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High temperature reaction of multiple eutectic-component system; The Case of solid metallic Zr and molten stainless steel-B$$_{4}$$C

墨田 岳大; 小畠 雅明; 高野 公秀; 池田 篤史

Materialia, 20, p.101197_1 - 101197_11, 2021/12

The eutectic melting, one of the fundamental phenomena in high temperature reactions involving liquid phases, is a primitive but important subject for both scientific and industrial fields associated with metallurgy. The present study aims at revealing the formation and reaction mechanisms of the multiple eutectic-component system consisting of solid metallic Zr and molten stainless steel- boron carbide (SS-B$$_{4}$$C) by combining multiple analytical methods (i.e. powder X-ray diffraction (PXRD), scanning electron microscopy- energy dispersive X-ray spectroscopy (SEM-EDS), and dynamic secondary ion mass spectrometry (D-SIMS)) with thermodynamical consideration. The results indicate that the solidified Zr-SS-B$$_{4}$$C mixture is composed of major phases of (Fe,Cr)$$_{2}$$Zr, (Fe,Cr,Ni)$$_{2}$$Zr, (Ni,Fe)Zr$$_{2}$$, ZrB$$_{2}$$, and a minor phase of ZrC. The results also reveal that the eutectic melting between solid metallic Zr and molten SS-B$$_{4}$$C can be described as the combination of diffusion kinetics and thermodynamic stability. That is, the initial formation of ZrC and ZrB$$_{2}$$ layers at the reaction interface significantly retards the diffusion of other SS-B$$_{4}$$C components (i.e. Cr, Fe, and Ni) into solid metallic Zr.


Tolerance of spin-Seebeck thermoelectricity against irradiation by swift heavy ions

岡安 悟; 針井 一哉*; 小畠 雅明; 吉井 賢資; 福田 竜生; 石田 真彦*; 家田 淳一; 齊藤 英治

Journal of Applied Physics, 128(8), p.083902_1 - 083902_7, 2020/08

 被引用回数:0 パーセンタイル:0(Physics, Applied)

The ion-irradiation tolerance of thermoelectric devices based on the spin Seebeck effect (SSE) was investigated by using 320 MeV gold ion (Au$$^{24+}$$) beams modeling cumulative damages due to fission products emitted from the surface of spent nuclear fuels. For this purpose, prototypical Pt/Y$$_3$$Fe$$_5$$O$$_{12}$$/Gd$$_3$$Ga$$_5$$O$$_{12}$$ SSE elements were irradiated with varying the dose level at room temperature and measured the SSE voltage of them. We confirmed that the thermoelectric and magnetic properties of the SSE elements are not affected by the ion-irradiation up to $$10^{10}$$ ions/cm$$^2$$ fluence and that the SSE signal is extinguished around $$10^{12}$$ ions/cm$$^2$$, in which the ion tracks almost fully cover the sample surface. We also performed the hard X-ray photoemission spectroscopy (HAXPES) measurements to understand the effects at the interface of Pt/Y$$_3$$Fe$$_5$$O$$_{12}$$. The HAXPES measurements suggest that the chemical reaction that diminishes the SSE signals is enhanced with the increase of the irradiation dose. The present study demonstrates that SSE-based devices are applicable to thermoelectric generation even in harsh environments for a long time period.


Electronic structure of trivalent compound EuPd$$_3$$ studied by soft X-ray angle-resolved photoemission spectroscopy

川崎 郁斗; 小畠 雅明; 藤森 伸一; 竹田 幸治; 山上 浩志; 仲村 愛*; 伊覇 航*; 辺土 正人*; 仲間 隆男*; 大貫 惇睦*

Journal of the Physical Society of Japan, 89(4), p.044704_1 - 044704_6, 2020/04

 被引用回数:1 パーセンタイル:34.55(Physics, Multidisciplinary)

EuPd$$_3$$ is a rare Eu-based compound, whose Eu ions are in a trivalent state. The electronic structure of EuPd$$_3$$ was investigated by angle-resolved photoemission spectroscopy (ARPES) using soft X rays. Eu$$^{3+}$$ components arising from the 4f$$^5$$ final state multiplet were clearly observed in the valence spectra, and no Eu$$^{2+}$$ components were observed within an experimental accuracy, confirming a robust Eu$$^{3+}$$ state. The band structure and Fermi surfaces revealed by ARPES measurements were compared to the band structure calculations based on the density-functional theory for LaPd$$_3$$ andYPd$$_3$$. We found that the calculation for LaPd$$_3$$ provides a better description for our ARPES results. The effective electron masses estimated from the ARPES spectra near the Fermi level are in good agreement with the corresponding cyclotron effective masses in previous de Haas-van Alphen experiments.


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:5 パーセンタイル:52.83(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.



小畠 雅明; 岡根 哲夫; 小林 啓介*

分光研究, 67(4), p.161 - 162, 2018/08



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:8 パーセンタイル:81.85(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:5 パーセンタイル:36.26(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:6 パーセンタイル:36.26(Materials Science, Multidisciplinary)

The electronic structures of U$$X_3$$ ($$X$$=Al, Ga, and In) were studied by photoelectron spectroscopy to understand the 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.


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:6 パーセンタイル:41.6(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:7 パーセンタイル:56.42(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.


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:1 パーセンタイル:14.48(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.



小畠 雅明; 小林 啓介*

Journal of the Vacuum Society of Japan, 58(2), p.43 - 49, 2015/02




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.

no journal, , 

体心正方晶(BaAl$$_4$$型)を持つEuAl$$_4$$は、T=15K付近で反強磁性体で、T=140Kでフェルミ面のネスティング効果による電荷密度波(CDW)を示唆する肩構造が電気抵抗に現れる興味深い物性をもつ物質である。この物性を理解するためにEuAl$$_4$$のバンド構造とフェルミ面に関する情報を得ることは物理的に重要である。そこで、本研究では、EuAl$$_4$$のバンド構造とフェルミ面の形状を実験的に決めることを目的とし、原子力機構専用ビームラインBL23SU(SPring-8)で軟X線角度分解光電子分光(SX-ARPES)実験を行った。その結果から、EuAl$$_4$$のEuは、2価であることが分かった。また、この物質の4${it f}$バンドはフェルミ準位以下の約1eVの所に存在した。そのため、フェルミ面は4${it f}$バンド以外の価電子からできていると考えられる。そこで、4${it f}$電子の価電子帯への寄与をより明確にするために、同じ結晶構造で${it f}$電子をもたないSrAl$$_4$$の電子状態と比較することが有効と考え、両者の電子構造について比較を行った。両者のフェルミ付近のバンド構造やフェルミ面の形状は、類似することが分かった。講演では、バンド計算と比較して、この化合物の電子状態について報告する。



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

no journal, , 



Electronic structure of UGa$$_3$$ studied by angle-resolved 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*

no journal, , 

遍歴反強磁性体であるUGa$$_3$$に対して角度分解光電子分光を行ってその電子状態を調べた。UGa$$_3$$$$T_{rm N}=$$67Kの反強磁性体であり、典型的なウラン化合物金属である。その電子状態に対して多くの研究があるにもかかわらず、その詳細な電子状態は明らかとなっていない。UGa$$_3$$のバンド構造とフェルミ面を実験的に明らかにし、フェルミ準位付近に5f電子に起因する準粒子バンドが存在することが明らかとなった。さらに測定温度を変化させることにより、反強磁性転移に伴う電子状態の変化を研究した。



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; 藤森 伸一

no journal, , 

反強磁性ウラン化合物UGa$$_{3}$$に対して軟X線ARPES (SX-ARPES)を行って、バンド構造とフェルミ面の導出を行った結果について報告する。UGa$$_{3}$$はTN=67Kの反強磁性体であるが、電子状態については研究例が少ないためほとんど明らかになっていない状況にある。実験の結果、フェルミ準位近傍にはU 5f電子に起因した狭いバンドが観測され、さらにR点周りに大きなホールフェルミ面を形成していることが明らかとなった。講演ではバンド計算との比較も示し、この化合物の電子状態について議論する。



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.

no journal, , 

角度分解光電子分光によりThRu$$_{2}$$Si$$_{2}$$のバンド構造およびフェルミ面の導出を行った結果について報告する。バンド計算の結果との比較を行い、その電子状態について議論する。さらにURu$$_{2}$$Si$$_{2}$$に対する実験結果との比較を行って、URu$$_{2}$$Si$$_{2}$$のバンド構造とフェルミ面におけるU 5f電子状態の寄与についても議論する。

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