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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


 被引用回数:3 パーセンタイル:66.42(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.


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


 被引用回数:1 パーセンタイル:92.85(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


Unveiling the impurity band induced ferromagnetism in the magnetic semiconductor (Ga,Mn)As

小林 正起*; 宗田 伊理也*; 竹田 幸治; 原田 慈久*; 藤森 淳*; Krempask$'y$, J.*; Schmitt, T.*; 大矢 忍*; 田中 雅明*; 尾嶋 正治*; et al.

Physical Review B, 89(20), p.205204_1 - 205204_8, 2014/05

 被引用回数:40 パーセンタイル:7.96(Materials Science, Multidisciplinary)

(Ga,Mn)As is a paradigm of a diluted magnetic semiconductor which shows ferromagnetism induced by doped hole carriers. With a few controversial models emerging from numerous experimental and theoretical studies, the mechanism of the ferromagnetism in (Ga,Mn)As still remains a puzzling enigma. In this article, we use soft X-ray angle-resolved photoemission spectroscopy to positively identify the ferromagnetic Mn 3d-derived impurity band (IB) in (Ga,Mn)As. The band appears dispersionless and hybridized with the light-hole band of the host GaAs. These findings conclude the picture of the valence-band structure of (Ga,Mn)As disputed for more than a decade. The nondispersive character of the IB and its location in vicinity of the valence-band maximum indicate that the Mn 3d-derived IB is formed as a split-off Mn-impurity state predicted by the Anderson.


Probing carbon edge exposure of iron phthalocyanine-based oxygen reduction catalysts by soft X-ray absorption spectroscopy

丹羽 秀治*; 斎藤 信*; 小林 正起*; 原田 慈久*; 尾嶋 正治*; 守屋 彰悟*; 松林 克征*; 難波江 裕太*; 黒木 重樹*; 池田 隆司; et al.

Journal of Power Sources, 223, p.30 - 35, 2013/02

 被引用回数:16 パーセンタイル:36.86(Chemistry, Physical)

固体高分子形燃料電池用の非白金で、安価で、高性能の炭素正極触媒をデザインするには、酸素還元反応の活性点を明らかにすることが重要である。しかしながら、このような複雑な系においては通常用いられる原子・電子構造プローブにより活性点を直接特定するのは困難である。本研究では、炭素1${it s}$X線吸収分光を用いて鉄フタロシアニンをもとにした触媒の炭素構造を観察し、$$pi^{ast}$$吸収端以下に炭素端の露出を意味する構造を見いだした。またその強度は酸素還元活性とよく相関することがわかった。これらの結果は、炭素1${it s}$X線吸収分光を用いることにより炭素正極触媒における酸素還元活性の評価が端の露出の観点から可能であることを示している。


Study on the oxygen adsorption property of nitrogen-containing metal-free carbon-based cathode catalysts for oxygen reduction reaction

木内 久雄*; 丹羽 秀治*; 小林 正起*; 原田 慈久*; 尾嶋 正治*; 畳開 真之*; 難波江 裕太*; 黒木 重樹*; 柿本 雅明*; 池田 隆司; et al.

Electrochimica Acta, 82(1), p.291 - 295, 2012/10

 被引用回数:10 パーセンタイル:63.21(Electrochemistry)

含窒素ポリアミド(PA)と窒素を含まないフェノール樹脂(PhRs)由来の金属を含まない炭素触媒への酸素吸着特性を調べた。電気化学分析及びラマン分光からPA由来の炭素触媒はPhRs由来の物よりもより高い2電子酸素還元活性を示し、またより多くの欠陥を含むことがわかった。${it In-situ}$X線光電子分光からグラファイト状窒素が酸素吸着に寄与しPA由来の触媒ではC=Oが主な成分であることがわかった。これらの実験結果はグラファイト状窒素の近傍に吸着したC=O成分が2電子酸素還元の活性点であることを示唆している。


Indirect contribution of transition metal towards oxygen reduction reaction activity in iron phthalocyanine-based carbon catalysts for polymer electrolyte fuel cells

小林 正起*; 丹羽 秀治*; 斎藤 信*; 原田 慈久*; 尾嶋 正治*; 大渕 博宣*; 寺倉 清之*; 池田 隆司; 腰越 悠香*; 尾崎 純一*; et al.

Electrochimica Acta, 74, p.254 - 259, 2012/07

 被引用回数:38 パーセンタイル:15.62(Electrochemistry)



Role of residual transition-metal atoms in oxygen reduction reaction in cobalt phthalocyanine-based carbon cathode catalysts for polymer electrolyte fuel cell

小林 正起*; 丹羽 秀治*; 原田 慈久*; 堀場 弘司*; 尾嶋 正治*; 大渕 博宣*; 寺倉 清之*; 池田 隆司; 腰越 悠香*; 尾崎 純一*; et al.

Journal of Power Sources, 196(20), p.8346 - 8351, 2011/10

 被引用回数:26 パーセンタイル:27.67(Chemistry, Physical)

コバルトフタロシアニンとフェノール樹脂の混合物の熱分解によって合成したコバルトフタロシアニン由来の炭素触媒中の炭素原子の電子構造をX線吸収微細構造分析と硬X線光電子分光を用いて調べた。Co K端XAFSスペクトルからほとんどのコバルト原子は金属状態であるが酸洗い後でも少量の酸化コバルト成分があることがわかった。また、XAFSとHXPESのプローブ長の違いから酸洗い後においてCoクラスタ凝集体の表面領域はおもに金属Coから構成されていることがわかった。酸洗い前後で電気化学的性質がほとんど変化しなかったことから、残存金属Co又は酸化Co自体は炭素カソード触媒の酸素還元反応活性にほとんど寄与しておらず、炭素や窒素等の軽元素がコバルトフタロシアニン由来炭素触媒の活性点を構成していると考えられる。


X-ray photoemission spectroscopy analysis of N-containing carbon-based cathode catalysts for polymer electrolyte fuel cells

丹羽 秀治*; 小林 正起*; 堀場 弘司*; 原田 慈久*; 尾嶋 正治*; 寺倉 清之*; 池田 隆司; 腰越 悠香*; 尾崎 純一*; 宮田 清蔵*; et al.

Journal of Power Sources, 196(3), p.1006 - 1011, 2011/02

 被引用回数:72 パーセンタイル:5.96(Chemistry, Physical)



Electronic structure and magnetism of the diluted magnetic semiconductor Fe-doped ZnO nanoparticles

片岡 隆史*; 小林 正起*; 坂本 勇太*; Song, G. S.*; 藤森 淳*; Chang, F.-H.*; Lin, H.-J.*; Huang, D. J.*; Chen, C. T.*; 大河内 拓雄*; et al.

Journal of Applied Physics, 107(3), p.033718_1 - 033718_7, 2010/02


 被引用回数:44 パーセンタイル:11.81(Physics, Applied)

We have studied the electronic structure of Fe-doped ZnO nanoparticles, which have been reported to show ferromagnetism at room temperature, by X-ray photoemission spectroscopy (XPS), resonant photoemission spectroscopy (RPES), X-ray absorption spectroscopy (XAS) and X-ray magnetic circular dichroism (XMCD). From the experimental and cluster-model calculation results, we find that Fe atoms are predominantly in the Fe$$^{3+}$$ ionic state with mixture of a small amount of Fe$$^{2+}$$ and that Fe$$^{3+}$$ ions are dominant in the surface region of the nanoparticles. It is shown that the room temperature ferromagnetism in the Fe-doped ZnO nanoparticles is primarily originated from the antiferromagnetic coupling between unequal amounts of Fe$$^{3+}$$ ions occupying two sets of nonequivalent positions in the region of the XMCD probing depth of $$sim$$2-3 nm.


Antiferromagnetic interaction between paramagnetic Co ions in the diluted magnetic semiconductor Zn$$_{1-x}$$Co$$_x$$O

小林 正起*; 石田 行章*; Hwang, J. I.*; 長船 義敬*; 藤森 淳*; 竹田 幸治; 岡根 哲夫; 斎藤 祐児; 小林 啓介*; 佐伯 洋昌*; et al.

Physical Review B, 81(7), p.075204_1 - 075204_7, 2010/02


 被引用回数:18 パーセンタイル:31.68(Materials Science, Multidisciplinary)

The magnetic properties of Zn$$_{1-x}$$Co$$_x$$O (x=0.07 and 0.10) thin films, which were homoepitaxially grown on a ZnO(0001) substrates with varying relatively high oxygen pressure, have been investigated using X-ray magnetic circular dichroism (XMCD) at Co 2p core-level absorption edge. The magnetic-field and temperature dependences of the XMCD intensity are consistent with the magnetization measurements, indicating that except for Co there are no additional sources for the magnetic moment, and demonstrate the coexistence of paramagnetic and ferromagnetic components in the homoepitaxial Zn$$_{1-x}$$Co$$_x$$O thin films. The analysis of the XMCD intensities using the Curie-Weiss law reveals the presence of antiferromagnetic interaction between the paramagnetic Co ions. Missing XMCD intensities and magnetization signals indicate that most of Co ions are nonmagnetic probably because they are strongly coupled antiferromagnetically with each other.



竹田 幸治; 小林 正起*; 岡根 哲夫; 大河内 拓雄*; 岡本 淳*; 斎藤 祐児; 小林 啓介*; 山上 浩志; 藤森 淳*; 田中 新*; et al.

放射光, 22(4), p.202 - 209, 2009/07

SPring-8 BL23SUで改良・整備を進めてきた軟X線磁気円二色性装置を用いて、希薄磁性半導体Ga$$_{1-x}$$Mn$$_{x}$$AsのMn元素の磁気的特性を系統的な温度・磁場依存性測定を行って調べた。その結果、Gaと置換されたMnイオンと結晶格子の隙間に入り込んだMnイオンの間には反強磁性相互作用が存在しており、キュリー温度と結晶格子の隙間に入り込んだMnイオンの量とは明らかに相関していて、Gaと置換されたMnイオンの強磁性秩序を結晶格子の隙間に入り込んだMnイオンが阻害していることがわかった。


Experimental observation of bulk band dispersions in the oxide semiconductor ZnO using soft X-ray angle-resolved photoemission spectroscopy

小林 正起*; Song, G.-S.*; 片岡 隆史*; 坂本 勇太*; 藤森 淳; 大河内 拓雄*; 竹田 幸治; 岡根 哲夫; 斎藤 祐児; 山上 浩志; et al.

Journal of Applied Physics, 105(12), p.122403_1 - 122403_4, 2009/06


 被引用回数:9 パーセンタイル:56.61(Physics, Applied)

ZnO is one of the most promising oxide semiconductors for applications to semiconductor electronics, especially for optical devices. Their inexpensiveness and environmental safety are also advantages for practical applications. The surface electronic structure of ZnO has been investigated so far using angle-resolved photoemission spectroscopy (ARPES) in the ultraviolet ray region (less than 150 eV), although those measurements are surface sensitive. Considering their potentiality of ZnO for extensive applications, it is desired to investigate the bulk electronic structure of ZnO experimentally. In this work, we have performed soft X-ray (SX) ARPES measurements on a ZnO thin film in order to probe the bulk electronic structure. All the obtained band dispersion reflects the hexagonal Brillouin zone of ZnO, indicating we succeeded in the observation of the band dispersion of ZnO by SX-ARPES.


Hybridization between the conduction band and 3$$d$$ orbitals in the oxide-based diluted magnetic semiconductor In$$_{2-x}$$V$$_x$$O$$_3$$

小林 正起*; 石田 行章*; Hwang, J. I.*; Song, G. S.*; 滝沢 優*; 藤森 淳; 竹田 幸治; 大河内 拓雄*; 岡根 哲夫; 斎藤 祐児; et al.

Physical Review B, 79(20), p.205203_1 - 205203_5, 2009/05

 被引用回数:4 パーセンタイル:74.29(Materials Science, Multidisciplinary)

The electronic structure of In$$_{2-x}$$V$$_x$$O$$_3$$ ($$x=0.08$$) has been investigated by photoemission spectroscopy and X-ray absorption spectroscopy (XAS). The V $$2p$$ core-level photoemission and XAS spectra revealed that the V ion is in the trivalent state, which is the same valence state as that of In in In$$_2$$O$$_3$$. The V $$3d$$ partial density of states obtained by the resonant photoemission technique showed a sharp peak above the O $$2p$$ band. While the O $$1s$$ XAS spectrum of In$$_{2-x}$$V$$_x$$O$$_3$$ was similar to that of In$$_2$$O$$_3$$, there were differences in the In $$3p$$ and $$3d$$ XAS spectra between the V-doped and pure In$$_2$$O$$_3$$. The observations give clear evidence for hybridization between the In-derived conduction band and the V $$3d$$ orbitals in In$$_{2-x}$$V$$_x$$O$$_3$$.


Systematic changes of the electronic structure of the diluted ferromagnetic oxide Li-doped Ni$$_{1-x}$$Fe$$_x$$O with hole doping

小林 正起*; Hwang, J. I.*; Song, G.*; 大木 康弘*; 滝沢 優*; 藤森 淳; 竹田 幸治; 藤森 伸一; 寺井 恒太*; 岡根 哲夫; et al.

Physical Review B, 78(15), p.155322_1 - 155322_4, 2008/10

 被引用回数:5 パーセンタイル:69.26(Materials Science, Multidisciplinary)

The electronic structure of Li-doped Ni$$_{1-x}$$Fe$$_x$$O has been investigated using photoemission spectroscopy (PES) and X-ray absorption spectroscopy (XAS). The Ni $$2p$$ core-level PES and XAS spectra were not changed by Li doping. In contrast, the Fe$$^{3+}$$ intensity increased with Li doping relative to the Fe$$^{2+}$$ intensity. However, the increase of Fe$$^{3+}$$ is only $$sim 5%$$ of the doped Li content, suggesting that most of the doped holes enter the O $$2p$$ and/or the charge-transferred configuration Ni $$3d^8underline{L}$$. The Fe $$3d$$ partial density of states and the host valence-band emission near valence-band maximum increased with Li content, consistent with the increase of electrical conductivity. Based on these findings, percolation of bound magnetic polarons is proposed as an origin of the ferromagnetic behavior.


Soft X-ray absorption and photoemission studies of ferromagnetic Mn-implanted 3$$C$$-SiC

Song, G.*; 小林 正起*; Hwang, J. I.*; 片岡 隆*; 滝沢 優*; 藤森 淳; 大河内 拓雄; 竹田 幸治; 岡根 哲夫; 斎藤 祐児; et al.

Japanese Journal of Applied Physics, 47(9), p.7113 - 7116, 2008/09

 被引用回数:2 パーセンタイル:87.89(Physics, Applied)

We have performed X-ray photoemission spectroscopy (XPS), X-ray absorption spectroscopy (XAS), and resonant photoemission spectroscopy (RPES) measurements of Mn-implanted 3$$C$$-SiC (3$$C$$-SiC:Mn) and carbon-incorporated Mn$$_{5}$$Si$$_{2}$$ (Mn$$_{5}$$Si$$_{2}$$:C). The Mn 2$$p$$ core-level XPS and XAS spectra of 3$$C$$-SiC:Mn and Mn$$_{5}$$Si$$_{2}$$:C were similar to each other and showed "intermediate" behaviors between the localized and itinerant Mn 3$$d$$ states. The intensity at the Fermi level was found to be suppressed in 3$$C$$-SiC:Mn compared with Mn$$_{5}$$Si$$_{2}$$:C. These observations are consistent with the formation of Mn$$_{5}$$Si$$_{2}$$:C clusters in the 3$$C$$-SiC host, as observed in a recent transmission electron microscopy study.


Electronic structure of Ga$$_{1-x}$$Cr$$_{x}$$N and Si-doping effects studied by photoemission and X-ray absorption spectroscopy

Song, G.*; 小林 正起*; Hwang, J. I.*; 片岡 隆*; 滝沢 優*; 藤森 淳; 大河内 拓雄; 竹田 幸治; 岡根 哲夫; 斎藤 祐児; et al.

Physical Review B, 78(3), p.033304_1 - 033304_4, 2008/07

 被引用回数:7 パーセンタイル:60.79(Materials Science, Multidisciplinary)

The electronic structure of the magnetic semiconductor Ga$$_{1-x}$$Cr$$_{x}$$N, and the effect of Si doping on it have been investigated by photoemission and soft X-ray absorption spectroscopy. We have confirmed that Cr in GaN is predominantly trivalent when substituting for Ga and that Cr 3$$d$$ states appear within the band gap of GaN just above the N 2$$p$$-derived valence-band maximum. As a result of Si doping, downward shifts of the core levels (except for Cr 2$$p$$) and the formation of new states near the Fermi level were observed, which we attribute to the upward chemical-potential shift and the formation of a small amount of Cr$$^{2+}$$ species caused by electron doping. Possibility of Cr-rich cluster growth by Si doping are discussed based on the spectroscopic and magnetization data.


Nature of magnetic coupling between Mn ions in as-grown Ga$$_{1-x}$$Mn$$_{x}$$As studied by X-ray magnetic circular dichroism

竹田 幸治; 小林 正起*; 岡根 哲夫; 大河内 拓雄; 岡本 淳*; 斎藤 祐児; 小林 啓介*; 山上 浩志; 藤森 淳; 田中 新*; et al.

Physical Review Letters, 100(24), p.247202_1 - 247202_4, 2008/06

 被引用回数:30 パーセンタイル:18.37(Physics, Multidisciplinary)



Local electronic structure of Cr in the II-VI diluted ferromagnetic semiconductor Zn$$_{1-x}$$Cr$$_x$$Te

小林 正起*; 石田 行章*; Hwang, J. I.*; Song, G. S.*; 藤森 淳; Yang, C. S.*; Lee, L.*; Lin, H.-J.*; Huang, D.-J.*; Chen, C. T.*; et al.

New Journal of Physics (Internet), 10, p.055011_1 - 055011_15, 2008/05

 被引用回数:11 パーセンタイル:37.82(Physics, Multidisciplinary)

The electronic structure of the Cr ions in the diluted ferromagnetic semiconductor Zn$$_{1-x}$$Cr$$_x$$Te ($$x$$=0.03 and 0.15) thin films has been investigated using X-ray magnetic circular dichroism (XMCD) and photoemission spectroscopy (PES). The line shape of the Cr $$2p$$ XMCD spectra is independent of $$H$$, $$T$$, and $$x$$, indicating that the ferromagnetism is originated from the same electronic states of the Cr ion. Cluster-model analysis indicates that the ferromagnetic XMCD signal is originated from Cr ions substituted for the Zn site. The Cr $$3d$$ partial density of states extracted using Cr $$2p to 3d$$ resonant PES shows a broad feature near the top of the valence band, suggesting strong $$s$$,$$p$$-$$d$$ hybridization. Based on these findings, we conclude that double exchange mechanism cannot explain the ferromagnetism in Zn$$_{1-x}$$Cr$$_{x}$$Te.


X-ray magnetic circular dichroism and photoemission studies of ferromagnetism in CaMn$$_{1-x}$$Ru$$_{x}$$O$$_{3}$$ thin films

寺井 恒太*; 吉井 賢資; 竹田 幸治; 藤森 伸一; 斎藤 祐児; 大和田 謙二; 稲見 俊哉; 岡根 哲夫; 有田 将司*; 島田 賢也*; et al.

Physical Review B, 77(11), p.115128_1 - 115128_6, 2008/03

 被引用回数:12 パーセンタイル:45.59(Materials Science, Multidisciplinary)

We have studied the electronic and magnetic properties of epitaxially grown CaMn$$_{1-x}$$Ru$$_{x}$$O$$_{3}$$ thin films ($em x em = 1.0, 0.75, 0.5) by soft X-ray absorption (XAS), soft X-ray magnetic circular dichroism (XMCD) and hard X-ray photoemission spectroscopy (HXPES) measurements. The XMCD studies indicated that the spin moments of Mn and Ru are aligned in opposite directions. The valence-band HXPES spectra revealed that the Ru 4{it d}$ $$t_{2g}$$ states around the Fermi level and the Mn 3${it d}$ $$t_{2g}$$ up-spin states centered $$sim$$ 2 eV below it, both of which showed systematic concentration dependences. From these results, we propose that the localized Mn 3${it d}$ $$t_{2g}$$ states and the itinerant Ru 4${it d}$ $$t_{2g}$$ band are antiferromagnetically coupled and give rise to the ferromagnetic ordering, in analogy to the mechanism proposed for double perovskite oxides such as Sr$$_{2}$$FeMoO$$_{6}$$.


Photoemission and X-ray absorption studies of valence states in (Ni,Zn,Fe,Ti)$$_3$$O$$_4$$ thin films exhibiting photoinduced magnetization

小林 正起*; 大木 康弘*; 滝沢 優*; Song, G. S.*; 藤森 淳; 竹田 幸治; 寺井 恒太*; 岡根 哲夫; 藤森 伸一; 斎藤 祐児; et al.

Applied Physics Letters, 92(8), p.082502_1 - 082502_3, 2008/02

 被引用回数:8 パーセンタイル:60.83(Physics, Applied)

By means of photoemission and X-ray absorption spectroscopy, we have studied the electronic structure of (Ni,Zn,Fe,Ti)$$_{3}$$O$$_{4}$$ thin films, which exhibits a cluster glass behavior with a spin-freezing temperature $$T_f$$ of $$sim 230$$ K and photo-induced magnetization (PIM) below $$T_f$$. The Ni and Zn ions were found to be in the divalent states. Most of the Fe and Ti ions in the thin films were trivalent (Fe$$^{3+}$$) and tetravalent (Ti$$^{4+}$$), respectively. While Ti doping did not affect the valence states of the Ni and Zn ions, a small amount of Fe$$^{2+}$$ ions increased with Ti concentration, consistent with the proposed charge-transfer mechanism of PIM.

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