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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

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

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

Progress of material characterization techniques based on neutron Bragg-edge transmission imaging

Wang, Y. W.*; 徐 平光; Su, Y. H.; Ma, Y. L.*; Wang, H. H.*

Physics Examination and Testing, 42(4), p.32 - 41, 2024/08

With the rapid technological development of large spallation neutron source facilities, the neutron beam flux obtained has been greatly improved and neutron imaging techniques have been further developed. Due to the limitation of neutron beam flux, conventional neutron imaging techniques require neutron beams with a wide wavelength range to obtain relatively high neutron beam flux conditions. Recently, spallation neutron sources using large proton accelerators have made it possible to obtain high-flux pulsed neutron beams. Energy (wavelength) resolved neutron imaging technique based on the Bragg edge effect (neutron Bragg edge transmission imaging technique) is expected to have a wide range of applications because of its high energy resolution, high spatial resolution, and ability to detect crystallographic information. The basic principle of this technique is briefly introduced. Several applications in the evaluation of residual strain, phase composition, dislocation density, and oriented structure are also reviewed to play an active role in promoting the wider applications of related technique.

論文

Microscopic insights of the extraordinary work-hardening due to phase transformation

Ma, Y.*; Naeem, M.*; Zhu, L.*; He, H.*; Sun, X.*; Yang, Z.*; He, F.*; Harjo, S.; 川崎 卓郎; Wang, X.-L.*

Acta Materialia, 270, p.119822_1 - 119822_13, 2024/05

We report an in situ neutron diffraction study of 316 L that reveals an extraordinary work-hardening rate (WHR) of $$sim$$7 GPa at 15 K. Detailed analyses show that the major contribution to the excellent strength and ductility comes from the transformation-induced plasticity (TRIP) effect, introduced by the austenite-to-martensite ($$gamma$$-to-$$alpha$$') phase transition. A dramatic increase in the WHR is observed along with the transformation; the WHR declined when the austenite phase is exhausted. During plastic deformation, the volume-fraction weighted phase stress and stress contribution from the $$alpha$$'-martensite increase significantly. The neutron diffraction data further suggest that the $$gamma$$-to-$$alpha$$' phase transformation was mediated by the $$varepsilon$$-martensite, as evidenced by the concurrent decline of the $$varepsilon$$ phase with the $$gamma$$ phase.

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

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

Crystal-liquid duality driven ultralow two-channel thermal conductivity in $$alpha$$-MgAgSb

Li, J.*; Li, X.*; Zhang, Y.*; Zhu, J.*; Zhao, E.*; 古府 麻衣子; 中島 健次; Avdeev, M.*; Liu, P.-F.*; Sui, J.*; et al.

Applied Physics Reviews (Internet), 11(1), p.011406_1 - 011406_8, 2024/03

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

The desire for intrinsically low lattice thermal conductivity ($$kappa_L$$) in thermoelectrics motivates numerous efforts on understanding the microscopic mechanisms of heat transport in solids. Here, based on theoretical calculations, we demonstrate that $$alpha$$-MgAgSb hosts low-energy localized phonon bands and avoided crossing of the rattler modes, which coincides with the inelastic neutron scattering result. Using the two-channel lattice dynamical approach, we find, besides the conventional contribution ($$sim$$70% at 300 K) from particlelike phonons propagating, the coherence contribution dominated by the wavelike tunneling of phonons accounts for $$sim$$30% of total $$kappa_L$$ at 300 K. By considering dual contributions, our calculated room-temperature $$kappa_L$$ of 0.64 Wm$$^{-1}$$K$$^{-1}$$ well agrees with the experimental value of 0.63 Wm$$^{-1}$$K$$^{-1}$$. More importantly, our computations give a nonstandard $$kappa_L propto T^{-0.61}$$ dependence, perfectly explaining the abnormal temperature-trend of $$sim T^{-0.57}$$ in experiment for $$alpha$$-MgAgSb. By molecular dynamics simulation, we reveal that the structure simultaneously has soft crystalline sublattices with the metavalent bonding and fluctuating liquid-like sublattices with thermally induced large amplitude vibrations. These diverse forms of chemical bonding arouse mixed part-crystal part-liquid state, scatter strongly heat-carrying phonons, and finally produce extremely low $$kappa_L$$. The fundamental research from this study will accelerate the design of ultralow-$$kappa_L$$ materials for energy-conversion applications.

論文

Microscopic origin of the spin-reorientation transition in the kagome topological magnet TbMn$$_{6}$$Sn$$_{6}$$

Huang, Z.*; Wang, W.*; Ye, H.*; Bao, S.*; Shangguan, Y.*; Liao, J.*; Cao, S.*; 梶本 亮一; 池内 和彦*; Deng, G.*; et al.

Physical Review B, 109(1), p.014434_1 - 014434_9, 2024/01

 被引用回数:0 パーセンタイル:0.01(Materials Science, Multidisciplinary)

TbMn$$_{6}$$Sn$$_{6}$$ is a correlated topological magnet with a Mn-based kagome lattice, in which a Chern gap opens at the Dirac point at low temperatures. The magnetic moment direction of the ferrimagnetic order changes from in the kagome plane to the out-of-plane upon cooling, which is essential for generating the Chern gap, but the underlying mechanism for the spin reorientation remains elusive. Here, we investigate the spin-reorientation transition in TbMn$$_{6}$$Sn$$_{6}$$ using neutron scattering. We provide direct evidence for the spin-reorientation transition and unveil the coexistence of two Tb modes at 200 K. To account for these results, we put forward a model based on SU(N) spin-wave theory, in which there is a temperature evolution of the ground state Tb $$4f$$ orbitals, driven by the crystalline electric field, single-ion anisotropy, and exchange interactions between Tb and Mn ions. Our findings shed light on the complex magnetism of TbMn$$_{6}$$Sn$$_{6}$$, despite its relatively simple ground state magnetic structure, and provide insights into the mechanisms for tuning magnetic topological materials.

論文

Stress corrosion cracking induced by the combination of external and internal hydrogen in Al-Zn-Mg-Cu alloy

Tang, J.*; Wang, Y.*; 藤原 比呂*; 清水 一行*; 平山 恭介*; 海老原 健一; 竹内 晃久*; 上椙 真之*; 戸田 裕之*

Scripta Materialia, 239, p.115804_1 - 115804_5, 2024/01

 被引用回数:0 パーセンタイル:0.00(Nanoscience & Nanotechnology)

Al-Zn-Mg-Cu合金の外部および内部水素(H)の組合せによって誘起される応力腐食割れ(SCC)の挙動をその場3次元評価技術を使い系統的に調べた。Al-Zn-Mg-Cu合金のSCCは水素濃度が臨界値を超える潜在的なクラック発生領域で発生・進展し、Hがナノスケール$$eta$$-MgZn$$_2$$析出物界面での原子結合を弱め巨視的な割れを引き起こしていることが分かった。さらに、水環境からき裂へ浸透した外部Hが、き裂先端近傍に勾配を持つH影響ゾーンを作ることでSCCにおいて重要な役割を果たすことや、あらかじめ存在する内部Hが、塑性変形に伴いき裂先端に向かうことでSCCにおけるき裂の発生と進展の両方に関与することも分かった。

論文

Cryogenic impact fracture behavior of a high-Mn austenitic steel using electron backscatter diffraction and neutron Bragg-edge transmission imaging

Wang, Y. W.*; Wang, H. H.*; Su, Y. H.; 徐 平光; 篠原 武尚

Materials Science & Engineering A, 887, p.145768_1 - 145768_13, 2023/11

 被引用回数:1 パーセンタイル:44.33(Nanoscience & Nanotechnology)

A unique impact fracture behavior is found in a high-Mn austenitic steel (24Mn-4Cr-0.4C-0.3Cu) in this work. The steel exhibits concurrent twinning-induced plasticity (TWIP) effect and the transformation-induced plasticity (TRIP) effect. By analyzing the load-deflection curves recorded during Charpy impact testing, the resistance to crack initiation and propagation is quantified from the absorbed energy. The high-Mn steel demonstrates good resistance to crack initiation at 273 K and 77 K. However, as the temperature decreases from 273 K to 77 K, there is an accelerated transition from stable crack growth to unstable crack growth during impact, resulting in the deterioration of resistance to crack propagation. The plastic deformation of the impact-tested samples, especially in the region close to the crack-path profile was quantitatively analyzed using neutron Bragg-edge transmission (BET) imaging. The deformation zones, divided by using the width of the 200 Bragg edge, exhibit good agreement with the impact absorbed energy characteristics obtained from dynamic load-deflection curves. Moreover, the unstable growth transition point was roughly determined on the impact-tested sample. Then, the electron backscatter diffraction (EBSD) technique is employed to examine the deformation microstructure along the crack-path in the impact-tested samples. The results revealed the dual roles of TRIP effect in impact toughness of the high-Mn steel. On one hand, the TRIP effect plays a positive role in improving resistance to crack initiation and propagation. On the other hand, the excessive accumulation of brittle $$varepsilon$$/$$alpha$$'-martensite caused by the enhanced TRIP effect at 77 K leads to quasi-cleavage fracture, thereby playing a negative role. Finally, we discussed the prominent toughening mechanisms associated with the TWIP and TRIP effects, which greatly impact the impact fracture behavior.

論文

Validation of the $$^{10}$$Be ground-state molecular structure using $$^{10}$$Be($$p,palpha$$)$$^{6}$$He triple differential reaction cross-section measurements

Li, P. J.*; Beaumel, D.*; Lee, J.*; Assi$'e$, M.*; Chen, S.*; Franchoo, S.*; Gibelin, J.*; Hammache, F.*; Harada, T.*; 延与 佳子*; et al.

Physical Review Letters, 131(21), p.212501_1 - 212501_7, 2023/11

$$^{10}$$Beのクラスター構造を($$p,palpha$$)反応を用いて調査した。三重微分断面積が実験的に測定され、Tohsaki-Horiuchi-Schuck-R$"o$pke波動関数の方法や反対称化分子動力学を用いた歪曲波インパルス近似計算と比較した。実験データと理論計算の顕著な一致が確認され、$$^{10}$$Beの比較的コンパクトな分子状態を確認した。

論文

Acoustically driven magnon-phonon coupling in a layered antiferromagnet

Lyons, T. P.*; Puebla, J.*; 山本 慧; Deacon, R. S.*; Hwang, Y.*; 石橋 幸治*; 前川 禎通*; 大谷 義近*

Physical Review Letters, 131(19), p.196701_1 - 196701_6, 2023/11

 被引用回数:2 パーセンタイル:72.40(Physics, Multidisciplinary)

Harnessing the causal relationships between mechanical and magnetic properties of van der Waals materials presents a wealth of untapped opportunity for scientific and technological advancement, from precision sensing to novel memories. This can, however, only be exploited if the means exist to efficiently interface with the magnetoelastic interaction. Here, we demonstrate acoustically-driven spin-wave resonance in a crystalline antiferromagnet, chromium trichloride, via surface acoustic wave irradiation. The resulting magnon-phonon coupling is found to depend strongly on sample temperature and external magnetic field orientation, and displays a high sensitivity to extremely weak magnetic anisotropy fields in the few mT range. Our work demonstrates a natural pairing between power-efficient strain-wave technology and the excellent mechanical properties of van der Waals materials, representing a foothold towards widespread future adoption of dynamic magneto-acoustics.

論文

Valley-selective phonon-magnon scattering in magnetoelastic superlattices

Liao, L.*; Puebla, J.*; 山本 慧; Kim, J.*; 前川 禎通*; Hwang, Y.*; Ba, Y.*; 大谷 義近*

Physical Review Letters, 131(17), p.176701_1 - 176701_6, 2023/10

 被引用回数:2 パーセンタイル:72.40(Physics, Multidisciplinary)

Phonons and magnons are engineered by periodic potential landscapes in phononic and magnonic crystals, and their combined studies may enable valley phonon transport tunable by the magnetic field. Through nonreciprocal surface acoustic wave transmission, we demonstrate valley-selective phonon-magnon scattering in magnetoelastic superlattices. The lattice symmetry and the out-of-plane magnetization component control the sign of nonreciprocity. The phonons in the valleys play a crucial role in generating nonreciprocal transmission by inducing helical strains that couple with the magnons. The transmission spectra show a nonreciprocity peak near a transmission gap, matching the phononic band structure. Our results open the way for manipulating valley phonon transport through periodically varying magnon-phonon coupling.

論文

PANDORA Project for the study of photonuclear reactions below $$A=60$$

民井 淳*; Pellegri, L.*; S$"o$derstr$"o$m, P.-A.*; Allard, D.*; Goriely, S.*; 稲倉 恒法*; Khan, E.*; 木戸 英治*; 木村 真明*; Litvinova, E.*; et al.

European Physical Journal A, 59(9), p.208_1 - 208_21, 2023/09

 被引用回数:2 パーセンタイル:79.22(Physics, Nuclear)

光核反応は原子核構造の観点からも応用の観点からも重要であるにも関わらず、その反応断面積は未だに不定性が大きい。近年、超高エネルギー宇宙線の起源を探るために、鉄よりも軽い原子核の光核反応断面積を正確に知る必要が指摘されている。この状況を打破するため、原子核物理の実験、理論、宇宙物理の共同研究となるPANDORAプロジェクトが始まった。本論文はその計画の概要をまとめたものである。原子核実験ではRCNP、iThembaによる仮想光子実験とELI-NPによる実光子実験などが計画されている。原子核理論では、乱雑位相近似計算、相対論的平均場理論、反対称化分子動力学、大規模殻模型計算などが計画されている。これらで得られた信頼性の高い光核反応データベースと宇宙線伝搬コードを組み合わせ、超高エネルギー宇宙線の起源の解明に挑む。

論文

Direct observation of topological magnon polarons in a multiferroic material

Bao, S.*; Gu, Z.-L.*; Shangguan, Y.*; Huang, Z.*; Liao, J.*; Zhao, X.*; Zhang, B.*; Dong, Z.-Y.*; Wang, W.*; 梶本 亮一; et al.

Nature Communications (Internet), 14, p.6093_1 - 6093_9, 2023/09

 被引用回数:2 パーセンタイル:72.40(Multidisciplinary Sciences)

Magnon polarons are novel elementary excitations possessing hybrid magnonic and phononic signatures, and are responsible for many exotic spintronic and magnonic phenomena. Despite long-term sustained experimental efforts in chasing for magnon polarons, direct spectroscopic evidence of their existence is hardly observed. Here, we report the direct observation of magnon polarons using neutron spectroscopy on a multiferroic Fe$$_{2}$$Mo$$_{3}$$O$$_{8}$$ possessing strong magnon-phonon coupling. Specifically, below the magnetic ordering temperature, a gap opens at the nominal intersection of the original magnon and phonon bands, leading to two separated magnon-polaron bands. Each of the bands undergoes mixing, interconverting and reversing between its magnonic and phononic components. We attribute the formation of magnon polarons to the strong magnon-phonon coupling induced by Dzyaloshinskii-Moriya interaction. Intriguingly, we find that the band-inverted magnon polarons are topologically nontrivial. These results uncover exotic elementary excitations arising from the magnon-phonon coupling, and offer a new route to topological states by considering hybridizations between different types of fundamental excitations.

論文

Level structures of $$^{56,58}$$Ca cast doubt on a doubly magic $$^{60}$$Ca

Chen, S.*; Browne, F.*; Doornenbal, P.*; Lee, J.*; Obertelli, A.*; 角田 佑介*; 大塚 孝治*; 茶園 亮樹*; Hagen, G.*; Holt, J. D.*; et al.

Physics Letters B, 843, p.138025_1 - 138025_7, 2023/08

 被引用回数:1 パーセンタイル:59.27(Astronomy & Astrophysics)

$$^{57,59}$$Scからの1陽子ノックアウト反応を用いて、$$^{56}$$Caと$$^{58}$$Caのガンマ崩壊を観測した。$$^{56}$$Caでは1456(12)keVの$$gamma$$線遷移が、$$^{58}$$Caでは1115(34)keVの遷移が観測された。どちらの遷移も暫定的に$$2^{+}_{1} rightarrow 0^{+}_{gs}$$と割り当てられた。有効核子間相互作用をわずかに修正した広い模型空間での殻模型計算では、$$2^{+}_{1}$$準位エネルギー、2中性子分離エネルギー、反応断面積が実験とよく一致し、N=34閉殻の上に新しい殻が形成されていることを裏付けた。その構成要素である$$0_{f5/2}$$$$0_{g9/2}$$軌道はほぼ縮退しており、これは$$^{60}$$Caが二重魔法核である可能性を排除し、Ca同位体のドリップラインを$$^{70}$$Caあるいはそれ以上にまで広げる可能性がある。

論文

${it In situ}$ neutron diffraction study on the deformation behavior of the plastic inorganic semiconductor Ag$$_{2}$$S

Wang, Y.*; Gong, W.; 川崎 卓郎; Harjo, S.; Zhang, K.*; Zhang, Z. D.*; Li, B.*

Applied Physics Letters, 123(1), p.011903_1 - 011903_6, 2023/07

 被引用回数:1 パーセンタイル:44.21(Physics, Applied)

Bulk Ag$$_{2}$$S is a plastic inorganic semiconductor at room temperature. It exhibits a compressive strain greater than 50%, which is highly different from brittle conventional counterparts, such as silicon. Here, we present the experimental investigation of the deformation behavior in a plastic inorganic semiconductor Ag$$_{2}$$S using ${it in situ}$ neutron diffraction during compressive deformation at room and elevated temperatures. At room temperature, the lattice strain partitioning among $$hkl$$-orientated grain families could be responsible for the significant work-hardening behavior in the bulk Ag$$_{2}$$S with a monoclinic structure. The rapid accumulation of lattice defects and remarkable development of the deformation texture suggest that dislocation slip promotes plasticity. At 453 K, a monoclinic phase transforms into a body-centered cubic phase. A stress plateau appears at $$sim$$-4.8 MPa, followed by a rehardening state. The deformation mode of bulk Ag$$_{2}$$S at the initial stage is likely attributable to the migration of silver ions, and as strain increases, it is closer to that of room temperature, leading to rehardening.

論文

The Development of a Multiphysics Coupled Solver for Studying the Effect of Dynamic Heterogeneous Configuration on Particulate Debris Bed Criticality and Cooling Characteristics

Li, C.-Y.; Wang, K.*; 内堀 昭寛; 岡野 靖; Pellegrini, M.*; Erkan, N.*; 高田 孝*; 岡本 孝司*

Applied Sciences (Internet), 13(13), p.7705_1 - 7705_29, 2023/07

 被引用回数:1 パーセンタイル:52.66(Chemistry, Multidisciplinary)

For a sodium-cooled fast reactor, the capability for stable cooling and avoiding re-criticality on the debris bed is essential for achieving in-vessel retention when severe accidents occur. However, an unexploited uncertainty still existed regarding the compound effect of the heterogeneous configuration and dynamic particle redistribution for the debris bed's criticality and cooling safety assessment. Therefore, this research aims to develop a numerical tool for investigating the effects of the different transformations of the heterogeneous configurations on the debris bed's criticality/cooling assessment. Based on the newly proposed methodology in this research, via integrating the Discrete Element Method (DEM) with Computational Fluid Dynamics (CFD) and Monte-Carlo-based Neutronics (MCN), the coupled CFD-DEM-MCN solver was constructed with the originally created interface to integrate two existing codes. The effects of the different bed configurations' transformations on the bed safety assessments were also quantitively confirmed, indicating that the effect of the particle-centralized fissile material had the dominant negative effect on the safety margin of avoiding re-criticality and particle re-melting accidents and had a more evident impact than the net bed-centralized effect. This coupled solver can serve to further assess the debris bed's safety via a multi-physics simulation approach, leading to safer SFR design concepts.

論文

Cu $$K$$-edge X-ray absorption fine structure study of $$T'$$-type $$RE$$$$_{2}$$CuO$$_{4+alpha-delta}$$ ($$RE$$ = Rare Earth); Toward unified understanding of electronic state of $$T'$$-type cuprate

Chen, Y.*; 浅野 駿*; Wang, T.*; Xie, P.*; 北山 慎之介*; 石井 賢司*; 松村 大樹; 辻 卓也; 谷口 貴紀*; 藤田 全基*

JPS Conference Proceedings (Internet), 38, p.011050_1 - 011050_6, 2023/05

To investigate the variation of the electronic state of $$T'$$-type cuprate due to annealing, we performed Cu $$K$$-edge X-ray absorption fine structure measurements on Pr$$_{2}$$CuO$$_{4+alpha-delta}$$ (PCO) and Pr$$_{1.3}$$La$$_{0.7}$$CuO$$_{4+alpha-delta}$$ (PLCO). The induced electrons due to annealing ($$n_{AN}$$) in PCO and PLCO were approximately 2$$delta$$, consistent with a model of electron doping to Mott insulator. Here, $$alpha$$ and $$delta$$ represent the amount of excess oxygen from the stoichiometric composition in the as-sintered compound and that of oxygen loss due to annealing, respectively. Furthermore, the energy of the Einstein oscillator ($$hbaromega_{E}$$) for the Cu-O$$_{p}$$ bond was evaluated by extended X-ray absorption fine structure analysis. (O$$_{p}$$ denotes the in-plane oxygen.) We found a small annealing effect on $$hbaromega_{E}$$ for both PCO and PLCO.

論文

Pressure engineering of van der Waals compound RhI$$_3$$; Bandgap narrowing, metallization, and remarkable enhancement of photoelectric activity

Fang, Y.*; Kong, L.*; Wang, R.*; Zhang, Z.*; Li, Z.*; Wu, Y.*; Bu, K.*; Liu, X.*; Yan, S.*; 服部 高典; et al.

Materials Today Physics (Internet), 34, p.101083_1 - 101083_7, 2023/05

 被引用回数:1 パーセンタイル:44.21(Materials Science, Multidisciplinary)

層状ファンデルワールスハライドは、外部圧力に対して特に敏感であるため、目的とする性質を持つ構造にチューンすることが可能となる。一方で、圧力に非常に敏感であるという特性は、同時に目的とする機能の実現に有害な相転移や格子歪みを引き起こす可能性があるためその操作は依然として困難である。この研究では、層状RhI$$_3$$結晶が持つ極めて弱い層間結合と高い機能可変性を観察した。5GPaという適度な圧力をかけると圧力誘起相転移が起こり、積層構造に変化が現れた。驚くべきことに、この相転移は、圧力に対してほぼ直線的なバンドギャップ減少という傾向に影響を与えなかった。また、より高い圧力では、1.3eVの赤方偏移というかなり大きな調整幅を伴う金属相が観測された。さらに、RhI$$_3$$のキャリア濃度は30GPaで4桁増加し、光電流は7.8GPaで5桁増加することが確認された。これらの結果は、ファンデルワールスハライドの層状構造という特異な特徴を生かした探索、調整、理解のための新たな機会を創出し、原子レベルの薄さを持つマテリアルバイデザインに基づく将来のデバイスとして有望である。

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, p.999 - 1006, 2023/05

 被引用回数:26 パーセンタイル:99.34(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.

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