arXiv subjects

Goro Shibata

Publications and source records attributed to Goro Shibata.

At least 19 recordsLinked to original sources

arXiv2026

CE-antiferromagnetic electronic structure in LaSr$_2$Mn$_2$O$_7$ revealed by micro-focused angle-resolved photoemission spectroscopy and tight-binding models

We have investigated the electronic structure of LaSr$_2$Mn$_2$O$_7$ in the CE-type antiferromagnetic (CE-AFM) state below the N\'eel temperature using micro-focused angle-resolved photoemission spectroscopy ($\mu$-ARPES) and tight-binding models. In agreement with the tight-binding calculations, we found a dispersive intensity around the X point in the $\mu$-ARPES spectra, where the A-type antiferromagnetic (A-AFM) phase has no bands experimentally and theoretically, demonstrating that we have successfully captured the signatures of the CE-AFM band structure for the first time. Many observed features can be explained by the CE-AFM tight-binding bands, although some of them and the overall near-Fermi level intensity mapping can be explained by the A-AFM band structure. This indicates that the CE-AFM domain size would be no larger than the beam footprint size of a $\sim\!20$~{\textmu}m scale.

cond-mat.str-el↗

arXiv2025

Fe contribution to the magnetic anisotropy of $L{1_0}$-ordered FePt thin films studied by angle-dependent x-ray magnetic circular dichroism

Among magnetic thin films with perpendicular magnetic anisotropy (PMA), $L1_0$-ordered FePt has attracted significant attention because of its exceptionally strong PMA. However, the microscopic origin of its strong PMA has not been elucidated experimentally. We have investigated the contribution of the Fe $3d$ electrons to its magnetic anisotropy energy by angle-dependent x-ray magnetic circular dichroism at the Fe $L_{2,3}$ edge. By this technique, one can deduce the magnetic dipole moment $m_\text{T}$, which represents the anisotropic spatial distribution of spin-polarized electrons, and the orbital moment anisotropy (OMA) of Fe $3d$ electrons. Detected finite $m_\text{T}$ indicates that the spin-polarized Fe $3d$ electrons are distributed preferentially in the out-of-plane direction of the films. This $m_\text{T}$ of Fe overwhelms the positive contribution of OMA to PMA, and reduces the PMA of $L1_0$-ordered FePt thin films, consistent with a previous first-principles calculation. The present result implies that a large positive contribution of the non-magnetic element Pt rather than Fe governs the PMA of $L1_0$-ordered FePt thin films.

cond-mat.mtrl-sci↗

arXiv2025

Possibility of ferro-octupolar order in Ba$_2$CaOsO$_6$ assessed by X-ray magnetic dichroism measurements

Localized $5d^2$ electrons in a cubic crystal field possess multipoles such as electric quadrupoles and magnetic octupoles. We studied the cubic double perovskite Ba$_2$CaOsO$_6$ containing the Os$^{6+}$ ($5d^2$) ions, which exhibits a phase transition to a `hidden order' below $T^* \sim$ 50 K, by X-ray absorption spectroscopy (XAS) and X-ray magnetic circular dichroism (XMCD) at the Os $L_{2,3}$ edge. The cubic ligand-field splitting between the $t_{2g}$ and $e_g$ levels of Os $5d$ was deduced by XAS to be $\sim$4 eV. Ligand-field (LF) multiplet calculation under fictitious strong magnetic fields indicated that the exchange interaction between nearest-neighbor octupoles should be as strong as $\sim$1.5 meV if a ferro-octupolar order is stabilized in the `hidden-ordered' state, consistent with the exchange interaction of $\sim$1 meV previously predicted theoretically using model and density functional theory calculations. The temperature dependence of the XMCD spectra was consistent with a $\sim$18 meV residual cubic splitting of the lowest $J_{\rm eff} =$ 2 multiplet state into the non-Kramers $E_g$ doublet ground state and the $T_{2g}$ triplet excited state.

cond-mat.str-el↗

arXiv2024

On the relationship between orbital moment anisotropy, magnetocrystalline anisotropy, and Dzyaloshinskii-Moriya interaction in W/Co/Pt trilayers

We have studied the Co layer thickness dependences of magnetocrystalline anisotropy (MCA), Dzyaloshinskii-Moriya interaction (DMI), and orbital moment anisotropy (OMA) in W/Co/Pt trilayers, in order to clarify their correlations with each other. We find that the MCA favors magnetization along the film normal and monotonically increases with decreasing effective magnetic layer thickness ($t_\mathrm{eff}$). The magnitude of the Dzyaloshinskii-Moriya exchange constant ($|D|$) increases with decreasing $t_\mathrm{eff}$ until $t_\mathrm{eff} \sim$1 nm, below which $|D|$ decreases. The MCA and $|D|$ scale with $1/t_\mathrm{eff}$ for $t_\mathrm{eff}$ larger than $\sim$1 nm, indicating an interfacial origin. The increase of MCA with decreasing $t_\mathrm{eff}$ continues below $t_\mathrm{eff}$ $\sim$ 1 nm, but with a slower rate. To clarify the cause of the $t_\mathrm{eff}$ dependences of MCA and DMI, the OMA of Co in W/Co/Pt trilayers is studied using x-ray magnetic circular dichroism (XMCD). We find non-zero OMA when $t_\mathrm{eff}$ is smaller than $\sim$0.8 nm. The OMA increases with decreasing $t_\mathrm{eff}$ more rapidly than what is expected from the MCA, indicating that factors other than OMA contribute to the MCA at small $t_\mathrm{eff}$. The $t_\mathrm{eff}$ dependence of the OMA also suggests that $|D|$ at $t_\mathrm{eff}$ smaller than $\sim$1 nm is not related to the OMA at the interface. We propose that the growth of Co on W results in a strain and/or texture that reduces the interfacial DMI, and, to some extent, MCA at small $t_\mathrm{eff}$.

cond-mat.mtrl-sci↗

arXiv2023

Origin of magnetically dead layers in spinel ferrites $M\text{Fe}_2\text{O}_4$ grown on $\text{Al}_2\text{O}_3$: Effects of post-deposition annealing studied by XMCD

We study the electronic and magnetic states of as-grown and annealed $M\text{Fe}_2\text{O}_4$(111)/$\text{Al}_2\text{O}_3$(111) ($M=\text{Co, Ni}$) thin films with various thicknesses grown on Si(111) substrates with the $γ$-$\text{Al}_2\text{O}_3$(111) buffer layers by using x-ray absorption spectroscopy (XAS) and x-ray magnetic circular dichroism (XMCD), to investigate magnetically dead layers in these films. Although the magnetically dead layers in the as-grown samples are formed near the interface with the $\text{Al}_2\text{O}_3$ buffer layer, we reveal that ferrimagnetic order is partially recovered by post-deposition annealing at 973 K for 48 hours in air. By analyzing the line shapes of the XAS and XMCD spectra, we conclude that, in the dead layers, there are a significant number of vacancies at the $T_d$ sites of the spinel structure, which may be the microscopic origin of the degraded ferrimagnetic order in the $M\text{Fe}_2\text{O}_4$(111) thin films.

cond-mat.mtrl-sci↗

arXiv2021

Reduced magnetocrystalline anisotropy of CoFe$_2$O$_4$ thin films studied by angle-dependent x-ray magnetic circular dichroism

Spinel-type CoFe$_2$O$_4$ is a ferrimagnetic insulator with the Néel temperature exceeding 790 K, and shows a strong cubic magnetocrystalline anisotropy (MCA) in bulk materials. However, when a CoFe$_2$O$_4$ film is grown on other materials, its magnetic properties are degraded so that so-called magnetically dead layers are expected to be formed in the interfacial region. We investigate how the magnetic anisotropy of CoFe$_2$O$_4$ is modified at the interface of CoFe$_2$O$_4$/Al$_2$O$_3$ bilayers grown on Si(111) using x-ray magnetic circular dichroism (XMCD). We find that the thinner CoFe$_2$O$_4$ films have significantly smaller MCA values than bulk materials. The reduction of MCA is explained by the reduced number of Co$^{2+}$ ions at the $O_h$ site reported by a previous study [Y. K. Wakabayashi $\textit{et al.}$, Phys. Rev. B $\textbf{96}$, 104410 (2017)].

cond-mat.mtrl-sci↗

arXiv2021

Large Orbital Magnetic Moment and Strong Perpendicular Magnetic Anisotropy in Heavily Intercalated Fe$_{x}$TiS$_2$

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 $μ_0H_\text{c} \simeq 1.0\ \text{T}$. 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 $\simeq 0.59\ μ_\text{B}\text{/Fe}$, to which, combined with the spin-orbit interaction and the trigonal crystal field, we attribute the strong magnetic anisotropy of Fe$_x$TiS$_2$.

cond-mat.mtrl-sci↗

arXiv2020

Anisotropic spin distribution and perpendicular magnetic anisotropy in the layered ferromagnetic semiconductor (Ba,K)(Zn,Mn)$_{2}$As$_{2}$

Perpendicular magnetic anisotropy of the new ferromagnetic semiconductor (Ba,K)(Zn,Mn)$_{2}$As$_{2}$ is studied by angle-dependent x-ray magnetic circular dichroism measurements. The large magnetic anisotropy with the anisotropy field of 0.85 T is deduced by fitting the Stoner-Wohlfarth model to the magnetic-field-angle dependence of the projected magnetic moment. Transverse XMCD spectra highlights the anisotropic distribution of Mn 3$d$ electrons, where the $d_{xz}$ and $d_{yz}$ orbitals are less populated than the $d_{xy}$ state because of the $D_{2d}$ splitting arising from the elongated MnAs$_{4}$ tetrahedra. It is suggested that the magnetic anisotropy originates from the degeneracy lifting of $p$-$d_{xz}$, $d_{yz}$ hybridized states at the Fermi level and resulting energy gain due to spin-orbit coupling when spins are aligned along the $z$ direction.

cond-mat.str-el↗

arXiv2020

Temperature evolution of magnetic phases near the thickness-dependent metal-insulator transition in La$_{1-x}$Sr$_x$MnO$_3$ thin films observed by XMCD

Perovskite-type manganites, which are well-known for their intriguing physical properties such as colossal magnetoresistance (CMR) and half metalicity, have been considered as candidate materials for spintronics. However, their ferromagnetic (FM) properties are often suppressed in thin films when the thickness is reduced down to several monolayers (MLs). In order to investigate how the magnetic phases evolve near the paramagnetic (PM)-to-FM phase transition boundary, we have performed temperature-dependent x-ray magnetic circular dichroism (XMCD) experiments on a La$_{1-x}$Sr$_{x}$MnO$_3$ (LSMO, $x=0.4$) thin film, whose thickness (8 ML) is close to the boundary between the FM-metallic and the PM-insulating phases. By utilizing the element-selectiveness of XMCD, we have quantitatively estimated the fractions of the PM and superparamagnetic (SPM) phases as well as the FM one as a function of temperature. The results can be reasonably described based on a microscopic phase-separation model.

cond-mat.mtrl-sci↗

arXiv2019

Giant perpendicular magnetic anisotropy in Ir/Co/Pt multilayers

We have studied the magnetic properties of multilayers composed of ferromagnetic metal Co and heavy metals with strong spin orbit coupling (Pt and Ir). Multilayers with symmetric (ABA stacking) and asymmetric (ABC stacking) structures are grown to study the effect of broken structural inversion symmetry. We compare the perpendicular magnetic anisotropy (PMA) energy of symmetric Pt/Co/Pt, Ir/Co/Ir multilayers and asymmetric Pt/Co/Ir, Ir/Co/Pt multilayers. First, the interface contribution to the PMA is studied using the Co layer thickness dependence of the effective PMA energy. Comparison of the interfacial PMA between the Ir/Co/Pt, Pt/Co/Ir asymmetric structures and Pt/Co/Pt, Ir/Co/Ir symmetric structures indicate that the broken structural inversion symmetry induced PMA is small compared to the overall interfacial PMA. Second, we find the magnetic anisotropy field is significantly increased in multilayers when the ferromagnetic layers are antiferromagnetically coupled via interlayer exchange coupling (IEC). Macrospin model calculations can qualitatively account for the relation between the anisotropy field and the IEC. Among the structures studied, IEC is the largest for the asymmetric Ir/Co/Pt multilayers: the exchange coupling field exceeds 3 T and consequently, the anisotropy field approaches 10 T. Third, comparing the asymmetric Ir/Co/Pt and Pt/Co/Ir structures, we find the IEC and, to some extent, the interface PMA are stronger for the former than the latter. X-ray magnetic circular dichroism studies suggest that the proximity induced magnetization in Pt is larger for the Ir/Co/Pt multilayers than the inverted structure, which may partly account for the difference in the magnetic properties. These results show the intricate relation between PMA, IEC and the proximity induced magnetization that can be exploited to design artificial structures with unique magnetic characteristics.

cond-mat.mtrl-sci↗

arXiv2019

Relationship between charge redistribution and ferromagnetism at the heterointerface between perovskite oxides LaNiO$_3$ and LaMnO$_3$

To investigate the relationship between the charge redistribution and ferromagnetism at the heterointerface between perovskite transition-metal oxides LaNiO$_3$ (LNO) and LaMnO$_3$ (LMO), we performed x-ray absorption spectroscopy and x-ray magnetic circular dichroism (XMCD) measurements. In the LNO/LMO heterostructures with asymmetric charge redistribution, the electrons donated from Mn to Ni ions are confined within one monolayer (ML) of LNO at the interface, whereas holes are distributed over 3-4 ML on the LMO side. A detailed analysis of the Ni-$L_{2,3}$ and Mn-$L_{2,3}$ XMCD spectra reveals that Ni magnetization is induced only by the Ni$^{2+}$ ions in the 1 ML LNO adjacent to the interface, while the magnetization of Mn ions is increased in the 3-4 ML LMO of the interfacial region. The characteristic length scale of the emergent (increased) interfacial ferromagnetism of the LNO (LMO) layers is in good agreement with that of the charge distribution across the interface, indicating a close relationship between the charge redistribution due to the interfacial charge transfer and the ferromagnetism of the LNO/LMO interface. Furthermore, the XMCD spectra clearly demonstrate that the vectors of induced magnetization of both ions are aligned ferromagnetically, suggesting that the delicate balance between the exchange interactions occurring inside each layer and across the interface may induce the canted ferromagnetism of Ni$^{2+}$ ions, resulting in weak magnetization in the 1 ML LNO adjacent to the interface.

cond-mat.str-el↗

arXiv2018

Electronic structure of the novel high-$T_{\rm C}$ ferromagnetic semiconductor (Ga,Fe)Sb: x-ray magnetic circular dichroism and resonance photoemission spectroscopy studies

The electronic structure and the magnetism of the novel ferromagnetic semiconductor (Ga,Fe)Sb, whose Curie temperature $T_{\rm C}$ can exceed room temperature, were investigated by means of x-ray absorption spectroscopy (XAS), x-ray magnetic circular dichroism (XMCD), and resonance photoemission spectroscopy (RPES). The line-shape analyses of the XAS and XMCD spectra suggest that the ferromagnetism is of intrinsic origin. The orbital magnetic moments deduced using XMCD sum rules were found to be large, indicating that there is a considerable amount of 3$d^{6}$ contribution to the ground state of Fe. From RPES, we observed a strong dispersive Auger peak and non-dispersive resonantly enhanced peaks in the valence-band spectra. The latter is a fingerprint of the correlated nature of Fe 3$d$ electrons, whereas the former indicates their itinerant nature. It was also found that the Fe 3$d$ states have finite contribution to the DOS at the Fermi energy. These states presumably consisting of majority-spin $p$-$d$ hybridized states or minority-spin $e$ states would be responsible for the ferromagnetic order in this material.

cond-mat.str-el↗

arXiv2018

Anisotropic Charge Distribution Induced by Spin Polarization in La$_{0.6}$Sr$_{0.4}$MnO$_{3}$ Thin Films Studied by X-ray Magnetic Linear Dichroism

Magnetic anisotropy of epitaxially grown thin films is affected by the strain from the substrates due to a combined effect of distorted electronic structure and spin-orbit interaction (SOI). As an inverse process, one expects an anisotropy of the electronic structure induced by magnetization in the presence of SOI. We have studied the charge-density anisotropy induced by magnetization in thin films of the ferromagnetic metal La$_{1-x}$Sr$_{x}$MnO$_3$ via x-ray magnetic linear dichroism (XMLD). XMLD measurements on thin films with various thicknesses have shown that the XMLD intensity is proportional to the square of the ferromagnetic moment. Using the XMLD sum rule and cluster-model calculation, it has been shown that more Mn 3$d$ electrons are distributed in orbitals elongated along the direction parallel to the spin polarization than in orbitals elongated in the direction perpendicular to it. The cluster-model calculation has shown that the effect of tensile strain from the SrTiO$_3$ substrate on the XMLD spectra is also consistent with the observed XMLD spectral line shapes.

cond-mat.mtrl-sci↗

arXiv2018

Local Magnetic States of the Weakly Ferromagnetic Iron-Based Superconductor Sr$_2$VFeAsO$_{3-δ}$ Studied by X-ray Magnetic Circular Dichroism

We have performed x-ray magnetic circular dichroism (XMCD) measurements on the iron-based superconductor Sr$_2$VFeAsO$_{3-δ}$ to study the origin of weak ferromagnetism (WFM) reported for this compound. While Fe 3$d$ electrons show a magnetic response similar to the other iron pnictides, signals from V 3$d$ electrons remain finite at zero magnetic field and may be responsible for the WFM.

cond-mat.str-el↗

arXiv2018

Systematic study of the electronic structure and the magnetic properties of a few-nm-thick epitaxial (Ni1-xCox)Fe2O4 (x = 0 - 1) layers grown on Al2O3(111)/Si(111) using soft X-ray magnetic circular dichroism: effects of cation distribution

We study the electronic structure and the magnetic properties of epitaxial (Ni1-xCox)Fe2O4(111) layers (x = 0 - 1) with thicknesses d = 1.7 - 5.2 nm grown on Al2O3(111)/Si(111) structures, to achieve a high value of inversion parameter y, which is the inverse-to-normal spinel-structure ratio, and hence to obtain good magnetic properties even when the thickness is thin enough for electron tunneling as a spin filter. We revealed the crystallographic (octahedral Oh or tetrahedral Td) sites and the valences of the Fe, Co, and Ni cations using experimental soft X-ray absorption spectroscopy and X-ray magnetic circular dichroism spectra and configuration-interaction cluster-model calculation. In all the (Ni1-xCox)Fe2O4 layers with d = about 4 nm, all Ni cations occupy the Ni2+ (Oh) site, whereas Co cations occupy the three different Co2+ (Oh), Co2+ (Td), and Co3+ (Oh) sites with constant occupancies. According to these features, the occupancy of the Fe3+ (Oh) cations decreases and that of the Fe3+ (Td) cations increases with decreasing x. Consequently, we obtained a systematic increase of y with decreasing x and achieved the highest y value of 0.91 for the NiFe2O4 layer with d = 3.5 nm. From the d dependences of y and magnetization in the d range of 1.7 - 5.2 nm, a magnetically dead layer is present near the NiFe2O4/Al2O3 interface, but its influence on the magnetization was significantly suppressed compared with the case of CoFe2O4 layers reported previously [Y. K. Wakabayasi et al., Phys. Rev. B 96, 104410 (2017)], due to the high site selectivity of the Ni cations. Since our epitaxial NiFe2O4 layer with d = 3.5 nm has a high y values (0.91) and a reasonably large magnetization (180 emu/cc), it is expected to exhibit a strong spin filter effect, which can be used for efficient spin injection into Si.

cond-mat.mtrl-sci↗

arXiv2018

Electronic States and Possible Origin of the Orbital-Glass State in a Nearly Metallic Spinel Cobalt Vanadate: An X-ray Magnetic Circular Dichroism Study

We have investigated the orbital states of the orbital-glassy (short-range orbital ordered) spinel vanadate Co$_{1.21}$V$_{1.79}$O$_{4}$ using x-ray absorption spectroscopy (XAS), x-ray magnetic circular dichroism (XMCD), and subsequent configuration-interaction cluster-model calculation. From the sign of the XMCD spectra, it was found that the spin magnetic moment of the Co ion is aligned parallel to the applied magnetic field and that of the V ion anti-parallel to it, consistent with neutron scattering studies. It was revealed that the excess Co ions at the octahedral site take the trivalent low-spin state, and induce a random potential to the V sublattice. The orbital magnetic moment of the V ion is small although finite, suggesting that the ordered orbitals mainly consists of real-number orbitals.

cond-mat.str-el↗

arXiv2017

Effect(s) of Cobalt Substitution in $L1_{0}$-(Fe,Co)Pt Thin Films

We have studied the effect of cobalt substitution in $L1_{0}$-Fe$_{1-x}$Co$_{x}$Pt films by means of x-ray magnetic circular dichroism (XMCD) and first-principles calculations. The magnetic moments of Fe ($\sim$2.5 $μ_{\rm B}$) and Co ($\sim$1.5 $μ_{\rm B}$) deduced using XMCD were almost unchanged upon Co doping, and the net magnetization decreases with increasing Co content. Calculation also showed that the 3$d$ electrons that have been added by Co substitution occupy only spin-down bands.

cond-mat.mtrl-sci↗

arXiv2017

Electronic structure and magnetic properties of magnetically dead layers in epitaxial CoFe2O4/Al2O3/Si(111) films studied by X-ray magnetic circular dichroism

Epitaxial CoFe2O4/Al2O3 bilayers are expected to be highly efficient spin injectors into Si owing to the spin filter effect of CoFe2O4. To exploit the full potential of this system, understanding the microscopic origin of magnetically dead layers at the CoFe2O4/Al2O3 interface is necessary. In this paper, we study the crystallographic and electronic structures and the magnetic properties of CoFe2O4(111) layers with various thicknesses (thickness d = 1.4, 2.3, 4, and 11 nm) in the epitaxial CoFe2O4(111)/Al2O3(111)/Si(111) structures using soft X-ray absorption spectroscopy (XAS) and X-ray magnetic circular dichroism (XMCD) combined with cluster-model calculation. The magnetization of CoFe2O4 measured by XMCD gradually decreases with decreasing thickness d and finally a magnetically dead layer is clearly detected at d = 1.4 nm. The magnetically dead layer has frustration of magnetic interactions which is revealed from comparison between the magnetizations at 300 and 6 K. From analysis using configuration-interaction cluster-model calculation, the decrease of d leads to a decrease in the inverse-to-normal spinel structure ratio and also a decrease in the average valence of Fe at the octahedral sites. These results strongly indicate that the magnetically dead layer at the CoFe2O4/Al2O3 interface originates from various complex networks of superexchange interactions through the change in the crystallographic and electronic structures. Furthermore, from comparison of the magnetic properties between d = 1.4 and 2.3 nm, it is found that ferrimagnetic order of the magnetically dead layer at d = 1.4 nm is restored by the additional growth of the 0.9-nm-thick CoFe2O4 layer on it.

cond-mat.mtrl-sci↗