Anomalous behavior of liquid molecules near solid nanoparticles; Novel interpretation on thermal conductivity enhancement in nanofluids

Hashimoto, Shunsuke*; Yamaguchi, Satoshi*; Harada, Masashi*; Nakajima, Kenji; Kikuchi, Tatsuya*; Oishi, Kazuki*

Journal of Colloid and Interface Science, 638, p.475 - 486, 2023/05

https://doi.org/10.1016/j.jcis.2023.01.101

Recently, it has been reported that anomalous improvement in the thermal conductivity of nanofluid composed of base liquids and dispersed solid nanoparticles, compared to the theoretically predicted value calculated from the particle fraction. Generally, the thermal conductivity values of gases and liquids are dominated by the mean free path of the molecules during translational motion. Herein, we present solid evidence showing the possible contribution of the vibrational behavior of liquid molecules around nanoparticles to increasing these thermal conductivities.

Mictomagnetism and suppressed thermal conduction of the prototype high-entropy alloy CrMnFeCoNi

Yang, J.*; Ren, W.*; Zhao, X.*; Kikuchi, Tatsuya*; Miao, P.*; Nakajima, Kenji; Li, B.*; Zhang, Z.*

Journal of Materials Science & Technology, 99, p.55 - 60, 2022/02

https://doi.org/10.1016/j.jmst.2021.04.077

High-entropy alloys are characteristic of extensive atomic occupational disorder on high-symmetric lattices, differing from traditional alloys. Here, we investigate magnetic and thermal transport properties of the prototype face-centered-cubic high-entropy alloy CrMnFeCoNi by combining physical properties measurements and neutron scattering. Direct-current (dc) and alternating-current (ac) magnetizations measurements indicate a mictomagnetic behavior with coexisting antiferromagnetic and ferromagnetic interactions in the entire temperature region and three anomalies are found at about 80, 50, and 20 K, which are related to the paramagnetic to antiferromagnetic transition, the antiferromagnetic to ferromagnetic transition, and the spin freezing, respectively. The electrical and thermal conductivities are significantly reduced compared to Ni and the temperature dependence of lattice thermal conductivity exhibits a glass-like plateau. Inelastic neutron scattering measurements suggest weak anharmonicity so that the thermal transport is expected to be dominated by the defect scattering.

Recent update of AMATERAS; A Cold-neutron disk-chopper spectrometer

Nakajima, Kenji; Kawamura, Seiko; Kofu, Maiko; Murai, Naoki; Inamura, Yasuhiro; Kikuchi, Tatsuya*; Wakai, Daisuke*

JPS Conference Proceedings (Internet), 33, p.011089_1 - 011089_7, 2021/03

https://doi.org/10.7566/JPSCP.33.011089

The recent update of AMATERAS, a cold-neutron disk-chopper spectrometer at Japan Proton Accelerator Research Complex (J-PARC), is reported. AMATERAS has been operating for a decade. Since 2017, some updates have been done or are underway, which include installing new detectors, replacing the vacuum system of the scattering chamber, and other works. We are also working on the re-investigation of the resolution function. Demonstration measurements were carried out at 1MW test operations done in 2018 and 2019. Plans of upgrading the spectrometer are currently being considered.

Mode distribution analysis for superionic melt of CuI by coherent quasielastic neutron scattering

Kawakita, Yukinobu; Kikuchi, Tatsuya*; Tahara, Shuta*; Nakamura, Mitsutaka; Inamura, Yasuhiro; Maruyama, Kenji*; Yamauchi, Yasuhiro*; Kawamura, Seiko; Nakajima, Kenji

JPS Conference Proceedings (Internet), 33, p.011071_1 - 011071_6, 2021/03

BB2019-1144.pdf:0.7MB

https://doi.org/10.7566/JPSCP.33.011071

CuI is a well-known superionic conductor in a high temperature solid phase where the mobile cations migrate between interstitial sites in the f.c.c. sublattice formed by iodine ions. Even in the molten state, it shows several features suggesting collective or cooperative ionic motion. MD results show that Cu diffuses much faster than I. The Cu-Cu partial structure factor have a FSDP which indicates a medium-range ordering of Cu ions. Moreover the Cu-Cu partial pair distribution deeply penetrates into the nearest neighboring Cu-I shell. To reveal origin such anomalous behaviors of molten CuI, we performed quaiselastic neutron scattering (QENS) by the disk-chopper spectrometer AMATERAS at MLF, J-PARC. To interpret the total dynamic structure factor obtained from coherent QENS, the mode distribution analysis was applied. It is found that the motion of iodine is a kind of fluctuating within an almost local area while Cu ions diffuse much faster than iodine ions.

Real time and real space analysis for coherent QENS and its application to liquid bismuth

Kikuchi, Tatsuya*; Kawakita, Yukinobu

Physica B; Condensed Matter, 567, p.51 - 54, 2019/08

https://doi.org/10.1016/j.physb.2019.01.022

Background issues encountered by cold-neutron chopper spectrometer AMATERAS

Kikuchi, Tatsuya*; Nakajima, Kenji; Kawamura, Seiko; Inamura, Yasuhiro; Nakamura, Mitsutaka; Wakai, Daisuke*; Aoyama, Kazuhiro*; Iwahashi, Takaaki*; Kambara, Wataru*

Physica B; Condensed Matter, 564, p.45 - 53, 2019/07

https://doi.org/10.1016/j.physb.2019.02.015

Details of the background, that is, unwanted signals accumulated by the data acquisition system of neutron instruments, observed by the cold-neutron chopper spectrometer AMATERAS installed at the Materials and Life Science Experimental Facility at J-PARC are reported. In the design phase of AMATERAS, we carefully considered the achievement of high signal-to-noise ratio, and possible countermeasures were implemented. Actually, recent scientific outputs from AMATERAS indicates that the spectrometer is one of excellent neutron instruments with low background. In spite of that, in nine years of AMATERAS operation, we have encountered unwanted signals due to various reasons, including gamma-rays emitted at materials on or near the beam line including the sample itself, scattered neutrons from the beam line devices, air scattering, electronic noise in data acquisition system, cosmic rays, T0 burst, and other unknown sources. In this report, we discuss the background observed by AMATERAS, especially in the conditions of without samples, comprehensively. The possible sources of these signals and the countermeasures considered against the above sources are discussed, which may be helpful to those who are engaged in other existing or planned neutron-scattering instruments.

Colossal barocaloric effects in plastic crystals

Li, B.*; Kawakita, Yukinobu; Kawamura, Seiko; Sugahara, Takeshi*; Wang, H.*; Wang, J.*; Chen, Y.*; Kawaguchi, Saori*; Kawaguchi, Shogo*; Ohara, Koji*; et al.

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

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

Refrigeration is of vital importance for modern society for example, for food storage and air conditioning- and 25 to 30% of the world's electricity is consumed for refrigeration. Current refrigeration technology mostly involves the conventional vapour compression cycle, but the materials used in this technology are of growing environmental concern because of their large global warming potential. As a promising alternative, refrigeration technologies based on solid-state caloric effects have been attracting attention in recent decades. However, their application is restricted by the limited performance of current caloric materials, owing to small isothermal entropy changes and large driving magnetic fields. Here we report colossal barocaloric effects (CBCEs) (barocaloric effects are cooling effects of pressure-induced phase transitions) in a class of disordered solids called plastic crystals. The obtained entropy changes in a representative plastic crystal, neopentylglycol, are about 389 joules per kilogram per kelvin near room temperature. Pressure-dependent neutron scattering measurements reveal that CBCEs in plastic crystals can be attributed to the combination of extensive molecular orientational disorder, giant compressibility and highly anharmonic lattice dynamics of these materials. Our study establishes the microscopic mechanism of CBCEs in plastic crystals and paves the way to next-generation solid-state refrigeration technologies.

Phonon dynamics of NaI investigated by G() analysis

Nakamura, Mitsutaka; Kikuchi, Tatsuya*; Kamazawa, Kazuya*; Kawakita, Yukinobu

Physica B; Condensed Matter, 551, p.351 - 354, 2018/12

BB2017-0467.pdf:0.48MB

https://doi.org/10.1016/j.physb.2017.12.057

The dynamic structure function in real space G() is deduced from the dynamical structure factor S() which can be obtained from inelastic neutron scattering measurement. In this study, we applied the G() analysis to NaI which is a typical alkali halide crystal. The optic and acoustic phonons of NaI are widely separated in energy because the difference in mass between the constituent atoms is large. These characteristic properties certainly help us to evaluate the G() features associated with the phonon modes. We measured the S() for NaI powder using the Fermi chopper spectrometer 4SEASONS at J-PARC, and converted S() into G() by newly developed software which utilizes the maximum entropy method. Our analysis clearly demonstrated the G() of TO mode oscillates out of phase with that of LA mode, which is physically reasonable. Further analyses will be given in the presentation.

Detailed study of the structure of the low-energy magnetic excitations in overdoped LaSrCuO

Ikeuchi, Kazuhiko*; Kikuchi, Tatsuya*; Nakajima, Kenji; Kajimoto, Ryoichi; Wakimoto, Shuichi; Fujita, Masaki*

Physica B; Condensed Matter, 536, p.717 - 719, 2018/05

https://doi.org/10.1016/j.physb.2017.11.022

To examine the detailed structure of low-energy magnetic excitations in a high-transition-temperature superconducting cuprate with heavily hole-doping, we performed inelastic neutron scattering experiments on LaSrCuO. We observed clear dispersion relations of the previously reported incommensurate (IC) magnetic correlations at = (0.5 , 0.5)/(0.5, 0.5 ). In addition, we show the emergence of continuum magnetic excitations with a ring shape centered at point in a constant energy spectrum at = 50 K. The radius of the ring ( = 0.109) is smaller than the incommensurability ( = 0.118). This suggests that the origin of the ring-like excitations is different from that of the IC magnetic correlations, and the low-energy magnetic excitations of the LaSrCuO system are inherently composed of these two kinds of excitations.

Retreat from stress; Rattling in a planar coordination

Suekuni, Koichiro*; Lee, C. H.*; Tanaka, Hiromi*; Nishibori, Eiji*; Nakamura, Atsushi*; Kasai, Hidetaka*; Mori, Hitoshi*; Usui, Hidetomo*; Ochi, Masayuki*; Hasegawa, Takumi*; et al.

Advanced Materials, 30(13), p.1706230_1 - 1706230_6, 2018/03

https://doi.org/10.1002/adma.201706230

Thermoelectric materials for highly efficient devices must satisfy conflicting requirements of high electrical conductivity and low thermal conductivity. In this paper, we studied the crystal structure and phonon dynamics of tetrahedrites (Cu,Zn)(Sb,As)S. The results revealed that the Cu atoms in a planar coordination are rattling, which effectively scatter phonons. These findings provide a new strategy for the development of highly efficient thermoelectric materials with planar coordination.