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Andrei Rogalev

Publications and source records attributed to Andrei Rogalev.

12 recordsLinked to original sources

Interfacial charge-transfer in 3d/5d complex oxide heterostructures

Interfacial charge transfer (ICT) provides a powerful route to engineer electronic phases in correlated oxide heterostructures, yet predictive design principles remain elusive. Here, we systematically investigate superlattices composed of the 5d spin-orbit coupled semimetal SrIrO3 and a series of correlated 3d perovskites (LaMnO3, LaFeO3, LaCoO3, and NdNiO3), thereby establishing a quantitative framework for ICT across 3d/5d interfaces. Combining element-specific x-ray absorption spectroscopy with spatially resolved electron energy loss spectroscopy, a homogeneous electron transfer from the 5d to the 3d layers is directly quantified, reaching up to 0.35 e per unit cell in the cobaltate superlattice. We show that the magnitude of ICT scales linearly with the difference in electronegativity between the transition-metal oxide layers, identifying electronegativity-driven band alignment as the dominant mechanism for ICT. Beyond interfacial doping, we find that strong 3d-5d hybridization induces a complete low-spin to high-spin conversion in the cobaltate layers, demonstrating interface-controlled spin-state engineering without chemical substitution. These results establish electronegativity mismatch as a predictive design parameter for correlated oxide interfaces and provide a materials platform for tailoring band filling, orbital hierarchy, and spin configurations in quantum oxide heterostructures, paving the way towards advanced oxide electronics and next-generation information technologies.

cond-mat.mtrl-sci

Ligand Mediated Magnetic Coupling Across Metamagnetic Transitions in CrPS4

Chromium thiophosphate (CrPS4) is a long-known material: a layered semiconducting antiferromagnet. Its recently discovered gate-tunable metamagnetic phase transitions, the remarkable positive and oscillating magnetoresistance as a tunnel barrier, and its Fano-resonance luminescence, elusive among the multitude of Cr3+ compounds, call for revisiting the understanding of its electronic structure, especially regarding how it relates to magnetic order. Here, we employ X-ray magnetic circular dichroism, implemented in both absorption and resonant inelastic X-ray spectroscopies, together with quantum many-body calculations, to unveil the role of metal-ligand covalency in mediating the metamagnetic transitions in CrPS4, using crystal-field and charge-transfer excitations as fingerprints of the evolving magnetic order. We reveal the role of extended superexchange paths involving P and S atoms, coupling interactions between the Cr spins across the different magnetic phases: antiferromagnetic, canted, and ferromagnetic. Our results elucidate the electronic states involved in these phases and provide prescriptions for engineering the metamagnetic phase diagram of CrPS4.

cond-mat.mtrl-sci

Spin and Orbital Magnetism in UH2 Thin Films Studied by X-ray Magnetic Circular Dichroism

Uranium dihydride UH2 is a metastable phase unknown in bulk form but accessible through thin-film synthesis. We prepared UH2 films by reactive dc sputtering on CaF2(001) or Si(001) substrates, the latter equipped with a Mo buffer layer to suppress a U-Si interdiffusion. On CaF2, UH2 adopts the fluorite-type structure with a near-[1 1 1] out-of-plane texture, four rotational domains, and a lattice parameter a = 539 +- 3 pm without measurable strain, whereas the Mo-buffered film is polycrystalline. X-ray photoelectron spectroscopy confirmed complete hydrogenation and minimal oxidation. Magnetization and XMCD measurements show ferromagnetic ordering with Curie temperatures of 120-130 K and a uranium 5f moment of 0.9 {\mu}B/U, dominated by the orbital contribution ({\mu}L ~ 1.4 {\mu}B, {\mu}S ~ -0.5 {\mu}B), in a good agreement with GGA+U computations, which otherwise overestimate absolute values of the spin and orbital components. The slightly reduced moment in thinner CaF2-supported films is attributed to surface U(IV) species. These results demonstrate that thin-film synthesis enables stabilization of UH2 and direct probing of 5f magnetism, opening pathways toward higher uranium hydrides and interface-engineered actinide systems.

cond-mat.mtrl-sci

Local magnetic and geometric structure in Mn-doped La(Fe,Si)13

Magnetic cooling has the potential to replace conventional gas compression refrigeration. Materials such as La(Fe,Si)$_{13}$ exhibit a sizeable first-order magnetocaloric effect, and it is possible to tailor the phase transition towards room temperature by Mn-H-doping, resulting in a large temperature range for operation. Within this work, we discuss variations of the electronic and lattice structure in La(Fe,Si)$_{13}$ with increasing Mn content utilizing X-ray magnetic circular dichroism (XMCD) and extended X-ray absorption fine structure spectroscopy (EXAFS). While XMCD shows a decrease of the magnetic polarization at the Fe K edge, low-temperature EXAFS measurements indicate increased positional disorder in the La environment that is otherwise absent for Fe and Mn. First-principles calculations link the positional disorder to an enlarged Mn-Si distance -- explaining the increased positional disorder in the La surrounding.

cond-mat.mtrl-sci

Static magnetic proximity effects and spin Hall magnetoresistance in Pt/Y$_{3}$Fe$_{5}$O$_{12}$ and inverted Y$_{3}$Fe$_{5}$O$_{12}$/Pt bilayers

The magnetic state of heavy metal Pt thin films in proximity to the ferrimagnetic insulator Y$_{3}$Fe$_{5}$O$_{12}$ has been investigated systematically by means of x-ray magnetic circular dichroism and x-ray resonant magnetic reflectivity measurements combined with angle-dependent magnetotransport studies. To reveal intermixing effects as the possible cause for induced magnetic moments in Pt, we compare thin film heterostructures with different order of the layer stacking and different interface properties. For standard Pt layers on Y$_{3}$Fe$_{5}$O$_{12}$ thin films, we do not detect any static magnetic polarization in Pt. These samples show an angle-dependent magnetoresistance behavior, which is consistent with the established spin Hall magnetoresistance. In contrast, for the inverted layer sequence, Y$_{3}$Fe$_{5}$O$_{12}$ thin films grown on Pt layers, Pt displays a finite induced magnetic moment comparable to that of all-metallic Pt/Fe bilayers. This magnetic moment is found to originate from finite intermixing at the Y$_{3}$Fe$_{5}$O$_{12}$/Pt interface. As a consequence, we found a complex angle-dependent magnetoresistance indicating a superposition of the spin Hall and the anisotropic magnetoresistance in these type of samples. Both effects can be disentangled from each other due to their different angle dependence and their characteristic temperature evolution.

cond-mat.mtrl-sci

Unraveling Bulk and Grain Boundary Electrical Properties in La0.8Sr0.2Mn1-yO3 Thin Films

Grain boundaries in Sr-doped LaMnO3 thin films have been shown to strongly influence the electronic and oxygen mass transport properties, being able to profoundly modify the nature of the material. The unique behaviour of the grain boundaries can be correlated with substantial modifications of the cation concentration at the interfaces, which can be tuned by changing the overall cationic ratio in the films. In this work, we study the electronic properties of La0.8Sr0.2Mn1-yO3 thin films with variable Mn content. The influence of the cationic composition on the grain boundary and grain bulk electronic properties is elucidated by studying the manganese valence state evolution using spectroscopy techniques and by confronting the electronic properties of epitaxial and polycrystalline films. Substantial differences in the electronic conduction mechanism are found in the presence of grain boundaries and depending on the manganese content. Moreover, the unique defect chemistry of the nanomaterial is elucidated by measuring the electrical resistance of the thin films as a function of oxygen partial pressure, disclosing the importance of the cationic local non-stoichiometry on the thin films behavior.

cond-mat.mtrl-sci

Probing Magnetic Sublattices in Multiferroic Ho$_{0.5}$Nd$_{0.5}$Fe$_{3}$(BO$_{3}$)$_{4}$ Single Crystal using X-ray Magnetic Circular Dichroism

Using element-specific X-ray magnetic circular dichroism (XMCD) technique we have studied different magnetic sublattices in a multiferroic Ho$_{0.5}$Nd$_{0.5}$Fe$_{3}$(BO$_{3}$)$_{4}$ single crystal. The XMCD measurements at the \emph{L}$_{2,3}$-edges of Ho and Nd, and at the Fe \emph{K}-edge have been performed at \emph{T}=2~K under a magnetic field up to 17~T applied along the trigonal \emph{c}-axis as well as in the basal \emph{ab}-plane. All three magnetic sublattices are shown to undergo a spin-reorientation transition under magnetic field applied along the \emph{c}-axis. On the contrary, when magnetic field is applied in the \emph{ab}-plane only the holmium atoms exhibit a magnetization jump. Thus, the element-specific magnetization curves revealed the Ho sublattice to be much stronger coupled to the Fe one than the Nd sublattice. The results demonstrate that the Ho$^{3+}$ subsystem plays even more dominant role in magnetic behavior of Ho$_{0.5}$Nd$_{0.5}$Fe$_{3}$(BO$_{3}$)$_{4}$ crystal than in pure HoFe$_{3}$(BO$_{3}$)$_{4}$ crystal.

cond-mat.mtrl-sci

Local noncentrosymmetric structure of Bi2Sr2CaCu2O8+y by X-ray magnetic circular dichroism at Cu K-edge XANES

The two-dimensional Bi2Sr2CaCu2O8+y (Bi2212), the most studied prototype cuprate superconductor, is a lamellar system made of a stack of two-dimensional corrugated CuO2 bilayers separated by Bi2O2+ySr2O2 layers. While the large majority of theories, proposed to interpret unconventional high Tc superconductivity in Bi2Sr2CaCu2O8+y, assume a centrosymmetric tetragonal CuO2 lattice for the [CuO2]Ca[CuO2] bilayer here we report new compelling results providing evidence for local noncentrosymmetric structure at the Cu site. We have measured polarized Cu K-edge XANES (x-ray absorption near edge structure) and the K-edge X-ray magnetic circular dichroism (XMCD) of a Bi2212 single crystal near optimum doping. The Cu K edge XMCD signal was measured at ID12 beamline of ESRF with the k-vector of x-ray beam parallel to c-axis i.e. with the electric field of x-ray beam E//ab, using a 17 T magnetic field parallel to the c-axis of a Bi2212 single crystal. Numerical simulations of the XMCD signal of Bi2212 by multiple scattering theory have shown agreement with the experimental XMCD signal only for the local structure with noncentrosymmetric Bb2b space group of Bi2Sr2CaCu2O8+y.

cond-mat.supr-con

High Resolution Hard X-ray Magnetic Imaging with Dichroic Ptychography

Imaging the magnetic structure of a material is essential to understanding the influence of the physical and chemical microstructure on its magnetic properties. Magnetic imaging techniques, however, have up to now been unable to probe 3D micrometer-sized systems with nanoscale resolution. Here we present the imaging of the magnetic domain configuration of a micrometre-thick FeGd multilayer with hard X-ray dichroic ptychography at energies spanning both the Gd L3 edge and the Fe K edge, providing a high spatial resolution spectroscopic analysis of the complex X-ray magnetic circular dichroism. With a spatial resolution reaching 45 nm, this advance in hard X-ray magnetic imaging is the first step towards the investigation of buried magnetic structures and extended three-dimensional magnetic systems at the nanoscale.

cond-mat.mtrl-sci

Comment on "Pt magnetic polarization on Y3Fe5O12 and magnetotransport characteristics"

In a recent Letter [Y.M. Lu et al., Phys. Rev. Lett. 110, 147207 (2013)], Lu et al. reported on "ferromagneticlike transport properties" of thin films of Pt, deposited ex situ via sputtering on the ferrimagnetic insulator Y3Fe5O12. The authors found a magnetoresistance in Pt displaying a hysteresis corresponding to the coercive field of Y3Fe5O12, consistent with the findings of other groups. While the latter interpreted their data in terms of the recently proposed spin-Hall magnetoresistance, Lu et al. attributed their observation to a magnetic proximity effect. To support this interpretation, they measured the X-ray magnetic circular dichroism (XMCD) at the Pt L2,3 edges from a Pt/Y3Fe5O12 sample with a Pt thickness of 1.5 nm and derived an average induced magnetic moment of 0.054 Bohr magnetons per Pt atom. This is contradictory to the results of our previous comprehensive XMCD study of three different Pt/Y3Fe5O12 samples with Pt thicknesses of 3, 7, and 10 nm from which we identified an upper limit of (0.003 +/- 0.001) Bohr magnetons per Pt [Geprägs et al., Appl. Phys. Lett. 101, 262407 (2012), arXiv:1211.0916].

cond-mat.mtrl-sci

Investigation of induced Pt magnetic polarization in Pt/Y3Fe5O12 bilayers

Using X-ray magnetic circular dichroism (XMCD) measurements, we explore the possible existence of induced magnetic moments in thin Pt films deposited onto the ferrimagnetic insulator yttrium iron garnet (Y3Fe5O12). Such a magnetic proximity effect is well established for Pt/ferromagnetic metal heterostructures. Indeed, we observe a clear XMCD signal at the Pt L3 edge in Pt/Fe bilayers, while no such signal can be discerned in XMCD traces of Pt/Y3Fe5O12 bilayers. Integrating the XMCD signals allows to estimate an upper limit for the induced Pt magnetic polarization in Pt/Y3Fe5O12 bilayers.

cond-mat.mtrl-sci

Structural relaxations around Ti, Cr and Fe impurities in alpha-Al2O3 probed by x-ray absorption near edge structure combined with first-principles calculations

We determine the structural relaxations around paramagnetic impurities (Ti, Cr, Fe) in corundum (alpha-Al2O3), by combining x-ray absorption near edge structure (XANES) experiments and ab initio calculations. The structural relaxations are found to be very local. We then show that XANES is sensitive to small variations in interatomic distances within the coordination shell of the absorbing atom. The experiments were carried out on single crystals of ruby and sapphires. Linear dichroic signals are essential to characterize the geometry of the impurity site. The calculations were performed within a self-consistent ``non muffin-tin'' framework, that uses pseudopotentials, plane-wave basis set, and the continued fraction for the absorption cross section.

cond-mat.mtrl-sci