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Micheau, C.; 上田 祐生; 元川 竜平; 阿久津 和宏*; 山田 悟史*; 山田 雅子*; Moussaoui, S. A.*; Makombe, E.*; Meyer, D.*; Berthon, L.*; et al.
Journal of Molecular Liquids, 401, p.124372_1 - 124372_12, 2024/05
Supramolecular organization of extractant molecules impacts metal ions separation behavior. Probing bulk and interfacial structures of the relevant systems is expected to provide key insights into the metal ion selectivity and kinetic aspects. The supramolecular features of two solvent extraction systems based on malonamide extractants, N,N,N′,N′-tetrahexylmalonamide (THMA) in toluene and N,N′-dimethyl-N,N′-dibutyl-2-tetradecylmalonamide (DBMA) in n-heptane, were studied using small-angle X-ray scattering for the organic bulk phases, as well as interfacial tension and neutron reflectivity measurements for the interfaces. In the bulk solution, THMA forms dimeric/trimeric associates but no aggregates in toluene, while DBMA forms large aggregates in n-heptane. On the other hand, THMA accumulates in a diffuse layer at the interface at high THMA concentration, whereas DBMA forms a compact but thinner layer. After Pd(II) extraction, the thickness of interfacial layers decreases in the case of THMA, and totally vanishes in the case of DBMA. Based on these new structural information, two mechanisms are proposed for Pd(II) and Nd(III) extraction with malonamides. In toluene, THMA associates slightly accumulate in the vicinity of the interface, then coordinate Pd(II) and diffuse into the organic bulk phase. In n-heptane, DBMA aggregates adsorb at the interface then pick up Nd(III) cations in their polar cores and finally diffuse into the bulk.
Baccou, J.*; Glantz, T.*; Ghione, A.*; Sargentini, L.*; Fillion, P.*; Damblin, G.*; Sueur, R.*; Iooss, B.*; Fang, J.*; Liu, J.*; et al.
Nuclear Engineering and Design, 421, p.113035_1 - 113035_16, 2024/05
被引用回数:0In the Best-Estimate Plus Uncertainty (BEPU) framework, the use of best-estimate code requires to go through a Verification, Validation and Uncertainty Quantification process (VVUQ). The relevance of the experimental data in relation to the physical phenomena of interest in the VVUQ process is crucial. Adequacy analysis of selected experimental databases addresses this problem. The outcomes of the analysis can be used to select a subset of relevant experimental data, to encourage designing new experiments or to drop some experiments from a database because of their substantial lack of adequacy. The development of a specific transparent and reproducible approach to analyze the relevance of experimental data for VVUQ still remains open and is the topic of this contribution. In this paper, the concept of adequacy initially introduced in the OECD/NEA SAPIUM (Systematic APproach for model Input Uncertainty quantification Methodology) activity is formalized. It is defined through two key properties, called representativeness and completeness, that allows considering the multifactorial dimension of the adequacy problem. A new systematic approach is then proposed to analyze the adequacy of a set of experimental databases. It relies on the introduction of two sets of criteria to characterize representativeness and completeness and on the use of multi-criteria decision analysis method to perform the analysis. Finally, the approach is applied in the framework of the new OECD/NEA ATRIUM activity which includes a set of practical IUQ exercises in thermal-hydraulics to test the SAPIUM guideline in determining input uncertainties and forward propagating them on an application case. It allows evaluating the adequacy of eight experimental databases coming from the Super Moby-dick, Sozzi-Sutherland and Marviken experiments and identifying the most adequate ones.
Meer, H.*; Wust, S.*; Schmitt, C.*; Herrgen, P.*; Fuhrmann, F.*; Hirtle, S.*; Bednarz, B.*; Rajan, A.*; Ramos, R.*; Nio, M. A.*; et al.
Advanced Functional Materials, 33(21), p.2213536_1 - 2213536_6, 2023/05
被引用回数:1 パーセンタイル:49.29(Chemistry, Multidisciplinary)The antiferromagnetic order in heterostructures of NiO/Pt thin films can be modified by optical pulses. After the irradiation with laser light, the optically induced creation of antiferromagnetic domains can be observed by imaging the created domain structure utilizing the X-ray magnetic linear dichroism effect. The effect of different laser polarizations on the domain formation can be studied and used to identify a polarization-independent creation of 180 domain walls and domains with 180 different Nel vector orientation. By varying the irradiation parameters, the switching mechanism can be determined to be thermally induced. This study demonstrates experimentally the possibility to optically create antiferromagnetic domains, an important step towards future functionalization of all optical switching mechanisms in antiferromagnets.
伊藤 あずさ; Karmaoui, M.*; Thirunavukkarasu, G.*; Hriljac, J. A.*
APL Materials (Internet), 11(4), p.041105_1 - 041105_9, 2023/04
被引用回数:0 パーセンタイル:0(Nanoscience & Nanotechnology)Composites of zeolite Na-chabazite particles with attached superparamagnetic nanoparticles of FeO and CoFeO ferrite spinels have been produced using a novel solvothermal route. These have been characterized by a combination of techniques including powder X-ray diffraction, X-ray fluorescence spectroscopy, Raman spectroscopy, vibrating sample magnetometry and both scanning and transmission electron microscopy. These confirm the nature of the attached nanoparticles and the microscope images show a good dispersion of nanoparticles with a narrow size range deposit uniformly on the surface of the zeolite particles. The magnetisation is of sufficient strength to allow magnetic separation from solution. Both time and pH dependent Cs uptake experiments show the magnetised systems are still excellent for the rapid uptake of Cs via an ion exchange process with no reduction in property due to the attached nanoparticles.
Yakushev, A.*; Lens, L.*; Dllmann, Ch. E.*; Khuyagbaatar, J.*; Jger, E.*; Krier, J.*; Runke, J.*; Albers, H. M.*; 浅井 雅人; Block, M.*; et al.
Frontiers in Chemistry (Internet), 10, p.976635_1 - 976635_11, 2022/08
被引用回数:11 パーセンタイル:80.03(Chemistry, Multidisciplinary)114番元素フレロビウム(Fl)は現在その化学的性質が研究されている最も重い元素である。Flに関する最初の化学実験では、Flは貴ガス的な性質を持つ元素であると報告された。一方、2番目の研究では、Flは揮発性金属の性質を示すと報告された。より信頼性の高い結論を得るため、我々は更なる実験的研究を行い、二酸化ケイ素と金表面におけるFlの吸着挙動を調べた。その結果、Flは揮発性金属の水銀よりも高い揮発性と低い反応性を示し、一方、貴ガスのラドンよりは反応性が高いことを明らかにした。
Arokiaswamy, J. A.*; Batra, C.*; Chang, J. E.*; Garcia, M.*; Herranz, L. E.*; Klimonov, I. A.*; Kriventsev, V.*; Li, S.*; Liegeard, C.*; Mahanes, J.*; et al.
IAEA-TECDOC-2006, 380 Pages, 2022/00
IAEAの共同研究プロジェクト「シビアアクシデント条件下におけるプロトタイプナトリウム冷却高速炉からの放射性物質の放出」は、シビアアクシデント条件下における、リファレンスとなるナトリウム冷却高速炉の施設内における放射性物質および燃料粒子の存在量の、異なる時間スケールにおける現実的な数値シミュレーションを目的として実施された。解析のスコープは3つに分割され、3つのワークパッケージ(WP)として定義された:(1)炉内ソースターム評価、(2)一次系/格納容器系境界のソースターム評価、および(3)格納容器内の現象分析。WP-1の参加機関の結果を比較すると、希ガスおよび放射性セシウムの放出割合、およびカバーガスへの放射性核種の放出割合はよく一致した。共通の圧力履歴を用いたWP-2の解析では、各機関の解析結果はよく一致し、いずれの機関の解析手法も同程度の精度を有することが示された。先行するWPにおける解析と分離するため、放出割合をあらかじめ設定したスタンドアロンケースがWP-3にて定義された。WP-3の全参加機関によるスタンドアロンケースの解析結果は全般的に一致した。
Khuyagbaatar, J.*; Yakushev, A.*; Dllmann, Ch. E.*; Ackermann, D.*; Andersson, L.-L.*; 浅井 雅人; Block, M.*; Boll, R. A.*; Brand, H.*; Cox, D. M.*; et al.
Physical Review C, 102(6), p.064602_1 - 064602_9, 2020/12
被引用回数:45 パーセンタイル:98.14(Physics, Nuclear)原子番号119及び120を持つ超重元素の合成を目指した探索実験を、それぞれTi+Bk及びTi+Cf核融合-粒子蒸発反応を用いて、ガス充填型反跳分離装置TASCAにて実施した。4ヶ月間におよぶビーム照射実験を行ったが、どちらの元素も検出されず、その生成断面積の上限値は65fb及び200fbであった。119, 120番元素が観測されなかった理由について、安定の島領域の超重元素の核分裂障壁の高さを予測する様々な理論計算値を用いて、核融合-粒子蒸発反応の概念を用いて議論した。
Meleshenkovskii, I.*; 小川 達彦; Sari, A.*; Carrel, F.*; Boudergui, K.*
Nuclear Instruments and Methods in Physics Research B, 483, p.5 - 14, 2020/11
被引用回数:5 パーセンタイル:44.4(Instruments & Instrumentation)核分裂性物質の検知を目的として、制動放射線を検知対象に照射して光核分裂反応を発生させ、放出される中性子線を観測する技術が注目されている。この技術で制動放射線を発生させるための電子加速器は、同等の性能を発揮する中性子源と比べて放射化や即発線量が低く、装置の小型化が容易という利点がある。一方、光核分裂反応は中性子誘導核分裂反応より断面積が低いため、電子線ターゲットや制動放射線の取り出し口、照射野などを最適化することが検知効率の向上に必要となる。本研究では、汎用モンテカルロ放射線輸送計算コードMCNPとPHITSを用いて、最適化に必要な要素を明らかにした。その結果、ターゲットでの制動放射線の生成は原子番号の高い元素の方が有利であるが、発生した光子がターゲット周辺で(,n)二次反応を起こし、中性子を生成するため、光子によって起こる早い光核分裂反応と、中性子による遅い核分裂が混在し、最終的な検出対象である核分裂の発生時間が広がる問題が明らかとなった。また、中性子を生じる二次反応は電子線ターゲットだけではなく、ターゲット周辺の遮蔽材でも発生するため、中性子放出スレッショルドが高い元素を遮蔽材として選択するなどの工夫が必要であることが明らかになった。
Song, C.*; Seo, O.*; 松村 大樹; 廣井 慧*; Cui, Y.-T.*; Kim, J.*; Chen, Y.*; Tayal, A.*; 草田 康平*; 小林 浩和*; et al.
RSC Advances (Internet), 10(34), p.19751 - 19758, 2020/05
被引用回数:0 パーセンタイル:0(Chemistry, Multidisciplinary)To unveil the origin of the hydrogen-storage properties of rhodium nanoparticles (Rh NPs), we investigated the dynamical structural change of Rh NPs using dispersive X-ray absorption fine structure spectroscopy (XAFS). The variation of the Rh-Rh interatomic distance and Debye-Waller factor of Rh NPs with a size of 4.0 and 10.5 nm during hydrogen absorption and desorption suggested that they have a different mechanism for hydrogen absorption, which is that the hydrogen absorption on the inner site has a greater contribution than that on a surface for Rh 4.0 nm. In the case of Rh 10.5 nm, it is opposed to Rh 4.0 nm. This study demonstrates a powerful XAFS method for observing small local structural changes of metal nanoparticles and its importance for understanding of the hydrogen-absorption properties of Rh NPs with an interesting hydrogenation mechanism.
Lokotko, T.*; Leblond, S.*; Lee, J.*; Doornenbal, P.*; Obertelli, A.*; Poves, A.*; Nowacki, F.*; 緒方 一介*; 吉田 数貴; Authelet, G.*; et al.
Physical Review C, 101(3), p.034314_1 - 034314_7, 2020/03
被引用回数:10 パーセンタイル:75.97(Physics, Nuclear)中性子過剰核であるCoに対する()ノックアウト反応が理化学研究所RIBFで測定された。 coincidenceの方法で準位構造が決定され、測定された包括的断面積および排他的断面積から暫定的ではあるがスピン・パリティが決定された。殻模型計算との比較により、Coの低励起状態には球形核と変形核が共存することが示唆された。
Baldrati, L.*; Gomonay, O.*; Ross, A.*; Filianina, M.*; Lebrun, R.*; Ramos, R.*; Leveille, C.*; Fuhrmann, F.*; Forrest, T. R.*; Maccherozzi, F.*; et al.
Physical Review Letters, 123(17), p.177201_1 - 177201_6, 2019/10
被引用回数:118 パーセンタイル:98.37(Physics, Multidisciplinary)We probe the current-induced magnetic switching of insulating antiferromagnet-heavy-metal systems, by electrical spin Hall magnetoresistance measurements and direct imaging, identifying a reversal occurring by domain wall (DW) motion. We observe switching of more than one-third of the antiferromagnetic domains by the application of current pulses. Our data reveal two different magnetic switching mechanisms leading together to an efficient switching, namely, the spin-current induced effective magnetic anisotropy variation and the action of the spin torque on the DWs.
Lam, T.-N.*; Chou, Y.-S.*; Chang, Y.-J.*; Sui, T.-R.*; Yeh, A.-C.*; Harjo, S.; Lee, S. Y.*; Jain, J.*; Lai, B.-H.*; Huang, E.-W.*
Crystals (Internet), 9(8), p.420_1 - 420_8, 2019/08
被引用回数:9 パーセンタイル:67.37(Crystallography)An equal-molar CoCrFeMnNi, face-centered-cubic (fcc) high-entropy alloy (HEA) and a nickel-based superalloy are studied using in situ neutron diffraction experiments. With continuous measurements, the evolution of diffraction peaks is collected for microscopic lattice strain analyses. Cyclic hardening and softening are found in both metallic systems. However, as obtained from the diffraction-peak-width evolution, the underneath deformation mechanisms are quite different. The CoCrFeMnNi HEA exhibits distinct lattice strain and microstructure responses under tension-compression cyclic loadings.
Khuyagbaatar, J.*; Yakushev, A.*; Dllmann, Ch. E.*; Ackermann, D.*; Andersson, L.-L.*; 浅井 雅人; Block, M.*; Boll, R. A.*; Brand, H.*; Cox, D. M.*; et al.
Physical Review C, 99(5), p.054306_1 - 054306_16, 2019/05
被引用回数:24 パーセンタイル:90.61(Physics, Nuclear)Ca+B融合反応を用いて117番元素(Ts)合成実験を行い、117番元素に起因すると思われる4つの崩壊連鎖を観測した。うち2つは長い崩壊連鎖で、Tsの崩壊に起因するものと同定された。他の2つは短い崩壊連鎖で、Tsの崩壊に起因すると考えると矛盾しない。今回の結果と過去の文献値を比較したところ、今回の我々の結果は過去の文献値をほぼ再現し、117番元素合成の事実を強く再確認する結果となった。
Dong, B.-W.*; Baldrati, L.*; Schneider, C.*; 新関 友彦*; Ramos, R.*; Ross, A.*; Cramer, J.*; 齊藤 英治; Klui, M.*
Applied Physics Letters, 114(10), p.102405_1 - 102405_5, 2019/03
被引用回数:11 パーセンタイル:52.56(Physics, Applied)We study the spin Hall magnetoresistance (SMR) in epitaxial -FeO/NiO(001)/Pt stacks, as a function of temperature and thickness of the antiferromagnetic insulating NiO layer. Upon increasing the thickness of NiO from 0 nm to 10 nm, we detect a sign change of the SMR in the temperature range between 10 K and 280 K. This temperature dependence of the SMR in our stacks is different compared to that of previously studied yttrium iron garnet/NiO/Pt, as we do not find any peak or sign change as a function of temperature. We explain our data by a combination of spin current reflection from both the NiO/Pt and -FeO/NiO interfaces and the thickness-dependent exchange coupling mode between the NiO and -FeO layers, comprising parallel alignment for thin NiO and perpendicular alignment for thick NiO.
Lens, L.*; Yakushev, A.*; Dllmann, Ch. E.*; 浅井 雅人; Ballof, J.*; Block, M.*; David, H. M.*; Despotopulos, J.*; Di Nitto, A.*; Eberhardt, K.*; et al.
Radiochimica Acta, 106(12), p.949 - 962, 2018/12
被引用回数:8 パーセンタイル:62.29(Chemistry, Inorganic & Nuclear)半減期449秒の短寿命同位体を用いて、水銀(Hg), タリウム(Tl), 鉛(Pb)の単一原子レベルでのSiO及びAu表面への固体吸着挙動をオンライン気相実験により調べた。超重元素Cn, Nh, Flの吸着エンタルピー測定のためのモデル実験として実施した。短寿命同位体はドイツ重イオン研究所の反跳核分離装置TASCAを用いて生成・分離した。生成核はヘリウムガス中に捕集された後、SiOあるいはAuで表面を覆われたSi検出器で作製されたガスクロマトグラフィーカラムへと導入した。短寿命Tl及びPb同位体は室温においてSiO表面に吸着し、Si検出器で測定することに成功した。一方、HgはSiO表面には吸着せず、Au表面に吸着した。この結果より、本実験のセットアップを用いることで短寿命Hg, Tl, Pb同位体の吸着特性を調べることができると証明され、この手法がCn, Nh, Flの実験にも適用できることが確認された。
Shand, C. M.*; Podolyk, Zs.*; Grska, M.*; Doornenbal, P.*; Obertelli, A.*; Nowacki, F.*; Otsuka, T.*; Sieja, K.*; Tostevin, J. A.*; Tsunoda, T.*; et al.
Physics Letters B, 773, p.492 - 497, 2017/10
被引用回数:25 パーセンタイル:87.8(Astronomy & Astrophysics)Low-lying states in neutron-rich Zn nuclei were measured for the first time via in-beam -ray spectroscopy at RIKEN. These include the 4 to 2 in Zn and the 2 to 0 and 4 to 2 in Zn. The reduced E() energies and increased E(4)/E(2) ratios at =52,54 compared to Zn attest that the magicity is confined just on the neutron number =50 only. The levels observed in Zn suggest the onset of deformation towards heavier Zn isotopes. The data were compared to state-of-the-art shell model calculations.
Morales, A. I.*; Benzoni, G.*; Watanabe, H.*; 角田 佑介*; Otsuka, T.*; 西村 俊二*; Browne, F.*; Daido, R.*; Doornenbal, P.*; Fang, Y.*; et al.
Physics Letters B, 765, p.328 - 333, 2017/02
被引用回数:33 パーセンタイル:92.56(Astronomy & Astrophysics)The level schemes of neutron-rich isotopes Co and Ni were populated in the decay of Fe and studied using -delayed -ray spectroscopy of the decay, at the RIBF in RIKEN, Japan. The experimental results were compared to state-of-the-art shell-model calculations, and indicate a dominance of prolate deformation in the low-lying states, coexisting with spherical states. The decay of the isobars is shown to progress in accordance to a new type of shell evolution, the so-called Type II, which involves many particle-hole excitations across energy gaps.
Lang, R.*; Li, T.*; 松村 大樹; Miao, S.*; Ren, Y.*; Cui, Y.-T.*; Tan, Y.*; Qiao, B.*; Li, L.*; Wang, A.*; et al.
Angewandte Chemie; International Edition, 55(52), p.16054 - 16058, 2016/12
Single-atom catalysts have the advantages of both homogeneous catalysts, such as "isolated sites", and heterogeneous catalysts, such as stability and reusability, and thus would be a promising alternative to traditional homogeneous catalysts. In the hydroformylation of olefins, single-atom Rh catalysts supported on ZnO nanowires demonstrate similar efficiency (TON 40000) compared to that of homogeneous Wilkinson's catalyst (TON 19000). HAADF-STEM and infrared CO chemisorption experiments identified isolated Rh atoms on the support. XPS and XANES spectra indicate that the electronic state of Rh is almost metallic. The catalysts are about one or two orders of magnitude more active than most reported heterogeneous catalysts and can be reused four times without an obvious decline in activity.
Morales, A. I.*; Benzoni, G.*; Watanabe, H.*; 西村 俊二*; Browne, F.*; Daido, R.*; Doornenbal, P.*; Fang, Y.*; Lorusso, G.*; Patel, Z.*; et al.
Physical Review C, 93(3), p.034328_1 - 034328_14, 2016/03
被引用回数:25 パーセンタイル:84.88(Physics, Nuclear)Low-lying excited states in Ni have been investigated at RIKEN by studying the decay of Co to Ni. Co was separated with BigRIPS, implanted into the WaS3ABi Silicon array, and the ray measured using the EURICA spectrometer. From the analysis, 60 new -ray transitions and 21 new levels in Ni were observed. The new experimental information is compared to shell-model calculations which include neutron excitation across the shell. The calculations reproduce rather well the observed states, implying that a clear understanding of these low-lying excitations has been achieved.
Geprgs, S.*; Kehlberger, A.*; Coletta, F.*; Qiu, Z.*; Guo, E.-J.*; Schulz, T.*; Mix, C.*; Meyer, S.*; Kamra, A.*; Althammer, M.*; et al.
Nature Communications (Internet), 7, p.10452_1 - 10452_6, 2016/02
被引用回数:155 パーセンタイル:97.39(Multidisciplinary Sciences)Magnons are the elementary excitations of a magnetically ordered system. Here, we show that the spin Seebeck effect is sensitive to the complexities of the magnon spectrum. The spin Seebeck effect is caused by a thermally excited spin dynamics that is converted to a voltage by the inverse spin Hall effect at the interface to a heavy metal contact. By investigating the temperature dependence of the spin Seebeck effect in the ferrimagnet gadlinium iron garnet, with a magnetic compensation point near room temperature, we demonstrate that high-energy exchange magnons play a key role in the spin Seebeck effect.