Possibility of ferro-octupolar order in BaCaOsO assessed by X-ray magnetic dichroism measurements

芝田 悟朗; 藤森 淳; 他10名*

Physical Review B, 113(16), p.165151_1 - 165151_7, 2026/04

https://doi.org/10.1103/mh1b-q11n

We studied the cubic double perovskite BaCaOsO containing the Os () ions, which exhibits a phase transition to a `hidden order' below K, by X-ray absorption spectroscopy (XAS) and X-ray magnetic circular dichroism (XMCD) at the Os edge. The cubic ligand-field splitting between the and levels of Os was deduced by XAS to be eV. The temperature dependence of the XMCD spectra was consistent with a meV residual cubic splitting of the lowest multiplet state into the non-Kramers doublet ground state and the triplet excited state. Ligand-field (LF) multiplet calculation under fictitious strong magnetic fields indicated that the exchange interaction between nearest-neighbor octupoles should be as strong as meV if a ferro-octupole order is stabilized in the `hidden-ordered' state, consistent with the exchange interaction of meV previously predicted theoretically using model and density functional theory calculations.

Orbital magnetic moments in FeCrS studied by X-ray magnetic circular dichroism

Verma, V. K.*; 芝田 悟朗; 藤森 淳*; 他8名*

Physical Review B, 112(10), p.104444_1 - 104444_8, 2025/09

https://doi.org/10.1103/hdzg-mn6r

We have investigated the element specific magnetic characteristics of single-crystal FeCrS using X-ray magnetic circular dichroism (XMCD). We have found that the Fe L2,3-edge XAS spectra do not exhibit clear multiplet structures, indicating strong hybridization between the Fe 3d and S 3p orbitals, leading to delocalized rather than localized electronic states. The Fe 3d and Cr 3d spin moments are antiferromagnetically coupled, consistent with the Goodenough-Kanamori rule. The orbital magnetic moments of Fe and Cr are determined to be -0.23 and -0.017 B/ion, respectively. The large orbital magnetic moment of Fe is due to the d6 configuration under the relatively weak tetrahedra crystal field at the Fe site, and the delocalized Fe electrons maintain the orbital degree of freedom in spite of their itinerant nature. On the other hand, the octahedral crystal-field splitting of the Cr 3d level is large enough to result in the quenching of the orbital moment of the Cr ion in FeCrS.

Hard X-ray photoemission study of bulk single-crystalline InGaZnO

芝田 悟朗; 他9名*

Applied Physics Letters, 126(24), p.241902_1 - 241902_6, 2025/06

https://doi.org/10.1063/5.0271655

We performed hard X-ray photoemission spectroscopy (HAXPES) experiments of bulk single-crystalline InGaZnO (sc-IGZO), which was recently synthesized via the optical floating zone method, in order to reveal the bulk intrinsic electronic structure. We find that oxygen vacancies are preferentially located around In atoms in as-grown crystals, which are filled out by post-annealing in an oxygen atmosphere. The subgap states near the valence-band maximum (VBM) were much weaker than those in the previous study even without oxygen annealing, which suggests that the loss of crystallinity is relevant to the formation of them in addition to the oxygen vacancies.

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

Chi, Z.*; 芝田 悟朗; 藤森 淳; 他15名*

Physical Review B, 110(18), p.184401_1 - 184401_8, 2024/11

https://doi.org/10.1103/PhysRevB.110.184401

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 (). The magnitude of the Dzyaloshinskii-Moriya exchange constant () increases with decreasing until 1 nm, below which decreases. The MCA and scale with 1/ for larger than nm, indicating an interfacial origin. Using X-ray magnetic circular dichroism (XMCD), we find non-zero OMA when is smaller than nm. The OMA increases with decreasing more rapidly than what is expected from the MCA, indicating that factors other than OMA contribute to the MCA at small .

Origin of magnetically dead layers in spinel ferrites FeO grown on AlO; Effects of postdeposition annealing studied by XMCD

野中 洋亮*; 若林 勇希*; 芝田 悟朗; 坂本 祥哉*; 池田 啓祐*; Chi, Z.*; Wan, Y.*; 鈴木 雅弘*; 田中 新*; 田中 雅明*; et al.

Physical Review Materials (Internet), 7(4), p.044413_1 - 044413_10, 2023/04

https://doi.org/10.1103/PhysRevMaterials.7.044413

We study the electronic and magnetic states of as-grown and annealed FeO(111)/AlO3(111) (Co, Ni) thin films with various thicknesses grown on Si(111) substrates with the -AlO(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 AlO buffer layer, we reveal that ferrimagnetic order is partially recovered by postdeposition 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 sites of the spinel structure, which may be the microscopic origin of the degraded ferrimagnetic order in the FeO thin films.

Cr doping-induced ferromagnetism in the spin-glass CdMnTe studied by X-ray magnetic circular dichroism

Verma, V.*; 坂本 祥哉*; 石川 弘一郎*; Singh, V. R.*; 石上 啓介*; 芝田 悟朗; 門野 利治*; 小出 常晴*; 黒田 真司*; 藤森 淳*

Physica B; Condensed Matter, 642, p.414129_1 - 414129_5, 2022/10

https://doi.org/10.1016/j.physb.2022.414129

The prototypical diluted magnetic semiconductor CdMnTe is a spin glass () or an antiferromagnet () but becomes ferromagnetic upon doping with a small amount of Cr atoms. To investigate the origin of the ferromagnetism in CdMnCrTe, we have studied its element specific magnetic properties by X-ray absorption spectroscopy (XAS) and X-ray magnetic circular dichroism (XMCD). Measured XAS and XMCD spectra indicate that both Cr and Mn atoms are divalent and that the magnetic moments of Cr and Mn are aligned parallel. By analyzing the element-specific magnetization curves, we conclude that Cr doping leads to the formation of ferromagnetic or superparamagnetic clusters consisting of several Cr ions surrounded by a much larger number of Mn ions.

Alternation of magnetic anisotropy accompanied by metal-insulator transition in strained ultrathin manganite heterostructures

小林 正起*; Anh, L. D.*; 鈴木 雅弘*; 金田-高田 真悟*; 竹田 幸治; 藤森 伸一; 芝田 悟朗*; 田中 新*; 田中 雅明*; 大矢 忍*; et al.

Physical Review Applied (Internet), 15(6), p.064019_1 - 064019_10, 2021/06

https://doi.org/10.1103/PhysRevApplied.15.064019

A fundamental understanding of the interfacial magnetic properties in ferromagnetic heterostructures is essential for utilizing ferromagnetic materials for spintronic device applications. Here, we investigate the interfacial magnetic and electronic structures of epitaxial single-crystalline LaAlO(LAO)/LaSrMnO(LSMO)/Nb:SrTiO(Nb:STO) heterostructures with varying LSMO layer thicknesses, in which the magnetic anisotropy strongly changes with the LSMO thickness due to the delicate balance between strains originating from both the Nb:STO and LAO layers, using X-ray magnetic circular dichroism and photoemission spectroscopy. We successfully detect the clear change of the magnetic behavior of the Mn ions concomitant with the thickness-dependent metal-insulator transition. Our results suggest that the double-exchange interaction induces ferromagnetism in the metallic LSMO film under tensile strain caused by the STO substrate, while the superexchange interaction determines the magnetic behavior in the insulating LSMO film under compressive strain originating from the top LAO layer. The change in strain, depending on LSMO layer thickness, is confirmed by scanning transmission electron microscopy. Based on those findings, the formation of a magnetic dead layer near the LAO/LSMO interface is attributed to competition between the superexchange interaction via Mn orbitals under compressive strain and the double-exchange interaction via the orbitals. These findings provide key aspects of ferromagnetic oxide heterostructures for the development of spintronic device applications.

Electronic structure of the high- ferromagnetic semiconductor (Ga,Fe)Sb; X-ray magnetic circular dichroism and resonance photoemission spectroscopy studies

坂本 祥哉*; Tu, N. T.*; 竹田 幸治; 藤森 伸一; Hai, P. N.*; Anh, L. D.*; 若林 勇希*; 芝田 悟朗*; 堀尾 眞史*; 池田 啓祐*; et al.

Physical Review B, 100(3), p.035204_1 - 035204_8, 2019/07

https://doi.org/10.1103/PhysRevB.100.035204

The electronic structure and the magnetism of the ferromagnetic semiconductor (Ga,Fe)Sb, whose Curie temperature 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 3 contribution to the ground state of Fe. From RPES, we observed a strong dispersive Auger peak and nondispersive resonantly enhanced peaks in the valence-band spectra. The latter is a fingerprint of the correlated nature of Fe 3 electrons, whereas the former indicates their itinerant nature. It was also found that the Fe 3 states have a finite contribution to the density of states at the Fermi energy. These states would be responsible for the ferromagnetic order in this material.

Cation distribution and magnetic properties in ultrathin (NiCo)FeO (x=0-1) layers on Si(111) studied by soft X-ray magnetic circular dichroism

若林 勇希*; 野中 洋亮*; 竹田 幸治; 坂本 祥哉*; 池田 啓祐*; Chi, Z.*; 芝田 悟朗*; 田中 新*; 斎藤 祐児; 山上 浩志; et al.

Physical Review Materials (Internet), 2(10), p.104416_1 - 104416_12, 2018/10

https://doi.org/10.1103/PhysRevMaterials.2.104416

We study the electronic structure and magnetic properties of epitaxial (NiCo)FeO(111) layers with thicknesses = 1.7 - 5.2 nm grown on AlO(111)/Si(111) structures. We revealed the crystallographic (octahedral or tetrahedral ) 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.

Magnetization process of the -type ferromagnetic semiconductor (In,Fe)As:Be studied by X-ray magnetic circular dichroism

坂本 祥哉*; Anh, L. D.*; Hai, P. N.*; 芝田 悟朗*; 竹田 幸治; 小林 正起*; 高橋 文雄*; 小出 常晴*; 田中 雅明*; 藤森 淳*

Physical Review B, 93(3), p.035203_1 - 035203_6, 2016/01

AA2016-0502.pdf:1.1MB

https://doi.org/10.1103/PhysRevB.93.035203

In order to investigate the mechanism of ferromagnetic ordering in the new -type magnetic semiconductor (In,Fe)As codoped with Be, we have performed X-ray absorption spectroscopy and X-ray magnetic circular dichroism (XMCD) studies. The spectral line shapes suggest that the ferromagnetism is intrinsic, originating from Fe atoms incorporated into the zinc-blende-type InAs lattice. The magnetization curves of Fe measured by XMCD were well reproduced by the superposition of a Langevin function representing superparamagnetic (SPM) behavior of nanoscale ferromagnetic domains and a -linear function representing Curie-Weiss paramagnetism even much above the Curie temperatures. The data at 20 K showed a deviation from the Langevin behavior, suggesting a gradual establishment of macroscopic ferromagnetism on lowering temperature. The existence of nanoscale ferromagnetic domains indicated by the SPM behavior suggests spatial fluctuations of Fe concentration on the nanoscale.