X-ray Magnetic Circular Dichroism Measurements Research Articles

Magnetic properties of the (Mo2/3R1/3)2AlC (R=Ho,Dy) i−MAX phases studied by x-ray magnetic circular dichroism and neutron diffraction

We report on the magnetic properties of single crystals of Ho- and Dy-based ${({\mathrm{Mo}}_{2/3}{R}_{1/3})}_{2}\mathrm{AlC} i\text{\ensuremath{-}}\mathrm{MAX}$ phases. In these nanolamellar compounds, where planes of $R$ and Mo arranged in a skewed triangular lattice are separated by planes of Al and C, geometrical frustration and magnetic exchange interactions lead to complex magnetic properties. Temperature-dependent bulk magnetization, specific heat, and resistivity measurements reveal two magnetic phase transitions in Dy $i\text{\ensuremath{-}}\mathrm{MAX}$ (15 and 12 K) and only one in Ho $i\text{\ensuremath{-}}\mathrm{MAX}$ (8.5 K). Strong magnetic anisotropy and metamagnetic transitions with a step at $\frac{1}{3}$ of saturation moment along the crystal $a$ axis are observed in field-dependent bulk magnetization curves. X-ray magnetic circular dichroism measurements unveil induced moments on Mo and Al, and a quantitative estimation of the orbital and spin moments of Mo based on magneto-optical sum rules suggests an unusual interaction between the $R 4f$ and the Mo $4d$ magnetic moments. Magnetic structures are derived from neutron diffraction measurements, revealing a zero-field incommensurate amplitude modulated order in both compounds, followed by an antiferromagnetic equal-moments structure at lower temperature for Dy $i\text{\ensuremath{-}}\mathrm{MAX}$. The bulk magnetization $\frac{1}{3}$ step is found to be linked to the flip of one $R$ moment out of three within the planes. Detailed phase diagrams for Ho and Dy $i\text{\ensuremath{-}}\mathrm{MAX}$ are derived from these measurements.

Study on FeCr thin film for a spintronic material with negative spin polarization

Negative spin polarization materials generate a spin current whose spin direction is opposite to the magnetization direction. This characteristic is technologically important because it increases the freedom in the design of spintronic devices. In this paper, we studied FeCr from the viewpoints of band structure, atomic magnetic moments, and local atomic arrangement to explore its potentiality as a negative spin polarization material. First-principles calculations on the disordered FeCr alloy predicted a high negative spin polarization, which was attributed to the band matching of the minority spin. We experimentally fabricated Fe1-xCrx thin films in the Cr concentration (x) range from 0.2 to 0.4 by sputter deposition and demonstrated inverse magnetoresistance using current-perpendicular-to-plane giant magnetoresistance (GMR) devices, which provided evidence of negative spin polarization. The spin polarization of Fe0.7Cr0.3 estimated from the GMR device measurements was −0.28 and fell below the calculated value. Synchrotron X-ray magnetic circular dichroism measurements showed a ferrimagnetic configuration of the Fe and Cr magnetic moments. The Fe moment showed a large moment over a wide Cr concentration range, whereas the Cr moment decreased with the Cr concentration, which agreed with the calculation result. Synchrotron Mössbauer spectroscopy measurements indicated the inhomogeneity of the FeCr composition even in the as-deposited state. Fe-rich regions were formed after annealing, reflecting the phase separation nature of the Fe-Cr system. Inhomogeneity was not considered in the calculation and could be the origin of the smaller negative spin polarization observed in the experiment.

Spark plasma sintering-assisted synthesis and high-Tc ferromagnetism of Mn-doped SiGe alloys

In this work, Mn-doped SiGe alloys with high Curie-temperature (TC) ferromagnetism are synthesized via spark plasma sintering (SPS). The structural characterizations indicate that the Mn-doped samples are composed of strained Si0.25Ge0.75 crystals due to the incorporation of substitutional Mn dopants in the SiGe lattice. The magnetization characterizations and X-ray magnetic circular dichroism (XMCD) measurements show that the Mn-doped samples exhibit Mn concentration-dependent ferromagnetism up to room temperature, owing to the spin and orbit magnetic moment contribution from the substitutional Mn acceptors. Furthermore, the magneto-transport measurements reveal anomalous Hall effect and complex magnetoresistance in the ferromagnetic Mn-doped samples. This study gives insight into the fabrication and magnetic properties of Mn-doped SiGe alloys prepared by SPS and may be useful for related spintronic applications.

Origin of Magnetization in Silica-coated Fe3O4 Nanoparticles Revealed by Soft X-ray Magnetic Circular Dichroism

Magnetite (Fe3O4) nanoparticles (NPs) and SiO2-coated Fe3O4 nanoparticles have successfully been synthesized using co-precipitation and modified Stöber methods, respectively. The samples were characterized using X-ray diffraction (XRD), Fourier transform infrared (FTIR) spectroscopy, high-resolution transmission electron microscopy (HRTEM), vibrating sample magnetometer (VSM) techniques, X-ray absorption spectroscopy (XAS), and X-ray magnetic circular dichroism (XMCD). XRD and FTIR data confirmed the structural configuration of a single-phase Fe3O4 and the successful formation of SiO2-coated Fe3O4 NPs. XRD also confirmed that we have succeeded to synthesize nano-meter size of Fe3O4 NPs. HRTEM images showed the increasing thickness of SiO2-coated Fe3O4 with the addition of the Tetraethyl Orthosilicate (TEOS). Room temperature VSM analysis showed the magnetic behaviour of Fe3O4 and its variations that occurred after SiO2 coating. The magnetic behaviour is further authenticated by XAS spectra analysis which cleared about the existence of SiO2 shells that have transformed the crystal as well as the local structures of the magnetite NPs. We have performed XMCD measurements, which is a powerful element-specific technique to find out the origin of magnetization in SiO2-coated Fe3O4 NPs, that verified a decrease in magnetization with increasing thickness of the SiO2 coating.Graphical Magnetite (Fe3O4) nanoparticles (NPs) and SiO2-coated Fe3O4 nanoparticles have successfully been synthesized using co-precipitation and modified Stöber methods, respectively. The samples were characterized using X-ray diffraction (XRD), Fourier transform infrared (FTIR) spectroscopy, high-resolution transmission electron microscopy (HRTEM), vibrating sample magnetometer (VSM) techniques, X-ray absorption spectroscopy (XAS), and X-ray magnetic circular dichroism (XMCD). XRD and FTIR data confirmed the structural configuration of a single-phase Fe3O4 and the successful formation of SiO2-coated Fe3O4 NPs. XRD also confirmed that we have succeeded to synthesize nano-meter size of Fe3O4 NPs. HRTEM images showed the increasing thickness of SiO2-coated Fe3O4 with the addition of the Tetraethyl Orthosilicate (TEOS). Room temperature VSM analysis showed the magnetic behaviour of Fe3O4 and its variations that occurred after SiO2 coating. The magnetic behaviour is further authenticated by XAS spectra analysis which cleared about the existence of SiO2 shells that have transformed the crystal as well as the local structures of the magnetite NPs. We have performed XMCD measurements, which is a powerful element-specific technique to find out the origin of magnetization in SiO2-coated Fe3O4 NPs, that verified a decrease in magnetization with increasing thickness of the SiO2 coating.

Strain-engineering of magnetic anisotropy in CoxNi1−x−SrTiO3/SrTiO3 (001) vertically assembled nanocomposites

Ultrathin ${\mathrm{Co}}_{x}{\mathrm{Ni}}_{1\ensuremath{-}x}$ alloy nanowires vertically embedded in ${\mathrm{SrTiO}}_{3}/{\mathrm{SrTiO}}_{3}\phantom{\rule{0.16em}{0ex}}(001)$ thin films were grown using a self-assembly approach based on sequential pulsed laser deposition. Due to vertical epitaxial coupling of the metallic and oxide phases, a large average tensile strain of up to 4% arises within the nanowires, which is evidenced using a combination of x-ray diffraction and transmission electron microscopy. Macroscopic magnetometry experiments are used to demonstrate that this huge deformation allows us to enhance the uniaxial anisotropy of the nanowires, leading to saturation field in excess of 1 T in the hard direction, large coercive field at low temperature along the easy axis, and to a blocking temperature exceeding 600 K in the case of nanowires with a diameter of 5 nm and 78% Co content. These data are complemented with angular dependent x-ray magnetic circular dichroism measurements at the Co and Ni ${L}_{2,3}$ edges. The value of the magnetic moment was extracted from these measurements by applying sum rules and the anisotropy of the orbital moment was investigated.

Van der Waals epitaxy growth of 2D ferromagnetic Cr(1+δ)Te2 nanolayers with concentration-tunable magnetic anisotropy

Cr(1+δ)Te2 are pseudo-layered compounds consisting of CrTe2 transition metal dichalcogenide (TMD) layers with additional (δ) self-intercalated Cr atoms. The recent search for ferromagnetic 2D materials revived the interest into chromium tellurides. Here, Cr(1+δ)Te2 nanolayers are epitaxially grown on MoS2 (0001), forming prototypical van der Waals heterostructures. Under optimized growth conditions, ultrathin films of only two TMD layers with a single intercalated Cr-layer are achieved, forming a 2D sheet with van der Waals surfaces. Detailed compositional and structural characterization by scanning tunneling microscopy, grazing incidence x-ray diffraction, and high-resolution Rutherford backscattering indicate the layer-by-layer growth and that the δ can be tuned by post-growth annealing in a range between ∼0.5 and 1. X-ray magnetic circular dichroism and magnetometry measurements demonstrate that all self-intercalated Cr(1+δ)Te2 nanolayers exhibit strong ferromagnetism with magnetic moments larger than 3μB per Cr-atom. The magnetic properties are maintained in the ultrathin limit of a material with a single intercalation layer. Interestingly, the magnetic anisotropy can be tuned from close to isotropic (δ = 1) to a desirable perpendicular anisotropy for low δ values. Thus, the bottom-up growth of these 2D Cr(1+δ)Te2 sheets is a promising approach for designing magnetic van der Waals heterostructures.

Cationic Ordering and Its Influence on the Magnetic Properties of Co-Rich Cobalt Ferrite Thin Films Prepared by Reactive Solid Phase Epitaxy on Nb-Doped SrTiO3(001).

Here, we present the (element-specific) magnetic properties and cation ordering for ultrathin Co-rich cobalt ferrite films. Two Co-rich films with different stoichiometry ( and ) have been formed by reactive solid phase epitaxy due to post-deposition annealing from epitaxial CoO/FeO bilayers deposited before on Nb-doped SrTiO(001). The electronic structure, stoichiometry and homogeneity of the cation distribution of the resulting cobalt ferrite films were verified by angle-resolved hard X-ray photoelectron spectroscopy. From X-ray magnetic circular dichroism measurements, the occupancies of the different sublattices were determined using charge-transfer multiplet calculations. For both ferrite films, a partially inverse spinel structure is found with increased amount of cations in the low-spin state on octahedral sites for the film. These findings concur with the results obtained by superconducting quantum interference device measurements. Further, the latter measurements revealed the presence of an additional soft magnetic phase probably due to cobalt ferrite islands emerging from the surface, as suggested by atomic force microscope measurements.

Ferrimagnetic–ferromagnetic phase transition in Mn4N films favored by non-magnetic In doping

The ferrimagnet Mn4N forms a family of compounds useful in spintronics. In a compound comprising non-magnetic and magnetic elements, one basically expects the compound to become ferromagnetic when the proportion of the magnetic element increases. Conversely, one does not expect ferromagnetism when the proportion of the non-magnetic element increases. Surprisingly, Mn4N becomes ferromagnetic at room temperature when the Mn content is decreased by the addition of In atoms, a non-magnetic element. X-ray magnetic circular dichroism measurement reveals that the magnetic moment of Mn atoms at face-centered sites, Mn(II), reverses between x= 0.15 and 0.27 and aligns parallel to that of Mn atoms at corner sites, Mn(I), at x = 0.27 and 0.41. The sign of the anomalous Hall resistivity also changes between x = 0.15 and 0.27 in accordance with the reversal of the magnetic moment of the Mn(II) atoms. These results can be interpreted using first-principles calculations, showing that the magnetic moment of Mn(II) sites which are the nearest neighbors to the In atom align to that of Mn(I) sites.

Integration of epitaxial La2/3Sr1/3MnO3 thin films on silicon-on-sapphire substrate for MEMS applications

We report the integration of high-quality epitaxial La2/3Sr1/3MnO3 (LSMO) thin films onto SrTiO3 buffered Silicon-on-Sapphire (SOS) substrates by combining state-of-the-art thin film growth techniques such as molecular beam epitaxy and pulsed laser deposition. Detailed structural, magnetic and electrical characterizations of the LSMO/STO/SOS heterostructures show that the LSMO film properties are competitive with those directly grown on oxide substrates. X-ray magnetic circular dichroism measurements on Mn L2,3 edges show strong dichroic signal at room temperature, and angular-dependent in-plane magnetic properties by magneto-optical Kerr magnetometry reveal isotropic magnetic anisotropy. Suspended micro-bridges were thus finally fabricated by silicon micromachining, thus demonstrating the potential use of integrating LSMO magnetic layer on industrially compatible SOS substrates for the development of applicative MEMS devices.

Single-domain perpendicular magnetization induced by the coherent O 2p -Ru 4d hybridized state in an ultra-high-quality SrRuO3 film

We investigated the Ru $4d$ and O $2p$ electronic structure and magnetic properties of an ultrahigh-quality $\mathrm{SrRu}{\mathrm{O}}_{3}$ film on $\mathrm{SrTi}{\mathrm{O}}_{3}$ grown by machine-learning assisted molecular-beam epitaxy. The high itinerancy and long quantum lifetimes of the quasiparticles in the Ru $4d$ ${t}_{2g}$-O $2p$ hybridized valence band are confirmed by observing the prominent well-screened peak in the Ru $3d$ core-level photoemission spectrum, the coherent peak near the Fermi energy in the valence-band spectrum, and quantum oscillations in the resistivity. The element-specific magnetic properties and the hybridization between the Ru $4d$ and O $2p$ orbitals were characterized by Ru ${M}_{2,3}$-edge and O $K$-edge soft x-ray absorption spectroscopy and x-ray magnetic circular dichroism measurements. The ultrahigh-quality $\mathrm{SrRu}{\mathrm{O}}_{3}$ film with the residual resistivity ratio of 86 shows the large orbital magnetic moment of oxygen ions induced by the strong orbital hybridization of the O $2p$ states with the spin-polarized Ru $4d$ ${t}_{2g}$ states. The film also shows single-domain perpendicular magnetization with an almost ideal remanent magnetization ratio of 0.97. These results provide detailed insights into the relevance between orbital hybridization and the perpendicular magnetic anisotropy in $\mathrm{SrRu}{\mathrm{O}}_{3}/\mathrm{SrTi}{\mathrm{O}}_{3}$ systems.

Intrinsic 2D-XY ferromagnetism in a van der Waals monolayer.

The physics and universality scaling of phase transitions in low-dimensional systems has historically been a topic of great interest. Recently, two-dimensional (2D) materials exhibiting intriguing long-range magnetic order have been in the spotlight. Although an out-of-plane anisotropy has been shown to stabilize 2D magnetic order, the demonstration of a 2D magnet with in-plane rotational symmetry has remained elusive. We constructed a nearly ideal easy-plane system, a single CrCl3 monolayer on graphene/6H-SiC(0001), and observed robust ferromagnetic ordering with critical scaling characteristic of a 2D-XY system. These observations indicate the realization of a finite-size Berezinskii-Kosterlitz-Thouless phase transition in a large-area, quasi–free-standing van der Waals monolayer magnet with an XY universality class. This offers a material platform to host 2D superfluid spin transport and topological magnetic textures.

Proximity-induced magnetism and the enhancement of damping in ferromagnetic/heavy metal systems

The relationship between proximity-induced magnetism (PIM) at the heavy metal/ferromagnet interface and spin-transport across such interfaces has generated significant debate. To investigate the link between the two, element specific x-ray magnetic circular dichroism and ferromagnetic resonance measurements were made on the same CoFe/Au/Pt and NiFe/Au/Pt thin film samples with varying Au thickness, with complementary SIMS analysis, which shows evidence of Ni diffusion from NiFe into the Pt. An approximately linear relationship is observed between the magnitude of Pt PIM and magnitude of damping enhancement in both systems. The results demonstrate that electronic hybridization of the heavy metal and ferromagnet is required for a full understanding of damping enhancement and interfacial spin-transport for spintronic devices.

Room Temperature Ferromagnetism of Monolayer Chromium Telluride with Perpendicular Magnetic Anisotropy.

The realization of long-range magnetic ordering in 2D systems can potentially revolutionize next-generation information technology. Here, the successful fabrication of crystalline Cr3 Te4 monolayers with room temperature (RT) ferromagnetism is reported. Using molecular beam epitaxy, the growth of 2D Cr3 Te4 films with monolayer thickness is demonstrated at low substrate temperatures (≈100 °C), compatible with Si complementary metal oxide semiconductor technology. X-ray magnetic circular dichroism measurements reveal a Curie temperature (Tc ) of v344 K for the Cr3 Te4 monolayer with an out-of-plane magnetic easy axis, which decreases to v240 K for the thicker film (≈7nm) with an in-plane easy axis. The enhancement of ferromagnetic coupling and the magnetic anisotropy transition is ascribed to interfacial effects, in particular the orbital overlap at the monolayer Cr3 Te4 /graphite interface, supported by density-functional theory calculations. This work sheds light on the low-temperature scalable growth of 2D nonlayered materials with RT ferromagnetism for new magnetic and spintronic devices.

Present Status of Rare-earth Free Ferrimagnet Mn4N and Future Prospects of Mn4N-based Compensated Ferrimagnets

The rare-earth-free ferrimagnet Mn4N has attractive features for spintronics applications, because it possesses a perpendicular magnetization, due to a relatively large magnetic anisotropy constant of ∼105 J m−3 and a small spontaneous magnetization of ∼100 kA m−1, and a large spin polarization (P = 0.8). More crucially, it is possible to reach the magnetic compensation at room temperature, by tuning its constituent elements in compounds such as Mn4−xNixN and Mn4−xCoxN. This is particularly interesting for spin-torque-based spintronics applications, because at the vicinity of the magnetization and/or angular momentum compensation points, the switching currents can be reduced significantly, thereby leading to lower switching energies and higher switching speed. In this review article, we emphasize the importance of epitaxial growth of Mn4N films by comparing the results obtained on two different substrates, MgO(001) and SrTiO3(001). We then present the achievement of ultrafast current-induced domain wall motion (CIDWM) in Mn4N microstrips, and study the magnetic compensations in Mn4−xNixN and Mn4−xCoxN at room temperature, proved by x-ray magnetic circular dichroism measurements. Finally, we offer future prospects for such Mn4N-based compensated

Diverse Structures and Magnetic Properties in Nonlayered Monolayer Chromium Selenide.

Thickness-dependent magnetic behavior has previously been observed in chemical vapor deposition-grown chromium selenide. However, the low-dimensional structure in nonlayered chromium selenide, which plays a crucial role in determining the low-dimensional magnetic order, needs further study. Here, we report the structure-dependent magnetic properties in monolayer CrSe2 and Cr2Se3 grown by molecular beam epitaxy. In the monolayer CrSe2, 1T-CrSe2 with a lattice constant of 3.3 Å has a metallic character, coexisting with the 1T″ phase with 2 × 2 surface periodicity. Monolayer CrSe2 can be transformed into Cr2Se3 with a lattice constant of 3.6 Å by annealing at 300 °C. X-ray magnetic circular dichroism (XMCD) measurements combined with DFT calculations reveal that while the MBE-grown monolayer CrSe2 is antiferromagnetic, monolayer Cr2Se3 is ferromagnetic with a Curie temperature of ∼200 K. This work demonstrates the structural diversity in nonlayered chromium selenide and the critical effect of different structures on its electronic and magnetic properties.

Voltage control of ferrimagnetic order and voltage-assisted writing of ferrimagnetic spin textures.

Voltage control of magnetic order is desirable for spintronic device applications, but 180° magnetization switching is not straightforward because electric fields do not break time-reversal symmetry. Ferrimagnets are promising candidates for 180° switching owing to a multi-sublattice configuration with opposing magnetic moments of different magnitudes. In this study we used solid-state hydrogen gating to control the ferrimagnetic order in rare earth-transition metal thin films dynamically. Electric field-induced hydrogen loading/unloading in GdCo can shift the magnetic compensation temperature by more than 100 K, which enables control of the dominant magnetic sublattice. X-ray magnetic circular dichroism measurements and ab initio calculations indicate that the magnetization control originates from the weakening of antiferromagnetic exchange coupling that reduces the magnetization of Gd more than that of Co upon hydrogenation. We observed reversible, gate voltage-induced net magnetization switching and full 180° Néel vector reversal in the absence of external magnetic fields. Furthermore, we generated ferrimagnetic spin textures, such as chiral domain walls and skyrmions, in racetrack devices through hydrogen gating. With gating times as short as 50 μs and endurance of more than 10,000 cycles, our method provides a powerful means to tune ferrimagnetic spin textures and dynamics, with broad applicability in the rapidly emerging field of ferrimagnetic spintronics.

Probing exchange bias at the surface of a doped ferrimagnetic insulator

With the realization of stress-induced perpendicular magnetic anisotropy, efficient spin-orbit torque switching, and room temperature topological Hall effect, interest in rare earth iron garnets has been revived in recent years for their potential in spintronic applications. In this study, we investigate the magnetic properties of micrometer-thick Bi and Ga substituted thulium iron garnets (BiGa:TmIG) grown by the liquid-phase epitaxy method. Above the magnetization compensation (MC) temperature, anomalous triple hysteresis is observed in BiGa:TmIG/Pt heterostructures by anomalous Hall effect measurements. X-ray magnetic circular dichroism and energy dispersive spectroscopy measurements reveal its origin as an internal exchange bias (EB) effect arising from inhomogeneities localized at the surface of the film. Possibly depending on the difference in thickness and defect realization of the EB layer, two types of magnetization reversal mechanisms, namely, the Stoner-Wohlfarth type and the reversible domain-wall motion type, are observed. Our results show that rich meta-magnetic phases exist in garnets close to MC, which can be robustly tuned by chemical composition engineering and conveniently probed by electrical transport measurements.

Microstructures and Interface Magnetic Moments in Mn2VAl/Fe Layered Films Showing Exchange Bias.

Heusler alloys are a material class exhibiting various magnetic properties, including antiferromagnetism. A typical application of antiferromagnets is exchange bias that is a shift of the magnetization curve observed in a layered structure consisting of antiferromagnetic and ferromagnetic films. In this study, a layered sample consisting of a Heusler alloy, MnVAl and a ferromagnet, Fe, is selected as a material system exhibiting exchange bias. Although the fully ordered MnVAl is known as a ferrimagnet, with an optimum fabrication condition for the MnVAl layer, the MnVAl/Fe layered structure exhibits exchange bias. The appearance of the antiferromagnetic property in the MnVAl is remarkable; however, the details have been unclear. To clarify the microscopic aspects on the crystal structures and magnetic moments around the MnVAl/Fe interface, cross-sectional scanning transmission electron microscope (STEM) observation, and synchrotron soft X-ray magnetic circular dichroism (XMCD) measurements were employed. The high-angle annular dark-field STEM images demonstrated clusters of MnVAl with the L2 phase distributed only around the interface to the Fe layer in the sample showing the exchange bias. Furthermore, antiferromagnetic coupling between the Mn- and Fe-moments were observed in element-specific hysteresis loops measured using the XMCD. The locally ordered L2 phase and antiferromagnetic Mn-moments in the MnVAl were suggested as important factors for the exchange bias.

Tunable room-temperature ferromagnetism in Co-doped two-dimensional van der Waals ZnO

The recent discovery of ferromagnetism in two-dimensional van der Waals crystals has provoked a surge of interest in the exploration of fundamental spin interaction in reduced dimensions. However, existing material candidates have several limitations, notably lacking intrinsic room-temperature ferromagnetic order and air stability. Here, motivated by the anomalously high Curie temperature observed in bulk diluted magnetic oxides, we demonstrate room-temperature ferromagnetism in Co-doped graphene-like Zinc Oxide, a chemically stable layered material in air, down to single atom thickness. Through the magneto-optic Kerr effect, superconducting quantum interference device and X-ray magnetic circular dichroism measurements, we observe clear evidences of spontaneous magnetization in such exotic material systems at room temperature and above. Transmission electron microscopy and atomic force microscopy results explicitly exclude the existence of metallic Co or cobalt oxides clusters. X-ray characterizations reveal that the substitutional Co atoms form Co2+ states in the graphitic lattice of ZnO. By varying the Co doping level, we observe transitions between paramagnetic, ferromagnetic and less ordered phases due to the interplay between impurity-band-exchange and super-exchange interactions. Our discovery opens another path to 2D ferromagnetism at room temperature with the advantage of exceptional tunability and robustness.

Large Orbital Magnetic Moment and Strong Perpendicular Magnetic Anisotropy in Heavily Intercalated FexTiS2

Titanium disulfide TiS$_2$, which is a member of the layered transition-metal dichalcogenides with the 1T-CdI$_2$-type crystal structure, is known to exhibit a wide variety of magnetism through intercalating various kinds of transition-metal atoms of different concentrations. Among them, Fe-intercalated titanium disulfide Fe$_x$TiS$_2$ is known to be ferromagnetic with strong perpendicular magnetic anisotropy (PMA) and large coercive fields ($H_\text{c}$). In order to study the microscopic origin of the magnetism of this compound, we have performed X-ray absorption spectroscopy (XAS) and X-ray magnetic circular dichroism (XMCD) measurements on single crystals of heavily intercalated Fe$_x$TiS$_2$ ($x\sim0.5$). The grown single crystals showed a strong PMA with a large $H_\text{c}$ of $\mu_0H_\text{c} \simeq 1.0\ \text{T}$. XAS and XMCD spectra showed that Fe is fully in the valence states of 2+ and that Ti is in an itinerant electronic state, indicating electron transfer from the intercalated Fe atoms to the host TiS$_2$ bands. The Fe$^{2+}$ ions were shown to have a large orbital magnetic moment of $\simeq 0.59\ \mu_\text{B}\text{/Fe}$, to which, combined with the spin-orbit interaction and the trigonal crystal field, we attribute the strong magnetic anisotropy of Fe$_x$TiS$_2$.