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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

https://doi.org/10.1103/PhysRevMaterials.7.044413
 被引用回数：0 パーセンタイル：0(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

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

https://doi.org/10.1016/j.physb.2022.414129
 被引用回数：4 パーセンタイル：53.42(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

https://doi.org/10.7566/JPSJ.91.064710
 被引用回数：0 パーセンタイル：0(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

Evolution of Fe 3$$d$$ impurity band state as the origin of high Curie temperature in the $$p$$-type ferromagnetic semiconductor (Ga,Fe)Sb

武田 崇仁*; 坂本 祥哉*; 荒木 恒星*; 藤澤 唯太*; Anh, L. D.*; Tu, N. T.*; 竹田 幸治; 藤森 伸一; 藤森 淳*; 田中 雅明*; et al.

Physical Review B, 102(24), p.245203_1 - 245203_8, 2020/12

https://doi.org/10.1103/PhysRevB.102.245203
 被引用回数：7 パーセンタイル：44.34(Materials Science, Multidisciplinary)

(Ga$$_{1-x}$$,Fe$$_x$$)Sb is one of the promising ferromagnetic semiconductors for spintronic device applications because its Curie temperature (Tc) is above 300 K when the Fe concentration $$x$$ is equal to or higher than 0.20. However, the origin of the high Tc in (Ga,Fe)Sb remains to be elucidated. To address this issue, we use resonant photoemission spectroscopy (RPES) and first-principles calculations to investigate the x dependence of the Fe 3$$d$$ states in (Ga$$_{1-x}$$,Fe$$_x$$)Sb ($$x$$ = 0.05, 0.15, and 0.25) thin films. The observed Fe 2$$p$$-3$$d$$ RPES spectra reveal that the Fe-3$$d$$ impurity band (IB) crossing the Fermi level becomes broader with increasing $$x$$, which is qualitatively consistent with the picture of double-exchange interaction. Comparison between the obtained Fe-3$$d$$ partial density of states and the first-principles calculations suggests that the Fe-3$$d$$ IB originates from the minority-spin ($$downarrow$$) $$e$$ states. The results indicate that enhancement of the double-exchange interaction between $$e_{downarrow}$$ electrons with increasing $$x$$ is the origin of the high Tc in (Ga,Fe)Sb.

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

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

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

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

https://doi.org/10.1103/PhysRevB.100.035204
 被引用回数：16 パーセンタイル：66.08(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

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

https://doi.org/10.7566/JPSJ.87.105001
 被引用回数：2 パーセンタイル：21.2(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

https://doi.org/10.1103/PhysRevMaterials.2.104416
 被引用回数：10 パーセンタイル：37.66(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 robust nanoscale ferromagnetism in Fe-doped Ge revealed by angle-resolved photoemission spectroscopy and first-principles calculation

坂本 祥哉*; 若林 勇希*; 竹田 幸治; 藤森 伸一; 鈴木 博人*; 伴 芳祐*; 山上 浩志; 田中 雅明*; 大矢 忍*; 藤森 淳*

Physical Review B, 95(7), p.075203_1 - 075203_5, 2017/02

https://doi.org/10.1103/PhysRevB.95.075203
 被引用回数：9 パーセンタイル：42.75(Materials Science, Multidisciplinary)

Ge$$_{1-x}$$Fe$$_x$$ (Ge:Fe) shows ferromagnetic behavior up to a relatively high temperature of 210 K and hence is a promising material for spintronic applications compatible with Si technology. We have studied its underlying electronic structure by soft X-ray angle-resolved photoemission spectroscopy measurements and first-principles supercell calculation. We observed finite Fe 3$$d$$ components in the states at the Fermi level ($$Erm_F$$) in a wide region of momentum space, and the $$Erm_F$$ was located $$sim$$0.35 eV above the valence-band maximum of the host Ge. Our calculation indicates that the $$Erm_F$$ is also within the deep acceptor-level impurity band induced by the strong $$p$$-$$d$$($$t_2$$) hybridization. We conclude that the additional minority-spin $$d(e)$$ electron characteristic of the Fe$$^{2+}$$ state is responsible for the short-range ferromagnetic coupling between Fe atoms.

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

https://doi.org/10.1103/PhysRevB.95.014417
 被引用回数：10 パーセンタイル：45.87(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

Volume-wise destruction of the antiferromagnetic Mott insulating state through quantum tuning

Frandsen, B. A.*; Liu, L.*; Cheung, S. C.*; Guguchia, Z.*; Khasanov, R.*; Morenzoni, E.*; Munsie, T. J. S.*; Hallas, A. M.*; Wilson, M. N.*; Cai, Y.*; et al.

Nature Communications (Internet), 7, p.12519_1 - 12519_8, 2016/08

https://doi.org/10.1038/ncomms12519
 被引用回数：33 パーセンタイル：77.26(Multidisciplinary Sciences)

RENiO$$_3$$ (RE = rare-earth element) and V$$_2$$O$$_3$$ are archetypal Mott insulator systems. When tuned by chemical substitution (RENiO$$_3$$) or pressure (V$$_2$$O$$_3$$), they exhibit a quantum phase transition (QPT) between an antiferromagnetic Mott insulating state and a paramagnetic metallic state. Because novel physics often appears near a Mott QPT, the details of this transition, such as whether it is first or second order, are important. Here, we demonstrate through muon spin relaxation/rotation experiments that the QPT in RENiO$$_3$$ and V$$_2$$O$$_3$$ is first order: the magnetically ordered volume fraction decreases to zero at the QPT, resulting in a broad region of intrinsic phase separation, while the ordered magnetic moment retains its full value until it is suddenly destroyed at the QPT. These findings bring to light a surprising universality of the pressure-driven Mott transition, revealing the importance of phase separation and calling for further investigation into the nature of quantum fluctuations underlying the transition.

論文

Room-temperature local ferromagnetism and its nanoscale expansion in the ferromagnetic semiconductor Ge$$_{1-x}$$Fe$$_{x}$$

若林 勇希*; 坂本 祥哉*; 竹田 幸治; 石上 啓介*; 高橋 文雄*; 斎藤 祐児; 山上 浩志; 藤森 淳*; 田中 雅明*; 大矢 忍*

Scientific Reports (Internet), 6, p.23295_1 - 23295_9, 2016/03

AA2016-0503.pdf:1.66MB

https://doi.org/10.1038/srep23295
 被引用回数：20 パーセンタイル：66.31(Multidisciplinary Sciences)

We investigate the local electronic structure and magnetic properties of the group-IV-based ferromagnetic semiconductor, Ge$$_{1-x}$$Fe$$_{x}$$ (GeFe), using soft X-ray magnetic circular dichroism. Our results show that the doped Fe 3$$d$$ electrons are strongly hybridized with the Ge 4$$p$$ states, and have a large orbital magnetic moment relative to the spin magnetic moment, namely $$m_{rm orb}$$/$$m_{rm spin}$$ $$approx$$ 0.1. We find that nanoscale local ferromagnetic regions, which are formed through ferromagnetic exchange interactions in the high-Fe-content regions of the GeFe films, exist even at room temperature, well above the Curie temperature of 20 - 100K. We observe the intriguing nanoscale expansion of the local ferromagnetic regions with decreasing temperature, followed by a transition of the entire film into a ferromagnetic state at the Curie temperature.

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

https://doi.org/10.1103/PhysRevB.93.035203
 被引用回数：18 パーセンタイル：63.01(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

Spin and orbital magnetic moments of Fe in the $$n$$-type ferromagnetic semiconductor (In,Fe)As

小林 正起*; Anh, L. D.*; Hai, P. N.*; 竹田 幸治; 坂本 祥哉*; 門野 利治*; 岡根 哲夫; 斎藤 祐児; 山上 浩志; 原田 慈久*; et al.

Applied Physics Letters, 105(3), p.032403_1 - 032403_4, 2014/07

AA2015-0418.pdf:0.82MB

https://doi.org/10.1063/1.4890733
 被引用回数：6 パーセンタイル：26.85(Physics, Applied)

The electronic and magnetic properties of Fe atoms in the ferromagnetic semiconductor (In,Fe)As codoped with Be have been studied by X-ray absorption spectroscopy (XAS) and X-ray magnetic circular dichroism (XMCD) at the Fe $$L_{2,3}$$ edge. The XAS and XMCD spectra showed simple spectral line shapes similar to Fe metal, but the ratio of the orbital and spin magnetic moments estimated using the XMCD sum rules was significantly larger than that of Fe metal, indicating a significant orbital moment of Fe 3$$d$$ electrons in (In,Fe)As:Be. The XMCD intensity as a function of magnetic field indicated hysteretic behavior of the superparamagnetic-like component due to discrete ferromagnetic domains. VC

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