Colossal barocaloric effects in plastic crystals

Li, B.*; 川北 至信; 河村 聖子; 菅原 武*; Wang, H.*; Wang, J.*; Chen, Y.*; 河口 沙織*; 河口 彰吾*; 尾原 幸治*; et al.

Nature, 567(7749), p.506 - 510, 2019/03

https://doi.org/10.1038/s41586-019-1042-5

冷却は現代社会では、世界における25-30%の電力が空調や食料保存に用いられるように、重要である。従来の気化、圧縮で冷却を行う方法は、温暖化などの観点から限界が来ている。有望な代替手段として固体の熱量効果を用いた冷却方法が注目を集めている。しかしながら、この方法は、現在候補に挙げられている物質ではエントロピー変化の小ささや巨大な磁場を必要とするところなどから性能に限界がある。そこで我々は柔粘性結晶における圧力誘起の相転移で冷却が起こる巨大圧力熱量効果を報告する。柔粘性結晶の一つであるネオペンチルグリコールのエントロピー変化は室温近傍において単位キログラム、単位温度あたり、約389ジュールであった。圧力下の中性子散乱実験の結果から、そのような巨大圧力熱量効果は分子配向の非秩序化、巨大な圧縮率、極めて非線形性の強い格子ダイナミクスの組み合わせに由来することが明らかになった。我々の研究により、柔粘性結晶における巨大圧力熱量効果発現の微視的機構が明らかとなり、次世代の固体を使った冷却技術の確立に筋道を付けることができた。

Liquid-like thermal conduction in intercalated layered crystalline solids

Li, B.; Wang, H.*; 川北 至信; Zhang, Q.*; Feygenson, M.*; Yu, H. L.*; Wu, D.*; 尾原 幸治*; 菊地 龍弥*; 柴田 薫; et al.

Nature Materials, 17(3), p.226 - 230, 2018/03

http://dx.doi.org/10.1038/s41563-017-0004-2

As a generic property, all substances transfer heat through microscopic collisions of constituent particles. A solid conducts heat through both transverse and longitudinal acoustic phonons, but a liquid employs only longitudinal vibrations. As a result, a solid is usually thermally more conductive than a liquid. In canonical viewpoints, such a difference also serves as the dynamic signature distinguishing a solid from a liquid. Here, we report liquid-like thermal conduction observed in the crystalline AgCrSe. The transverse acoustic phonons are completely suppressed by the ultrafast dynamic disorder while the longitudinal acoustic phonons are strongly scattered but survive, and are thus responsible for the intrinsically ultralow thermal conductivity. This scenario is applicable to a wide variety of layered compounds with heavy intercalants in the van der Waals gaps, manifesting a broad implication on suppressing thermal conduction. These microscopic insights might reshape the fundamental understanding on thermal transport properties of matter and open up a general opportunity to optimize performances of thermoelectrics.

Super-absorbent polymer valves and colorimetric chemistries for time-sequenced discrete sampling and chloride analysis of sweat via skin-mounted soft microfluidics

Kim, S. B.*; Zhang, Y.*; Won, S. M.*; Bandodkar, A. J.*; 関根 由莉奈; Xue, Y.*; Koo, J.*; Harshman, S. W.*; Martin, J. A.*; Park, J. M.*; et al.

Small, 14(12), p.1703334_1 - 1703334_11, 2018/03

https://doi.org/10.1002/smll.201703334

This paper introduces super absorbent polymer valves and colorimetric sensing reagents as enabling components of soft, skin-mounted microfluidic devices designed to capture, store and chemically analyze sweat released from eccrine glands. The valving technology enables robust means for guiding the flow of sweat from an inlet location into a collection of isolated reservoirs, in a well-defined sequence. Analysis in these reservoirs involves a color responsive indicator of chloride concentration with a formulation tailored to offer stable operation with sensitivity optimized for the relevant physiological range. Evaluations on human subjects with comparisons against ex situ analysis illustrate the practical utility of these advances.

Atomically dispersed Pt on the surface of Ni particles; Synthesis and catalytic function in hydrogen generation from aqueous ammonia-borane

Li, Z.*; He, T.*; 松村 大樹; Miao, S.*; Wu, A.*; Liu, L.*; Wu, G.*; Chen, P.*

ACS Catalysis, 7(10), p.6762 - 6769, 2017/10

http://dx.doi.org/10.1021/acscatal.7b01790

We report herein that the single-atom alloy (SAA) made of atomically dispersed Pt on the surface of Ni particles (Pt is surrounded by Ni atoms) exhibits improved catalytic activity on the hydrolytic dehydrogenation of ammonia-borane, a promising hydrogen storage method for onboard applications. Specifically, an addition of 160 ppm of Pt leads to ca. 3-fold activity improvement in comparison to that of pristine Ni/CNT catalyst. The turnover frequency based on the isolated Pt is 12000 mol mol min, which is about 21 times the value of the best Pt-based catalyst ever reported. Our simulation results indicate that the high activity achieved stems from the synergistic effect between Pt and Ni, where the negatively charged Pt (Pt) and positively charged Ni (Ni) in the Pt-Ni alloy are prone to interact with H and OH of HO molecules, respectively, leading to an energetically favorable reaction pathway.

Shell evolution beyond =28 and =50; Spectroscopy of Zn

Shand, C. M.*; Podolyk, Zs.*; Grska, M.*; Doornenbal, P.*; Obertelli, A.*; Nowacki, F.*; Otsuka, T.*; Sieja, K.*; Tostevin, J. A.*; Tsunoda, T.*; et al.

Physics Letters B, 773, p.492 - 497, 2017/10

http://dx.doi.org/10.1016/j.physletb.2017.09.001

Low-lying states in neutron-rich Zn nuclei were measured for the first time via in-beam -ray spectroscopy at RIKEN. These include the 4 to 2 in Zn and the 2 to 0 and 4 to 2 in Zn. The reduced E() energies and increased E(4)/E(2) ratios at =52,54 compared to Zn attest that the magicity is confined just on the neutron number =50 only. The levels observed in Zn suggest the onset of deformation towards heavier Zn isotopes. The data were compared to state-of-the-art shell model calculations.

Observation of magnetoelastic effects in a quasi-one-dimensional spiral magnet

Wang, C.*; Daiwei, Y.*; Liu, X.*; Chen, R.*; Du, X.*; Hu, B.*; Wang, L.*; 飯田 一樹*; 蒲沢 和也*; 脇本 秀一; et al.

Physical Review B, 96(8), p.085111_1 - 085111_5, 2017/08

AA2017-0274.pdf:1.02MB

http://dx.doi.org/10.1103/PhysRevB.96.085111

This paper presents a systematic study of spin and lattice dynamics in the quasi-one-dimensional spiral magnet CuBr, using Raman scattering in conjunction with infrared and neutron spectroscopy. Along with the development of spin correlations upon cooling, we observe a rich set of broad Raman bands at energies that correspond to phonon-dispersion energies near the one-dimensional magnetic wave vector. The low-energy bands further exhibit a distinct intensity maximum at the spiral magnetic ordering temperature.

decay of unbound neutron-hole states in Sn

Vaquero, V.*; Jungclaus, A.*; Doornenbal, P.*; Wimmer, K.*; Gargano, A.*; Tostevin, J. A.*; Chen, S.*; Ncher, E.*; Sahin, E.*; 志賀 慶明*; et al.

Physical Review Letters, 118(20), p.202502_1 - 202502_5, 2017/05

http://dx.doi.org/10.1103/PhysRevLett.118.202502

Excited states in Sn were populated following one-neutron knockout reaction from an unstable Sn beam at the RIBF laboratory in RIKEN. In addition to the already known rays, additional strength was observed for the first time in the excitation-energy range 3.5-5.5 MeV. Since the neutron separation energy of Sn is low, this observation provides direct evidence for the radioactive decay of neutron-unbound states in this nucleus. The ability of decay to compete with neutron emission was attributed to a mismatch between the wave functions of the initial and final states in the neutron emission case. These findings suggest that in the region south-east of Sn, nuclear structure effects play a significant role in the decay of unbound states, which are instead usually ignored in the evaluation of neutron-emission probabilities in astrophysical simulations.

A Multiscale Bayesian data integration approach for mapping air dose rates around the Fukushima Daiichi Nuclear Power Plant

Wainwright, Haruko*; 関 暁之; Chen, J.*; 斎藤 公明

Proceedings of International Waste Management Symposia 2017 (WM 2017) (Internet), 8 Pages, 2017/03

地上での測定による歩行サーベイと走行サーベイと上空から測定による航空機サーベイの複数タイプの空間線量率データを統合した。これらデータは領域・解像度・精度などに違いがあるが、本論文で用いた手法により、異質な空間の構造を地理統計的に表現し、さらに階層ベイズモデルを使って統一した手順で統合している。ベイズ手法は予測の不確実性を定量化し、信頼区間を提供することで意思決定に役立つ。ここでは、避難指示区域周辺の高い空間線量率を示す領域についてデータ統合し、高解像度な空間線量率の地図を提供した。

Are there signatures of harmonic oscillator shells far from stability?; First spectroscopy of Zr

Paul, N.*; Corsi, A.*; Obertelli, A.*; Doornenbal, P.*; Authelet, G.*; Baba, H.*; Bally, B.*; Bender, M.*; Calvet, D.*; Chteau, F.*; et al.

Physical Review Letters, 118(3), p.032501_1 - 032501_7, 2017/01

http://dx.doi.org/10.1103/PhysRevLett.118.032501

The first measurement of rays emitted by the very neutron rich nuclei Mo (Z=42) and Zr (Z=40) was carried out at the RIBF facility at RIKEN. These data shine light on the postulated N=70 harmonic oscillator shell. If the spin-orbit splitting which gives rise to the N=82 shell gap is reduced in very neutron-rich nuclei, the harmonic oscillator gap at N=70 should open instead. However, both the measured energy of the first excited state Mo and Zr, respectively 235(7) keV and 185(11) keV, and their E(4)/E(2) ratio, indicate that these nuclei are good rotors, and exclude the shell stabilization scenario at Z=40 and N=70. These results were compared to state-of-the-art density functional theoretical calculations using Gogny and Skyrme effective interactions.

Volume-wise destruction of the antiferromagnetic Mott insulating state through quantum tuning

Frandsen, B. A.*; Liu, L.*; Cheung, S. C.*; Guguchia, Z.*; Khasanov, R.*; Morenzoni, E.*; Munsie, T. J. S.*; Hallas, A. M.*; Wilson, M. N.*; Cai, Y.*; et al.

Nature Communications (Internet), 7, p.12519_1 - 12519_8, 2016/08

http://dx.doi.org/10.1038/ncomms12519

RENiO (RE = rare-earth element) and VO are archetypal Mott insulator systems. When tuned by chemical substitution (RENiO) or pressure (VO), they exhibit a quantum phase transition (QPT) between an antiferromagnetic Mott insulating state and a paramagnetic metallic state. Because novel physics often appears near a Mott QPT, the details of this transition, such as whether it is first or second order, are important. Here, we demonstrate through muon spin relaxation/rotation experiments that the QPT in RENiO and VO is first order: the magnetically ordered volume fraction decreases to zero at the QPT, resulting in a broad region of intrinsic phase separation, while the ordered magnetic moment retains its full value until it is suddenly destroyed at the QPT. These findings bring to light a surprising universality of the pressure-driven Mott transition, revealing the importance of phase separation and calling for further investigation into the nature of quantum fluctuations underlying the transition.