X-ray Magnetic Circular Dichroism Experiments Research Articles

Quantifying the orbital-to-spin moment ratio under dynamic excitation

The orbital component of magnetization dynamics, e.g., excited by ferromagnetic resonance (FMR), may generate “orbitronic” effects in nanomagnetic devices. Yet, distinguishing orbital dynamics from spin dynamics remains a challenge. Here, we employ x-ray magnetic circular dichroism (XMCD) to quantify the ratio between the orbital and spin components of FMR-induced dynamics in a Ni80Fe20 film. By applying the XMCD sum rules at the Ni L3,2 edges, we obtain an orbital-to-spin ratio of 0.108 ± 0.005 for the dynamic magnetization. This value is consistent with 0.102 ± 0.008 for the static magnetization, probed with the same x-ray beam configuration as the dynamic XMCD experiment. The demonstrated method presents a possible path to disentangle orbitronic effects from their spintronic counterparts in magnetic media.

Investigating the electronic states of UTe2 using X-ray spectroscopy

The recent discovery of superconductivity in paramagnetic UTe2 turns spotlight on a serious candidate for spin-triplet state. To draw a complete picture of the superconducting state in UTe2 precise knowledge of the electronic properties of the 5 f states of Uranium is missing. We report on x-ray absorption and magnetic circular dichroism experiments performed at the U M4,5 edges at 2.7 K. At ambient pressure the 5 f electron count is found to be in-between 2.6 and 2.8. Partial delocalization of the 5 f electrons is further confirmed by the reduced value of the U orbital to spin magnetic moment ratio. The 5 f count is reduced by as large as 7 percent at the transition to a magnetically ordered state at Pc ≈ 1.5 GPa. At pressures above 4 GPa, the 5 f count increases back towards U3+ in the tetragonal phase. The observed “valence instabilities” and their interplay with magnetism seem to be important ingredients to understand the electronic structure in UTe2 in different phases.

Nonmonotonous temperature fluctuations of the orbital moment and spin-orbit coupling in multiferroic gallium ferrite thin films

Temperature dependent x-ray absorption spectroscopy and x-ray magnetic circular dichroism experiments were performed at the Fe ${L}_{2,3}$ edges to unveil the magnetic orbital moment and spin-orbit coupling (SOC) behavior in thin films of the multiferroic ${\mathrm{Ga}}_{0.6}{\mathrm{Fe}}_{1.4}{\mathrm{O}}_{3}$ (GFO) compound. A thorough analysis of the data evidenced a nonmonotonous behavior for both magnetic orbital moment and SOC with a minimum at approximately 120 K, accompanied with indications of disturbances of the magnetic exchange and electric field dipole. Resonant photoemission spectroscopy experiments performed at the Fe ${L}_{2,3}$ edges rendered an important modification of the crystal field configuration around this temperature value, pointing to a temperature-driven structural trigonal distortion. These instabilities can be compared to those observed in other iron oxides, in particular, during transitions such as the Verwey transition, with the difference that on GFO they do not have any impact on the macroscopic magnetic properties, such as the coercive field and the global magnetization. This work demonstrates that the absence of instabilities in magnetism at the macroscopic scale does not guarantee the absence of fluctuations at the atomic scale. Such atomic-scale fluctuations of the SOC are undoubtedly shown here and have an impact on the spin Hall magnetoresistance response of the films. This point is of importance for prospective applications of GFO in spin-orbitronics.

Experimental confirmation of the delayed Ni demagnetization in FeNi alloy

Element-selective techniques are central for the understanding of ultrafast spin dynamics in multi-element materials, such as magnetic alloys. Recently, however, it turned out that the commonly used technique of the transverse magneto-optical Kerr effect (T-MOKE) in the extreme ultraviolet range may have issues with unwanted crosstalk between different elemental signals and energy-dependent non-linear response. This problem can be sizeable, which puts recent observations of ultrafast spin transfer from Fe to Ni sites in FeNi alloys into question. In this study, we investigate the Fe-to-Ni spin transfer in a crosstalk-free time-resolved x-ray magnetic circular dichroism (XMCD) experiment with a reliable time reference. With XMCD near the absorption maxima, we find a very similar Fe and Ni dynamics as with T-MOKE from identical samples. Considering the potential non-linearities of the T-MOKE response, such a good agreement in our findings is remarkable. Our data provide the ongoing discussion about ultrafast spin-transfer mechanisms in FeNi systems with a broader experimental basis.

Element-specific magnetic hysteresis loops observed in hexagonal ErFeO3 thin films

We investigated the magnetic properties of multiferroic hexagonal ErFeO3 thin films by using x-ray magnetic circular dichroism (XMCD) and synchrotron Mössbauer spectroscopy. In order to reveal the element-specific magnetic properties, temperature-dependent XMCD experiments were conducted at the Fe L 2,3 and Er M 4,5-edges. Apparent magnetic hysteresis loops appear for both ions below the Néel temperature, which suggests the existence of ferromagnetism. The temperature evolutions of the coercive field and spontaneous magnetization for both ions show similar behavior. These results indicate that Fe ions influence the magnetism of Er ions. Our results deepen the understanding of the physical properties of hexagonal rare-earth ferrite system.

5f states in UGa2 probed by x-ray spectroscopies

The $5f$-based ferromagnet $\mathrm{U}{\mathrm{Ga}}_{2}$ with the Curie temperature ${T}_{\mathrm{C}}=125\phantom{\rule{0.16em}{0ex}}\mathrm{K}$ was investigated by x-ray absorption spectroscopy (XAS) and x-ray magnetic circular dichroism (XMCD) experiments at the $\mathrm{U}--{M}_{4,5}$ and Ga--K edges. The position of the $\mathrm{U}--{M}_{4}$ white line, determined in the high-energy resolution fluorescence detection XAS, suggests that $\mathrm{U}{\mathrm{Ga}}_{2}$ is neither a localized $5{f}^{2}$ nor an itinerant system with $5f$ occupancy close to ${n}_{5f}=3$. The analysis of the acquired ${M}_{4,5}$ XANES and XMCD spectra indicates the $5f$ occupancy close to 2.5 and a large orbital magnetic moment of the uranium $5f$ states (3.18 ${\ensuremath{\mu}}_{\mathrm{B}}$) that is partly compensated by the antiparallel spin moment (1.31 ${\ensuremath{\mu}}_{\mathrm{B}}$). Thus, the total $5f$ magnetic moment of 1.87 ${\ensuremath{\mu}}_{\mathrm{B}}$ is obtained, which is smaller than the known bulk magnetization of 3.0 ${\ensuremath{\mu}}_{\mathrm{B}}$ per formula unit, while the magnetic moments of the Ga atoms are negligible. Several methods based on density-functional theory were applied and the obtained results were compared with XAS spectral features, the Sommerfeld coefficient of the electronic specific heat, and the size of the U moments and $5f$ occupancies. A clear correlation is revealed between the $\mathrm{U}--{M}_{4}$ white-line position of three metallic uranium compounds and the calculated uranium ionicity. It is demonstrated that only electronic structure methods taking appropriate care of orbital magnetism and related atomic multiplet effects can successfully describe all considered properties.

Induced magnetization in Cu atoms at the Fe-Co/Cu3Au(001) interface: X-ray magnetic circular dichroism experiments and theoretical results

The induced magnetization in Cu atoms at the interface between ferromagnetic (FM) Fe/Co ultrathin films and a nonmagnetic (NM) Cu3Au(001) substrate was explored by the investigation of two structures of five alternated Fe and Co monoatomic layers with different stacking orders with a Fe or a Co layer in direct contact with the Cu3Au(001) surface. First principles calculations were applied to disentangle the origin of magnetic proximity effects at these FM/NM interfaces. The hybridization between the electronic states of the FM layers, resulting in a pronounced widening of the d-bands of the local density of states of Fe-Co interface atoms, has a fundamental effect in the spin-polarization of the NM substrate. X-ray magnetic circular dichroism measurements at the L2,3-edges of Fe, Co and Cu allowed to extract the spin and orbital magnetic moments of Fe and Co, and to measure extremely low magnetic moments induced in Cu atoms. It is shown that the magnetism is induced only in the Cu and Au atoms at the first CuAu monolayer at the very surface of the substrate, i.e., the Cu XMCD signal is due to only 0.5 ML magnetic Cu atoms.

Direct observation of the magnetic ordering process in the ferromagnetic semiconductor Ga1−xMnxAs via soft x-ray magnetic circular dichroism

In order to understand the mechanism of the ferromagnetism in the ferromagnetic semiconductor Ga1−xMnxAs [(Ga,Mn)As], we have investigated the magnetic behavior on a microscopic level through systematic temperature (T)- and magnetic field (H)-dependent soft x-ray magnetic circular dichroism (XMCD) experiments at the Mn L2,3 absorption edges. The T and H dependences of XMCD intensities have been analyzed using a model consisting of the ferromagnetic (FM), paramagnetic, and superparamagnetic (SPM) components. Intriguingly, we have found a common behavior for the ferromagnetic ordering process in (Ga,Mn)As samples with different Mn concentrations (4% and 10.8%) and different Curie temperature (TC) values (65, 120, and 164 K). In particular, the SPM component develops well above TC, indicating that local FM regions are formed well above TC. The present findings indicate that the onset of ferromagnetic ordering is triggered by local electronic states around the substitutional Mn ions rather than uniform electronic states considered by mean-field theories. Insight into the most representative ferromagnetic semiconductor, (Ga,Mn)As, provided by the present study will be an important step in understanding the mechanism of ferromagnetic ordering in various ferromagnetic semiconductor families.

A versatile X-ray phase retarder for lock-in XMCD measurements.

X-ray magnetic circular dichroism (XMCD) is a technique commonly used to probe magnetic properties of materials with element and orbital selectivity, which requires the use of circularly polarized (CP) X-rays. It is possible to accomplish XMCD experiments with fixed CP and alternating the magnetic fieldorientation, but most reliable data are obtained when alternating the magnetization orientation and the polarization between right and left helicities. A versatile strategy has been developed to perform XMCD experiments using a hard X-ray quarter-wave plate, at both polychromatic dispersive and conventional monochromatic optics, in combination with synchronous data acquisition. The switching frequency waveform is fed into a lock-in amplifier to detect andamplify the XMCD signal. The results on a reference sample demonstrate an improvement in data quality and acquisition time. The instrumentation successfully generated 98% of CP X-rays switching the beam helicity at 13 Hz, with the possibility of faster helicity switching once it is installed at the new Brazilian fourth-generation source, SIRIUS.

The Synthesis of a Quasi-One-Dimensional Iron-Based Telluride with Antiferromagnetic Chains and a Spin Glass State.

The report on the superconductivity of the two-legged spin ladders BaFe2S3 and BaFe2Se3 has established 123-type iron chalcogenides as a novel subgroup in the iron-based superconductor family and has stimulated the continuous exploration of other iron-based materials with new structures and potentially novel properties. In this paper, we report the systematic study of a new quasi-one-dimensional (1D) iron-based compound, Ba9Fe3Te15, including its synthesis and magnetic properties. The high-pressure synthesized Ba9Fe3Te15 crystallized in a hexagonal structure that mainly consisted of face-sharing FeTe6 octahedral chains running along the c axis, with a lattice constant of a = 10.23668 Å; this led to weak interchain coupling and an enhanced one-dimensionality. The systematic static and dynamic magnetic properties were comprehensively studied experimentally. The dc magnetic susceptibility showed typical 1D antiferromagnetic characteristics, with a Tmax at 190 K followed by a spin glass (SG) state with freezing at Tf ≈ 6.0 K, which were also unambiguously proved by ac susceptibility measurements. Additionally, X-ray magnetic circular dichroism (XMCD) experiments revealed an unexpected orbital moment for Fe2+, i.e., 0.84 μB per Fe in Ba9Fe3Te15. The transport property is electrically insulating, with a thermal activation gap of 0.32 eV. These features mark Ba9Fe3Te15 as an alternative type of iron-based compound, providing a diverse candidate for high-pressure studies in order to pursue some emerging physics.

Anomalous and topological Hall effects in epitaxial thin films of the noncollinear antiferromagnet Mn3Sn

Noncollinear antiferromagnets with a D0$_{19}$ (space group = 194, P6$_{3}$/mmc) hexagonal structure have garnered much attention for their potential applications in topological spintronics. Here, we report the deposition of continuous epitaxial thin films of such a material, Mn$_{3}$Sn, and characterize their crystal structure using a combination of x-ray diffraction and transmission electron microscopy. Growth of Mn$_{3}$Sn films with both (0001) c-axis orientation and (40$\bar{4}$3) texture is achieved. In the latter case, the thin films exhibit a small uncompensated Mn moment in the basal plane, quantified via magnetometry and x-ray magnetic circular dichroism experiments. This cannot account for the large anomalous Hall effect simultaneously observed in these films, even at room temperature, with magnitude $\sigma_{\mathrm{xy}}$ ($\mu_{0}H$ = 0 T) = 21 $\mathrm{\Omega}^{-1}\mathrm{cm}^{-1}$ and coercive field $\mu_{0}H_{\mathrm{C}}$ = 1.3 T. We attribute the origin of this anomalous Hall effect to momentum-space Berry curvature arising from the symmetry-breaking inverse triangular spin structure of Mn$_{3}$Sn. Upon cooling through the transition to a glassy ferromagnetic state at around 50 K, a peak in the Hall resistivity close to the coercive field indicates the onset of a topological Hall effect contribution, due to the emergence of a scalar spin chirality generating a real-space Berry phase. We demonstrate that the polarity of this topological Hall effect, and hence the chiral-nature of the noncoplanar magnetic structure driving it, can be controlled using different field cooling conditions.

Nature of the magnetism of iridium in the double perovskite Sr2CoIrO6

We report on our investigation on the magnetism of the iridate double perovskite Sr$_2$CoIrO$_6$, a nominally Ir$^{5+}$ Van Vleck $J_{eff}=0$ system. Using x-ray absorption (XAS) and x-ray magnetic circular dichroism (XMCD) spectroscopy at the Ir-$L_{2,3}$ edges, we found a nearly zero orbital contribution to the magnetic moment and thus an apparent breakdown of the $J_{eff}=0$ ground state. By carrying out also XAS and XMCD experiments at the Co-$L_{2,3}$ edges and by performing detailed full atomic multiplet calculations to simulate all spectra, we discovered that the compound consists of about 90% Ir$^{5+}$ ($J_{eff}=0$) and Co$^{3+}$ ($S=2$) and 10% Ir$^{6+}$ ($S=3/2$) and Co$^{2+}$ ($S=3/2$). The magnetic signal of this minority Ir$^{6+}$ component is almost equally strong as that of the main Ir$^{5+}$ component. We infer that there is a competition between the Ir$^{5+}$-Co$^{3+}$ and the Ir$^{6+}$-Co$^{2+}$ configurations in this stoichiometric compound.

Pressure-induced first-order magnetic phase transition and Yb ordered moment in YbCu2Si2

We report on high-pressure x-ray absorption near edge structure and x-ray magnetic circular dichroism (XMCD) measurements at the Yb ${L}_{3}$ edge on ${\mathrm{YbCu}}_{2}{\mathrm{Si}}_{2}$. This intermetallic is a well-known intermediate valence compound which shows a pressure-induced paramagnetic-ferromagnetic phase transition at about 8 GPa. The pressure dependence of the Yb magnetization has been determined by following the evolution with pressure of the maximum of the dichroic signal at the energy corresponding to the electric quadrupole ($2{p}_{3/2}\ensuremath{-}4f$) transitions. The observed XMCD deduced magnetization curves confirm the ferromagnetic nature of the high-pressure phase as well as the first-order nature of the transition. The Yb ordered moment deduced from XMCD which amounts to about $1.25{\ensuremath{\mu}}_{B}$ at 8.7 GPa and 2.7 K is in very good agreement with the one estimated by M\"ossbauer spectroscopy for the magnetically ordered component of the spectra. This observation indicates that the paramagnetic and ferromagnetic phases coexist only in a narrow pressure range in our XMCD experiment. This is not the case for the M\"ossbauer measurements, which show that the paramagnetic component vanishes only at 20 GPa. Our results clarify the existing discrepancy with dc magnetization measurements that reported values of the Yb moment more than two times smaller. We propose that these apparent contradictory results are due to different experimental conditions which influence the range of coexistence of the paramagnetic and ferromagnetic phases, as found in many similar situations and frequently addressed in the literature.

Soft x-ray spectroscopic endstation at beamline 08U1A of Shanghai Synchrotron Radiation Facility.

A spectroscopic endstation with magnetic field, voltage, and low temperature control has been installed and commissioned at the soft X-ray beamline 08U1A of Shanghai Synchrotron Radiation Facility, which can obtain a magnetic field up to ±0.53 T, applied current and bias voltage, and cryogenic temperatures down to 14 K with a Gifford-McMahon cycle cryocooler. The endstation can perform soft X-ray absorption spectroscopy methods including total electron yield, fluorescence yield, and X-ray excited optical luminance. Combined with an elliptically polarized undulator and the in situ conditions, the endstation can effectively perform X-ray magnetic circular and linear dichroism experiments in the soft X-ray range between photon energies of 250 and 2000 eV.

Microscopic Nature of the First-Order Field-Induced Phase Transition in the Strongly Anisotropic Ferrimagnet HoFe_{5}Al_{7}.

We report on x-ray magnetic circular dichroism experiments in pulsed fields up to 30T to follow the rotations of individual magnetic moments through the field-induced phase transition in the ferrimagnet HoFe_{5}Al_{7}. Near the ground state, we observe simultaneous stepwise rotations of the Ho and Fe moments and explain them using a two-sublattice model for an anisotropic ferrimagnet with weak intersublattice exchange interactions. Near the compensation point, we find two phase transitions. The additional magnetization jump reflects the fact that the Ho moment is no longer rigid as the applied field acts against the intersublattice exchange field.

Enhanced spin–orbit torque via interface engineering in Pt/CoFeB/MgO heterostructures

Spin–orbit torque facilitates efficient magnetisation switching via an in-plane current in perpendicularly magnetised heavy-metal/ferromagnet heterostructures. The efficiency of spin–orbit-torque-induced switching is determined by the charge-to-spin conversion arising from either bulk or interfacial spin–orbit interactions or both. Here, we demonstrate that the spin–orbit torque and the resultant switching efficiency in Pt/CoFeB systems are significantly enhanced by an interfacial modification involving Ti insertion between the Pt and CoFeB layers. Spin pumping and X-ray magnetic circular dichroism experiments reveal that this enhancement is due to an additional interface-generated spin current of the non-magnetic interface and/or improved spin transparency achieved by suppressing the proximity-induced moment in the Pt layer. Our results demonstrate that interface engineering affords an effective approach to improve spin–orbit torque and thereby magnetisation switching efficiency.

Ultralow-temperature device dedicated to soft X-ray magnetic circular dichroism experiments.

A new ultralow-temperature setup dedicated to soft X-ray absorption spectroscopy and X-ray magnetic circular dichroism (XMCD) experiments is described. Two experiments, performed on the DEIMOS beamline (SOLEIL synchrotron), demonstrate the outstanding performance of this new platform in terms of the lowest achievable temperature under X-ray irradiation (T = 220 mK), the precision in controlling the temperature during measurements as well as the speed of the cooling-down and warming-up procedures. Moreover, owing to the new design of the setup, the eddy-current power is strongly reduced, allowing fast scanning of the magnetic field in XMCD experiments; these performances lead to a powerful device for X-ray spectroscopies on synchrotron-radiation beamlines facilities.

Co/Ni multilayers for spintronics: High spin polarization and tunable magnetic anisotropy

In this paper we analyze in details the electronic properties of (Co/Ni) multilayers, a model system for spintronics devices. We use magneto-optical Kerr (MOKE), spin-polarized photoemission spectroscopy (SRPES), x-ray magnetic circular dichroism (XMCD) and anomalous surface diffraction experiments to investigate the electronic properties and perpendicular magnetic anisotropy (PMA) in [Co(x)/Ni(y)] single-crystalline stacks grown by molecular beam epitaxy.

Element-specific observation of the ferromagnetic ordering process in UCoAl via soft x-ray magnetic circular dichroism

We have performed soft x-ray magnetic circular dichroism (XMCD) experiments on the itinerant-electron metamagnet UCoAl at the U $4d\ensuremath{-}5f({N}_{4,5})$ and Co $2p\ensuremath{-}3d({L}_{2,3})$ absorption edges in order to investigate the magnetic properties of the U $5f$ and Co $3d$ electrons separately. From the line shape of the XMCD spectrum, it is deduced that the orbital magnetic moment of the Co $3d$ electrons is unusually large. Through the systematic temperature $(T)$- and magnetic field $(H)$-dependent XMCD measurements, we have obtained two types of the magnetization curve as a function of $H$ and $T$ (M-H curve and M-T curve, respectively). The metamagnetic transition from a paramagnetic state to a field-induced ferromagnetic state was clearly observed under 15 K at ${H}_{\mathrm{M}}$. The value of the ${H}_{\mathrm{M}}$ and its $T$ dependence agree well between the U and Co sites, and the bulk magnetization. Whereas, we have discovered the remarkable differences in the M-H and M-T curves between the U and Co sites. The present findings clearly show that the role of the Co $3d$ electrons should be considered more carefully in order to understand the origin of the magnetic ordering in UCoAl.

Proximity effects across oxide-interfaces of superconductor-insulator-ferromagnet hybrid heterostructure

A case study of electron tunneling or charge-transfer-driven orbital ordering in superconductor (SC)-ferromagnet (FM) interfaces has been conducted in heteroepitaxial YBa2Cu3O7(YBCO)/La0.67Sr0.33MnO3(LSMO) multilayers interleaved with and without an insulating SrTiO3(STO) layer between YBCO and LSMO. X-ray magnetic circular dichroism experiments revealed anti-parallel alignment of Mn magnetic moments and induced Cu magnetic moments in a YBCO/LSMO multilayer. As compared to an isolated LSMO layer, the YBCO/LSMO multilayer displayed a (50%) weaker Mn magnetic signal, which is related to the usual proximity effect. It was a surprise that a similar proximity effect was also observed in a YBCO/STO/LSMO multilayer, however, the Mn signal was reduced by 20%. This reduced magnetic moment of Mn was further verified by depth sensitive polarized neutron reflectivity. Electron energy loss spectroscopy experiment showed the evidence of Ti magnetic polarization at the interfaces of the YBCO/STO/LSMO multilayer. This crossover magnetization is due to a transfer of interface electrons that migrate from Ti(4+)−δ to Mn at the STO/LSMO interface and to Cu2+ at the STO/YBCO interface, with hybridization via O 2p orbitals. So charge-transfer driven orbital ordering is the mechanism responsible for the observed proximity effect and Mn-Cu anti-parallel coupling in YBCO/STO/LSMO. This work provides an effective pathway in understanding the aspect of long range proximity effect and consequent orbital degeneracy parameter in magnetic coupling.