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論文

Strong low-energy rattling modes enabled liquid-like ultralow thermal conductivity in a well-ordered solid

Liu, P.-F.*; Li, X.*; Li, J.*; Zhu, J.*; Tong, Z.*; 古府 麻衣子*; 楡井 真実; Xu, J.*; Yin, W.*; Wang, F.*; et al.

National Science Review, 11(12), p.nwae216_1 - nwae216_10, 2024/12

 被引用回数:13 パーセンタイル:94.32(Multidisciplinary Sciences)

Crystalline solids exhibiting inherently low lattice thermal conductivity ($$kappa_{rm L}$$) are of great importance in applications such as thermoelectrics and thermal barrier coatings. However, $$kappa_{rm L}$$ cannot be arbitrarily low and is limited by the minimum thermal conductivity related to phonon dispersions. In this work, we report the liquid-like thermal transport in a well-ordered crystalline CsAg$$_5$$Te$$_3$$, which exhibits an extremely low $$kappa_{rm L}$$ value of $$sim$$ 0.18 Wm$$^{-1}$$K$$^{-1}$$. On the basis of first-principles calculations and inelastic neutron scattering measurements, we find that there are lots of low-lying optical phonon modes at $$sim$$ 3.1 meV hosting the avoided-crossing behavior with acoustic phonons. These strongly localized modes are accompanied by weakly bound rattling Ag atoms with thermally induced large amplitudes of vibrations. Using the two-channel model, we demonstrate that coupling of the particle-like phonon modes and the heat-carrying wave-like phonons is essential for understanding the low $$kappa_{rm L}$$, which is heavily deviated from the $$1/T$$ temperature dependence of the standard Peierls theory. In addition, our analysis indicates that the soft structural framework with liquid-like motions of the fluctuating Ag atoms is the underlying cause that leads to the suppression of the heat conduction in CsAg$$_5$$Te$$_3$$. These factors synergistically account for the ultralow $$kappa_{rm L}$$ value. Our results demonstrate that the liquid-like heat transfer could indeed exist in a well-ordered crystal.

論文

Brightening triplet excitons enable high-performance white-light emission in organic small molecules via integrating n-$$pi^*/pi$$-$$pi^*$$ transitions

Yang, Q.*; Yang, X.*; Wang, Y.*; Fei, Y.*; Li, F.*; Zheng, H.*; Li, K.*; Han, Y.*; 服部 高典; Zhu, P.*; et al.

Nature Communications (Internet), 15, p.7778_1 - 7778_9, 2024/09

 被引用回数:11 パーセンタイル:88.19(Multidisciplinary Sciences)

明るい一重項励起子と三重項励起子を同時に発現する発光材料は、オプトエレクトロニクス、サイネージ、情報暗号化において大きな可能性を秘めている。しかしながら、高性能の白色発光を実現するためには、蛍光と燐光の寄与が不均衡であることが大きな障害となっている。ここでは、水素結合の協同効果による圧力処理エンジニアリングによって、n-$$pi^*/pi$$-$$pi^*$$遷移の混合を実現し、イソフタル酸(IPA)中で三重項状態の発光を7%から40%に高めることで、この課題に対処した。加圧処理したIPAでは、蛍光と燐光のハイブリッドに基づく優れた白色発光が得られ、フォトルミネッセンス量子収率は当初の19%(青色発光)から75%に増加した。その場での高圧IRスペクトル、X線回折、中性子回折から、圧力の上昇に伴い水素結合が連続的に強化されることが明らかになった。さらに、この強化された水素結合は、圧力処理後も常圧条件下まで保持され、バランスの取れた一重項/三重項励起子集団のための効率的な系間交差を目的としたIPAに与え、効率的な白色発光をもたらした。この研究は、有機低分子の三重項状態を明るくするルートを提案するだけでなく、一重項励起子と三重項励起子の比率を調節して、高性能の白色発光を構築するものである。

論文

Anomalous dislocation response to deformation strain in CrFeCoNiPd high-entropy alloys with nanoscale chemical fluctuations

Ying, H.*; Yang, X.*; He, H.*; Yan, A.*; An, K.*; Ke, Y.*; Wu, Z.*; Tang, S.*; Zhang, Z.*; Dong, H.*; et al.

Scripta Materialia, 250, p.116181_1 - 116181_7, 2024/09

 被引用回数:2 パーセンタイル:36.18(Nanoscience & Nanotechnology)

Nanoscale chemical fluctuations and their effect on the deformation behavior of CrFeCoNi-based high-entropy alloys (HEAs) were investigated using small-angle scattering and in situ neutron diffraction measurements. Small-angle scattering results demonstrated the presence of nano ($$>$$10 nm) chemical fluctuations in the as-prepared CrFeCoNiPd HEAs, which was attributed to the negative mixing of enthalpy and the significant atomic radius difference between Pd and the constituent elements in the CrFeCoNi-based alloys. Subsequent tensile tests demonstrated that the yield and tensile strengths of the as-prepared CrFeCoNiPd HEA surpass those of the as-prepared CrMnFeCoNi HEA. Neutron diffraction data analysis revealed an anomalous response of dislocation evolution with the strain.

論文

Archie's cementation factors for natural rocks; Measurements and insights from diagenetic perspectives

Yuan, X.*; Hu, Q. H.*; Fang, X.*; Wang, Q. M.*; Ma, Y.*; 舘 幸男

Sedimentary Geology, 465, p.106633_1 - 106633_14, 2024/05

 被引用回数:0 パーセンタイル:0.00(Geology)

Archie's cementation factor, m, is a critical parameter for petrophysical studies, and the value is influenced by several factors such as the shape, type, and size of grains, degrees of diagenesis, and associated pore structure. Using integrated experimental and theoretical approaches, the goal of this study is to obtain the cementation factor of rocks (both reservoir rock and caprock) and assess the impact of diagenesis processes on the values of the cementation factor. Thirteen samples of geologically diverse rocks (six mudstones, four fossiliferous limestones, two marbles, and one sandstone) were selected to achieve these research objectives. Two approaches, the diffusion of gas tracers and the Bosanquet formula calculation using pore-throat sizes from mercury intrusion porosimetry analyses, were used to derive the cementation factors of these rock samples. These rocks were categorized into two groups based on the correlation between average pore-throat diameter and diffusivity, and an exponential-law relationship between the cementation factor and porosity was determined for these sample groups. In addition, thin-section petrography and field emission-scanning electron microscopy observations were utilized to investigate diagenetic processes, with four diagenetic patterns being established: (1) strong compaction, strong cementation, and weak dissolution-diagenesis pattern; (2) weak compaction, medium cementation, and weak dissolution-diagenesis pattern; (3) weak compaction, medium cementation, and strong dissolution-diagenesis pattern; and (4) fracture-matrix pattern. The results indicated that diagenetic processes and microfractures contribute to the variability in the cementation factors in these rock samples.

論文

Petrophysical properties of representative geological rocks encountered in carbon storage and utilization

Hu, Q.*; Wang, Q. M.*; Zhang, T.*; Zhao, C.*; Iltaf, K. H.*; Liu, S. Q.*; 深津 勇太

Energy Reports (Internet), 9, p.3661 - 3682, 2023/12

 被引用回数:11 パーセンタイル:64.37(Energy & Fuels)

This study evaluates petrophysical properties of representative geological rocks in the context of injectivity, storage space, and caprock integrity for effective utilization and long-term storage of carbon dioxide. A total of 10 geological rocks were selected as representative storage media for consideration as saline aquifers & depleted oil and gas reservoirs, basalts, and cap rocks, as well as utilization in organic-rich shale and coal seams. An integrated suite of laboratory tests, including liquid immersion porosimetry, gas expansion porosimetry, grain size distribution, mercury intrusion porosimetry, and gas diffusion, were performed on these various rock samples. The results exhibit a disparity of petrophysical properties among two broad groups of rocks: rocks selected for possible storage of CO$$_{2}$$ have porosities of $$sim$$10-25%, permeabilities of $$sim$$10$$^{-16}$$-10$$^{-13}$$ m$$^{2}$$, $$mu$$m-sized pore-throat size distribution, and mostly good pore connectivity; in contrast, the potential caprocks have porosities of $$sim$$0.5-5%, permeabilities of $$sim$$10$$^{-20}$$-10$$^{-18}$$ m$$^{2}$$, pore throat sizes of $$<$$50 nm, and probably poorly connected pore networks. An understanding of the measured facets of pore structure and contribution of fractures is also critical in the context of different testing principles and data interpretation of petrophysical analyses, as well as observational scales in the laboratory and field, and therefore reliable confidence of CO$$_{2}$$ storage and utilization performance. Our work further illustrates the controlling influence of grain size distribution and geological processes on pore size distribution and pore connectivity for a wide range of rock types and lithologies, and particularly presents the extent and behavior of CO$$_{2}$$ gas diffusion with a custom-designed apparatus for a holistic understanding of various petrophysical attributes of widely different geological rocks.

論文

Extreme phonon anharmonicity underpins superionic diffusion and ultralow thermal conductivity in argyrodite Ag$$_{8}$$SnSe$$_{6}$$

Ren, Q.*; Gupta, M. K.*; Jin, M.*; Ding, J.*; Wu, J.*; Chen, Z.*; Lin, S.*; Fabelo, O.*; Rodriguez-Velamazan, J. A.*; 古府 麻衣子; et al.

Nature Materials, 22(8), p.999 - 1006, 2023/08

 被引用回数:78 パーセンタイル:99.19(Chemistry, Physical)

Ultralow thermal conductivity and fast ionic diffusion endow superionic materials with excellent performance both as thermoelectric converters and as solid-state electrolytes. Yet the correlation and interdependence between these two features remain unclear owing to a limited understanding of their complex atomic dynamics. Here we investigate ionic diffusion and lattice dynamics in argyrodite Ag$$_{8}$$SnSe$$_{6}$$ using synchrotron X-ray and neutron scattering techniques along with machine-learned molecular dynamics. We identify a critical interplay of the vibrational dynamics of mobile Ag and a host framework that controls the overdamping of low-energy Ag-dominated phonons into a quasi-elastic response, enabling superionicity. Concomitantly, the persistence of long-wavelength transverse acoustic phonons across the superionic transition challenges a proposed 'liquid-like thermal conduction' picture. Rather, a striking thermal broadening of low-energy phonons, starting even below 50 K, reveals extreme phonon anharmonicity and weak bonding as underlying features of the potential energy surface responsible for the ultralow thermal conductivity ($$<$$ 0.5 Wm$$^{-1}$$K$$^{-1}$$) and fast diffusion. Our results provide fundamental insights into the complex atomic dynamics in superionic materials for energy conversion and storage.

論文

Pressure-modulated magnetism and negative thermal expansion in the Ho$$_2$$Fe$$_{17}$$ intermetallic compound

Cao, Y.*; Zhou, H.*; Khmelevskyi, S.*; Lin, K.*; Avdeev, M.*; Wang, C.-W.*; Wang, B.*; Hu, F.*; 加藤 健一*; 服部 高典; et al.

Chemistry of Materials, 35(8), p.3249 - 3255, 2023/04

 被引用回数:4 パーセンタイル:20.33(Chemistry, Physical)

静水圧や化学圧力は、結晶構造を変化させる効率的な刺激であり、材料科学において電気的、磁気的特性のチューニングによく利用されている。しかし、化学圧力は定量化が困難であり、これら両者の定量的な対応関係はまだよくわかっていない。本研究では、負の熱膨張(NTE)を持つ永久磁石の候補である金属間化合物を調べた。放射光X線その場観察により、AlをドープしたHo$$_2$$Fe$$_{17}$$に負の化学圧力があることを明らかにし、単位セル体積の温度・圧力依存性を用いそれを定量的に評価した。また、磁化測定と中性子回折測定を組み合わせることで、磁気秩序に対する化学圧力と静水圧の違いを比較した。興味深いことに、圧力はNTEの抑制と増強を制御するために使用することができた。電子状態計算から、圧力がFermiレベル(EF)に対する主要バンドの上部に影響を与えたことを示しており、これは磁気安定性に影響を与え、それが磁気とNTEを調節する上で重要な役割を果たしていることがわかった。本研究は、圧力の影響を理解し、それを利用して機能性材料の特性を制御する良い例を示している。

論文

Pore connectivity influences mass transport in natural rocks; Pore structure, gas diffusion and batch sorption studies

Yuan, X.*; Hu, Q.*; Lin, X.*; Zhao, C.*; Wang, Q.*; 舘 幸男; 深津 勇太; 濱本 昌一郎*; Siitari-Kauppi, M.*; Li, X.*

Journal of Hydrology, 618, p.129172_1 - 129172_15, 2023/03

 被引用回数:6 パーセンタイル:58.63(Engineering, Civil)

Mass transport in geomedia as influenced by the pore structure is an important phenomenon. Six rocks (granodiorite, limestone, two chalks, mudstone, and dolostone) with different extents of heterogeneity at six different particle sizes were studied to describe the effects of pore connectivity on mass transport. The multiple methods applied were porosity measurement, gas diffusion test, and batch sorption test of multiple ions. Porosity measurement results reveal that with decreasing particle sizes, the effective porosities for the "heterogenous" group (granodiorite and limestone) increase, whereas the porosities of "homogeneous" group (chalks, mudstone, and dolostone) roughly remain constant. Gas diffusion results show that the intraparticle gas diffusion coefficient among these two groups, varying in the magnitude of 10$$^{-8}$$ to 10$$^{-6}$$ m$$^{2}$$/s. The batch sorption work displays a different affinity of these rocks for tracers, which are related to their mineral components. For granodiorite, mudstone, and dolostone, the adsorption capacity increases as the particle size decreases, due to higher specific surface area in smaller particle-size. In general, this integrated research of grain size distribution, rock porosity, intraparticle diffusivity, and ionic sorption capacity gives insights into the pore connectivity effect on both gas diffusion and chemical transport behaviors for different lithologies and/or different particle sizes.

論文

Micro- to nano-scale areal heterogeneity in pore structure and mineral compositions of a sub-decimeter-sized Eagle Ford Shale

Wang, Q.*; Hu, Q.*; Zhao, C.*; Yang, X.*; Zhang, T.*; Ilavsky, J.*; Kuzmenko, I.*; Ma, B.*; 舘 幸男

International Journal of Coal Geology, 261, p.104093_1 - 104093_15, 2022/09

 被引用回数:12 パーセンタイル:69.82(Energy & Fuels)

To understanding the spatial heterogeneity of mineral and pore structure variations in fine-grained shale, microscale X-ray fluorescence (micro-XRF) mapping, (ultra-) small-angle X-ray scattering [(U)SAXS] and wide-angle X-ray scattering were applied for two samples from a piece of Eagle Ford Shale in South Texas. Thin section petrography and field emission-scanning electron microscopy, X-ray diffraction (XRD), total organic carbon, and pyrolysis were also utilized to investigate the potential spatial heterogeneity of pore types, mineral and organic matter compositions for both samples. Overall, the siliceous-carbonate mineral contents in these carbonate-rich Eagle Ford Shale vary between laminations at mm scales. By analyzing six selected sub-samples on each of two samples with X-ray scattering and XRD techniques, nm-sized pores are mainly interparticle ones in the higher calcite regions, where the porosity is also relatively lower, while the lower calcite regions consist of both interparticle and intraparticle pore types with higher porosity. Finally, the micro-XRF and (U)SAXS are combined to generate porosity distribution maps to provide more insights about its heterogeneity related to the laminations and fractures at our observational scales.

論文

Structure of an aqueous RbCl solution in the gigapascal pressure range by neutron diffraction combined with empirical potential structure refinement modeling

Zhang, W. Q.*; 山口 敏男*; Fang, C. H.*; 吉田 亨次*; Zhou, Y. Q.*; Zhu, F. Y.*; 町田 真一*; 服部 高典; Li, W.*

Journal of Molecular Liquids, 348, p.118080_1 - 118080_11, 2022/02

 被引用回数:3 パーセンタイル:24.49(Chemistry, Physical)

3mol/kgのRbCl水溶液におけるイオンの水和・会合と水素結合した水の構造を、298K/0.1MPa, 298K/1GPa, 523K/1GPa, 523K/4GPaにおける中性子回折と経験的ポテンシャル構造精密化モデリングにより調べた。その結果、構造パラメータは温度と圧力に依存していることがわかった。高圧・高温条件では、Rb$$^+$$とCl$$^-$$の第二水和層がより明確になる。第一水和層におけるRb$$^+$$の平均酸素配位数は、配位距離を0.290nmから0.288nmに縮めながら、常圧では6.3だったのが、4GPaでは8.9に増加した。第一水和シェルのCl$$^-$$の平均酸素配位数は、常圧で5.9、4GPaで9.1と圧力により増加し、対応する配位距離は0.322nmから0.314nmへと減少した。Rb$$^+$$と中心の水分子の第一溶媒和シェルにおける水双極子の配向は圧力に敏感であるが、Cl$$^-$$の第一溶媒和シェルにおける水双極子の配向は温度圧力によらずあまり変化しなかった。Rb$$^+$$-Cl$$^-$$の隣接イオンペアの数は、温度が高くなると減少し、圧力が高くなると増加する。水分子は密に詰まっており、極限状態では水分子の四面体水素結合ネットワークはもはや存在しない。

論文

The $$^{59}$$Fe(n,$$gamma$$)$$^{60}$$Fe cross section from the surrogate ratio method and its effect on the $$^{60}$$Fe nucleosynthesis

Yan, S. Q.*; Li, X. Y.*; 西尾 勝久; Lugaro, M.*; Li, Z. H.*; 牧井 宏之; Pignatari, M.*; Wang, Y. B.*; Orlandi, R.; 廣瀬 健太郎; et al.

Astrophysical Journal, 919(2), p.84_1 - 84_7, 2021/10

 被引用回数:5 パーセンタイル:33.27(Astronomy & Astrophysics)

The long-lived $$^{60}$$Fe (with a half-life of 2.62 Myr) is a crucial diagnostic of active nucleosynthesis in the Milky Way galaxy and in supernovae near the solar system. The neutron-capture reaction $$^{59}$$Fe(n,$$gamma$$)$$^{60}$$Fe on $$^{59}$$Fe (half-life=44.5 days) is the key reaction for the production of $$^{60}$$Fe in massive stars. This reaction cross section has been previously constrained by the Coulomb dissociation experiment, which offered partial constraint on the E1 $$gamma$$-ray strength function but a negligible constraint on the M1 and E2 components. In this work, for the first time, we use the surrogate ratio method to experimentally determine the $$^{59}$$Fe(n,$$gamma$$)$$^{60}$$Fe cross sections in which all the components are included. We derived a Maxwellian-averaged cross section of 27.5$$pm$$3.5 mb at $$kT$$ = 30 keV and 13.4$$pm$$1.7 mb at $$kT$$ = 90 keV, roughly 10%-20% higher than previous estimates. We analyzed the impact of our new reaction rates in nucleosynthesis models of massive stars and found that uncertainties in the production of $$^{60}$$Fe from the $$^{59}$$Fe(n,$$gamma$$)$$^{60}$$Fe rate are at most 25$$%$$. We conclude that stellar physics uncertainties now play a major role in the accurate evaluation of the stellar production of $$^{60}$$Fe.

論文

Suppressed lattice disorder for large emission enhancement and structural robustness in hybrid lead iodide perovskite discovered by high-pressure isotope effect

Kong, L.*; Gong, J.*; Hu, Q.*; Capitani, F.*; Celeste, A.*; 服部 高典; 佐野 亜沙美; Li, N.*; Yang, W.*; Liu, G.*; et al.

Advanced Functional Materials, 31(9), p.2009131_1 - 2009131_12, 2021/02

 被引用回数:33 パーセンタイル:82.86(Chemistry, Multidisciplinary)

有機-無機ハロゲン化物ペロブスカイトは非常に柔らかいために、圧力などの外部刺激により格子定数を容易に変化させることができ、有用な光電特性を引き出すのに有効である。一方でこの特性は、多少の加圧でも、格子を歪ませてしまい、光と物質の相互作用を弱め、それによる性能の低下を引き起こす。そこで本研究では、代表的な物質であるヨウ化メチルアンモニウム鉛に対して圧力効果および同位体効果を調べ、それらが格子歪を抑制することが分かった。このことは、それらが、これまで得られなかったような光学的,機械的特性を持つ物質を得る手段として有効であることを示している。

論文

Influence of pH, competing ions, and salinity on the sorption of strontium and cobalt onto biogenic hydroxyapatite

Handley-Sidhu, S.*; Mullan, T. K.*; Grail, Q.*; Albadarneh, M.*; 大貫 敏彦; Macaskie, L. E.*

Scientific Reports (Internet), 6, p.23361_1 - 23361_8, 2016/03

 被引用回数:65 パーセンタイル:86.55(Multidisciplinary Sciences)

微生物起源アパタイトは、Sr$$^{2+}$$およびCo$$^{2+}$$の吸着において、非生物的に合成したアパタイトよりも優れた性能を示した。微生物起源アパタイトの有する非晶質のCaリン酸塩の表面が、その原因である。したがって、生物起源アパタイトは、汚染地下水の浄化材料として優れている。

論文

Port-based plasma diagnostic infrastructure on ITER

Pitcher, C. S.*; Barnsley, R.*; Bertalot, L.*; Encheva, A.*; Feder, R.*; Friconneau, J. P.*; Hu, Q.*; Levesy, B.*; Loesser, G. D.*; Lyublin, B.*; et al.

Fusion Science and Technology, 64(2), p.118 - 125, 2013/08

 被引用回数:5 パーセンタイル:36.22(Nuclear Science & Technology)

ITERにおいて計測装置を設置するための基盤構造である上部及び水平ポートプラグの共通部分に関する統合設計をまとめたものである。本設計は、ITER機構が組織した各国数名からなる設計タスクフォースにより実施され、ポートプラグの成立に必要なすべての作業を網羅したものである。検討の結果、一つのポートプラグに複数の計測装置が入る水平ポートプラグでは、計測器毎の干渉を避けると同時に保守を考慮した3から6のユニット構造を提案し、さらに発生する電磁力の低減をはかった。また、真空容器外のインタースペースやポートセルへの設置についても考慮し、ポートプラグ及び計測装置の一体化の検討を行った。会議では懸案となっている中性子遮蔽性能の改善策についても併せて報告する。

論文

Diluted ferromagnetic semiconductor Li(Zn,Mn)P with decoupled charge and spin doping

Deng, Z.*; Zhao, K.*; Gu, B.; Han, W.*; Zhu, J. L.*; Wang, X. C.*; Li, X.*; Liu, Q. Q.*; Yu, R. C.*; 後神 達郎*; et al.

Physical Review B, 88(8), p.081203_1 - 081203_5, 2013/08

 被引用回数:77 パーセンタイル:91.56(Materials Science, Multidisciplinary)

We report the discovery of a diluted magnetic semiconductor, Li(Zn,Mn)P, in which charge and spin are introduced independently via lithium off-stoichiometry and the isovalent substitution of Mn$$^{2+}$$ for Zn$$^{2+}$$, respectively. Isostructural to (Ga,Mn)As, Li(Zn,Mn)P was found to be a ${it p}$-type ferromagnetic semiconductor with excess lithium providing charge doping. First-principles calculations indicate that excess Li is favored to partially occupy the Zn site, leading to hole doping. Ferromagnetism with Curie temperature up to 34 K is achieved while the system still shows semiconducting transport behavior.

論文

Nuclear engineering of diagnostic port plugs on ITER

Pitcher, C. S.*; Barnsley, R.*; Feder, R.*; Hu, Q.*; Loesser, G. D.*; Lyublin, B.*; Padasalagi, S.*; Pak, S.*; Reichle, R.*; 佐藤 和義; et al.

Fusion Engineering and Design, 87(5-6), p.667 - 674, 2012/08

 被引用回数:12 パーセンタイル:63.74(Nuclear Science & Technology)

The nuclear engineering infrastructure for port-based diagnostics on ITER is presented, including the equatorial and upper port plug generic designs, the adopted modular concept, the loads and associated load response and the remote handling.

論文

Li(Zn,Mn)As as a new generation ferromagnet based on a I-II-V semiconductor

Deng, Z.*; Jin, C. Q.*; Liu, Q. Q.*; Wang, X. C.*; Zhu, J. L.*; Feng, S. M.*; Chen, L. C.*; Yu, R. C.*; Arguello, C.*; 後神 達郎*; et al.

Nature Communications (Internet), 2, p.1425_1 - 1425_5, 2011/08

 被引用回数:172 パーセンタイル:93.60(Multidisciplinary Sciences)

(Ga,Mn)Asは典型的な強磁性III-V族半導体として知られている。これは3価のGa原子を2価のMnで置き換えたものであるが、化学的溶解度が限られているため準安定であり、薄膜でしか製作できないものであった。また電子ドープも行うことができなかった。この困難な条件を超えるため、Masekらは理論的にI-II-V族半導体LiZnAsを提案した。この物質では原子価が等しい(Zn,Mn)の置き換えによる磁性の発現とLi濃度を過剰あるいは不足させることによるキャリアードープを独立に制御可能である。本研究では世界で初めてバルクな状態でのLi$$_{1+y}$$(Zn$$_{1-x}$$Mn$$_x$$)Asの合成に成功した。わずかにLiを過剰にすることで、50Kまでの温度で強磁性が現れること、またp型のキャリアーを持つことが観測され、これらの結果を報告した。

口頭

Quantifying isolated pore space in geological barrier materials

Hu, Q.*; Wang, Q.*; Oware, P.*; 舘 幸男; 深津 勇太; Ilavsky, J.*; Almer, J.*

no journal, , 

Pore connectivity is important in controlling fluid flow and mass transport in porous natural rocks. A different extent of pore connectivity can be reflected in the proportion of isolated pore space not connected to the surface of natural rocks. This work presents the multi-approach and multi-scale laboratory studies to investigating the proportion of isolated pore space of, and its resultant anomalous fluid flow and radionuclide movement in, generic geological barrier materials. The samples include mudstone from Wakkanai formation, Opalinus clay from Mt. Terri as well as granodiorite from Grimisel, salt rock from Waste Isolation Pilot Plant in New Mexico, and welded tuff in Yucca Mountain. The independent quantification of both (1) surface-accessible pore space with various probing fluids (e.g., micron-scale tracer mapping using laser ablation-ICP-MS); and (2) total porosity by small angle X-ray scattering. Our complementary approaches provide a rich toolbox for tackling the pore structure characteristics in geological barrier materials, and associated fluid flow and radionuclide transport.

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Decimeter-scale laboratory studies of thermal, mechanical, hydrological and chemical processes in near-field systems of generic geological waste repositories

Hu, Q. H.*; Zhang, T.*; Shen, Y. Q.*; 舘 幸男; 深津 勇太; Borglin, S.*; Chang, C.*; Hampton, J.*

no journal, , 

In a deep geological repository of high-level nuclear wastes, the near-field systems consist of waste packages, buffer materials, and natural barrier systems. It is expected that the initial thermal loading after waste emplacement will last several hundred years. It is important to investigate the effects of this thermal loading on the near-field components under in situ stress conditions, in terms of thermal-hydrological-mechanical-chemical (THMC) processes and subsequent radionuclide retention and migration. Preliminary tests have been performed via integrated combinations of buffer materials and host rocks, at nm-dm scales, subjected to a range of elevated temperatures under true-triaxial conditions, which is complemented by a suite of nano-petrophysical characterization approaches such as small-angle neutron/X-ray scattering techniques to quantify total pore space and sample size-dependent effective porosity. For multiple-approach radionuclide retention and migration tests before- and after-THMC experiments, a complementary range of tests will include batch, column, and gas diffusion for granular samples, as well as gas/liquid diffusion and fractured core transport tests for intact rock samples under different temperature and pressure conditions.

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Effects of biotite on diffusion and sorption of cations in crystalline rocks by through-diffusion and laser-ablation ICP-MS experiments

深津 勇太; Hu, Q.*; 舘 幸男

no journal, , 

Matrix diffusion and sorption are key processes to predict the transport of radionuclides in crystalline rocks for geological repository. Based on the previous studies, cationic sorption onto biotite would play an important role to evaluate the sorption and diffusivity of radionuclides in crystalline rock. In order to investigate the impact of sorption of cations in biotite on the diffusivity, in this study, we conducted through-diffusion tests of Cs$$^{+}$$, Co$$^{2+}$$ and Sr$$^{2+}$$ for several types of crystalline rocks, and compared the results in different concentrations of K$$^{+}$$ that is one of the major cations of groundwater and also strong competitor for Cs$$^{+}$$ sorption onto biotite. Moreover, the elemental maps of multiple tracers sorbed onto biotite of these rocks were directly obtained by using a laser ablation (LA)-ICP-MS, which provides microscale distribution of tracer elements within the rocks.

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