arXiv subjects

F. Wilhelm

Publications and source records attributed to F. Wilhelm.

At least 19 recordsLinked to original sources

arXiv2025

Extremely asymmetric diffraction as a method of determining magneto-optical constants for X-rays near absorption edges

The spectral dependence of the Bragg peak position under conditions of extremely asymmetric diffraction has been analyzed in the kinematical and dynamical approximations of the diffraction theory. Simulations have been performed for the L$_3$ absorption edge of yttrium in a single crystal YFe$_2$ film; they have shown that the magneto optical constants (or, equivalently, the dispersion corrections to the atomic scatter ing factor) for hard X rays can be determined from this dependence. Comparison with the experimental data obtained for a Nb(4 nm)/YFe$_2$(40 nm $\langle 110 \rangle$)/Fe(1.5 nm)/Nb(50 nm)/sapphire sample at the European Synchrotron Radiation Facility has been made.

cond-mat.mtrl-sci↗

arXiv2023

A multi-stage, first-order phase transition in LaFe11.8Si1.2: interplay between the structural, magnetic and electronic degrees of freedom

Alloys with a first-order magnetic transition are central to solid-state refrigeration technology, sensors and actuators, or spintronic devices. The discontinuous nature of the transition in these materials is a consequence of the coupling between the magnetic, electronic and structural subsystems, but in a real experiment, it is difficult to observe and analyze the simultaneous evolution of all the subsystems. As a result, it is very hard to determine the main mechanisms of the transition and purposefully develop these advanced magnetic materials. To resolve this issue, we changed the existing paradigm and conducted simultaneous measurements of the macroscopic properties - magnetization, temperature change of the sample, longitudinal and transversal magnetostrictions - to reveal the rich details of the magneto-structural, first-order transition occurring in the prototypical alloy LaFe11.8Si1.2. We complement these findings with experiments on the atomistic scale, i.e., x-ray absorption spectroscopy (XAS), x-ray magnetic circular dichroism (XMCD) and M\"ossbauer spectroscopy, and then combine them with first-principles calculations to reveal the full complexity and two-stage nature of the transition. This new approach can be successfully extended to a large class of advanced magnetic materials that exhibit analogous transformations.

cond-mat.mtrl-sci↗

arXiv2022

Valence state and lattice incorporation of Ni in Zn/Co-based magnetic oxides

Ni incorporation has been studied in a comprehensive range of Zn/Co-based magnetic oxides to elucidate it valence state and lattice incorporation. The resulting structural and magnetic properties are studied in detail. To the one end Ni in incorporated by in-diffusion as well as reactive magnetron co-sputtering in wurtzite ZnO where only the Ni-diffused ZnO exhibits significant conductivity. This is complemented by Ni and Co codoping of ZnO leading. To the other end, the ZnCo$_2$O$_4$ spinel is co-doped with varying amounts of Ni. In the wurtzite oxides Ni is exclusively found on tetrahedral lattice sites in its formal 2+ oxidation state as deep donor. It behaves as an anisotropic paramagnet and a limited solubility of Ni about 10\% is found. Due to its smaller magnetic moment it can induce partial uncompensation of the Co magnetic moments due to antiferromagnetic coupling. In the spinel Ni is found to be incorporated in its formal 3+ oxidation state on octahedral sites and couples antiferromagnetically to the Co moments leading again to magnetic uncompensation of the otherwise antiferromagnetic ZnCo$_2$O$_4$ spinel and to ferrimagnetism at higher Ni concentrations. Increasing Ni even further leads to phase separation of cubic NiO resulting in an exchange-biased composite magnetic oxide.

cond-mat.mtrl-sci↗

arXiv2020

Spin state crossover in Co3BO5

The magnetic contribution of the Co3+ ions in Co3BO5 has been investigated using the Co (K-edge) XMCD, dc magnetic susceptibility, and heat capacity measurements. The crystal structure of Co3BO5 single crystal has been solved in detail at the T range 296-703 K. The results have been supplemented by the GGA+U calculations.

cond-mat.mtrl-sci↗

arXiv2018

Magnetic, electronic and transport properties of high-pressure-synthesized chiralmagnets Mn$_{1-x}$Rh$_x$Ge (B20)

We report on structural, magnetic and transport properties of a new set of the high-pressuresynthesized compounds Mn$_{1-x}$Rh$x$Ge ($0 \leq x \leq 1$) with the chiral magnetic ordering. The magnetic and transport properties depend substantially on the concentration of rhodium (x) and the pressure. The saturation magnetic moment corresponds to a known high-spin value for pristine MnGe (x = 0) and decreases almost linearly with increasing concentration $x$. In addition, XMCD spectra taken at 10 K and 2 T indicate magnetic polarization of the Rh 4d electron states and Ge $4p$ states, which decreases with $x$, too. In rhodium rich compounds ($x \geq 0.5$) the temperature of the magnetic ordering increases significantly with pressure, whereas in manganese rich compounds ($x < 0.5$) the temperature decreases. Three different tendencies are also found for several structural and transport properties. In the intermediate range ($0.3 \leq x \leq 0.7$) samples are semiconducting in the paramagnetic phase, but become metallic in the magnetically ordered state. We carried out ab initio density-functional calculations of Mn$_{1-x}$Rh$_x$Ge at various concentrations $x$ and traced the evolution of electronic and magnetic properties. The calculation results are in good agreement with the measured magnetic moments and qualitatively explain the observed trends in transport properties.

cond-mat.str-el↗

arXiv2018

Probing the $J_{eff}=0$ ground state and the Van Vleck paramagnetism of the Ir$^{5+}$ ions in the layered Sr$_2$Co$_{0.5}$Ir$_{0.5}$O$_4$

We report a combined experimental and theoretical x-ray magnetic circular dichroism (XMCD) spectroscopy study at the Ir-$L_{2,3}$ edges on the Ir$^{5+}$ ions of the layered hybrid solid state oxide Sr$_2$Co$_{0.5}$Ir$_{0.5}$O$_4$ with the K$_2$NiF$_4$ structure. From theoretical simulation of the experimental Ir-$L_{2,3}$ XMCD spectrum, we found a deviation from a pure $J_{eff}=0$ ground state with an anisotropic orbital-to-spin moment ratio ($L_x/2S_x$ = 0.43 and $L_z/2S_z$ = 0.78). This deviation is mainly due to multiplet interactions being not small compared to the cubic crystal field and due to the presence of a large tetragonal crystal field associated with the crystal structure. Nevertheless, our calculations show that the energy gap between the singlet ground state and the triplet excited state is still large and that the magnetic properties of the Ir$^{5+}$ ions can be well described in terms of singlet Van Vleck paramagnetism.

cond-mat.str-el↗

arXiv2017

Probing magnetism in the vortex phase of PuCoGa$_5$ by X-ray magnetic circular dichroism

We have measured X-ray magnetic circular dichroism (XMCD) spectra at the Pu $M_{4,5}$ absorption edges from a newly-prepared high-quality single crystal of the heavy fermion superconductor $^{242}$PuCoGa$_{5}$, exhibiting a critical temperature $T_{c} = 18.7~{\rm K}$. The experiment probes the vortex phase below $T_{c}$ and shows that an external magnetic field induces a Pu 5$f$ magnetic moment at 2 K equal to the temperature-independent moment measured in the normal phase up to 300 K by a SQUID device. This observation is in agreement with theoretical models claiming that the Pu atoms in PuCoGa$_{5}$ have a nonmagnetic singlet ground state resulting from the hybridization of the conduction electrons with the intermediate-valence 5$f$ electronic shell. Unexpectedly, XMCD spectra show that the orbital component of the $5f$ magnetic moment increases significantly between 30 and 2 K; the antiparallel spin component increases as well, leaving the total moment practically constant. We suggest that this indicates a low-temperature breakdown of the complete Kondo-like screening of the local 5$f$ moment.

cond-mat.str-el↗

arXiv2016

Microscopic mechanism of the giant magnetocaloric effect in MnCoGe alloys probed by XMCD

One important aspect of the magneto-structural transition in MnCoGe and related materials is the reduction in saturation magnetization from the orthorhombic to the hexagonal phase. Here, by combining an element specific magnetization probe such as x-ray magnetic circular dichroism and band structure calculations, we show that the magnetic moment instability between orthorhombic and hexagonal structures originates from a reduction in the Mn sub-lattice magnetization. The consequences of the moment instability for the magnetocaloric effect are discussed.

cond-mat.str-el↗

arXiv2015

Absence of magnetic proximity effects in magnetoresistive Pt/CoFe2O4 hybrid interfaces

Ultra-thin Pt films grown on insulating ferrimagnetic CoFe2O4 (111) epitaxial films display a magnetoresistance upon rotating the magnetization of the magnetic layer. We report here X-ray magnetic circular dichroism (XMCD) recorded at Pt-L2,3 and Pt-M3 edges. The results indicate that the Pt magnetic moment, if any, is below the detection limit (< 0.001 {\mu}$_B$/Pt), thus strongly favoring the view that the presence of CoFe2O4 does not induce the formation of magnetic moments in Pt. Therefore, the observed magnetoresistance cannot be attributed to some sort of proximity-induced magnetic moments at Pt ions and subsequent magnetic-field dependent scattering. It thus follows that either bulk (spin Hall and Inverse spin Hall Effects) or interface (Rashba) spin-orbit related effects dominate the observed magnetoresistance. Furthermore, comparison of bulk magnetization and XMCD data at (Fe,Co)-L2,3 edges suggests the presence of some spin disorder in the CoFe2O4 layer which may be relevant for the observed anomalous non-saturating field-dependence of spin Hall magnetoresistance.

cond-mat.mtrl-sci↗

arXiv2015

Electronic tuneability of a structurally rigid surface intermetallic and Kondo lattice: CePt$_5$ / Pt(111)

We present an extensive study of structure, composition, electronic and magnetic properties of Ce--Pt surface intermetallic phases on Pt(111) as a function of their thickness. The sequence of structural phases appearing in low energy electron diffraction (LEED) may invariably be attributed to a single underlying intermetallic atomic lattice. Findings from both microscopic and spectroscopic methods, respectively, prove compatible with CePt$_5$ formation when their characteristic probing depth is adequately taken into account. The intermetallic film thickness serves as an effective tuning parameter which brings about characteristic variations of the Cerium valence and related properties. Soft x-ray absorption (XAS) and magnetic circular dichroism (XMCD) prove well suited to trace the changing Ce valence and to assess relevant aspects of Kondo physics in the CePt$_5$ surface intermetallic. We find characteristic Kondo scales of the order of 10$^2$ K and evidence for considerable magnetic Kondo screening of the local Ce $4f$ moments. CePt$_5$/Pt(111) and related systems therefore appear to be promising candidates for further studies of low-dimensional Kondo lattices at surfaces.

cond-mat.str-el↗

arXiv2015

Twisted phase of the orbital-dominant ferromagnet SmN in a GdN/SmN heterostructure

The strong spin-orbit interaction in the rare-earth elements ensures that even within a ferromagnetic state there is a substantial orbital contribution to the ferromagnetic moment, in contrast to more familiar transition metal systems, where the orbital moment is usually quenched. The orbital-dominant magnetization that is then possible within rare-earth systems facilitates the fabrication of entirely new magnetic heterostructures, and here we report a study of a particularly striking example comprising interfaces between GdN and SmN. Our investigation reveals a twisted magnetization arising from the large spin-only magnetic moment in GdN and the nearly zero, but orbital-dominant, moment of SmN. The unusual twisted phase is driven by (i) the similar ferromag- netic Gd-Gd, Sm-Sm and Gd-Sm exchange interactions, (ii) a SmN Zeeman interaction 200 times weaker than that of GdN, and (iii) the orbital-dominant SmN magnetic moment. The element specificity of X-ray magnetic circular dichroism (XMCD) is used in seperate modes probing both bulk and surface regions, revealing the depth profile of the twisting magnetization.

cond-mat.mtrl-sci↗

arXiv2015

Magnetic polarization of the americium $J = 0$ ground state in AmFe$_{2}$

Trivalent americium has a non-magnetic ($J$ = 0) ground state arising from the cancelation of the orbital and spin moments. However, magnetism can be induced by a large molecular field if Am$^{3+}$ is embedded in a ferromagnetic matrix. Using the technique of x-ray magnetic circular dichroism, we show that this is the case in AmFe$_2$. Since $\langle J_z \rangle$ = 0, the spin component is exactly twice as large as the orbital one, the total Am moment is opposite to that of Fe, and the magnetic dipole operator $\langle T_{z} \rangle$ can be determined directly; we discuss the progression of the latter across the actinide series.

cond-mat.str-el↗

arXiv2015

Assessment of the U and Co magnetic moments in UCoGe by X-ray magnetic circular dichroism

The ferromagnetic superconductor UCoGe has been investigated by high field X-ray magnetic circular dichroism (XMCD) at the U-M$_{4,5}$ and Co/Ge-K edges. The analysis of the branching ratio and XMCD at the U-M$_{4,5}$ edges reveals that the U-5$f$ electrons count is close to 3. The orbital ($\sim0.70\,\mu_B$) and spin ($\sim-0.30\,\mu_B$) moments of U at 2.1K and 17T (H//c) have been determined. Their ratio ($\sim-2.3$) suggests a significant delocalization of the 5$f$ electron states. The similar field dependences of the local U/Co and the macroscopic magnetization indicate that the Co moment is induced by the U moment. The XMCD at the Co/Ge-K edges reveal the presence of small Co-4$p$ and Ge-4$p$ orbital moments parallel to the macroscopic magnetization. In addition, the Co-3$d$ moment is estimated to be at most of the order of 0.1$\mu_B$ at 17T. Our results rule out the possibility of an unusual polarisability of the U and Co moments as well as their antiparallel coupling. We conclude that the magnetism which mediates the superconductivity in UCoGe is driven by U.

cond-mat.str-el↗

arXiv2014

Low temperature magnetic properties of NpNi$_5$

We present the result of an extended experimental characterization of the hexagonal intermetallic Haucke compound NpNi$_{5}$. By combining macroscopic and shell-specific techniques, we determine the 5$f$-shell occupation number $n_f$ close to 4 for the Np ions, together with orbital and spin components of the ordered moment in the ferromagnetic phase below T$_C$ = 16 K ($μ_{S}$ = -1.88~$μ_{B}$ and $μ_{L}$ = 3.91~$μ_{B}$). The apparent coexistence of ordered and disordered phases observed in the Mössbauer spectra is explained in terms of slow relaxation between the components of a quasi-triplet ground state. The ratio between the expectation value of the magnetic dipole operator and the spin magnetic moment ($3\langle T_{z}\rangle/ \langle S_{z}\rangle$ = +1.43) is positive and large, suggesting a localized character of the 5$f$ electrons. The angular part of the spin-orbit coupling ($\langle\vec{\ell}\cdot\vec{s}\rangle$ = -5.55) is close to the value of -6.25 calculated for trivalent Np ions in intermediate coupling approximation. The results are discussed against the prediction of first-principle electronic structure calculations based on the spin-polarized local spin density approximation plus Hubbard interaction, and of a mean field model taking into account crystal field and exchange interactions.

cond-mat.str-el↗

arXiv2013

Spin pumping damping and magnetic proximity effect in Pd and Pt spin-sink layers

We investigated the spin pumping damping contributed by paramagnetic layers (Pd, Pt) in both direct and indirect contact with ferromagnetic Ni$_{81}$Fe$_{19}$ films. We find a nearly linear dependence of the interface-related Gilbert damping enhancement $\Delta\alpha$ on the heavy-metal spin-sink layer thicknesses t$_\textrm{N}$ in direct-contact Ni$_{81}$Fe$_{19}$/(Pd, Pt) junctions, whereas an exponential dependence is observed when Ni$_{81}$Fe$_{19}$ and (Pd, Pt) are separated by \unit[3]{nm} Cu. We attribute the quasi-linear thickness dependence to the presence of induced moments in Pt, Pd near the interface with Ni$_{81}$Fe$_{19}$, quantified using X-ray magnetic circular dichroism (XMCD) measurements. Our results show that the scattering of pure spin current is configuration-dependent in these systems and cannot be described by a single characteristic length.

cond-mat.mes-hall↗

arXiv2013

Europium nitride: A novel diluted magnetic semiconductor

Europium nitride is semiconducting and contains non-magnetic \3+, but sub-stoichiometric EuN has Eu in a mix of 2+ and 3+ charge states. We show that at \2+ ~concentrations near 15-20% EuN is ferromagnetic with a Curie temperature as high as 120 K. The \3+ ~polarization follows that of the \2+, confirming that the ferromagnetism is intrinsic to the EuN which is thus a novel diluted magnetic semiconductor. Transport measurements shed light on the likely exchange mechanisms.

cond-mat.mtrl-sci↗

arXiv2013

Emergence of ferromagnetism and Jahn-Teller distortion in low Cr-substituted LaMnO3

The emergence of a ferromagnetic component in $LaMnO_{3}$ with low Cr-for-Mn substitution has been studied by x-ray absorption spectroscopy and x-ray magnetic circular dichroism at the Mn and Cr K edges. The local magnetic moment strength for the Mn and Cr are proportional to each other and follows the macroscopic magnetization. The net ferromagnetic components of $Cr^{3+}$ and $Mn^{3+}$ are found antiferromagnetically coupled. Unlike hole doping by La site substitution, the inclusion of $Cr^{3+}$ ions up to x = 0.15 does not decrease the Jahn-Teller (JT) distortion and consequently does not significantly affect the orbital ordering. This demonstrates that the emergence of the ferromagnetism is not related to JT weakening and likely arises from a complex orbital mixing.

cond-mat.str-el↗

arXiv2013

X-ray magnetic circular dichroism experiments and theory of transuranium Laves phase compounds

The actinide cubic Laves compounds NpAl2, NpOs2, NpFe2, and PuFe2 have been examined by X-ray magnetic circular dichroism (XMCD) at the actinide M4,5 absorption edges and Os L2,3 absorption edges. The XMCD experiments performed at the M4,5 absorption edges of Np and Pu allow us to determine the spectroscopic branching ratio, which gives information on the coupling scheme in these materials. In all materials the intermediate coupling scheme is found appropriate. Comparison with the SQUID data for NpOs2 and PuFe2 allows a determination of the individual orbital and spin magnetic moments and the magnetic dipole contribution mmd. The resulting orbital and spin magnetic moments are in good agreement with earlier values determined by neutron diffraction, and the values of mmd are non-negligible, and close to those predicted for intermediate coupling. There is a comparatively large induced moment on the Os atom in NpOs2 such that the Os contribution to the total moment per formula unit is ~30% of the total. The spin and orbital moments at the Os site are parallel, in contrast to the anti-parallel configuration of Os impurities in 3d ferromagnetic transition metals. Calculations using the LDA+U technique are reported. The ab initio computed XMCD spectra show good agreement with experimental spectra for small values (0-1eV) of the Hubbard U parameter, which underpins that 5f electrons in these compounds are relatively delocalized.

cond-mat.str-el↗