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Journal Articles

Temperature dependence of ortho-positronium annihilation in room temperature ionic liquids

Hirade, Tetsuya; Michishio, Koji*; Kobayashi, Yoshinori*; Oshima, Nagayasu*

Acta Physica Polonica A, 137(2), p.109 - 112, 2020/02

 Times Cited Count:0 Percentile:100(Physics, Multidisciplinary)

Recently, it was reported that the positronium (Ps) bubble in Room Temperature Ionic Liquids (RTILs) showed some phenomena that were very different from them observed in other molecular liquids. Now the reason of these interesting phenomena is being understood. The structure caused by the ionic interaction between anions and cations can exist even at the higher temperatures than the melting temperatures. It was the reason why the oscillation of Ps bubble was observed at the temperatures near the melting temperatures in RTILs. The temperature dependence of the Ps bubble size estimated by the triplet Ps ($$ortho$$-Ps) pick-off annihilation lifetime indicated that there was a nano-meter structure remained by ionic interactions even at high temperatures. The $$ortho$$-Ps pick-off annihilation lifetime will be a strong tool to study nano-structure in RTILs.

Journal Articles

Positronium in room temperature ionic liquids

Hirade, Tetsuya

AIP Conference Proceedings 2182, p.030007_1 - 030007_5, 2019/12

There are many new application of room temperature ionic liquids (RTILs) for many different fields. One of them is reprocessing spent nuclear fuels and then research of irradiation effects on RTILs are very important. The positron annihilation techniques are very strong tool to investigate fast reactions of excess electrons. Positron annihilation age-momentum correlation (AMOC) experiment was applied to deepen understanding the phenomena occurred at very young positron ages. We clarified that Ps bubble formation in RTILs was very slow and, finally, oscillation of Ps bubble was observed just after the Ps formation at near melting temperatures. These results can indicate that Ps formation occurred in very short time in RTILs. The phenomena observed by Ps just in RTILs will be discussed.

Journal Articles

Development of an online measurement system using an alpha liquid scintillation counter and a glass-based microfluidic solvent extraction device for plutonium analysis

Yamamoto, Masahiko; Taguchi, Shigeo; Do, V. K.; Kuno, Takehiko; Surugaya, Naoki

Applied Radiation and Isotopes, 152, p.37 - 44, 2019/10

 Times Cited Count:1 Percentile:56.06(Chemistry, Inorganic & Nuclear)

An online measurement system using an alpha liquid scintillation counter ($$alpha$$-LSC) coupled to microchip solvent extraction has been developed. A flow-through cell of $$alpha$$-LSC has been prepared by packing PTFE tube into glass tube to combine microchip. Two-phase flow in microchannel has been stabilized by using coiled tube. The Pu in organic phase has been mixed with scintillation cocktail by T-junction connectors. The system separates and detects Pu by online with detection limit of 6.5 Bq/mL, generating only $$mu$$L-level wastes.

Journal Articles

Controlled deuterium labelling of imidazolium ionic liquids to probe the fine structure of the electrical double layer using neutron reflectometry

Akutsu, Kazuhiro*; Cagnes, M.*; Tamura, Kazuhisa; Kanaya, Toshiji*; Darwish, T. A.*

Physical Chemistry Chemical Physics, 21(32), p.17512 - 17516, 2019/08

 Times Cited Count:1 Percentile:75.85(Chemistry, Physical)

We combined the deuterium labeling and neutron reflectivity techniques to determine the fine structure of the electric double layer structure in an imidazolium ionic liquid (IL). For this, a simple and large scale deuteration method for imidazolium ILs was developed, where the deuteration level can be systematically controlled.

Journal Articles

Anomalous structure of liquid Bi studied by coherent QENS and time-space correlation analysis

Kawakita, Yukinobu; Kikuchi, Tatsuya*

Hamon, 29(2), p.91 - 94, 2019/05

Bismuth (Bi) has a double-layered structure based on Peierls distortion in crystalline phase. Complicated static structure in liquid phase which cannot be interpreted by a simple packing model has been conjectured that Peierls distortion may remain even in liquid phase. We measured quasi-elastic neutron scattering (QENS) of liquid Bi by using AMATERAS installed at BL14 beamport of Materials and Life Science Experimental Facility (MLF) in J-PARC and analyzed coherent QENS spectra. A time-space correlation function revealed that the nearest neighboring shell followed by a shoulder-like structure at longer side consists of four contributions of short and long correlations with relatively long relaxation time of a few tens pico second and medium-ranged and the longest correlations with a short relaxation time of sub-pico second, which is a direct observation of the existing layered structure in liquid Bi. In this article, we report the above scientific results and the method to analyze coherent QENS by the time-space correlation function.

Journal Articles

Spin correlations of quantum spin liquid and quadrupole-ordered states of Tb$$_{2+x}$$Ti$$_{2-x}$$O$$_{7+y}$$

Kadowaki, Hiroaki*; Wakita, Mika*; F${aa}$k, B.*; Ollivier, J.*; Kawamura, Seiko; Nakajima, Kenji; Lynn, J. W.*

Physical Review B, 99(1), p.014406_1 - 014406_12, 2019/01

 Times Cited Count:3 Percentile:40.4(Materials Science, Multidisciplinary)

Spin correlations of the frustrated pyrochlore oxide Tb$$_{2+x}$$Ti$$_{2-x}$$O$$_{7+y}$$ have been investigated by using inelastic neutron scattering on single-crystalline samples (x = -0.007, 0.000, and 0.003), which have the putative quantum-spin-liquid (QSL) or electric-quadrupolar ground states. Spin correlations, which are notably observed in nominally elastic scattering, show short-range correlations around $$Gamma$$ points, tiny antiferromagnetic Bragg scattering at L and $$Gamma$$ points, and pinch-point-type structures around $$Gamma$$ points. The short-range spin correlations were analyzed using a random-phase approximation (RPA) assuming the paramagnetic state and two-spin interactions among Ising spins. These analyses have shown that the RPA scattering intensity well reproduces the experimental data using temperature- and x-dependent coupling constants of up to tenth-neighbor site pairs. This suggests that no symmetry breaking occurs in the QSL sample and that a quantum treatment beyond the semiclassical RPA approach is required. Implications of the experimental data and the RPA analyses are discussed.

Journal Articles

Anomaly of structural relaxation in complex liquid metal of bismuth; Dynamic correlation function of coherent quasi-elastic neutron scattering

Kawakita, Yukinobu; Kikuchi, Tatsuya*; Inamura, Yasuhiro; Tahara, Shuta*; Maruyama, Kenji*; Hanashima, Takayasu*; Nakamura, Mitsutaka; Kiyanagi, Ryoji; Yamauchi, Yasuhiro*; Chiba, Kaori*; et al.

Physica B; Condensed Matter, 551, p.291 - 296, 2018/12

 Times Cited Count:6 Percentile:43.39(Physics, Condensed Matter)

There are elemental liquid metals with complex structures far from the hard sphere (HS) packing model. Liquid Bi has an asymmetric first peak in the structure factors S(Q). The pair distribution function g(r) exhibits strange distance ratio of 1:2 between the first and the second peaks. Since a HS model with two kinds of radius produces asymmetry of the main peak in S(Q), existence of short-lived covalent bonds was discussed. Contrarily, modulation of the atomic distribution by the Friedel oscillations of shielding electrons around metallic ions was discussed. To examine its bonding nature from viewpoints of dynamic correlation functions, we have measured neutron quasielastic scattering of liquid Bi by using cold disk chopper spectrometer installed at MLF of J-PARC. The van Hove function revealed that the shoulder structure located at a longer side of the first peak in g(r) exhibits a longer relaxation time than the main structures such as the first and second peaks.

Journal Articles

Positronium in room temperature ionic liquids

Hirade, Tetsuya

Yodenshi Kagaku, (11), p.33 - 40, 2018/09

The positron injected in insulating materials thermalizes at the end part of its track and forms Positronium (Ps) with one of excess electrons within $$sim$$ 1 ps. Therefore, Ps formation can be a tool to investigate very fast processes like excess electron solvation in liquids. Many phenomena appeared in radiation chemistry researches for room temperature ionic liquids (ILs) are interesting and important for the application. Positron annihilation lifetime (PAL) measurements in ILs were carried out and anomalously long lifetime values of the shortest lifetime component were found in ILs. PAL and positron annihilation age-momentum correlation (AMOC) measurements were performed to clarify the reason of these anomalously long lifetime values and Ps bubble oscillation was finally discovered. Recent progresses are introduced with showing some results.

Journal Articles

Neutron source

Takada, Hiroshi

Kasokuki Handobukku, p.330 - 333, 2018/04

Spallation neutron source provides thermal and cold neutrons for materials researches. Those neutrons are obtained by slowing down the neutrons generated in a neutron production target by injecting high energy protons in surrounding reflector and moderators. This article introduces basic characteristics of the neutron production target at first, and then explains the characteristics of moderator, especially the design to generate high intensity and high quality neutron pulses with narrow width in the moderators used in the 1-MW spallation neutron source at J-PARC. Furthermore, the design procedure of the spallation neutron source is described.

Journal Articles

Positron annihilation in the near surface of room temperature ionic liquids

Hirade, Tetsuya; O'Rourke, B. E.*; Kobayashi, Yoshinori*

Journal of Physics; Conference Series, 791(1), p.012029_1 - 012029_4, 2017/02

 Times Cited Count:1 Percentile:43.44

We tried to observe the positron annihilation rates near surface of (room temperature ionic liquids) IL's, such as N,N,N-trimethyl-N-propylammonium bis(trifluoromethanesulfonyl)imide (TMPA-TFSI) by use of the perpendicular slow positron beamline installed at AIST. The vaper pressure of TMPA-TFSI is very small and hence it is possible to measure the positron annihilation rate in vacuum chamber directly. This represents the first energy variable experimental results of the positron annihilation rate at the near surface of an IL. The triplet positronium annihilation rate seems to be larger at nearer region to the surface of the IL's.

Journal Articles

Exotic field induced quantum phase transition of the kagome lattice antiferromagnet

Sakai, Toru; Nakano, Hiroki*

Physics Procedia, 75, p.821 - 828, 2015/12

 Times Cited Count:0 Percentile:100

The magnetization process of the S=1/2 kagome-lattice antiferromagnet is investigated using the numerical diagonalization up to 42-spin clusters. The critical exponent analysis confirms the unconventional magnetization behavior around the 1/3 magnetization plateau-like anomaly; the field derivative is infinite at the low-field side, while it is zero at the high-field side. We also confirm that a magnetization jump appears at 1/3 of the saturation magnetization in distorted kagome-lattice antiferromagnets.

Journal Articles

A Hybrid framework of first principles molecular orbital calculations and a three-dimensional integral equation theory for molecular liquids; Multi-center molecular Ornstein-Zernike self-consistent field approach

Kido, Kentaro; Kasahara, Kento*; Yokogawa, Daisuke*; Sato, Hirofumi*

Journal of Chemical Physics, 143(1), p.014103_1 - 014103_9, 2015/07

 Times Cited Count:2 Percentile:89.91(Chemistry, Physical)

Journal Articles

Positronium bubble oscillation in room temperature ionic liquids; Temperature dependence

Hirade, Tetsuya

Journal of Physics; Conference Series, 618(1), p.012004_1 - 012004_5, 2015/06

 Times Cited Count:3 Percentile:18.37

Positronium (Ps; a bound state of positron and electron) has a negative work function in materials and forms a bubble state in liquids. On the way of stable bubble state, the bubble grows and probably oscillates. The usual fast bubble formation has not been observed with the time resolution of the positron annihilation methods that is usually 100-200 pico-seconds. There had been many anomalous phenomena observed in the room temperature ionic liquids (RTIL). Recently it was found that very slow bubble formation caused these anomalous phenomena. And hence the oscillation of the Ps bubble was successfully observed by the change of the annihilation rate of the triplet Ps that is affected by the size of the bubble. The oscillation and the decay of the bubble give the information of the viscoelastic properties at the sub-nano scale. The temperature dependence of the oscillation has been also successfully indicated.

JAEA Reports

The Uranium waste fluid processing examination by liquid and liquid extraction method using the emulsion flow method

Kanda, Nobuhiro; Daiten, Masaki; Endo, Yuji; Yoshida, Hideaki; Mita, Yutaka; Naganawa, Hirochika; Nagano, Tetsushi; Yanase, Nobuyuki

JAEA-Technology 2015-007, 43 Pages, 2015/03


The centrifuge which has the subtlety information concerning the nuclear nonproliferation used for uranium enrichment technical development exists in the uranium enrichment facilities of Ningyo-toge Environmental Engineering Center, Japan Atomic Energy Agency. This centrifugal is performing separation processing of the radioactive material adhering to the surface of parts by wet decontamination of ultrasonic cleaning by dilute sulfuric acid and water, etc. By removing the uranium contained in waste fluid, generated sludge reduces activity concentration. And the possibility of reduction of sludge processing is examined. For this reason, from the 2007 fiscal year, Nuclear Science and Engineering Directorate and cooperation are aimed at, and development of the extraction separation technology of the "uranium" by the emulsion flow method is furthered. The test equipment using the developed emulsion flow method was tested. And dilute sulfuric acid and water were used for the examination as actual waste fluid. The result checked whether the various performances in Basic test carried out in Nuclear Science and Engineering Directorate would be obtained.

Journal Articles

Cross sections, stopping powers, and energy loss rates for rotational and phonon excitation processes in liquid water by electron impact

Kai, Takeshi; Yokoya, Akinari; Ukai, Masatoshi*; Watanabe, Ritsuko

Radiation Physics and Chemistry, 108, p.13 - 17, 2015/03

 Times Cited Count:9 Percentile:24.34(Chemistry, Physical)

Role of secondary electrons on DNA damage have not been understood sufficiently because there still exists a lack of cross section of rotational and phonon excitation in the liquid phase for precise simulation of the electron behavior. We calculated cross sections, stopping powers, and energy loss rates for the excitations in liquid water. The values for rotation are less by three orders of magnitude than those in the gas phase, while the values for phonon are close to those reported for amorphous ice. Thermalization process has so far been estimated from an assumption that the energy loss rates do not depend strongly on the energy below 1 eV. However, we found that the energy loss rates depend significantly on the energy. This fact indicates that the thermalization time will be longer than the previously estimated time, and we predict that thermalization process strongly involve in subsequent hydrated and chemical processes. The data set provide here is expected to useful to make the role of the secondary electrons on DNA damage much clear.

Journal Articles

Material issues relating to high power spallation neutron sources

Futakawa, Masatoshi

IOP Conference Series; Materials Science and Engineering, 74(1), p.012001_1 - 012001_7, 2015/02

 Times Cited Count:2 Percentile:23.89

Innovative researches using neutrons are being performed at the Materials and Life Science Experimental Facility, MLF, at the Japan Proton Accelerator Research Complex, J-PARC, in which a mercury target system is installed for MW-class pulse spallation neutron sources. The structural materials of the mercury target are subjected to irradiation damage due to protons and neutrons, very high cycle fatigue damages due to repeated pressure waves caused by the proton beam bombardment in mercury and so-called liquid metal embrittlement. That is, the structural materials must be said to be exposed to the extremely severe environments. In the paper, research and development relating to the material issues in the high power spallation neutron sources that has been performed so far at J-PARC is summarized.

Journal Articles

Actively convected liquid metal divertor

Shimada, Michiya; Hirooka, Yoshihiko*

Nuclear Fusion, 54(12), p.122002_1 - 122002_7, 2014/12

 Times Cited Count:22 Percentile:16.52(Physics, Fluids & Plasmas)

Tungsten is considered to be the most promising material for divertor in a fusion reactor. Tungsten divertor can withstand the heat loads of ITER, but the heat loads of DEMO divertor is a challenge. Pulsive heat loads as those associated with disruption could melt tungsten targets. The surface would not be flat after subsequent resolidification, which would significantly deteriorate its heat handling capability. Furthermore, DBTT of tungsten is rather high: $$sim$$ 400$$^{circ}$$C, which would become even higher after neutron irradiation, possibly resulting in cracks in tungsten. Our proposal is to use liquid metal for the divertor target material and actively circulate it with $$j$$ $$times$$ $$B$$ force. A simplified analysis of mhd equation in a cylindrical geometry suggests that the engineering requirement is modest. This analysis suggests that this new divertor concept merits further investigation.

Journal Articles

Status of development of Lithium Target Facility in IFMIF/EVEDA project

Wakai, Eiichi; Kondo, Hiroo; Kanemura, Takuji; Hirakawa, Yasushi; Furukawa, Tomohiro; Hoashi, Eiji*; Fukada, Satoshi*; Suzuki, Akihiro*; Yagi, Juro*; Tsuji, Yoshiyuki*; et al.

Proceedings of Plasma Conference 2014 (PLASMA 2014) (CD-ROM), 2 Pages, 2014/11

In the IFMIF/EVEDA (International Fusion Materials Irradiation Facility/ Engineering Validation and Engineering Design Activity), the validation tests of the EVEDA lithium test loop with the world's highest flow rate of 3000 L/min was succeeded in generating a 100 mm-wide and 25 mm-thick free-surface lithium flow steadily under the IFMIF operation condition of a high-speed of 15 m/s at 250$$^{circ}$$C in a vacuum of 10 $$^{-3}$$ Pa. Some excellent results of the recent engineering validations including lithium purification, lithium safety, and remote handling technique were obtained, and the engineering design of lithium facility was also evaluated. These results will advance greatly the development of an accelerator-based neutron source to simulate the fusion reactor materials irradiation environment as an important key technology for the development of fusion reactor materials.

Journal Articles

Effect of liquid-sheet thickness on detection sensitivity for laser-induced breakdown spectroscopy of aqueous solution

Oba, Hironori; Saeki, Morihisa; Wakaida, Ikuo; Tanabe, Rie*; Ito, Yoshiro*

Optics Express (Internet), 22(20), p.24478 - 24490, 2014/10

 Times Cited Count:11 Percentile:40.74(Optics)

For aqueous-solution-based elemental analysis, we used a thin liquid sheet ($$mu$$m-scale thickness) in laser-induced breakdown spectroscopy with nanosecond laser pulses. Laser-induced plasma is emitted by focusing a pulsed Nd:YAG laser (1064 nm) on a 5- to 80-$$mu$$m-thick liquid sheet in air. To optimize the conditions for detecting elements, we studied how the signal-to-background ratio (SBR) for H$$alpha$$ Balmer and Na-neutral emission lines depends on the liquid-sheet thickness. The SBR of the H$$alpha$$ Balmer and Na-neutral lines was maximized for a sheet thickness of $$sim$$20 $$mu$$m at the laser energy of 100 mJ. The hydrodynamics of liquid flow induced by the laser pulse was analyzed by laser flash shadowgraph imaging. Time-resolved observation of the hydrodynamics and plasma emission suggests that the dependence of the SBR on the liquid-sheet thickness is correlated with the volume of flowing liquid that interacts with the laser pulses.

367 (Records 1-20 displayed on this page)