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論文

Investigating eutectic behavior and material relocation in B$$_{4}$$C-stainless steel composites using the improved MPS method

Ahmed, Z.*; Wu, S.*; Sharma, A.*; Kumar, R.*; 山野 秀将; Pellegrini, M.*; 横山 諒*; 岡本 孝司*

International Journal of Heat and Mass Transfer, 250, p.127343_1 - 127343_17, 2025/11

The study aims to measure boron concentration through the unidirectional diffusion of boron within the stainless steel (SS) layers while evaluating the updated model ability to replicate melt relocation behavior and geometry. In the current MPS simulations, one scenario employed dummy walls as heat sources, while another scenario used SS surface particles as heat sources to avoid interference with the melt flow as it reached the bottom of the specimen.

論文

Magnetism of kagome metals (Fe$$_{1-x}$$Co$$_x$$)Sn studied by $$mu$$SR

Cai, Y.*; Yoon, S.*; Sheng, Q.*; Zhao, G.*; Seewald, E. F.*; Ghosh, S.*; Ingham, J.*; Pasupathy, A. N.*; Queiroz, R.*; Lei, H.*; et al.

Physical Review B, 111(21), p.214412_1 - 214412_17, 2025/06

We study the magnetic properties of the metallic kagome system (Fe$$_{1-x}$$Co$$_x$$)Sn by a combination of muon spin relaxation ($$mu$$SR), magnetic susceptibility, and scanning tunneling microscopy (STM) measurements in single crystal specimens with Co concentrations $$x$$ = 0, 0.11, 0.8. In the undoped antiferromagnetic compound FeSn, we find possible signatures for a previously unidentified phase that sets in at $$T^{*}sim 50$$~K, well beneath the Neel temperature $$T_{N}sim 376$$~K as indicated by a peak in the relaxation rate 1/$$T_1$$ observed in zero field (ZF) and longitudinal field (LF) $$mu$$SR measurements, with a corresponding anomaly in the ac and dc susceptibility, and an increase in the static width 1/$$T_2$$ in ZF-$$mu$$SR measurements. No signatures of spatial symmetry breaking are found in STM down to 7~K. Related to the location and motion of muons in FeSn, we confirmed a previous report that about 40% of the implanted muons reside at a field-cancelling high symmetry site at $$T < 250$$~K, while an onset of thermal hopping changes the site occupancy at higher temperatures. In Fe$$_{0.89}$$Co$$_{0.11}$$Sn, where disorder eliminated the field-cancellation effect, all the implanted muons exhibit precession and/or relaxation in the ordered state. In Fe$$_{0.2}$$Co$$_{0.8}$$Sn, we find canonical spin glass behavior with freezing temperature $$T_gsim 3.5$$~K; the ZF and LF-$$mu$$SR time spectra exhibit results similar to those observed in dilute alloy spin glasses CuMn and AuFe, with a critical behavior of $$1/T_1$$ at $$T_g$$ and $$1/T_1to 0$$ as $$Tto 0$$. The absence of spin dynamics at low temperatures makes a clear contrast to the spin dynamics observed by $$mu$$SR in many geometrically frustrated spin systems on insulating kagome, pyrochlore, and triangular lattices. The spin glass behavior of CoSn doped with dilute Fe moments is shown to originate primarily from the randomness of doped Fe moments rather than due to geometrical frustration of the underlying lattice.

論文

Synthesis of BaSiH$$_6$$ hydridosilicate at high pressures; A Bridge to BaSiH$$_8$$ polyhydride

Beyer, D. C.*; Spektor, K.*; Vekilova, O. Y.*; Grins, J.*; Barros Brant Carvalho, P. H.*; Leinbach, L. J.*; Sannemo-Targama, M.*; Bhat, S.*; Baran, V.*; Etter, M.*; et al.

ACS Omega (Internet), 10(15), p.15029 - 15035, 2025/04

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

SiH$$_6$$八面体部位を特徴とするヒドリドケイ酸塩は、水素貯蔵と水素化物イオン伝導に関連する潜在的な性質を持つかなり新しい化合物のクラスである。ここでは、Zintl相水素化物BaSiH$$_{sim 1.8}$$を4GPa以上の圧力でH$$_2$$流体と反応させ、その後常圧まで減圧して得られた新しい代表的なBaSiH$$_6$$について報告する。SiH$$_{6}^{2-}$$イオンはBa$$^{2+}$$対イオンによって八面体に配位している。Ba原子とSi原子の配置は理想的なfcc NaCl構造からわずかにずれている。IRとラマンスペクトルからSiH$$_{6}^{2-}$$の屈曲と伸縮モードがそれぞれ800-1200と1400-1800cm$$^{-1}$$の範囲で観測された。BaSiH$$_6$$は95$$^circ$$Cまで熱的に安定であり、それ以上ではBaH$$_2$$とSiに分解する。DFT計算により、直接バンドギャップは2.5eVであることが示された。BaSiH$$_6$$の発見により、ギガパスカル圧力(10GPa以下)のシリサイドの水素化反応からアクセス可能なヒドリドケイ酸塩の化合物クラスが固まった。BaSiH$$_6$$の構造的性質は、超伝導ポリハイドライドBaSiH$$_8$$を予測されるより高い圧力で水素化するための中間体(あるいは前駆体)であることを示唆している。

論文

Radiation heating effects on B$$_{4}$$C-SS eutectic melting and its relocation behaviour

Ahmed, Z.*; Sharma, A. K.*; Pellegrini, M.*; 山野 秀将; 岡本 孝司*

Arabian Journal for Science and Engineering, 50(5), p.3361 - 3371, 2025/03

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

This study pioneers the use of radiative heating for high-resolution visualisation and quantification of the eutectic melt composition, providing a novel approach to observing the melting and candling phenomena. Key findings include two distinct failure processes: SS cladding detachment forming molten droplets and fragmentation of B$$_{4}$$ pellets, with sintering observed in B$$_{4}$$ powder.

論文

Unusual low-temperature ductility increase mediated by dislocations alone

Naeem, M.*; Ma, Y.*; Tian, J.*; Kong, H.*; Romero-Resendiz, L.*; Fan, Z.*; Jiang, F.*; Gong, W.; Harjo, S.; Wu, Z.*; et al.

Materials Science & Engineering A, 924, p.147819_1 - 147819_10, 2025/02

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

Face-centered cubic (fcc) medium-/high-entropy alloys (M/HEAs) typically enhance strength and ductility at cryogenic temperatures via stacking faults, twinning, or martensitic transformation. However, in-situ neutron diffraction on VCoNi MEA at 15 K reveals that strain hardening is driven solely by rapid dislocation accumulation, without these mechanisms. This results in increased yield strength, strain hardening, and fracture strain. The behavior, explained by the Orowan equation, challenges conventional views on cryogenic strengthening in fcc M/HEAs and highlights the role of dislocation-mediated plasticity at low temperatures.

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:12 パーセンタイル:91.22(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

Enhanced cryogenic mechanical properties of heterostructured CrCoNi multicomponent alloy; Insights from ${it in situ}$ neutron diffraction

Naeem, M.*; Ma, Y.*; Knowles, A. J.*; Gong, W.; Harjo, S.; Wang, X.-L.*; Romero Resendiz, L.*; 他6名*

Materials Science & Engineering A, 916, p.147374_1 - 147374_8, 2024/11

 被引用回数:2 パーセンタイル:63.37(Nanoscience & Nanotechnology)

Heterostructured materials (HSMs) improve the strength-ductility trade-off of alloys, but their cryogenic performance under real-time deformation is unclear. We studied heterostructured CrCoNi medium-entropy alloy via ${it in situ}$ neutron diffraction at 77 K and 293 K. A significant mechanical mismatch between fine and coarse grains led to an exceptional yield strength of 918 MPa at 293 K, increasing to 1244 MPa at 77 K with a uniform elongation of 34%. This strength-ductility synergy at 77 K is attributed to high dislocation pile-up density, increased planar faults, and martensitic transformation. Compared to homogeneous alloys, HSMs show promise for enhancing cryogenic mechanical performance in medium-/high-entropy alloys.

論文

Simulation and performance of $$^{99}$$Mo/$$^{99m}$$Tc radioisotope separation by modified extraction method

Pratama, C.*; 藤田 善貴; Saptiama, I.*; Marlina, M.*; Triyatna, F.*; Ilhami, A.*; Maria, C. P.*; 土谷 邦彦; Teguh, A.*; Prasetyo, I.*

Journal of Physics; Conference Series, 2828, p.012025_1 - 012025_12, 2024/10

核医学検査薬として用いられるテクネチウム-99m($$^{99m}$$Tc)は、モリブデン-99($$^{99}$$Mo)の娘核種として生成される。本研究では$$^{99}$$Mo/$$^{99m}$$Tc製造プロセスの分配係数(Kd)を決定し、$$^{99m}$$Tc抽出プロセスにおいて溶媒として用いるメチルエチルケトン(MEK)の抽出効率を評価することを目的とする。日本原子力研究開発機構(JAEA)と共同で実施した、$$^{99m}$$Tcの代替としてレニウム(Re)を使用した予備試験では、$$^{99m}$$Tc抽出プロセスでの最適条件を明らかにした。このデータに基づき、インドネシア国立研究イノベーション庁(BRIN)において$$^{99}$$Mo/$$^{99m}$$Tcを用いたホット試験を実施した結果、MEKによる$$^{99m}$$Tc抽出率は100%を超え、$$^{99m}$$Tc溶出工程では97.81%の回収率を達成した。さらに、ホットセルでのシミュレーションと設備の改善を実施したが、$$^{99m}$$Tc抽出回収率は44.86%、$$^{99m}$$Tc溶出回収率は90.62%であった。この計算の結果、分配係数(Kd-$$^{99m}$$Tc)は0.45だった。また、得られた$$^{99m}$$Tc溶液の放射性核種と放射化学純度はそれぞれ99.90%及び99.80%と優れていた。これらの結果は、日本及びインドネシアの$$^{99}$$Mo/$$^{99m}$$Tcの輸入依存を低減し、$$^{99m}$$Tcの国産化に貢献する。

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

Study on eutectic melting behavior of control rod materials in severe accidents of sodium-cooled fast reactors, 4; Analyzing Eutectic Melting and Relocation Dynamics in B$$_{4}$$C-stainless steel using the Moving Particle Semi-Implicit (MPS) Method

Ahmed, Z.*; Wu, S.*; Pellegrini, M.*; 岡本 孝司*; Sharma, A.*; 山野 秀将

Proceedings of 14th International Topical Meeting on Nuclear Reactor Thermal-Hydraulics, Operation, and Safety (NTHOS-14) (Internet), 14 Pages, 2024/08

本解析では、いったん共晶反応が起こると、ステンレス鋼(SS)へボロンが拡散していくことを示す。単価ホウ素(B$$_{4}$$C)とSSの界面で溶融が開始し、融体はSS被覆管を伝って流下する。また、昇温するにつれて、融体内のボロン濃度が上昇することがわかった。炉心内のB$$_{4}$$C侵入の効果を理解するため、更新されたMPS法によって、共晶反応モデルの計算能力がシビアアクシデントを模擬した制御棒の共晶反応及びその後の再配置を効果的に解析できることを示した。

論文

Numerical intercomparison of PHITS and Geant4 Monte Carlo codes for fast neutron inelastic scattering applications

Meleshenkovskii, I.*; Van den Brandt, K.*; 小川 達彦; Datema, C.*; Mauerhofer, E.*

European Physical Journal Plus (Internet), 139, p.565_1 - 565_9, 2024/07

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

速中性子散乱による非破壊分析は物質の成分分析手法として有用であるが、分析に用いられる中性子ビームや測定器には様々なパラメータがあり、実際の応用のためにはモンテカルロ放射線輸送計算コードによるシミュレーションなどで最適化する必要がある。しかし、モンテカルロ放射線輸送計算コードは核データや反応モデルによって散乱反応の観測量を計算していることから、既存コードが速中性子散乱を正確に描像できるかどうか、またコード間で観測量にどれほどの差異が生じるかは、信頼性の高いシミュレーションのために必要となる。そこで本研究では、世界的に広く用いられているモンテカルロ放射線輸送計算コードとしてPHITSとGeant4を例にとり、速中性子散乱における観測量を計算して相互に比較した。標的としてはホウ素、鉄、ネオジム、ディスプロシウムを用い、これらが2.5MeVの中性子に照射された際に、標的から出射する中性子のエネルギースペクトルを計算した。また、中性子照射された標的から生じるガンマ線を検出することを想定し、100keVから9000keVのガンマ線を、CeBrガンマ線検出器で検知した場合の波高スペクトルを計算した。これらの計算の結果、標的からの出射中性子スペクトルはホウ素ターゲットの場合に弾性散乱ピークと非弾性散乱成分の間に両コードで異なる傾向が見えるほかは、よく合致することが分かった。この傾向についても、弾性散乱の計算アルゴリズムの違いが原因であることが示唆されている。

論文

Study on the difference between B$$_{4}$$C powder and B$$_{4}$$C pellet regarding the eutectic reaction with stainless steel

Hong, Z.*; Ahmed, Z.*; Pellegrini, M.*; 山野 秀将; Erkan, N.*; Sharma, A. K.*; 岡本 孝司*

Progress in Nuclear Energy, 171, p.105160_1 - 105160_13, 2024/06

 被引用回数:4 パーセンタイル:93.24(Nuclear Science & Technology)

本研究では、B$$_{4}$$C粉末とステンレス鋼(SS)間との共晶反応はB$$_{4}$$C粉ペレットとSS間とのそれより相当に速いことが分かった。粉末及びペレットに対して導出された反応速度定数は参考文献値によく一致している。また、粉末とペレットの場合の詳細微細構造をSEM/EDSを用いて組成分析を行った。粉末の場合、(Fe,Cr)Bからなる反応層として厚肉層が見られた。一方、ペレットの場合、2つの反応層が見られた。

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

 被引用回数:9 パーセンタイル:95.42(Materials Science, Multidisciplinary)

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

Eutectic melting and relocation behavior of B$$_{4}$$C pellet-stainless steel under radiative heating

Ahmed, Z.*; Sharma, A. K.*; Pellegrini, M.*; 山野 秀将; 叶野 翔*; 岡本 孝司*

Ceramics International, 50(10), p.17665 - 17680, 2024/05

 被引用回数:2 パーセンタイル:58.08(Materials Science, Ceramics)

本研究では、2つの独特な破損メカニズムを同定した。一つはB$$_{4}$$Cペレットからステンレス鋼が分離した後に溶融液滴が形成する。もう一つはおそらく熱応力によってB$$_{4}$$Cペレットが複数個に破壊される。可視化技術と界面抵抗解析によって共晶温度を正確に捉えた。

論文

Probing deformation behavior of a refractory high-entropy alloy using ${it in situ}$ neutron diffraction

Zhou, Y.*; Song, W.*; Zhang, F.*; Wu, Y.*; Lei, Z.*; Jiao, M.*; Zhang, X.*; Dong, J.*; Zhang, Y.*; Yang, M.*; et al.

Journal of Alloys and Compounds, 971, p.172635_1 - 172635_7, 2024/01

 被引用回数:2 パーセンタイル:12.80(Chemistry, Physical)

The grain orientation-dependent lattice strain evolution of a (TiZrHfNb)$$_{98}$$$$N_2$$ refractory high-entropy alloy (HEA) during tensile loading has been investigated using ${it in situ}$ neutron diffraction. The equivalent strain-hardening rate of each of the primary $$<hkl>$$-oriented grain families was found to be relatively low, manifesting the macroscopically weak work-hardening ability of such a body-centered cubic (BCC)-structured HEA. This finding is indicative of a dislocation planar slip mode that is confined in a few single-slip planes and leads to in-plane softening by high pile-up stresses.

論文

Visualization experiments of radiation heating on the eutectic reaction between B$$_{4}$$C-SS and its relocation behavior

Ahmed, Z.*; Sharma, A. K.*; Pellegrini, M.*; 山野 秀将; 岡本 孝司*

Proceedings of Saudi International Conference On Nuclear Power Engineering (SCOPE2023) (Internet), 8 Pages, 2023/11

本研究では、共晶反応とそれに続くボロン移動の融体構造について、輻射加熱を使って定量的な高解像度可視化手法によって観察した。実験は、1150$$^{circ}$$Cから1372$$^{circ}$$Cの温度範囲で実機の制御棒設計を模擬したステンレス鋼(SS)管と炭化ホウ素(B$$_{4}$$C)ペレットを用いて実施した。正確な可視化技術によって、共晶溶融開始タイミングとその温度を同定し、ペレットとパウダーのケースで差異を指摘した。

論文

Key role of temperature on delamination in solid-state additive manufacturing via supersonic impact

Wang, Q.*; Ma, N.*; Huang, W.*; Shi, J.*; Luo, X.-T.*; 冨高 宙*; 諸岡 聡; 渡邊 誠*

Materials Research Letters (Internet), 11(9), p.742 - 748, 2023/09

 被引用回数:2 パーセンタイル:25.24(Materials Science, Multidisciplinary)

Cold spray (CS) has emerged as a representative of solid-state additive manufacturing (AM) via supersonic impact. It enables a high deposition rate of solid-state microparticles. Delamination, however, tends to occur when depositing too thick; this remains to be conquered. Here, a CS-like process, warm spray (WS), was presented. Interestingly, it was found that the appropriate increase in particle temperature can effectively reduce the residual stress amplitude, relieving the concentrated tensile stress and safeguarding the additively manufactured components from interfacial delamination even when depositing too thick. The key role of temperature on delamination was identified in solid-state AM via supersonic impact.

論文

A One-third magnetization plateau phase as evidence for the Kitaev interaction in a honeycomb-lattice antiferromagnet

Shangguan, Y.*; Bao, S.*; Dong, Z.-Y.*; Xi, N.*; Gao, Y.-P.*; Ma, Z.*; Wang, W.*; Qi, Z.*; Zhang, S.*; Huang, Z.*; et al.

Nature Physics, 19(12), p.1883 - 1889, 2023/09

 被引用回数:19 パーセンタイル:94.19(Physics, Multidisciplinary)

The magnetization of a quantum magnet can be pinned at a fraction of its saturated value by collective effects. One example of such a plateau phase is found in spin-1/2 triangular-lattice antiferromagnets. They feature strong geometrical frustration and the plateau phase therein is often interpreted as arising from an order-by-disorder mechanism driven by quantum fluctuations. Here we observe a one-third magnetization plateau under an applied magnetic field in the spin-1 antiferromagnet Na$$_{3}$$Ni$$_{2}$$BiO$$_{6}$$ with a honeycomb lattice, which, with conventional magnetic interactions, would not be geometrically frustrated. Based on our elastic neutron scattering measurements, we propose the spin structure of the plateau phase to be an unusual partial spin-flop ferrimagnetic order. Our theoretical calculations indicate that bond-anisotropic Kitaev interactions are the source of frustration that produces the plateau. These results suggest that Kitaev interactions provide a different route to frustration and phases driven by quantum fluctuations in high-spin magnets.

論文

First observation of $$^{28}$$O

近藤 洋介*; Achouri, N. L.*; Al Falou, H.*; Atar, L.*; Aumann, T.*; 馬場 秀忠*; Boretzky, K.*; Caesar, C.*; Calvet, D.*; Chae, H.*; et al.

Nature, 620(7976), p.965 - 970, 2023/08

 被引用回数:27 パーセンタイル:94.86(Multidisciplinary Sciences)

非常に中性子が過剰な原子核$$^{28}$$Oは、陽子、中性子ともに魔法数であることから古くからその性質に興味が持たれていたが、酸素の最後の束縛核$$^{24}$$Oよりも中性子が4個も多いため、これまで観測されてこなかった。この論文では、理化学研究所RIBFにて$$^{29}$$Fからの1陽子ノックアウト反応によって$$^{28}$$Oを生成し、そこから放出される中性子を測定することによって初めてその観測に成功した。核構造の観点からは、$$^{28}$$Oでは二重閉殻が保たれているか興味が持たれていたが、実験で得られた分光学的因子が殻模型計算で予言されて程度の大きいことから、閉殻構造をもたない可能性が高いことがわかった。

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:76 パーセンタイル:99.20(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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