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論文

Incommensurate antiferromagnetism in UTe$$_2$$ under pressure

Knafo, W.*; Thebault, T.*; Raymond, S.*; Manuel, P.*; Khalyavin, D. D.*; Orlandi, F.*; Ressouche, E.*; Beauvois, K.*; Lapertot, G.*; 金子 耕士; et al.

Physical Review X, 15(2), p.021075_1 - 021075_16, 2025/05

The discovery of multiple superconducting phases in UTe$$_2$$ boosted research on correlated-electron physics. This heavy-fermion paramagnet was rapidly identified as a reference compound to study the interplay between magnetism and unconventional superconductivity with multiple degrees of freedom. The proximity to a ferromagnetic quantum phase transition was initially proposed as a driving force to triplet-pairing superconductivity. However, we find here that long-range incommensurate antiferromagnetic order is established under pressure. The propagation vector k$$_{rm m}$$ = (0.07, 0.33, 1) of the antiferromagnetic phase is close to a wavevector where antiferromagnetic fluctuations have previously been observed at ambient pressure. These elements support that UTe$$_2$$ is a nearly-antiferromagnet at ambient pressure. Our work appeals for theories modelling the evolution of the magnetic interactions and electronic properties, driving a correlated paramagnetic regime at ambient pressure to a long-range antiferromagnetic order under pressure. A deeper understanding of itinerant-f-electrons magnetism in UTe$$_2$$ will be a key for describing its unconventional superconducting phases.

論文

Surface and interfacial aggregation states in thin films of a polystyrene/polyrotaxane blend

田口 美岐*; 宮田 登*; 宮崎 司*; 青木 裕之; Ozawa, Satoru*; 長谷川 龍一 *; 盛満 裕真*; 川口 大輔*; 山本 悟*; 田中 敬二*

Polymer Journal, 7 Pages, 2025/03

 被引用回数:0 パーセンタイル:0.00(Polymer Science)

Polyrotaxane (PR) exhibits unique mechanical properties due to the ability of its cyclic molecules to move or slide along the axial chain. Thus, to design advanced polymer-based composite materials and organic devices, it is crucial to better understand the aggregation states at the surface and substrate interface in polymer films containing PR. Here, we report the depth profile of PR along the direction normal to the interface when it is mixed with polystyrene (PS). Neutron reflectivity and X-ray photoelectron spectroscopy revealed that PS and PR segregated at the surface and substrate interface, respectively, and that the extent of segregation depended on the length of PS. The surface enrichment of PS is driven by both energy and entropy, whereas the enrichment of PR at the substrate interface is energy driven.

論文

Neutron reflectometry study on the interfacial layer of epoxy resin to improve adhesion strength

Liu, Y.*; 宮田 登*; 宮崎 司*; 春藤 淳臣*; 川口 大輔*; 田中 敬二*; 青木 裕之

ACS Applied Materials & Interfaces, 8 Pages, 2025/00

The performance of structural adhesives is strongly influenced by the interfacial structure between the adhesive and adherend. In this study, we developed a nanometric stable interfacial layer derived from an epoxy resin system containing excess hardener. This layer, formed on solid substrates, exhibited excellent structural stability, even after extensive solvent washing. Neutron reflectometry (NR) was employed to investigate its structure under both dry and humid conditions, revealing a robust and well-defined interface that suppressed moisture accumulation at the adherend interface. FT-IR spectroscopy confirmed an excess of unreacted amino groups in the adsorbed layer, enabling further curing reactions with freshly applied epoxy resin. Re-coating experiments demonstrated that the adsorbed layer remained intact after thermal curing, suggesting strong interfacial compatibility. Notably, the presence of the adsorbed layer led to a significant enhancement in adhesive performance. Lap shear tests showed that the adhesion strength of the epoxy resin nearly doubled when the adsorbed layer was introduced at the interface. This approach does not rely on external coupling agents or primers, but instead utilizes a homologous material system to tailor interfacial properties through molecular-level design. The strategy presented here offers a practical and scalable method for improving adhesion in epoxy systems. By directly engineering the adhesive interface using components intrinsic to the epoxy formulation, this method enables reliable and enhanced bonding performance without altering the bulk material.

論文

$$^{149}$$Sm synchrotron-radiation-based M$"{o}$ssbauer and $$mu^+$$SR studies of Sm$$_3$$Ru$$_4$$Ge$$_{13}$$

筒井 智嗣; 伊藤 孝; 中村 仁*; 吉田 実生*; 小林 義男*; 依田 芳卓*; 中村 惇平*; 幸田 章宏*; 東中 隆二*; 青木 大*; et al.

Interactions (Internet), 245(1), p.55_1 - 55_9, 2024/12

$$^{149}$$Sm SR-based M$"{o}$ssbauer and muon spin relaxation ($$mu^+$$SR) spectroscopies have been applied to Sm$$_3$$Ru$$_4$$Ge$$_{13}$$. The temperature dependence of the $$^{149}$$Sm SR-based M$"{o}$ssbauer spectra in the paramagnetic state implies the presence of dynamical nuclear Zeeman and/or quadrupole interactions. The time differential $$mu^+$$SR spectra also exhibit a marked temperature dependence in the paramagnetic state, indicating the presence of magnetic fluctuation in Sm$$_3$$Ru$$_4$$Ge$$_{13}$$ at least. These results in the present work infer that the dynamical hyperfine interactions observed using the mutually complementary spectroscopic methods are connected with the mechanism of the heavy fermion behavior in Sm$$_3$$Ru$$_4$$Ge$$_{13}$$.

論文

Influence of MC carbides on pitting corrosion resistance of weld metal in austenitic stainless steels

門井 浩太*; 冠野 裕大*; 青木 聡; 井上 裕滋*

ISIJ International, 64(9), p.1450 - 1456, 2024/07

 被引用回数:0 パーセンタイル:0.00(Metallurgy & Metallurgical Engineering)

オーステナイトステンレス鋼の溶接金属中の孔食に及ぼす化学組成の影響について検討した。クロムおよびモリブデンを多く含む試験片は、再活性化率が低いことが示された。チタンの添加は、耐孔食性を著しく低下させた。クロム欠乏領域はM$$_{23}$$C$$_{6}$$やTiCのような炭化物の近くに形成された。また、凝固時に生成したTiC相がM$$_{23}$$C$$_{6}$$析出の核となった。M$$_{23}$$C$$_{6}$$の析出により、クロムの拡散による空乏領域が発生し、耐孔食性の劣化を誘発した。

論文

In-plane movement of isolated poly(methacrylate) chains on a hydrophilic solid surface

Kawano, Masayuki*; 盛満 裕真*; Liu, Y.*; 宮田 登*; 宮崎 司*; 青木 裕之; 川口 大輔*; 山本 悟*; 田中 敬二*

Macromolecules, 57(14), p.6625 - 6633, 2024/07

 被引用回数:0 パーセンタイル:0.00(Polymer Science)

A better understanding of the dynamic behavior of polymer chains on solid surfaces is indispensable for the design and construction of high-performance polymer composites. We herein visualized the in-plane movement of isolated poly(methyl methacrylate) (PMMA) and poly(tert-butyl methacrylate) (PtBMA) single chains on hydrophilic silicon wafers under ambient conditions by atomic force microscopy. Isolated PMMA chains adsorbed to the substrate, whereas PtBMA chains diffused, the degree of which was dependent on the humidity. Neutron reflectivity revealed the formation of a layer of condensed water on the substrate. All-atomistic molecular dynamics simulations implied that the diffusivity difference of the two polymers was based on the submerged depth in which a part of a chain existed. That is, the interaction of a polymer with the surface of the hydrophilic substrate primarily governs its lateral movement, or adsorption behavior, facilitated by the presence of water.

論文

A Focusing supermirror for time-of-flight grazing-incidence small-angle neutron scattering measurement

山崎 大; 丸山 龍治; 青木 裕之; 花島 隆泰*; 阿久津 和宏*; 宮田 登*; 曽山 和彦

Quantum Beam Science (Internet), 9(2), p.20_1 - 20_12, 2024/06

This study developed a neutron-beam focusing supermirror for grazing-incidence small-angle neutron scattering (GISANS) measurements. It was fabricated by depositing NiC/Ti supermirror film with ion-beam sputtering on a precise elliptic surface of fused quartz figured using the elastic emission machining technique. Neutron measurements at a pulsed neutron reflectometer BL17 of MLF, J-PARC successfully demonstrated that the focusing supermirror enhances a beam intensity twentyfold compared with an optimally collimated beam, achieving the signal-to-background ratio of the focal spot as high as 500. The mirror can be readily installed and used at BL17.

論文

Field-induced insulator-metal transition in EuTe$$_2$$

竹内 徹也*; 本多 史憲*; 青木 大*; 芳賀 芳範; 木田 孝則*; 鳴海 康雄*; 萩原 政幸*; 金道 浩一*; 軽部 皓介*; 播磨 尚朝*; et al.

Journal of the Physical Society of Japan, 93(4), p.044708_1 - 044708_10, 2024/04

 被引用回数:0 パーセンタイル:0.00(Physics, Multidisciplinary)

Electrical and magnetic properties of divalent europium antiferromagnet EuTe$$_2$$ are studied on single crystals grown from Te-flux method. Antiferromagnetism occurs at 11 K with an insulating ground state. Application of magnetic field induces a sudden resistance drop leading to a phase transition to metallic state. Energy band calculations reveal the appearance of a Fermi surface pocket with Te-5p character induced by the polarized Eu moments.

論文

Reinforcement of superconductivity by quantum critical fluctuations of metamagnetism in UTe$$_2$$

常盤 欣文; Opletal, P.; 酒井 宏典; 神戸 振作; 山本 悦嗣; 木俣 基*; 淡路 智*; 佐々木 孝彦*; 青木 大*; 芳賀 芳範; et al.

Physical Review B, 109(14), p.L140502_1 - L140502_6, 2024/04

 被引用回数:6 パーセンタイル:86.08(Materials Science, Multidisciplinary)

超伝導体UTe$$_2$$の常伝導状態を$$b$$軸磁場に対するエントロピー解析によって調べた。メタ磁性揺らぎ(空間一様、$$Q=0$$)による磁場によるエントロピーの強い増加が観測された。この磁場依存性は遍歴メタ磁性の量子臨界性に関するHertz-Millis-Moriya理論によってよく記述される。特に、量子臨界領域の下界は超伝導転移温度$$T_c(B)$$の最小値の位置とよく一致する。この結果は、$$Q=0$$の揺らぎが超伝導を強めることを示唆している。

論文

Synthesis of heat-resistant living polymer particles by one-step reversible addition-fragmentation chain transfer precipitation polymerization of styrene and $$N$$-phenylmaleimide

山崎 駿*; 金子 直矢*; 加藤 敦也*; 渡邉 航平*; 青木 大輔*; 谷口 竜王*; 唐津 孝*; 上田 祐生; 元川 竜平; 大倉 滉生*; et al.

Polymer, 298, p.126846_1 - 126846_11, 2024/04

 被引用回数:4 パーセンタイル:70.06(Polymer Science)

Synthesis of heat-resistant, living polymer particles via one-step reversible addition-fragmentation chain transfer precipitation polymerization (RAFTPP) of styrene and $$N$$-phenylmaleimide is reported. Gel permeation chromatography and nuclear magnetic resonance spectroscopy confirmed that the polymerization proceeded in a living manner. The scanning electron microscopy results showed that the monodisperse P(St-PhMI) RAFTPP particles with a diameter of 1.88 micrometer were successfully synthesized. The P(St-PhMI) RAFTPP showed excellent thermal stability with a high glass transition temperature and a 5 percent weight loss temperature. The surface concentration of the RAFT groups was determined to be 0.181 groups/square-nanometer due to fragmentation of the RAFT groups exposed on the particles. The small-angle neutron scattering measurements showed the particle formation mechanism, in which the swollen, growing polymer chains were consumed for particle formation. The introduction of grafted chains by surface-initiated RAFT polymerization demonstrated the possibility of further functionalization of P(St-PhMI) RAFTPP particles by exploiting their living nature.

論文

Longitudinal spin fluctuations driving field-reinforced superconductivity in UTe$$_2$$

徳永 陽; 酒井 宏典; 神戸 振作; Opletal, P.; 常盤 欣文; 芳賀 芳範; 北川 俊作*; 石田 憲二*; 青木 大*; Knebel, G.*; et al.

Physical Review Letters, 131(22), p.226503_1 - 226503_7, 2023/12

 被引用回数:11 パーセンタイル:85.32(Physics, Multidisciplinary)

Our measurements of $$^{125}$$Te NMR relaxations reveal an enhancement of electronic spin fluctuations above $$mu_0H^*sim15$$~T, leading to their divergence in the vicinity of the metamagnetic transition at $$mu_0H_mapprox35$$~T, below which field-reinforced superconductivity appears when a magnetic field ($$H$$) is applied along the crystallographic $$b$$ axis. The NMR data evidence that these fluctuations are dominantly longitudinal, providing a key to understanding the peculiar superconducting phase diagram in $$H|b$$, where such fluctuations enhance the pairing interactions.

論文

Impact of the Ce$$4f$$ states in the electronic structure of the intermediate-valence superconductor CeIr$$_3$$

藤森 伸一; 川崎 郁斗; 竹田 幸治; 山上 浩志; 雀部 矩正*; 佐藤 芳樹*; 清水 悠晴*; 仲村 愛*; Maruya, A.*; 本間 佳哉*; et al.

Electronic Structure (Internet), 5(4), p.045009_1 - 045009_7, 2023/11

The electronic structure of the $$f$$-based superconductor $$mathrm{CeIr_3}$$ was studied by photoelectron spectroscopy. The energy distribution of the $$mathrm{Ce}~4f$$ state was revealed by the $$mathrm{Ce}~3d-4f$$ resonant photoelectron spectroscopy. The $$mathrm{Ce}~4f$$ state was mostly distributed in the vicinity of the Fermi energy, suggesting the itinerant character of the $$mathrm{Ce}~4f$$ state. The contribution of the $$mathrm{Ce}~4f$$ state to the density of states (DOS) at the Fermi energy was estimated to be nearly half of that of the$$mathrm{Ir}~5d$$ states, implying that the $$mathrm{Ce}~4f$$ state has aconsiderable contribution to the DOS at the Fermi energy. The $$mathrm{Ce}~3d$$ core-level and $$mathrm{Ce}~3d$$ X-ray absorption spectra were analyzed based on a single-impurity Anderson model. The number of the $$mathrm{Ce}~4f$$ state in the ground state was estimated to be 0.8-0.9, which is much larger than the values obtained in the previous studies (i.e., 0-0.4).

論文

Magnetic and fermi surface properties of semimetals EuAs$$_3$$ and Eu(As$$_{1-x}$$P$$_x$$)$$_3$$

大貫 惇睦*; 軽部 皓介*; 青木 大*; 仲村 愛*; 本間 佳哉*; 松田 達磨*; 芳賀 芳範; 竹内 徹也*

Journal of the Physical Society of Japan, 92(11), p.114703_1 - 114703_12, 2023/11

 被引用回数:1 パーセンタイル:23.32(Physics, Multidisciplinary)

Single crystal samples of a series of semimetallic magnet Eu(As$$_{1-x}$$P$$_x$$)$$_3$$ have successfully grown. By measuring magnetization, Hall resistivity and de Haas-van Alphen oscillations, large anomalous Hall resistivity arising from peculiar magnetic phase diagram was identified.

論文

Superconducting spin reorientation in spin-triplet multiple superconducting phases of UTe$$_2$$

金城 克樹*; 藤林 裕己*; 松村 拓輝*; 堀 文哉*; 北川 俊作*; 石田 憲二*; 徳永 陽; 酒井 宏典; 神戸 振作; 仲村 愛*; et al.

Science Advances (Internet), 9(30), p.2736_1 - 2736_6, 2023/07

 被引用回数:14 パーセンタイル:88.25(Multidisciplinary Sciences)

Superconducting (SC) state has spin and orbital degrees of freedom, and spin-triplet superconductivity shows multiple SC phases because of the presence of these degrees of freedom. However, the observation of spin-direction rotation occurring inside the SC state (SC spin rotation) has hardly been reported. Uranium ditelluride, a recently found topological superconductor, exhibits various SC phases under pressure: SC state at ambient pressure (SC1), high-temperature SC state above 0.5 gigapascal (SC2), and low-temperature SC state above 0.5 gigapascal (SC3). We performed nuclear magnetic resonance (NMR) and ac susceptibility measurements on a single-crystal uranium ditelluride. The b axis spin susceptibility remains unchanged in SC2, unlike in SC1, and decreases below the SC2-SC3 transition with spin modulation. These unique properties in SC3 arise from the coexistence of two SC order parameters. Our NMR results confirm spin-triplet superconductivity with SC spin parallel to b axis in SC2 and unveil the remaining of spin degrees of freedom in SC uranium ditelluride.

論文

Neutron reflectometry analysis of condensed water layer formation at a solid interface of epoxy resins under high humidity

Liu, Y.*; 宮田 登*; 宮崎 司*; 春藤 淳臣*; 川口 大輔*; 田中 敬二*; 青木 裕之

Langmuir, 39(29), p.10154 - 10162, 2023/06

 被引用回数:11 パーセンタイル:74.82(Chemistry, Multidisciplinary)

Water absorbed by epoxy resins from a humid atmosphere considerably influences their structure and properties. Examining the effects of absorbed water on epoxy resins at their interfaces with solid substrates is crucial because of their adhesive applications in various fields. The spatial distribution of absorbed water in epoxy resin thin films under high humidity was investigated in this study by neutron reflectometry. Water molecules were found to accumulate at the SiO$$_{2}$$/epoxy resin interface after exposure at a relative humidity of 85% for 8 h. The formation of an ca.1 nm-thick condensed water layer was observed, and the thickness of this layer varied with curing conditions of epoxy systems. Furthermore, the water accumulation at the interface was noted to be affected by high-temperature and high-humidity environments. The formation of the condensed water layer is presumed to be related to the features of the polymer layer near the interface. The construction of the interface layer of epoxy resin would be affected by the interface constraint effect on the cross-linked polymer chain during the curing reaction. This study provides essential information for understanding the factors influencing the accumulation of water at the interface in epoxy resins. In the practical application, the process of improving the construction of epoxy resin near the interface would be a reasonable solution to resist the water accumulation in the interface.

論文

Large reduction in the $$a$$-axis knight shift on UTe$$_2$$ with $$T_c$$ = 2.1 K

松村 拓輝*; 藤林 裕己*; 金城 克樹*; 北川 俊作*; 石田 憲二*; 徳永 陽; 酒井 宏典; 神戸 振作; 仲村 愛*; 清水 悠晴*; et al.

Journal of the Physical Society of Japan, 92(6), p.063701_1 - 063701_5, 2023/05

 被引用回数:36 パーセンタイル:98.12(Physics, Multidisciplinary)

Spin susceptibility in the superconducting (SC) state was measured in the higher-quality sample of uranium-based superconductor UTe$$_2$$ by using Knight-shift measurements for a magnetic field $$H$$ along all three crystalline axes. In the higher-quality sample, the SC transition temperature $$T_c$$ is about 2.1 K, and the residual electronic term in the specific heat is almost zero. The NMR linewidth becomes narrower and is almost half of that in the previous sample with $$T_csim$$1.6 K when $$H//a$$ and $$c$$. Although the Knight-shift behavior was not so different from the previous results for $$H//b$$, and $$c$$, a large reduction in Knight shift along the $$a$$ axis was observed, in contrast with the previous $$a$$-axis Knight shift result. We discuss the origin of the difference between the previous and present results, and the possible SC state derived from the present results.

論文

Low-temperature magnetic fluctuations investigated by $$^{125}$$Te-NMR on the uranium-based superconductor UTe$$_2$$

藤林 裕己*; 金城 克樹*; 仲嶺 元輝*; 北川 俊作*; 石田 憲二*; 徳永 陽; 酒井 宏典; 神戸 振作; 仲村 愛*; 清水 悠晴*; et al.

Journal of the Physical Society of Japan, 92(5), p.053702_1 - 053702_5, 2023/05

 被引用回数:7 パーセンタイル:77.36(Physics, Multidisciplinary)

To investigate the static and dynamic magnetic properties on the uranium-based superconductor UTe$$_2$$, we measured the NMR Knight shift $$K$$ and the nuclear spin lattice relaxation rate 1/$$T_1$$ in $$H//a$$ by $$^{125}$$Te-NMR on a $$^{125}$$Te-enriched single-crystal sample. 1/$$T_1$$$$T$$ in $$H//a$$ is much smaller than 1/$$T_1$$$$T$$ in $$H //b$$ and c, and magnetic fluctuations along each axis are derived from the 1/$$T_1$$$$T$$ measured in $$H$$ parallel to all three crystalline axes. The magnetic fluctuations are almost identical at two Te sites and isotropic at high temperatures, but become anisotropic below 40 K, where heavy-fermion state is formed.

論文

Field induced multiple superconducting phases in UTe$$_2$$ along hard magnetic axis

酒井 宏典; 常盤 欣文; Opletal, P.; 木俣 基*; 淡路 智*; 佐々木 孝彦*; 青木 大*; 神戸 振作; 徳永 陽; 芳賀 芳範

Physical Review Letters, 130(19), p.196002_1 - 196002_6, 2023/05

 被引用回数:24 パーセンタイル:96.14(Physics, Multidisciplinary)

$$T_{rm c}$$=2.1Kのウラン2テルル化物単結晶における超伝導相図を磁気困難軸である結晶$$b$$軸方向に磁場をかけて調べた。電気抵抗と交流帯磁率を同時に測定した結果、低磁場超伝導(LFSC)相と高磁場超伝導(HFSC)相が、対照的な磁場-角度依存性をもつことがわかった。結晶の純良性が上がったことにより、LFSC相の上部臨界磁場は上昇したものの、HFSC相が現れる特徴磁場$$H^{ast}$$は、単結晶の純良性に関わらず、15Tと一定であることがわかった。また、$$H^{ast}$$近傍のLFSC相内に、弱い渦糸ピン留め力で特徴づけられる中間超伝導相を示唆する新たな相線の形跡を捉えた。

論文

Magnetic properties of single crystalline Tb$$_5$$Sb$$_3$$

北折 暁*; 金澤 直也*; 木田 孝則*; 鳴海 康雄*; 萩原 政幸*; 金道 浩一*; 竹内 徹也*; 仲村 愛*; 青木 大*; 芳賀 芳範; et al.

Journal of the Physical Society of Japan, 92(2), p.024702_1 - 024702_6, 2023/02

 被引用回数:1 パーセンタイル:23.32(Physics, Multidisciplinary)

Magnetic properties of Tb$$_5$$Sb$$_3$$ are reported. Unlike previous investigations on a polycrystal showing multiple phase transitions, the present single crystal sample shows a single transition 133 K. It is also shown that the magnetic hysteresis increases at low temperatures.

論文

Change of superconducting character in UTe$$_{2}$$ induced by magnetic field

金城 克樹*; 藤林 裕己*; 北川 俊作*; 石田 憲二*; 徳永 陽; 酒井 宏典; 神戸 振作; 仲村 愛*; 清水 悠晴*; 本間 佳哉*; et al.

Physical Review B, 107(6), p.L060502_1 - L060502_5, 2023/02

 被引用回数:21 パーセンタイル:92.66(Materials Science, Multidisciplinary)

UTe$$_2$$ is a recently discovered spin-triplet superconductor. One of the characteristic features of UTe$$_2$$ is a magnetic field ($$H$$)-boosted superconductivity above 16 T when H is applied exactly parallel to the $$b$$ axis. To date, this superconducting (SC) state has not been thoroughly investigated, and the SC properties as well as the spin state of this high-$$H$$ SC (HHSC) phase are not well understood. In this letter, we performed AC magnetic susceptibility and nuclear magnetic resonance measurements and found that, up to 24.8 T, the HHSC state has bulk nature and is quite sensitive to the $$H$$ angle and that its SC character is different from that in the low-$$H$$ SC (LHSC) state. The dominant spin component of the spin-triplet pair is along the $$a$$ axis in the LHSC state but is changed in the HHSC state along the $$b$$ axis. Our results indicate that $$H$$-induced multiple SC states originate from the remaining spin degrees of freedom.

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