Nested antiferromagnetic spin fluctuations and non-Fermi-liquid behavior in electron-doped CeCoNiIn

Sakai, Hironori; Tokunaga, Yo; Kambe, Shinsaku; Zhu, J.-X.*; Ronning, F.*; Thompson, J. D.*; Kotegawa, Hisashi*; To, Hideki*; Suzuki, Kohei*; Oshima, Yoshiki*; et al.

Physical Review B, 106(23), p.235152_1 - 235152_8, 2022/12

https://doi.org/10.1103/PhysRevB.106.235152

We investigate the electronic state of Ni-substituted CeCoNiIn by nuclear quadrupole and magnetic resonance (NQR/NMR) techniques. The heavy fermion superconductivity below K for is suppressed by Ni substitutions, and reaches zero for . The In NQR spectra for and 0.25 can be explained by simulating the electrical field gradient that is calculated for a virtual supercell with density functional theory. The spin-lattice relaxation rate indicates that Ni substitution weakens antiferromagnetic correlations that are not localized near the substituent but instead are uniform in space. The temperature () dependence of for shows a maximum around K and decreases toward almost zero when temperature is further reduced as if a gap might be opening in the magnetic excitation spectrum; however, the magnetic specific heat and the static magnetic susceptibility evolve smoothly through with a dependence. The peculiar T dependence of and non-Fermi-liquid specific heat and susceptibility can be interpreted in a unified way by assuming nested antiferromagnetic spin fluctuations in a quasi-two-dimensional electronic system.

Temperature dependence of positron annihilation lifetime in near-surface and bulk of room-temperature ionic liquid observed by a slow positron beam

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

Chemical Physics Letters, 795, p.139507_1 - 139507_4, 2022/05

https://doi.org/10.1016/j.cplett.2022.139507

We obtained the temperature dependence up to 150C of the triplet positronium (-Ps) lifetime in N,N,N-Trimethyl-N-propylammonium bis(trifluoromethanesulfonyl)imide (TMPA-TFSI) by the vertical slow positron beamline installed at AIST. Positrons penetrate into the liquid surface of TMPA-TFSI with the positron energies of 2 keV and 12 keV to investigate at the near-surface and the balk. The surface structure was visible at 150C, 120C above the melting temperature. The -Ps lifetime became shorter at higher temperatures for both positron energies. Similar temperature dependence had appeared just in water as the result of the reaction of -Ps and radiolysis products such as the OH radicals. The temperature dependence observed for TMPA-TFSI suggested that the chemical reaction of -Ps occurred.

First study on Nihonium (Nh, Element 113) chemistry at TASCA

Yakushev, A.*; Lens, L.*; Dllmann, C. E.*; Block, M.*; Nagame, Yuichiro*; Sato, Tetsuya; Toyoshima, Atsushi*; 42 of others*

Frontiers in Chemistry (Internet), 9, p.753738_1 - 753738_9, 2021/11

https://doi.org/10.3389/fchem.2021.753738

Nihonium (Nh, element 113) and flerovium (Fl, element 114) are the first superheavy elements in which the 7p shell is occupied. High volatility and inertness were predicted for Fl due to the strong relativistic stabilization of the closed 7p sub-shell, which originates from a large spin-orbit splitting between the 7p and 7p orbitals. One unpaired electron in the outermost 7p sub-shell in Nh is expected to give rise to a higher chemical reactivity. Theoretical predictions of Nh reactivity are discussed, along with results of the first experimental attempts to study Nh chemistry in the gas phase. The experimental observations verify a higher chemical reactivity of Nh atoms compared to its neighbor Fl and call for the development of advanced setups. First tests of a newly developed detection device miniCOMPACT with highly reactive Fr isotopes assure that effective chemical studies of Nh are within reach.

Simple pretreatment method for tritium measurement in environmental water samples using a liquid scintillation counter

Nakasone, Shunya*; Yokoyama, Sumi*; Takahashi, Tomoyuki*; Ota, Masakazu; Kakiuchi, Hideki*; Sugihara, Shinji*; Hirao, Shigekazu*; Momoshima, Noriyuki*; Tamari, Toshiya*; Shima, Nagayoshi*; et al.

Plasma and Fusion Research (Internet), 16, p.2405035_1 - 2405035_5, 2021/02

https://doi.org/10.1585/pfr.16.2405035

Removal of impurities such as organic and other types of dissolved matters from environmental water samples is required for precise analysis of tritium with a liquid scintillation counting method. In general, a distillation method is a conventional one for tritium analysis in environmental water samples, but is a time-consuming process that takes 24 hours for removal of impurities. We have proposed a rapid pretreatment method for tritium analysis, that uses ion exchange resins. In this study, we performed batch experiments, to evaluate the effectiveness of the ion exchange resins on the tritium measurement. The results obtained demonstrated that removal of impurities in the sample water by ion exchange resins can be achieved during a short period of time (i.e., in 5 min).

Preliminary investigation of pretreatment methods for liquid scintillation measurements of environmental water samples using ion exchange resins

Nakasone, Shunya*; Yokoyama, Sumi*; Takahashi, Tomoyuki*; Ota, Masakazu; Kakiuchi, Hideki*; Sugihara, Shinji*; Hirao, Shigekazu*; Momoshima, Noriyuki*; Tamari, Toshiya*; Shima, Nagayoshi*; et al.

Plasma and Fusion Research (Internet), 15, p.2405027_1 - 2405027_3, 2020/05

https://doi.org/10.1585/pfr.15.2405027

A quick preprocessing system for tritium analysis of environmental samples is important to judge environmental influence of tritium releases due to accident or tritium-handling facilities. Analysis of tritium in water samples with liquid scintillation counting method requires removal of impurities such as organic matter and ion species from water samples. Generally, a distillation method is adopted as a pretreatment of analysis for tritium; however, the distillation method is a time-consuming process. The aim of this study is to evaluate a rapid pretreatment method for tritium analysis with ion exchange resin. From batch and column experiments that used inland water and ion exchange resin, we confirmed removals of impurities of the water sample and that the removal of impurities was possible for a short time (by 5 minutes).

Optimization of an isothermal gas-chromatographic setup for the chemical exploration of dubnium (Db, Z = 105) oxychlorides

Chiera, N. M.; Sato, Tetsuya; Tomitsuka, Tomohiro; Asai, Masato; Ito, Yuta; Shirai, Kaori*; Suzuki, Hayato; Tokoi, Katsuyuki; Toyoshima, Atsushi; Tsukada, Kazuaki; et al.

Journal of Radioanalytical and Nuclear Chemistry, 320(3), p.633 - 642, 2019/06

https://doi.org/10.1007/s10967-019-06505-w

An isothermal gas-chromatographic (IGC) device has been developed and tested for on-line gas phase studies of volatile oxychlorides of short-lived group-5 transition metals. Radioisotopes of niobium and tantalum, produced in nuclear fusion evaporation reactions, are directly flushed into the IGC setup by an inert gas-jet. Oxychloride compounds are formed by the addition of SOCl and O. Parameters influencing the formation and transport of NbOCl and TaOCl are investigated. For nuclides with half-lives () of about 30 s, an overall efficiency of 7% is obtained, rendering the IGC setup suitable for the chemical exploration of Db( = 34s).

Formation and thermochemical properties of oxychlorides of niobium (Nb) and tantalum (Ta); Towards the gas-phase investigation of dubnium (Db) oxychloride

Chiera, N. M.; Sato, Tetsuya; Tomitsuka, Tomohiro; Asai, Masato; Suzuki, Hayato*; Tokoi, Katsuyuki; Toyoshima, Atsushi; Tsukada, Kazuaki; Nagame, Yuichiro

Inorganica Chimica Acta, 486, p.361 - 366, 2019/02

https://doi.org/10.1016/j.ica.2018.10.032

The formation of NbOCl and TaOCl and their adsorption behavior on quartz surfaces was explored by applying an isothermal gas-chromatographic method. Trace amounts of short-lived Nb and Ta isotopes were used. Adsorption enthalpy values () at zero surface coverage of -(NbOCl) = 102 4 kJ/mol and -(TaOCl) = 128 5 kJ/mol were determined by analyzing the chromatographic behavior of the Nb andTa complexes with a Monte-Carlo simulation method based on an adsorption-desorption kinetic model.By applying an empirical correlation, the experimental values were successively related to the macroscopic standard sublimation enthalpy, , as a measure of the volatility of each substance. The inferred sublimation enthalpies are in agreement with tabulated thermochemical values. Thus, the linear empirical correlation between and for metal-oxychlorides was updated with the inclusion of the present data. According to the predicted (DbOCl), a (DbOCl) value of 135 2 kJ/mol was extrapolated. The future accomplishment of comparative studies with DbOCl under the same experimental conditions will provide valuable information on the volatility trend in Group-5 elements, together with an indication on the magnitude of relativistic effects on the electronic structure of dubnium.

First ionization potentials of Fm, Md, No, and Lr; Verification of filling-up of 5f electrons and confirmation of the actinide series

Sato, Tetsuya; Asai, Masato; Borschevsky, A.*; Beerwerth, R.*; Kaneya, Yusuke*; Makii, Hiroyuki; Mitsukai, Akina*; Nagame, Yuichiro; Osa, Akihiko; Toyoshima, Atsushi; et al.

Journal of the American Chemical Society, 140(44), p.14609 - 14613, 2018/11

https://doi.org/10.1021/jacs.8b09068

The first ionization potential (IP) yields information on valence electronic structure of an atom. IP values of heavy actinides beyond einsteinium (Es, Z = 99), however, have not been determined experimentally so far due to the difficulty in obtaining these elements on scales of more than one atom at a time. Recently, we successfully measured IP of lawrencium (Lr, Z = 103) using a surface ionization method. The result suggests that Lr has a loosely-bound electron in the outermost orbital. In contrast to Lr, nobelium (No, Z = 102) is expected to have the highest IP among the actinide elements owing to its full-filled 5f and the 7s orbitals. In the present study, we have successfully determined IP values of No as well as fermium (Fm, Z = 100) and mendelevium (Md, Z = 101) using the surface ionization method. The obtained results indicate that the IP value of heavy actinoids would increase monotonically with filling electrons up in the 5f orbital like heavy lanthanoids.

Study of fission using multi-nucleon transfer reactions

Nishio, Katsuhisa; Hirose, Kentaro; Vermeulen, M. J.; Makii, Hiroyuki; Orlandi, R.; Tsukada, Kazuaki; Asai, Masato; Toyoshima, Atsushi; Sato, Tetsuya; Nagame, Yuichiro; et al.

EPJ Web of Conferences, 163, p.00041_1 - 00041_6, 2017/11

https://doi.org/10.1051/epjconf/201716300041

First ionization potential of the heaviest actinide lawrencium, element 103

Sato, Tetsuya; Asai, Masato; Borschevsky, A.*; Stora, T.*; Sato, Nozomi*; Kaneya, Yusuke; Tsukada, Kazuaki; Dllmann, C. E.*; Eberhardt, K.*; Eliav, E.*; et al.

EPJ Web of Conferences, 131, p.05001_1 - 05001_6, 2016/12

https://doi.org/10.1051/epjconf/201613105001

Ionization efficiency in a surface ionization process depends on the first ionization potential of the atom. Based on the dependence, the ionization potential of the atom can be determined. We measured ionization efficiencies of fermium, einsteinium, mendelevium, and lawrencium by using a newly developed gas-jet coupled surface ion-source. The ionization potential of the elements have not been determined so far due to their low production rates and/or their short half-lives. Based on a relationship between the ionization efficiency and the ionization potential obtained via measurements of short-lived lanthanide isotopes, the ionization potentials of these actinide elements have been successfully determined.