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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
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.
堀池 優貴*; 青木 裕之; 大内 誠*; 寺島 崇矢*
Journal of the American Chemical Society, 147(8), p.6727 - 6738, 2025/02
被引用回数：0 パーセンタイル：0.00(Chemistry, Multidisciplinary)Herein, we report water-intercalated and humidity-responsive lamellar materials obtained from the self-assembly of sodium acrylate (ANa)/alkyl acrylate (RA) random copolymers. The random copolymers efficiently absorbed water into the hydrophilic ANa/main chain phase from the outer environment to form lamellar structures consisting of the water-intercalated hydrophilic segments and the hydrophobic side chains. The lamellar formation involves controlling the weight fraction of hydrophilic segments containing water to 40-70 wt% by the RA content, hydrophobic side chains, and the amount of absorbed water. The domain spacing can be controlled in the range of 2-6 nm. More interestingly, the lamellar materials reversibly afford expansion and contraction of the domain spacing in the sub-1 nm level via the absorption and release of water, in response to relative humidity. The multilayered lamellar formation process via the intercalation of water was analyzed in situ by neutron reflectometry and atomic force microscopy measurements under humid conditions. The polymer film further served as a moisture-sensitive actuator that macroscopically induces deformation responsive to humidity.
山本 勝宏*; 今井 達也*; 河合 純希*; 伊藤 恵利*; 宮崎 司*; 宮田 登*; 山田 悟史*; 瀬戸 秀紀*; 青木 裕之
ACS Applied Materials & Interfaces, 16(48), p.66782 - 66791, 2024/11
被引用回数：0 パーセンタイル：0.00(Nanoscience & Nanotechnology)In this study, a silicon-based copolymer, poly(tris(trimethylsiloxy)-3-methacryloxypropylsilane)-co-poly(N,N-dimethyl acrylamide), thin film was subjected to plasma surface treatment to make its surface hydrophilic (biocompatible). Neutron reflectivity (NR) measurement of the plasma-treated thin film showed a decrease in the film thickness (etching width: similar to 20 nm) and an increase in the scattering length density (SLD) near the surface (similar to 15 nm). The region with a considerably high SLD adsorbed water (D
O) from its saturated vapor, indicating its superior surface hydrophilicity. Nevertheless of the hydrophilicity, the swelling of the thin film was suppressed. Hard X-ray photoelectron spectroscopy (HAXPES) performed at various takeoff angles revealed that the thin-film surface (similar to 20 nm depth) underwent extensive oxidation. NR and HAXPES analysis quantitatively yielded the depth profiling of elemental compositions in a few tens of nm scale. Si oxidation and hydrogen elimination (probably CH
groups) in the vicinity of the surface region increased the SLD and decreased the hydrophobicity. A combination of Soft X-ray photoelectron spectroscopy and NR measurements revealed the surface chemical composition and mass density. It was considered that the surface near the film was chemically composed close to SiO, forming a gel-like (three-dimensional network) structure that is hydrophilic and suppresses swelling due to moisture, indicating it can be expected to maintain stable hydrophilicity on the film surface.
宮崎 司*; 宮田 登*; 有馬 寛*; 下北 啓輔*; 山本 勝宏*; 竹中 幹人*; 中西 洋平*; 柴田 基樹*; 青木 裕之; 山田 悟史*; et al.
Colloids and Surfaces A; Physicochemical and Engineering Aspects, 701, p.134928_1 - 134928_8, 2024/11
被引用回数：0 パーセンタイル：0.00(Chemistry, Physical)Isotactic polypropylene (PP) thin films deposited on Si substrates were subjected to neutron reflectivity (NR) measurements under various humidity conditions to evaluate the isothermal adsorption of water accumulated between the PP layer and Si substrate, with focus on the temperature-dependence of the adsorption isotherm. The adsorption of accumulated water followed a single type II isotherm according to the Brunauer-Emmett-Teller (BET) classification, regardless of temperature. This can be attributed to the weak interactions between the PP layer and Si substrate, and between the PP layer and water molecules. Hydrophobic PP does not significantly interact with water molecules and the hydrophilic Si surface. Therefore, the interfacial water molecules are simply adsorbed on the native oxide layer on Si via simple interaction between the water molecules and the silicon oxide surface without being affected by the PP layer. Consequently, the adsorption isotherm of the accumulated water follows the single type II adsorption isotherm regardless of temperature, similar to the adsorption isotherm of water simply adsorbed on exposed silica surfaces. These weak interactions of the PP layer with the Si surface and water molecules also lead to fast diffusion kinetics for the accumulated water along the interface.
, 
, 
and 
mesons through their angular-dependent two-body decay modesPark, I. W.*; 佐甲 博之; 青木 和也*; Gubler, P.; Lee, S. H.*
Journal of Subatomic Particles and Cosmology (Internet), 1-2, p.100014_1 - 100014_11, 2024/11
The mass shift a spin-1 particle moving in the nuclear medium will depend on its polarization direction. To study polarization-independent mass shifts in the medium, we explore methods to isolate each polarization direction of spin-1 mesons through the angular-dependent two-body decay modes. Specifically, we study 
, 
, 
, 
and 
(
) decays. Concerning and mesons, since both particles have vacuum widths smaller than 100 MeV, they are ideal candidates for experimentally measuring chiral partners. The simultaneous observation of mass shifts of these chiral partners would provide valuable insights into the contribution of chiral symmetry breaking to the generation of hadron masses.
守田 圭介; 青木 健; 清水 厚志; 佐藤 博之
Proceedings of 31st International Conference on Nuclear Engineering (ICONE31) (Internet), 6 Pages, 2024/11
High temperature gas-cooled reactor (HTGR) is expected to use nuclear heat to wide range of industrial applications such as hydrogen production, which is capable of high temperature heat supply with inherent safe characteristics. JAEA started a High Temperature engineering Test Reactor (HTTR) heat application test project to develop coupling technologies between HTGR and a hydrogen production plant necessary to achieve large-scale, carbon-free hydrogen production. One of the key technologies is a safety evaluation method which can simulate an impact of explosion hazards induced in the hydrogen production plant on reactor facility because HTGR hydrogen production system contains large amount of combustible gases such as hydrogen. A computational fluid dynamics code FLACS has been sufficiently validated for dispersion and explosion of combustible gases such as hydrogen and methane worldwide, however, only few attempts have been made for validation of analysis in closed area with small space. A leak of combustible gases to the piping in HTGR hydrogen production system may occur in case of abnormal condition in hydrogen production plant and therefore an explosion in the piping must be considered. This paper describes the validation of FLACS by analyzing explosion experiments in straight piping and complex piping aiming to establish a safety evaluation method for analyzing explosions of combustible gases in piping.
町田 晃彦*; 齋藤 寛之*; 杉本 秀彦*; 服部 高典; 佐野 亜沙美; 遠藤 成輝*; 片山 芳則*; 飯塚 理子*; 佐藤 豊人*; 松尾 元彰*; et al.
Nature Communications (Internet), 15, p.8861_1 - 8861_2, 2024/10
被引用回数：0 パーセンタイル：0.00(Multidisciplinary Sciences)前回の論文(Nature Commun. 5, 5063 (2014))では、988Kと6.3GPaで収集した中性子粉末回折パターンのリートベルト精密化によって、fcc Fe金属格子に溶解したD原子のサイト占有率を調べた。fcc金属格子には、八面体サイトと四面体サイトの2つのD原子収容可能な格子間サイトがある。リートベルト精密化により、D原子は主に八面体サイトを0.532占有し、わずかに四面体サイトを0.056占有することがわかった。その後、Antonov (Phys. Rev. Mater. 2019))による密度汎関数理論(DFT)計算の結果、四面体サイトの占有エネルギーは八面体サイトの占有エネルギーよりも著しく高く、988Kの高温でも四面体サイトの占有は起こりにくいことがわかった。消衰補正は粉末回折パターンに適用されることはまれであり、前回の精密化には含まれていなかった。その結果、八面体の占有率は0.60に増加し、四面体の占有率はゼロに減少した。D原子の八面体サイトのみの占有は、以前の結果とは対照的ではあるが、DFT計算と一致している。
青木 健; 長谷川 武史; 倉林 薫; 野本 恭信; 清水 厚志; 佐藤 博之; 坂場 成昭
Proceedings of 11th International Topical Meeting on High Temperature Reactor Technology (HTR 2024), 6 Pages, 2024/10
原子力機構はHTTR(高温工学試験研究炉)及び水素製造施設を接続するHTTR-熱利用試験を計画している。本研究は、HTTR-熱利用試験施設の安全設計及び安全解析の成果を報告する。安全設計では、期待する安全機能に基づき構築物・系統及び機器の安全重要度分類を定めた。予備安全解析では、RELAP5コードを用いた熱流動解析を行った。予備安全解析は、蒸気発生器の伝熱管破損を除くHTTR-熱利用試験で新たに想定される事象が既設のHTTRの許認可ベース事象に包絡されること、並びに、新たな許認可ベース事象の候補は安全解析の判断基準を満足することを明らかにした。
内田 和杜*; 増田 造*; 原 伸太郎*; 松尾 陽一*; Liu, Y.*; 青木 裕之; 浅野 吉彦*; 宮田 一輝*; 福間 剛士*; 小野 俊哉*; et al.
ACS Applied Materials & Interfaces, 16(30), p.39104 - 39116, 2024/07
被引用回数：1 パーセンタイル：0.00(Nanoscience & Nanotechnology)Zwitterionic MPC polymer coatings effectively deter blood coagulation and protein buildup on medical devices. Researchers synthesized MPC copolymers containing a cross-linking unit (MPTMSi) plus one of four hydrophobic anchoring groups (MPTSSi, BMA, EHMA, LMA) and applied them to PDMS, PP, and PMP. These treatments yielded uniformly hydrophilic, electrically neutral surfaces. Protein adsorption tests showed that PMBSi (BMA) best resisted fluorescently labeled BSA, while PMLSi (LMA) was comparatively weaker, although all four coatings minimized platelet adhesion. Further analyses linked these differences in protein adsorption to varying swelling behaviors in water. Indeed, PMLSi absorbed more water, allowing some protein infiltration yet still repelling platelets. When tested under circulating flow to mimic shear stress, PMMMSi (MPTSSi) and PMLSi coatings on PP and PMP demonstrated excellent durability and platelet repellency. Overall, this study highlights how hydrophobic moieties can boost both hemocompatibility and stability of MPC-based coatings, promising improved performance in medical devices requiring low protein fouling, reduced platelet adhesion, and long-term reliability.
下北 啓輔*; 山本 勝宏*; 宮田 登*; 柴田 基樹*; 中西 洋平*; 荒川 勝利*; 竹中 幹人*; 木田 拓充*; 徳満 勝久*; 田中 亮*; et al.
Langmuir, 40(30), p.15758 - 15766, 2024/07
被引用回数：0 パーセンタイル：0.00(Chemistry, Multidisciplinary)To investigate the structure of the interface between polyethylene films and substrates, the neutron reflectivity (NR) of deuterated polyethylene (dPE) thin films deposited on Si substrates was measured, demonstrating water accumulation at the interface, even under ambient conditions. After leaching the thermally annealed dPE films in hot p-xylene, NR measurements were conducted on the layers remaining on the substrate, clearly revealing that the adsorption layer of dPE grew during annealing and consisted of two layers, an inner adsorption layer and an outer adsorption layer, as previously proposed for amorphous polymers. The inner adsorption layer was approximately 3.7 nm thick with a density comparable to that of the bulk. The outer adsorption layer was several nanometers thick and appeared to grow insufficiently on top of the inner adsorption layer under the annealing conditions examined in this study. This study clarifying the growth of the adsorption layer of polyethylene at the interface with an inorganic substrate is useful for improving the performance of polymer/inorganic filler nanocomposites due to the wide utility of crystalline polyolefins as polymer matrix materials in nanocomposites.
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.
筋田 涼太*; 青木 裕之; 竹中 幹人*; 大内 誠*; 寺島 崇矢*
ACS Macro Letters (Internet), 13(6), p.747 - 753, 2024/06
被引用回数：1 パーセンタイル：47.49(Polymer Science)Herein, we report the water-assisted self-assembly of alternating copolymers bearing imidazolium cations and hydrophobic groups to create water-compatible and nanostructured materials. The copolymers efficiently absorbed water into the cationic segments from the outer environments, depending on the relative humidity. The absorbed water serves as hydrophilic molecules to modulate the weight fraction of hydrophilic/hydrophobic units in the samples. Thus, the morphologies and domain spacing of the nanostructures can be controlled by not only the side chains, but also the amount of absorbed water. The self-assembly of the cationic copolymers, developed herein, afforded universal access to various morphologies, including lamella, gyroid, and cylinder, in addition to the precision control of the domain spacing at the 0.01 nm level.
and mesons through their angular-dependent decay modesPark, I. W.*; 佐甲 博之; 青木 和也*; Gubler, P.; Lee, S. H.*
Physical Review D, 109(11), p.114042_1 - 114042_10, 2024/06
被引用回数：0 パーセンタイル：0.00(Astronomy & Astrophysics)Observing the mass shifts of chiral partners will provide invaluable insight into the role of chiral symmetry breaking in the generation of hadron masses. Because both the and mesons have vacuum widths smaller than 100 MeV, they are ideal candidates for realizing mass shift measurements. On the other hand, the different momentum dependence of the longitudinal and transverse modes smear the peak positions. In this work, we analyze the angular dependence of the two-body decays of both the and . It is found that the longitudinal and transverse modes of the can be isolated by observing the pseudoscalar decay in either the forward or perpendicular directions, respectively. For the decaying into a vector meson and a pseudoscalar meson, one can accomplish the same goal by further observing the polarization of the vector meson through its angular dependence on the two pseudoscalar meson decay.
森 悠一郎*; 鍵 裕之*; 青木 勝敏*; 高野 将大*; 柿澤 翔*; 佐野 亜沙美; 舟越 賢一*
Earth and Planetary Science Letters, 634, p.118673_1 - 118673_8, 2024/05
被引用回数：1 パーセンタイル：58.96(Geochemistry & Geophysics)水素による鉄の体積膨張に対するケイ素の効果を調べるため、高圧高温下でのhcp-Fe
Si
の中性子回折実験とX線回折実験を行った。中性子回折実験は重水素化hcp-FeSiに対して13.5GPa, 900K及び12.1GPa, 300Kで行い、得られたプロファイルからリートベルト解析を用いて水素占有率を決定した。hcp-Fe-SiのP-V-T状態方程式を組み合わせることにより、hcp-FeSiの水素による体積膨張が純粋なhcp鉄の体積膨張よりも10%大きいことを示した。得られた値を用いて、内核の密度欠損を再現できる水素量を見積もったところ、シリコンの影響がない場合に比べて50%減少した。hcp-FeSiで内核の密度欠損を再現した場合、内核と外核で可能な水素量xはそれぞれ0.07と0.12-0.15と計算された。
Ikami, Takaya*; 青木 裕之; 寺島 崇矢*
ACS Macro Letters (Internet), 13(4), p.446 - 452, 2024/04
被引用回数：0 パーセンタイル：0.00(Polymer Science)Microphase separation of random copolymers, as well as that of high 
; low N block copolymers, is promising to construct sub-10-nm structures into materials. Herein, we designed statistical copolymers consisting of 2-hydroxyethyl acrylate (HEA) and N-octadecylacrylamide (ODAAm) to produce crystallization and hydrogen bond-assisted lamellar structure materials. The copolymers not only formed a crystalline lamellar structure with 3-4 nm domain spacing but also maintained an amorphous lamellar structure via phase transition above the melting temperature up to approximately 100 
C. The key is to introduce hydrogen-bonding amide junctions between the octadecyl groups and the polymer backbones, by which the polymer chains are physically fixed at the interface of lamellar structures even above the melting temperature. The stabilization of the lamellar structure by the amide units is also supported by the fact that the lamellar structure of all-acrylate random copolymers bearing hydroxyethyl and crystalline octadecyl groups is disordered above the melting temperature. By spin-coating on a silicon substrate, the HEA/ODAAm copolymer formed a multilayered lamellar thin film consisting of a hydrophilic hydroxyethyl/main chain phase and a hydrophobic octadecyl phase. The structure and order-disorder transition were analyzed by neutron reflectivity.
高野 将大*; 鍵 裕之*; 森 悠一郎*; 青木 勝敏*; 柿澤 翔*; 佐野 亜沙美; 飯塚 理子*; 土屋 卓*
Journal of Mineralogical and Petrological Sciences (Internet), 119(1), p.240122_1 - 240122_9, 2024/00
被引用回数：0 パーセンタイル：0.00(Mineralogy)硫化鉄(FeS)の高圧高温下での水素化は、水素と硫黄が地球や他の地球型惑星のコアの軽元素として有望な候補であることから注目されている。これまでのFeSの水素化反応に関する報告では、出発物質の化学組成は十分に明らかにされていなかった。本研究では、Fe1.000S(トロイライト)を出発物質としたFe-S-H系の高温高圧条件下での中性子回折とX線回折のその場測定を報告する。決定された占有率は、以前の研究で報告されたものより著しく低く、FeSの水素化は硫化鉄の化学組成に強く影響されることを示している。
O/HO vapor generator for contrast-variation neutron scattering有馬 寛*; 高田 慎一; 笠井 聡*; 大内 啓一*; 森川 利明*; 宮田 登*; 宮崎 司*; 青木 裕之; 岩瀬 裕希*; 廣井 孝介; et al.
Journal of Applied Crystallography, 56(6), p.1802 - 1812, 2023/12
被引用回数：4 パーセンタイル：73.01(Chemistry, Multidisciplinary)The contrast-variation technique in neutron scattering experiments plays a pivotal role in distinguishing partial structures within multi-component complexes, facilitating the elucidation of distinct sample constituents. This differentiation is achieved using different isotopes, namely hydrogen and deuterium, which possess varying neutron scattering characteristics. This study presents a novel vapor generator designed for neutron scattering experiments, enabling continuous control of the DO/HO ratio of the vapor. This feature is especially useful for contrast-variation studies. The generator features two saturators and four mass flow controllers, allowing for the rapid and independent generation of DO/HO vapors. Additionally, the incorporation of the two-temperature method ensures accurate dew point control within a margin of 
0.2Cdp. This setup proves useful for conducting time-resolved experiments and can accelerate research on functional polymers, such as polymer electrolyte membranes for fuel cells, where water potential assumes critical importance.
筋田 涼太*; 今井 彩帆里*; 大内 誠*; 青木 裕之; 寺島 崇矢*
Macromolecules, 56(23), p.9738 - 9749, 2023/12
被引用回数：3 パーセンタイル：34.80(Polymer Science)Constructing ordered ionic nanostructures into bulk polymers and thin films is an important technique to create functional materials, such as polyelectrolytes and proton- and ion-conducting materials, for various applications. Herein, we report microphase separation of cationic homopolymers bearing alkyl ammonium bromides to create sub-4 nm lamellar materials, where an ionic phase is alternatingly layered with a hydrophobic alkyl phase and serves as a channel for water intercalation. We prepared cationic homopolymers with linear or branched alkyl pendants (octyl or 2-ethylhexyl group: C8-eicosyl or 2-octyldodecyl group: C20) via the free radical polymerization of 2-(dimethylamino)ethyl acrylate (DMAEA), followed by the quaternization of the polyDMAEA with corresponding alkyl bromides. The homopolymers carrying linear hexadecyl, octadecyl, and eicosyl groups were crystalline at room temperature, whereas the others were amorphous. The homopolymers bearing linear alkyl pendants longer than the decyl group or branched alkyl pendants larger than the 2-butyloctyl group formed lamellar structures by the self-assembly of the side chains. The domain spacing can be controlled between 2.5 and 3.7 nm by tuning the pendant structures and are smaller than that formed by the corresponding random copolymers. A cationic homopolymer bearing crystalline octadecyl groups maintained lamellar structures up to 
210 
C far beyond the melting temperature (50 C). The cationic homopolymer further formed a multilayered lamellar thin film on a silicon substrate, in which the cationic layers absorbed water under humid conditions and reversibly released the water therefrom in a N gas atmosphere.
青木 裕之
波紋, 33(4), p.142 - 145, 2023/11
In recent years, there has been a strong demand for more advanced adhesion technologies. Neutron reflectometry (NR) is a powerful tool to examine the structure of the adhesion interface because of the large penetration depth to materials and the isotope-dependent contrast mechanism. Examining the effects of absorbed water on epoxy adhesives 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 by NR. The in situ NR measurement revealed the formation of an ~1 nm-thick condensed water layer at the interface with an adherend in a humid atmosphere at a relative humidity of 85%. Water absorbed by epoxy adhesives from a humid atmosphere considerably influences their structure and properties; therefore, the results of NR indicate that the effect of water at the adhesion interface should be considered to develop the adhesion technology. The recent advances in NR overcome the limitation in the applicable field in the conventional NR measurements and would unveil the further information on the fundamental mechanism of the adhesion phenomena.
橋本 慧*; 塩飽 透*; 青木 裕之; 横山 英明*; 眞弓 皓一*; 伊藤 耕三*
Science Advances (Internet), 9(47), p.eadi8505_1 - eadi8505_8, 2023/11
被引用回数：44 パーセンタイル：97.60(Multidisciplinary Sciences)The demand for mechanically robust polymer-based electrolytes is increasing for applications to wearable devices. Young's modulus and breaking energy are essential parameters for describing the mechanical reliability of electrolytes. The former plays a vital role in suppressing the short circuit during charge-discharge, while the latter indicates crack propagation resistance. However, polymer electrolytes with high Young's moduli are generally brittle. In this study, a tough slide-ring solid polymer electrolyte (SR-SPE) breaking through this trade-off between stiffness and toughness is designed on the basis of strain-induced crystallization (SIC) and phase separation. SIC makes the material highly tough (breaking energy, 80 to 100 megajoules per cubic meter). Phase separation in the polymer enhanced stiffness (Young's modulus, 10 to 70 megapascals). The combined effect of phase separation and SIC made SR-SPE tough and stiff, while these mechanisms do not impair ionic conductivity. This SIC strategy could be combined with other toughening mechanisms to design tough polymer gel materials.
