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論文

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, p.184401_1 - 184401_8, 2024/11

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 ($$t_{rm eff}$$). The magnitude of the Dzyaloshinskii-Moriya exchange constant ($$|D|$$) increases with decreasing $$t_{rm eff}$$ until $$T_{rm eff}$$ $$sim$$ 1 nm, below which $$|D|$$ decreases. The MCA and $$|D|$$ scale with 1/$$T_{rm eff}$$ for $$t_{rm eff}$$ larger than $$sim 1$$ nm, indicating an interfacial origin. Using X-ray magnetic circular dichroism (XMCD), we find non-zero OMA when $$t_{rm eff}$$ is smaller than $$sim 0.8$$ nm. The OMA increases with decreasing $$t_{rm eff}$$ more rapidly than what is expected from the MCA, indicating that factors other than OMA contribute to the MCA at small $$t_{rm eff}$$.

論文

Origin of magnetically dead layers in spinel ferrites $$M$$Fe$$_2$$O$$_4$$ grown on Al$$_2$$O$$_3$$; 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

 被引用回数:3 パーセンタイル:37.82(Materials Science, Multidisciplinary)

We study the electronic and magnetic states of as-grown and annealed $$M$$Fe$$_2$$O$$_4$$(111)/Al$$_2$$O3(111) ($$M =$$Co, Ni) thin films with various thicknesses grown on Si(111) substrates with the $$gamma$$-Al$$_2$$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 Al$$_2$$O$$_3$$ 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 $$T_d$$ sites of the spinel structure, which may be the microscopic origin of the degraded ferrimagnetic order in the $$M$$Fe$$_2$$O$$_4$$ thin films.

論文

垂直磁気異方性を示す鉄挿入遷移金属ダイカルコゲナイドFe$$_x$$TaS$$_2$$のX線磁気円二色性による研究; Fe$$_x$$TiS$$_2$$との比較

芝田 悟朗; Won, C.*; Kim, J.*; 野中 洋亮*; 池田 啓祐*; Wan, Y.*; 鈴木 雅弘*; 小出 常晴*; 田中 新*; Cheong, S.-W.*; et al.

Photon Factory Activity Report 2022 (インターネット), 2 Pages, 2023/00

Feをインターカレートした遷移金属ダイカルコゲナイド化合物Fe$$_x$$TiS$$_2$$およびFe$$_x$$TaS$$_2$$は、巨大な保磁力および垂直磁気異方性を示す強磁性体になることが知られている。我々は以前、Fe$$_x$$TiS$$_2$$についてのX線磁気円二色性(XMCD)実験の結果から、Fe$$^{2+}$$の凍結していない軌道磁気モーメントが結晶場の1次摂動によって直接磁気異方性エネルギーを生むことを明らかにした。今回、Fe$$_x$$TiS$$_2$$よりもさらに強い磁気異方性を示す遷移金属ダイカルコゲナイドFe$$_x$$TaS$$_2$$について同様にXMCD実験を行い、磁気異方性の強さが何によって左右されているかを探ることを試みた。

論文

Cr doping-induced ferromagnetism in the spin-glass Cd$$_{1-x}$$Mn$$_x$$Te 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

 被引用回数:5 パーセンタイル:46.34(Physics, Condensed Matter)

The prototypical diluted magnetic semiconductor Cd$$_{1-x}$$Mn$$_x$$Te is a spin glass ($$x < 0.6$$) or an antiferromagnet ($$x > 0.6$$) but becomes ferromagnetic upon doping with a small amount of Cr atoms. To investigate the origin of the ferromagnetism in Cd$$_{1-x-y}$$Mn$$_x$$Cr$$_y$$Te, 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.

論文

Magnetic properties and electronic configurations of Mn ions in the diluted magnetic semiconductor Ba$$_{1-x}$$K$$_x$$(Zn$$_{1-y}$$Mn$$_y$$)$$_2$$As$$_2$$ studied by X-ray magnetic circular dichroism and resonant inelastic X-ray scattering

鈴木 博人*; Zhao, G.*; 岡本 淳*; 坂本 祥哉*; Chen, Z.-Y.*; 野中 洋亮*; 芝田 悟朗; Zhao, K.*; Chen, B.*; Wu, W.-B.*; et al.

Journal of the Physical Society of Japan, 91(6), p.064710_1 - 064710_5, 2022/06

 被引用回数:0 パーセンタイル:0.00(Physics, Multidisciplinary)

The magnetic properties and the electronic excitations of the new diluted magnetic semiconductor Ba$$_{1-x}$$K$$_x$$(Zn$$_{1-y}$$Mn$$_y$$)$$_2$$As$$_2$$ have been studied by X-ray magnetic circular dichroism (XMCD) and resonant inelastic X-ray scattering (RIXS). The sum rule analysis of the XMCD spectra indicates that the Mn atoms are in the high-spin configurations of $$d^5$$, whereas the presence of competing ferromagnetic and antiferromagnetic interactions between the Mn ions reduces the net spin moment. Based on a comparison of the RIXS line shapes with those of Ga$$_{1-x}$$Mn$$_x$$As, it is concluded that the ground state of Mn in Ba$$_{1-x}$$K$$_x$$(Zn$$_{1-y}$$Mn$$_y$$)$$_2$$As$$_2$$ consists of both the $$3d^5 underline{L}$$ and $$3d^5$$ electron configurations.

論文

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

 被引用回数:7 パーセンタイル:48.63(Physics, Applied)

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$$_3$$(LAO)/La$$_{0.6}$$Sr$$_{0.4}$$MnO$$_3$$(LSMO)/Nb:SrTiO$$_3$$(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 $$3d_{3z^2-r^2}$$ orbitals under compressive strain and the double-exchange interaction via the $$3d_{x^2-y^2}$$ orbitals. These findings provide key aspects of ferromagnetic oxide heterostructures for the development of spintronic device applications.

論文

Electronic structure of the high-$$T_{rm C}$$ 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

 被引用回数:16 パーセンタイル:62.18(Materials Science, Multidisciplinary)

The electronic structure and the magnetism of the 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 3$$d^{6}$$ 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$$d$$ electrons, whereas the former indicates their itinerant nature. It was also found that the Fe 3$$d$$ 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.

論文

Electronic structure of the high-$$T_{rm C}$$ 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

The electronic structure and the magnetism of the 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 3$$d^{6}$$ 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$$d$$ electrons, whereas the former indicates their itinerant nature. It was also found that the Fe 3$$d$$ states have a finite contribution to the density of states 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.

論文

Local magnetic states of the weakly ferromagnetic iron-based superconductor Sr$$_{2}$$VFeAsO$$_{3-delta}$$ studied by X-ray magnetic circular dichroism

堀尾 眞史*; 竹田 幸治; 並木 宏允*; 片桐 隆雄*; 若林 勇希*; 坂本 祥哉*; 野中 洋亮*; 芝田 悟朗*; 池田 啓祐*; 斎藤 祐児; et al.

Journal of the Physical Society of Japan, 87(10), p.105001_1 - 105001_2, 2018/10

 被引用回数:2 パーセンタイル:19.88(Physics, Multidisciplinary)

We have performed X-ray magnetic circular dichroism (XMCD) measurements on the iron-based superconductor Sr$$_{2}$$VFeAsO$$_{3-delta}$$ to study the origin of weak ferromagnetism (WFM) reported for this compound. While Fe 3d electrons show a magnetic response similar to the other iron pnictides, signals from V 3d electrons remain finite at zero magnetic field and may be responsible for the WFM.

論文

Cation distribution and magnetic properties in ultrathin (Ni$$_{1-x}$$Co$$_{x}$$)Fe$$_{2}$$O$$_{4}$$ (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

 被引用回数:13 パーセンタイル:40.50(Materials Science, Multidisciplinary)

We study the electronic structure and magnetic properties of epitaxial (Ni$$_{1-x}$$Co$$_{x}$$)Fe$$_{2}$$O$$_{4}$$(111) layers with thicknesses $$d$$ = 1.7 - 5.2 nm grown on Al$$_{2}$$O$$_{3}$$(111)/Si(111) structures. We revealed the crystallographic (octahedral $$O_{h}$$ or tetrahedral $$T_{d}$$) 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.

論文

Origin of the large positive magnetoresistance of Ge$$_{1-x}$$Mn$$_{x}$$ granular thin films

若林 勇希*; 秋山 了太*; 竹田 幸治; 堀尾 眞史*; 芝田 悟朗*; 坂本 祥哉*; 伴 芳祐*; 斎藤 祐児; 山上 浩志; 藤森 淳*; et al.

Physical Review B, 95(1), p.014417_1 - 014417_6, 2017/01

 被引用回数:11 パーセンタイル:46.65(Materials Science, Multidisciplinary)

Ge$$_{1_x}$$Mn$$_x$$ (GeMn) granular thin films are a unique and promising material for spintronic applications owing to their large positive magnetoresistance (MR). The microscopic origin of the MR has not yet been clarified. Here, we develop a method to separately investigate the magnetic properties of the nanoparticles and the matrix, utilizing the extremely high sensitivity of X-ray magnetic circular dichroism (XMCD) to the local magnetic state of each atom. We find that the MR ratio is proportional to the product of the magnetizations originating from the nanoparticles and the matrix. This result indicates that the spin-polarized holes in the nanoparticles penetrate into the matrix and that these holes undergo first order magnetic scattering by the paramagnetic Mn atoms in the matrix, which induces the large MR.

論文

Magnetization process of the $$n$$-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

 被引用回数:19 パーセンタイル:62.92(Materials Science, Multidisciplinary)

In order to investigate the mechanism of ferromagnetic ordering in the new $$n$$-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 $$T$$-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.

論文

Thickness-dependent magnetic properties and strain-induced orbital magnetic moment in SrRuO$$_{3}$$ thin films

石上 啓介*; 吉松 公平*; 豊田 大介*; 滝沢 優*; 吉田 鉄平*; 芝田 悟朗*; 原野 貴幸*; 高橋 文雄*; 門野 利治*; Verma, V. K.*; et al.

Physical Review B, 92(6), p.064402_1 - 064402_5, 2015/08

 被引用回数:47 パーセンタイル:84.28(Materials Science, Multidisciplinary)

Thin films of the ferromagnetic metal SrRuO$$_{2}$$ (SRO) show a varying easy magnetization axis depending on the epitaxial strain, and undergo a metal-to-insulator transition with decreasing film thickness. We have investigated the magnetic properties of SRO thin films with varying thicknesses fabricated on SrTiO$$_{3}$$(001) substrates by soft X-ray magnetic circular dichroism at the Ru M2,3 edge. Results have shown that, with decreasing film thickness, the film changes from ferromagnetic to nonmagnetic at around 3 monolayer thickness, consistent with previous magnetization and magneto-optical Kerr effect measurements. The orbital magnetic moment perpendicular to the film was found to be 0.1$$mu$$B/Ru, and remained nearly unchanged with decreasing film thickness while the spin magnetic moment decreases. A mechanism for the formation of the orbital magnetic moment is discussed based on the electronic structure of the compressively strained SRO film.

論文

Orbital magnetic moment and coercivity of SiO$$_2$$-coated FePt nanoparticles studied by X-ray magnetic circular dichroism

高橋 文雄*; 門野 利治*; 山本 真平*; Singh, V. R.*; Verma, V.*; 石上 啓介*; 芝田 悟朗*; 原野 貴幸*; 竹田 幸治; 岡根 哲夫; et al.

Physical Review B, 90(2), p.024423_1 - 024423_5, 2014/07

AA2015-0417.pdf:0.45MB

 被引用回数:11 パーセンタイル:43.49(Materials Science, Multidisciplinary)

We have investigated the spin and orbital magnetic moments of Fe in FePt nanoparticles in the $$L1_{0}$$-ordered phase coated with SiO$$_2$$ by X-ray absorption spectroscopy (XAS) and X-ray magnetic circular dichroism (XMCD) measurements at the Fe $$L_{2,3}$$ absorption edges. The magnetic coercivity (H$$_{c}$$) was found to be as large as 1.8 T at room temperature, 3 times larger than the thin film value and 50 times larger than that of the gas phase condensed nanoparticles. The hysteresis curve is well explained by the Stoner-Wohlfarth model for noninteracting single-domain nanoparticles with the H$$_{c}$$ distributed from 1 to 5 T.

論文

Thickness-dependent ferromagnetic metal to paramagnetic insulator transition in La$$_{0.6}$$Sr$$_{0.4}$$MnO$$_3$$ thin films studied by X-ray magnetic circular dichroism

芝田 悟朗*; 吉松 公平*; 坂井 延寿*; Singh, V. R.*; Verma, V.*; 石上 啓介*; 原野 貴幸*; 門野 利治*; 竹田 幸治; 岡根 哲夫; et al.

Physical Review B, 89(23), p.235123_1 - 235123_5, 2014/06

AA2015-0419.pdf:0.33MB

 被引用回数:25 パーセンタイル:67.96(Materials Science, Multidisciplinary)

Metallic transition-metal oxides undergo a metal-to-insulator transition (MIT) as the film thickness decreases across a critical thickness of several monolayers (MLs), but its driving mechanism remains controversial. We have studied the thickness-dependent MIT of the ferromagnetic metal La$$_{0.6}$$Sr$$_{0.4}$$MnO$$_3$$ by X-ray absorption spectroscopy and X-ray magnetic circular dichroism. The results suggest that the ferromagnetic phase gradually and most likely inhomogeneously turns into the paramagnetic phase and both phases abruptly become insulating at the critical thickness.

口頭

Chemical state elucidation of trace nuclides in microparticles using scanning transmission X-ray microscopy

渡辺 勇輔; 芝田 悟朗; 小畠 雅明; 小荒井 一真; 竹田 幸冶

no journal, , 

本研究では福島第一原子力発電所事故由来の放射性物質や廃炉によって発生する廃棄物中の放射性核種の化学状態解明を目的として、SPring-8・RI実験棟に設置された走査型透過X線顕微鏡(STXM)を用いた微小粒子分析手法の開発を実施した。環境中において放射性核種を吸着しその移行挙動に影響を与える河川懸濁粒子を対象にSTXMを用いた粒子の性状把握と、粒子中微量元素の化学状態分析を行った。pHや元素組成が異なる上流と下流の2地点で採取した河川懸濁粒子中のFeとAlの元素分布とX線吸収スペクトルを測定した。酸性を示す上流で採取した試料ではFeとAlは別々に分布しており、Feは3価として存在していることが示された。一方下流の中性の河川水から採取した試料は2価のFeが多く存在しており、Alの分布と強い相関を示した。STXMを用いた粒子中元素分布と化学形態の比較により、上流から下流にかけてpHの変化に伴い粒子の形成プロセスが異なることが示唆された。

口頭

日本原子力研究開発機構専用ビームラインSPring-8 BL23SUにおける軟X線走査型透過X線顕微鏡の導入

竹田 幸治; 芝田 悟朗; 土井 玲祐; 矢板 毅

no journal, , 

日本原子力研究開発機構は、大型放射光施設SPring-8において放射性物質の取り扱いが可能なRI実験棟に引き込まれた硬X線(BL22XU)および軟X線(BL23SU)の2本の専用ビームラインを運用している。本発表ではRI実験棟BL23SUの最下流に設置・整備してきた走査型透過X線顕微鏡(STXM)装置を紹介する。BL23SUでは、400$$sim$$1900eVの光を利用でき、N、O、Al、Si等のK吸収端、3d遷移金属のL吸収端、4f希土類のM吸収端、ウランのN吸収端が分布し、幅広い元素を研究対象にできる。本装置は、福島第一原子力発電所の廃炉作業に資するための放射性物質(核燃料物質を含む)の分析や希土類抽出技術の開発、アクチノイド基礎科学研究等の展開を目的として導入されたが、外部ユーザーによる供用装置としての利用も可能である。本装置のハードウェア設計はTolek Tyliszczak氏によりなされ、測定ソフトウェアはLabVIEWにより独自開発を行った。当日は本装置概要と現状、および電子顕微鏡との相補利用など今後の計画についても報告する。

口頭

Scanning transmission X-ray microscope system at SPring-8 BL23SU RI Laboratory

芝田 悟朗; 竹田 幸治; 小林 徹; 矢板 毅

no journal, , 

Recently, a scanning transmission X-ray microscope (STXM) system has been installed at the JAEA beamline BL23SU in the RI Laboratory. STXM is an experimental technique which combines the X-ray microscopy and X-ray absorption spectroscopy in the transmission mode. One can obtain information about the electronic states of the targeted elements with a spatial resolution of $$sim 30$$ nm which enables the analysis of spatially inhomogeneous samples and particles with small concentration. A wide range of elements can be targeted for research, including lanthanides, actinides, and 3$$d$$ transition metals. This STXM system is aimed for developing JAEA's original researches such as analysis of radioactive materials and basic actinide science. In this presentation, we will introduce the design concepts of our STXM system and the scientific results so far obtained.

口頭

Perpendicular magnetic anisotropy of iron-intercalated transition-metal disulfides studied by X-ray magnetic circular dichroism

芝田 悟朗

no journal, , 

Layered transition-metal dichalcogenides with the 1T-CdI$$_2$$-type crystal structure are known to exhibit a wide variety of electric and magnetic properties by intercalating various transition-metal atoms of different concentrations between adjacent layers. Among them, iron-intercalated titanium disulfides Fe$$_x$$TiS$$_2$$ and tantalum disulfides Fe$$_x$$TaS$$_2$$ are ferromagnets which exhibits strong perpendicular magnetic anisotropy (PMA) with large coercive fields of a few tesla. It is reported that Fe$$_x$$TaS$$_2$$ shows stronger PMA than Fe$$_x$$TiS$$_2$$, presumably due to the stronger spin-orbit interaction (SOI) of Ta. In the present study, in order to elucidate the microscopic origin of the strong PMA in these compounds, the electronic structure and magnetism of single-crystalline Fe$$_x$$TiS$$_2$$ and Fe$$_x$$TaS$$_2$$ have been investigated via X-ray absorption spectroscopy (XAS) and X-ray magnetic circular dichroism (XMCD). From the spectral line shapes of XAS and XMCD, the valence of Fe is shown to be essentially 2+, whereas Ti is in an itinerant electronic state between 3+ and 4+. This shows that electrons are doped from the intercalated Fe atoms into the host TiS$$_2$$ and TaS$$_2$$. Notably, clear differences in the spectral line shapes of XMCD at the Fe $$L_{2,3}$$ edges are observed between Fe$$_x$$TiS$$_2$$ and Fe$$_x$$TaS$$_2$$ despite the similarity of the crystal structures. This may be attributed to the different SOI strength between these compounds. Based on the configuration-interaction cluster-model calculations, the observed changes in the spectral line shapes can be qualitatively reproduced by virtually increasing SOI of Fe 3$$d$$ electrons.

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硬X線磁気円二色性によるBa$$_2$$CaOsO$$_6$$の磁気転移・多極子秩序に関する研究

芝田 悟朗; 林 浩章*; 河村 直己*; 岡本 淳*; Huang, D.-J.*; Streltsov, S.*; 山浦 一成*; 藤森 淳*

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近年、スピン-軌道相互作用(SOI)の強い立方晶$$(5d)^n$$電子系における多極子秩序状態が盛んに議論されている。その中で$$(5d)^2$$系ダブルペロブスカイト(DP)型酸化物Ba$$_2$$CaOsO$$_6$$は、$$T^{*}sim$$50Kで帯磁率の異常を示し、$$mu$$SRによる$$T^{*}$$以下での時間反転対称性の破れも確認されている一方で、中性子散乱では$$T^{*}$$以下で反強磁性ピークが観測されないという特異な磁性を示す。これと結晶構造が最低温まで立方晶であることから、磁気八極子秩序の可能性が指摘されており、その理論的な予言もなされているが、DP型結晶で$$(5d)^2$$系は四極子秩序を示すという理論予測もあり、$$T^{*}$$以下での秩序状態について合意は得られていない。本研究では、Os $$L_{2,3}$$端硬X線磁気円二色性(XMCD)により、磁場中におけるBa$$_2$$CaOsO$$_6$$多結晶のOs 5$$d$$電子状態の解明を試みた。観測されたXMCDスペクトルは、3$$d$$, 4$$d$$電子系のXMCDスペクトルと異なり、$$L_2$$端で比較的大きなXMCD ($$sim$$1%)を示すのに対して$$L_3$$端のXMCDは弱く($$sim$$0.1%)、強いSOIによる大きな軌道磁気モーメントの存在が示唆された。X線吸収(XAS), XMCDスペクトルの概形は立方晶を仮定した原子多重項計算によって再現することができ、XASの2本のピーク分裂が$$10Dq$$ ($$sim$$4eV)を反映していること、他の5$$d$$電子系と同様にクーロン相互作用は弱くSOIが強いことが示された。

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