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Hard X-ray photoelectron spectroscopy study of Pt/Y$$_{3}$$Fe$$_{5}$$O$$_{12}$$

小畠 雅明; 吉井 賢資; 福田 竜生; 川崎 郁斗; 岡根 哲夫; 山上 浩志; 矢板 毅; 針井 一哉; 家田 淳一; 岡安 悟; et al.

JPS Conference Proceedings (Internet), 30, p.011192_1 - 011192_6, 2020/03

スピンゼーベック効果を示す系として注目されているPt/Y$$_{3}$$Fe$$_{5}$$O$$_{12}$$(YIG)系に対し、放射光を用いた硬X線光電子分光(HAXPES)により表面及び界面の電子状態測定を行った。本系ではスピンゼーベック効果のほかに特異な性質を示すことが報告されている。例えば、外部磁場が存在しない状況でもホール効果を発現する。この起源として、YIG中のFe$$^{3+}$$イオンがPt膜に染み出し、磁性を持つ金属間化合物を生成している可能性が提案されている。そこでHAXPESの分析深さを利用し、界面近傍の鉄イオン等の電子状態を測定した。Ptの厚みが2nm, 5nm, 8nm, 10nmの試料を測定したところ、2nmと5nmの試料において鉄イオンの分析を行うことができた。Fe 1s光電子スペクトルからは、鉄イオンが3+のものと金属的な0価に近い2つの状態が存在することが判明し、上記の可能性を支持する結果が得られた。Pt 4fやO 1sスペクトルなども測定しており、詳しい結果は当日報告する。


Manifestation of electron correlation effect in 5$$f$$ states of uranium compounds revealed by 4$$d$$-5$$f$$ resonant photoelectron spectroscopy

藤森 伸一; 小畠 雅明; 竹田 幸治; 岡根 哲夫; 斎藤 祐児; 藤森 淳; 山上 浩志; 芳賀 芳範; 山本 悦嗣; 大貫 惇睦*

Physical Review B, 99(3), p.035109_1 - 035109_5, 2019/01

 被引用回数:9 パーセンタイル:48.37(Materials Science, Multidisciplinary)

In the present study, we have elucidated the nature of the electron correlation effect in uranium compounds by imaging the partial $$mathrm{U}~5f$$ density of states (pDOS) of typical itinerant, localized, and heavy fermion uranium compounds by using the $$mathrm{U}$$ 4$$d$$-5$$f$$ resonant photoemission spectroscopy. Obtained $$mathrm{U}~5$$ pDOS exhibit a systematic trend depending on the physical properties of compounds: Although the coherent peak at the Fermi level can be explained by the band-structure calculation, an incoherent peak emerges on the higher binding energy side ($$lesssim 1~mathrm{eV}$$) in the cases of localized and heavy fermion compounds. The intensity and energy position of the incoherent peak is increased and shifted to a higher binding energy as the localization of the $$mathrm{U}~5$$ state increases. These behaviors are consistent with the prediction of the Mott metal-insulator transition, suggesting that the Hubbard-$$U$$ type mechanism takes an essential role in the $$5f$$ electronic structure of actinide materials.


Electronic structure of URu$$_2$$Si$$_2$$ studied by photoelectron spectroscopy (INVITED)

藤森 伸一; 竹田 幸治; 岡根 哲夫; 斎藤 祐児; 藤森 淳; 山上 浩志; 芳賀 芳範; 山本 悦嗣; 大貫 惇睦*

Progress in Nuclear Science and Technology (Internet), 5, p.82 - 85, 2018/11

One of the most remarkable properties of actinide compounds is the coexistence of superconductivity and magnetic ordering which has been realized in several strongly-correlated uranium based compounds. In these compounds, both superconductivity and magnetic ordering originate from U 5f states. To understand the origin of the coexistence as well as the mechanism of the superconductivity, it is essential to reveal their U 5f electronic structures. In this presentation, the U 5f electronic structures of heavy Fermion superconductors UPd$$_2$$Al$$_3$$ and URu$$_2$$Si$$_2$$ studied by photoelectron spectroscopy using soft X-rays from SPring-8 BL23SU are presented. For UPd$$_2$$Al$$_3$$, U 4d-5f resonant photoemission experiment was performed, and its partial U 5f spectrum was revealed experimentally. Furthermore, we have applied the three-dimentional ARPES to the hidden order compound URu$$_2$$Si$$_2$$, and revealed its complete 3D electronic structure in the paramagnetic phase. Their electronic structures are discussed based on these results.


Soft X-ray magnetic circular dichroism study on UGe$$_{2}$$

竹田 幸治; 岡根 哲夫; 斎藤 祐児; 山上 浩志; 山本 悦嗣; 芳賀 芳範

Progress in Nuclear Science and Technology (Internet), 5, p.171 - 174, 2018/11

In order to investigate the electronic and magnetic states of UGe$$_{2}$$ element-specifically, we have performed soft X-ray magnetic circular dichroism experiments at the U N$$_{4,5}$$ and Ge L$$_{2,3}$$ absorption edges. We have detected the XMCD signals at both the U and Ge sites and observed clear hysteresis loops in the ferromagnetic (FM) state at T = 5.5 K. From the branching ratio B, it is found that the occupation number of 5f electrons (n$$^{5f}$$) in UGe$$_{2}$$ is close to 3. In addition, applying the magneto-optical sum rules analysis to the XMCD spectrum at the U N$$_{4,5}$$ edges, the ratio of orbital magnetic moment to the spin magnetic moment (-M$$_{L}$$/M$$_{S}$$) is estimated to be 2.17. These values of B and -M$$_{L}$$/M$$_{S}$$ are comparable compared with the results of other FM superconductors: URhGe and UCoGe



小畠 雅明; 岡根 哲夫; 小林 啓介*

分光研究, 67(4), p.161 - 162, 2018/08



Element-specific observation of the ferromagnetic ordering process in UCoAl via soft X-ray magnetic circular dichroism

竹田 幸治; 斎藤 祐児; 岡根 哲夫; 山上 浩志; 松田 達磨*; 山本 悦嗣; 芳賀 芳範; 大貫 惇睦*

Physical Review B, 97(18), p.184414_1 - 184414_7, 2018/05


 被引用回数:1 パーセンタイル:10.9(Materials Science, Multidisciplinary)

We have performed soft X-ray magnetic circular dichroism (XMCD) experiments on the itinerant-electron metamagnet UCoAl at the U 4$$d$$-5$$f$$ ($$N_mathrm{4, 5}$$) and Co 2$$p$$-3$$d$$ ($$L_mathrm{2, 3}$$) absorption edges in order to investigate the magnetic properties of the U 5$$f$$ and Co 3$$d$$ electrons separately. From the line shape of the XMCD spectrum, it is deduced that the orbital magnetic moment of the Co 3$$d$$ electrons is unusually large. Through the systematic temperature ($$T$$)- and magnetic field ($$H$$)-dependent XMCD measurements, we have obtained two types of the magnetization curve as a function of $$H$$ and $$T$$ (M-H curve and M-T curve, respectively). The metamagnetic transition from a paramagnetic state to a field-induced ferromagnetic state was observed clearly under 15 K at $$H_mathrm{M}$$. The value of the $$H_mathrm{M}$$ and its $$T$$-dependence agree well between the U and Co sites, and the bulk magnetization. Whereas, we have discovered the remarkable differences in the M-H and M-T curves between the U and Co sites. The present findings show clearly that the role of the Co 3$$d$$ electrons should be considered more carefully in order to understand the origin of the magnetic ordering in UCoAl.


Chemical form analysis of reaction products in Cs-adsorption on stainless steel by means of HAXPES and SEM/EDX

小畠 雅明; 岡根 哲夫; 中島 邦久; 鈴木 恵理子; 大和田 謙二; 小林 啓介*; 山上 浩志; 逢坂 正彦

Journal of Nuclear Materials, 498, p.387 - 394, 2018/01

 被引用回数:16 パーセンタイル:86.58(Materials Science, Multidisciplinary)



Electronic structure of ThRu$$_2$$Si$$_2$$ studied by angle-resolved photoelectron spectroscopy; Elucidating the contribution of U 5$$f$$ states in URu$$_{2}$$Si$$_{2}$$

藤森 伸一; 小畠 雅明; 竹田 幸治; 岡根 哲夫; 斎藤 祐児; 藤森 淳; 山上 浩志; 松本 裕司*; 山本 悦嗣; 立岩 尚之; et al.

Physical Review B, 96(12), p.125117_1 - 125117_9, 2017/09

 被引用回数:8 パーセンタイル:40.31(Materials Science, Multidisciplinary)

The Fermi surface and band structure of $$mathrm{ThRu}_2mathrm{Si}_2$$ have been studied by angle resolved photoelectron spectroscopy (ARPES) with the incident photon energies of $$hnu$$ = 665-735 eV. Detailed band structure and the three-dimensional shape of the Fermi surface were derived experimentally, and they are quantitatively explained by the band-structure calculation based on the density functional approximation. Comparison of the experimental ARPES spectra of $$mathrm{ThRu}_2mathrm{Si}_2$$ with those of $$mathrm{URu}_2mathrm{Si}_2$$ shows that they have considerably different spectral profiles particularly in the energy range of $$E_mathrm{B} = E_mathrm{F}$$ - 1 eV. Some energy bands with their energy dispersions of about 1 eV observed in $$mathrm{URu}_2mathrm{Si}_2$$ are missing in the ARPES spectra of $$mathrm{ThRu}_2mathrm{Si}_2$$ measured along the same high symmetry line of Brillouin zone, suggesting that U 5$$f$$ states form these bands in $$mathrm{URu}_2mathrm{Si}_2$$. The relationship between the ARPES spectra of $$mathrm{URu}_2mathrm{Si}_2$$ and $$mathrm{ThRu}_2mathrm{Si}_2$$ is very different from the case between $$mathrm{CeRu}_2mathrm{Si}_2$$ and $$mathrm{LaRu}_2mathrm{Si}_2$$ where their intrinsic difference is limited only in the very vicinity of the Fermi energy. The present result argues that the U 5$$f$$ electrons in $$mathrm{URu}_2mathrm{Si}_2$$ have strong hybridization with ligand states, and essentially have an itinerant character.


Electronic structures of U$$X_3$$ ($$X$$=Al, Ga, and In) studied by photoelectron spectroscopy

藤森 伸一; 小畠 雅明; 竹田 幸治; 岡根 哲夫; 斎藤 祐児; 藤森 淳; 山上 浩志; 芳賀 芳範; 山本 悦嗣; 大貫 惇睦*

Physical Review B, 96(11), p.115126_1 - 115126_10, 2017/09

 被引用回数:7 パーセンタイル:36.67(Materials Science, Multidisciplinary)

The electronic structures of U$$X_3$$ ($$X$$=Al, Ga, and In) were studied by photoelectron spectroscopy to understand the relationship between their electronic structure and magnetic properties. The band structures and Fermi surfaces of UAl$$_3$$ and UGa$$_3$$ were revealed experimentally by angle-resolved photoelectron spectroscopy (ARPES), and they were compared with the result of band structure calculations. The topologies of the Fermi surfaces and the band structures of UAl$$_3$$ and UGa$$_3$$ were explained reasonably well by the calculation, although bands near the Fermi level ($$E_mathrm{F}$$) were renormalized owing to the finite electron correlation effect. The topologies of the Fermi surfaces of UAl$$_3$$ and UGa$$_3$$ are very similar to each other, except for some minor differences. Such minor differences in their Fermi surface or electron correlation effect might take an essential role in their magnetism.


Element specific electronic states and spin-flip-like behavior of Ce in (Ce$$_{0.2}$$Gd$$_{0.8}$$)Ni composed of heavy fermion CeNi and ferri-magnet GdNi through XMCD method

矢野 一雄*; 岡根 哲夫; 竹田 幸治; 山上 浩志; 藤森 淳; 西村 克彦*; 佐藤 清雄*

Physica B; Condensed Matter, 515, p.118 - 125, 2017/06

 被引用回数:1 パーセンタイル:6.18(Physics, Condensed Matter)

CeNi, GdNi、並びにCe$$_{0.2}$$Gd$$_{0.8}$$Niについて、構成元素の電子状態を軟X線吸収磁気円二色性(XMCD)測定により調べた。実験の結果、この系では、Gd 4f電子だけでなく、NI 3d電子並びにCe 4f電子も磁性も有しており、NI並びにCeの磁気モーメントはGdの磁気モーメントとは反平行にカップリングしていることがわかった。Ceの磁気モーメントは、いったん飽和した後、2T以上の磁場領域で減少していくが、これはスピンフリップ挙動と考えられる。サムルール解析からは、Gd 4f電子とNi 3d電子に小さい軌道磁気モーメントが残っていることが示唆された。


Results and progress of fundamental research on FP chemistry

逢坂 正彦; 中島 邦久; 三輪 周平; Di Lemma, F. G.*; 宮原 直哉; 鈴木 知史; 鈴木 恵理子; 岡根 哲夫; 小畠 雅明

Proceedings of 8th European Review Meeting on Severe Accident Research (ERMSAR 2017) (Internet), 11 Pages, 2017/05



Electronic structure and correlation in $$beta$$-Ti$$_3$$O$$_5$$ and $$lambda$$-Ti$$_3$$O$$_5$$ studied by hard X-ray photoelectron spectroscopy

小林 啓介*; 田口 宗孝*; 小畠 雅明; 田中 健司*; 所 裕子*; 大門 寛*; 岡根 哲夫; 山上 浩志; 池永 英司*; 大越 慎一*

Physical Review B, 95(8), p.085133_1 - 085133_7, 2017/02


 被引用回数:13 パーセンタイル:54.99(Materials Science, Multidisciplinary)

We have conducted hard X-ray photoelectron spectroscopy investigations of the electronic structure changes and electron correlation phenomena which take place upon the photoinduced reversible phase transition between $$beta$$- and $$lambda$$-Ti$$_3$$O. From valence band spectra of $$beta$$- and $$lambda$$-Ti$$_3$$O$$_5$$, we have identified the bipolaron caused by the $$sigma$$-type bonding of $$d_{xy}$$ orbitals in $$beta$$-Ti$$_3$$O$$_5$$ and the $$pi$$ stacking between the $$d_{xy}$$ orbitals between different Ti sites in $$lambda$$-Ti$$_3$$O$$_5$$, previously predicted by $textit{ab initio}$ calculations. On the other hand, the Ti $$2p$$ and Ti $$1s$$ core level spectra exhibit nonlocal screening satellite features, which are typical spectroscopic signs of strong electron correlation in the coherent Ti $$t_{2g}$$ states. Correlation in the valence band also manifests to reduce the plasmon energy, which results in an enhancement of the valence electron mass by a factor of 2.7.


Results and progress of fundamental research on fission product chemistry; Progress report in 2015

逢坂 正彦; 三輪 周平; 中島 邦久; Di Lemma, F. G.*; 鈴木 知史; 宮原 直哉; 小畠 雅明; 岡根 哲夫; 鈴木 恵理子

JAEA-Review 2016-026, 32 Pages, 2016/12




Electronic structure of EuAl$$_4$$ studied by photoelectron spectroscopy

小畠 雅明; 藤森 伸一; 竹田 幸治; 岡根 哲夫; 斎藤 祐児; 小林 啓介*; 山上 浩志; 仲村 愛*; 辺土 正人*; 仲間 隆男*; et al.

Journal of the Physical Society of Japan, 85(9), p.094703_1 - 094703_6, 2016/09

 被引用回数:11 パーセンタイル:61.24(Physics, Multidisciplinary)

The electronic structure of a divalent $$mathrm{Eu}$$ compound EuAl$$_4$$, which shows the charge density wave transition at $$T_{mathrm{CDW}} = 140~mathrm{K}$$, was studied by the hard X-ray angle-integrated photoelectron spectroscopy (HAXPES) and the soft X-ray angle resolved photoelectron spectroscopy (ARPES). The valence band and core-level spectra obtained by the HAXPES are consistent with the divalent nature of Eu atoms in EuAl$$_4$$. Furthermore, the Fermi surface as well as the band structure in the vicinity of the Fermi Energy ($$E_{rm F}$$) of EuAl$$_4$$ are very similar to those of its isostructural divalent $$mathrm{Sr}$$ compound SrAl$$_4$$, which does not have $$4f$$ electrons. These suggest that Eu atoms are divalent in EuAl$$_4$$, and $$4f$$ electrons are completely localized with $$mathrm{Eu}~4f^7$$ electronic configuration in the ground state. The ARPES spectra measured along the $$Gamma$$-$$(Sigma)$$-Z high-symmetry line did not show significant temperature dependences above and below $$T_{mathrm{CDW}}$$ within the energy resolution of $$80-90~mathrm{meV}$$. Moreover, the Fermi surface mapping along the $$k_z$$ direction showed that both of EuAl$$_4$$ and SrAl$$_4$$ have highly three-dimensional electronic structures, suggesting that the nesting of Fermi surface is not straightforward. The Fermi surface and band structure of SrAl$$_4$$ were well explained by the band-structure calculation based on the local density approximation.


Electronic structures of uranium compounds studied by soft X-ray photoelectron spectroscopy

藤森 伸一; 竹田 幸治; 岡根 哲夫; 斎藤 祐児; 藤森 淳; 山上 浩志; 芳賀 芳範; 山本 悦嗣; 大貫 惇睦

Journal of the Physical Society of Japan, 85(6), p.062001_1 - 062001_33, 2016/06

 被引用回数:31 パーセンタイル:84.12(Physics, Multidisciplinary)

The electronic structures of uranium-based compounds are studied by photoelectron spectroscopies with soft X-ray synchrotron radiation. Angle-resolved photoelectron spectroscopy with soft X-rays made it possible to directly observe their bulk band structures and Fermi surfaces. It is shown that the band structure and Fermi surface of itinerant compounds are quantitatively explained by the band-structure calculation treating all U 5$$f$$ electrons as being itinerant. Furthermore, the overall electronic structures of heavy Fermion compounds are also explained by the band-structure calculation although there exist some disagreements which might be originated from the electron correlation effect. This suggests that the itinerant description of U $$5f$$ states is an appropriate starting point for their description. The local electronic structures of uranium site are probed by the core-level photoelectron spectroscopy with soft X-rays. The comparisons of core-level spectra of these compounds with typical itinerant and localized compounds suggest that the local electronic structures of most of itinerant and heavy Fermion compounds are close to U 5$$f^3$$ configuration.


Recent progress of soft X-ray photoelectron spectroscopy studies of uranium compounds

藤森 伸一; 竹田 幸治; 岡根 哲夫; 斎藤 祐児; 藤森 淳; 山上 浩志; 山本 悦嗣; 芳賀 芳範; 大貫 惇睦

Journal of Electron Spectroscopy and Related Phenomena, 208, p.105 - 110, 2016/04

 被引用回数:1 パーセンタイル:8.8(Spectroscopy)



Hard X-ray photoelectron spectroscopy study for transport behavior of CsI in heating test simulating a BWR severe accident condition; Chemical effects of boron vapors

岡根 哲夫; 小畠 雅明; 佐藤 勇*; 小林 啓介*; 逢坂 正彦; 山上 浩志

Nuclear Engineering and Design, 297, p.251 - 256, 2016/02

 被引用回数:2 パーセンタイル:20.4(Nuclear Science & Technology)

Transport behavior of CsI in the heating test, which simulated a BWR severe accident, was investigated by hard X-ray photoelectron spectroscopy (HAXPES) with an emphasis on the chemical effect of boron vapors. CsI deposited on metal tube at temperatures ranging from 150$$^{circ}$$C to 750$$^{circ}$$C was reacted with vapor/aerosol B$$_2$$O$$_3$$, and the chemical form of reaction products on the sample surface was examined from the HAXPES spectra of core levels, e.g., Ni 2p, Cs 3d and I 3d levels, and valence band. For the samples at $$sim$$300$$^{circ}$$C, while the chemical form of major product on the sample surface without an exposure to B$$_2$$O$$_3$$ was suggested to be CsI from the HAXPES spectra, an intensity ratio of Cs/I was dramatically reduced at the sample surface after the reaction with B$$_2$$O$$_3$$. The results suggest the possibility of significant decomposition of deposited CsI induced by the chemical reaction with B$$_2$$O$$_3$$ at specific temperatures.


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:42 パーセンタイル:83.68(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.


Electronic structures of ferromagnetic superconductors UGe$$_{2}$$ and UCoGe studied by angle-resolved photoelectron spectroscopy

藤森 伸一; 大河内 拓雄*; 川崎 郁斗*; 保井 晃*; 竹田 幸治; 岡根 哲夫; 斎藤 祐児; 藤森 淳; 山上 浩志; 芳賀 芳範; et al.

Physical Review B, 91(17), p.174503_1 - 174503_9, 2015/05

 被引用回数:23 パーセンタイル:68.99(Materials Science, Multidisciplinary)



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:6 パーセンタイル:27.34(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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