of uncompensated and quasiloose spins on antisites and at interfaces. Using x-ray magnetic circular dichroism (XMCD), we have measured the spin and orbital contribution to the susceptibility in the direction perpendicular to the in-plane magnetic moments of a Mn$_2$Au(001) film and in fields up to 8 T. By performing these measurements at a low temperature of 7 K and at room temperature, we were able to separate the loose spin contribution from the susceptibility of AF coupled spins. The value of the AF exchange constant obtained with this method for a 10 nm thick Mn$_2$Au(001) film equals to (24 $\pm$ 5) meV.

Cooperative effects determine the spin-state bistability of spin-crossover molecules (SCMs). Herein, the ultimate scale limit at which cooperative spin switching becomes effective is investigated in a complex [Fe(H2B(pz)2)2(bipy)] deposited on a highly oriented pyrolytic graphite surface, using x-ray absorption spectroscopy. This system exhibits a complete thermal- and light-induced spin transition at thicknesses ranging from submonolayers to multilayers. On increasing the coverage from 0.35(4) to 10(1) monolayers, the width of the temperature-induced spin transition curve narrows significantly, evidencing the buildup of cooperative effects. While the molecules at the submonolayers exhibit an apparent anticooperative behavior, the multilayers starting from a double-layer exhibit a distinctly cooperative spin switching, with a free-molecule-like behavior indicated at around a monolayer. These observations will serve as useful guidelines in designing SCM-based devices.

When ferromagnetic films become ultrathin, key properties such as the Curie temperature and the saturation magnetization are usually depressed. This effect is thoroughly investigated in magnetic oxides such as half-metallic manganites, but much less in ferrimagnetic insulating perovskites such as rare-earth titanates RTiO3 , despite their appeal to design correlated 2D electron gases. Here, the magnetic properties of epitaxial DyTiO3 thin films are reported. While films thicker than about 50 nm show a bulk-like response, at low thickness a surprising increase of the saturation magnetization is observed. This behavior is described using a classical model of a "dead layer" but assuming that this layer is actually "living," that is, it responds to the magnetic field with a strong paramagnetic susceptibility. Through depth-dependent X-ray absorption and photoemission spectroscopy, it is shown that the "living-dead layer" corresponds to surface regions where magnetic (S = 1/2) Ti3+ ions are replaced by nonmagnetic Ti4+ ions. Hysteresis cycles at the Dy M 5 and Ti L 3 edges indicate that the surface Ti4+ ions decouple the Dy3+ ions, thus unleashing their strong paramagnetic response. Finally, it is shown how capping the DyTiO3 film can help increase the Ti3+ content near the surface and thus recover a better ferrimagnetic behavior.

We undertook a comparative study on optimizing the position accuracy of pnCCDs for single X-ray photon measurements. Various methods were analyzed by Monte Carlo simulations and related to experimental data obtained with a focused X-ray beam. Even with low energy photons of 1320 eV, a position accuracy much smaller than the actual pixel size of 48 μm × 48 μm can be achieved. This is possible since signal charges from a single photon interaction spread into more than one pixel, allowing a reconstruction of the original point of interaction. We found that a) making a decision on which pixels to use for the reconstruction and b) choosing a centroiding algorithm for carrying out the reconstruction were particularly crucial. For a) we introduce a new and superior method using a two step analysis with an adaptive pattern. It is compared to using a threshold or a fixed pattern. For b) we present a Center-of-Gravity method with a Gaussian correction taking into account the shape of the signal charge cloud. Both methods are also optimized for fast execution by implementing lookup tables rather than time consuming calculations. Our results show that with the appropriate analysis an uncertainty of the position measurement of better than 3.0 μm rms for 1320 eV photons is possible.

Christian Balz, 2, ∗ Bella Lake, 2 A.T.M. Nazmul Islam, Yogesh Singh, Jose A. Rodriguez-Rivera, 5 Tatiana Guidi, Elisa M. Wheeler, Giovanna G. Simeoni, and Hanjo Ryll Helmholtz-Zentrum Berlin für Materialien und Energie, 14109 Berlin, Germany Institut für Festkörperphysik, Technische Universität Berlin, 10623 Berlin, Germany† Indian Institute of Science Education and Research (IISER) Mohali, Knowledge City, Sector 81, Mohali 140306, India NIST Center for Neutron Research, National Institute of Standards and Technology, 20899 Gaithersburg, USA Department of Materials Science, University of Maryland, College Park, 20742 Maryland, USA ISIS Facility, STFC Rutherford Appleton Laboratory, Oxfordshire OX11 0QX, UK Institut Laue-Langevin, 38042 Grenoble, France Heinz Maier-Leibnitz Zentrum, Technische Universitat München, 85748 Garching, Germany (Dated: April 20, 2017)

A spin liquid is a new state of matter with topological order where the spin moments continue to fluctuate coherently down to the lowest temperatures rather than develop static long-range magnetic order as found in conventional magnets. For spin liquid behavior to arise in a material the magnetic Hamiltonian must be ``frustrated'', where the combination of lattice geometry, interactions, and anisotropies gives rise to competing spin arrangements in the ground state. Theoretical Hamiltonians which produce spin liquids are spin ice, the Kitaev honeycomb model, and the kagome antiferromagnet. Spin liquid behavior, however, in real materials is rare because they can only approximate these Hamiltonians and often have weak higher-order terms that destroy the spin liquid state. ${\mathrm{Ca}}_{10}{\mathrm{Cr}}_{7}{\mathrm{O}}_{28}$ is a new quantum spin liquid candidate with magnetic ${\mathrm{Cr}}^{5+}$ ions that possess quantum spin number $S=\textonehalf{}$. The spins are entirely dynamic in the ground state and the excitation spectrum is broad and diffuse, as is typical of spinons which are the excitations of a spin liquid. In this paper we determine the Hamiltonian of ${\mathrm{Ca}}_{10}{\mathrm{Cr}}_{7}{\mathrm{O}}_{28}$ using inelastic neutron scattering under high magnetic field to induce a field-polarized paramagnetic ground state and spin-wave excitations that can be fitted to extract the interactions. We further explore the phase diagram by using inelastic neutron scattering and heat capacity measurements and establish the boundaries of the spin liquid phase as a function of magnetic field and temperature. Our results show that ${\mathrm{Ca}}_{10}{\mathrm{Cr}}_{7}{\mathrm{O}}_{28}$ consists of distorted kagome bilayers with several isotropic ferromagnetic and antiferromagnetic interactions where, unexpectedly, the ferromagnetic interactions are stronger than the antiferromagnetic ones. This complex Hamiltonian does not correspond to any known spin liquid model and points to new directions in the search for quantum spin liquid behavior.