Sato, Tetsuya; Nagame, Yuichiro*
Nihon Butsuri Gakkai-Shi, 78(2), p.64 - 72, 2023/02
The study of the chemistry of superheavy elements, which are located in the heavy extremes of the periodic table, has made considerable progress over the past 20 years, and new approaches based on various ideas have recently been developed. Research groups in Japan have also made significant contributions to the development of research on superheavy elements. Recently, notable results have been reported for the transactinide elements rutherfordium (element 104), dubnium (element 105), and seaborgium (element 106), and the heavy actinides with atomic numbers exceeding 100. The review will focus on the recent main results of these elements. This review outlines the main recent results and touches on future prospects.
Orlandi, R.; Makii, Hiroyuki; Nishio, Katsuhisa; Hirose, Kentaro; Asai, Masato; Tsukada, Kazuaki; Sato, Tetsuya; Ito, Yuta; Suzaki, Fumi; Nagame, Yuichiro*; et al.
Physical Review C, 106(6), p.064301_1 - 064301_11, 2022/12
Yakushev, A.*; Lens, L.*; Dllmann, Ch. E.*; Khuyagbaatar, J.*; Jger, E.*; Krier, J.*; Runke, J.*; Albers, H. M.*; Asai, Masato; Block, M.*; et al.
Frontiers in Chemistry (Internet), 10, p.976635_1 - 976635_11, 2022/08
Flerovium (Fl, element 114) is the heaviest element chemically studied so far. The first chemical experiment on Fl suggested that Fl is a noble-gas-like element, while the second studies suggested that Fl has a volatile-metal-like character. To obtain more reliable conclusion, we performed further experimental studies on Fl adsorption behavior on Si oxide and gold surfaces. The present results suggest that Fl is highly volatile and less reactive than the volatile metal, Hg, but has higher reactivity than the noble gas, Rn.
Sato, Tetsuya; Nagame, Yuichiro*
Radiochimica Acta, 110(6-9), p.441 - 451, 2022/07
We describe our recent achievements in the effective production of low-energy ion-beams of the elements at the end of the actinide series, fermium (Fm, atomic number Z = 100), mendelevium (Md, Z = 101), nobelium (No, Z = 102), and lawrencium (Lr, Z = 103), using a surface ionization ion-source installed in the ISOL (Isotope Separator On-Line) at the Tandem accelerator facility of JAEA (Japan Atomic Energy Agency). Then the successful measurements of the first ionization potentials (IP) of these elements with the ISOL setup are reviewed. The measured IP values increased up to No via Fm and Md, while that of Lr was the lowest among the actinides. Based on the variation of the IP1 values of the heavy actinides with the atomic number in comparison with those of the heavy lanthanides, the results clearly demonstrated that the 5f orbitals are fully filled at No, and the actinide series ends with Lr. Furthermore, the IP value of Lr provoked controversy over its position in the Periodic Table, so a short introduction to this issue is presented. The feasibility of the extension of chemical studies to still heavier elements with their ion-beams generated by ISOL is briefly discussed.
Gtz, M.*; Yakushev, A.*; Gtz, S.*; Di Nitto, A.*; Dllmann, Ch. E.*; Asai, Masato; Kindler, B.*; Krier, J.*; Lommel, B.*; Nagame, Yuichiro*; et al.
Radiochimica Acta, 110(2), p.75 - 86, 2022/02
The study of volatile superheavy element carbonyl complexes requires more efficient methods because the yield of transactinide elements decreases with increasing atomic number. This is achieved by using a newly developed double chamber system to separate the recoil chamber and the reaction one, thereby avoiding the decomposition of reactive molecules by the projectile ion beam, which hinders the synthesis of carbonyl complexes. The feasibility of this method was verified by synthesizing 5d metal short-lived isotopes as homologous element isotopes of the light transactinide elements Sg, Bh, Hs, and Mt at the Japan Atomic Energy Agency tandem accelerator and conducting model experiments.
Chiera, N. M.*; Sato, Tetsuya; Eichler, R.*; Tomitsuka, Tomohiro; Asai, Masato; Adachi, Sadia*; Dressler, R.*; Hirose, Kentaro; Inoue, Hiroki*; Ito, Yuta; et al.
Angewandte Chemie; International Edition, 60(33), p.17871 - 17874, 2021/08
The formation and the chemical characterization of single atoms of dubnium (Db, element 105), in the form of its volatile oxychloride, was investigated using the on-line gas phase chromatography technique, in the temperature range 350 - 600 C. Under the exact same chemical conditions, comparative studies with the lighter homologs of group-5 in the Periodic Table clearly indicate the volatility sequence being NbOCl TaOCl DbOCl. From the obtained experimental results, thermochemical data for DbOCl were derived. The present study delivers reliable experimental information for theoretical calculations on the chemical properties of transactinides.
Nagame, Yuichiro*; Sato, Tetsuya; Kratz, J. V.*
Kirk-Othmer Encyclopedia of Chemical Technology (Internet), 52 Pages, 2020/09
This article gives a brief summary of the recent progress in the synthesis of new elements as well as heavy nuclei far from the stability line and in the studies of exotic nuclear decay properties including nuclear fission of heavy nuclei and chemical characterization of heavy actinides and transactinides. Experimental techniques of single-atom detection after in-flight separation with electromagnetic separators have made a breakthrough in discovery of new heavy isotopes. Development of automated rapid chemical separation apparatuses performing one atom-at-a-time chemistry has also considerably contributed to the progress of chemical studies of the transactinides. Some key experiments exploring new frontiers of the production and chemical characterization of heavy actinides and transactinides using state-of-the-art techniques are demonstrated. A short historical perspective of actinide and transactinide elements and some prospects of extending nuclear and chemical studies of heavy elements in the future are briefly presented.
Grund, J.*; Asai, Masato; Blaum, K.*; Block, M.*; Chenmarev, S.*; Dllmann, Ch. E.*; Eberhardt, K.*; Lohse, S.*; Nagame, Yuichiro*; Nagy, Sz.*; et al.
Nuclear Instruments and Methods in Physics Research A, 972, p.164013_1 - 164013_8, 2020/08
We report on the successful coupling of the Penning-trap mass spectrometry setup TRIGA-TRAP to the research reactor TRIGA Mainz. This offers the possibility to perform direct high-precision mass measurements of short-lived nuclei produced in neutron-induced fission of a U target located near the reactor core. An aerosol-based gas-jet system is used for efficient transport of short-lived neutron-rich nuclei from the target chamber to a surface ion source. In conjunction with new ion optics and extended beam monitoring capabilities, the experimental setup has been fully commissioned. The design of the surface ion source, efficiency studies and first results are presented.
Ghys, L.*; Andreyev, A. N.; Huyse, M.*; Van Duppen, P.*; Antalic, S.*; Barzakh, A.*; Capponi, L.*; Cocolios, T. E.*; Cubiss, J.*; Derkx, X.*; et al.
Physical Review C, 100(5), p.054310_1 - 054310_13, 2019/11
Radiochimica Acta, 107(9-11), p.803 - 819, 2019/09
Schdel, M.*; Nagame, Yuichiro
Radiochimica Acta, 107(7), p.561 - 585, 2019/07
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
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).
Barzakh, A. E.*; Cubiss, J. G.*; Andreyev, A. N.; Seliverstov, M. D.*; Andel, B.*; Antalic, S.*; Ascher, P.*; Atanasov, D.*; Beck, D.*; Biero, J.*; et al.
Physical Review C, 99(5), p.054317_1 - 054317_9, 2019/05
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
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.
Lens, L.*; Yakushev, A.*; Dllmann, Ch. E.*; Asai, Masato; Ballof, J.*; Block, M.*; David, H. M.*; Despotopulos, J.*; Di Nitto, A.*; Eberhardt, K.*; et al.
Radiochimica Acta, 106(12), p.949 - 962, 2018/12
Online gas-solid adsorption studies with single atom quantities of Hg, Tl, and Pb on SiO and Au surfaces were carried out using short-lived radioisotopes with half-lives in the range of 4-49 s. This is a model study to measure adsorption enthalpies of superheavy elements Cn, Nh, and Fl. The short-lived isotopes were produced and separated by the gas-filled recoil separator TASCA at GSI. The products were stopped in He gas, and flushed into gas chromatography columns made of Si detectors whose surfaces were covered by SiO or Au. The short-lived Tl and Pb were successfully measured by the Si detectors with the SiO surface at room temperature. On the other hand, the Hg did not adsorb on the SiO surface, but adsorbed on the Au surface. The results demonstrated that the adsorption properties of short-lived Hg, Tl, and Pb could be studied with this setup, and that this method is applicable to the experiment for Cn, Nh, and Fl.
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
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.
Radioisotopes, 67(10), p.507 - 526, 2018/10
Recent studies of the chemical separation and characterization experiments of the first three transactinide elements, rutherfordium (Rf), dubnium (Db) and seaborgium (Sg), conducted atom-at-a-time in liquid phases, are reviewed. A short description on experimental techniques based on partition methods, specifically automated rapid chemical separation systems, as well as on assessment of role of relativistic effects is also given. Perspectives for liquid phase chemistry experiments on heavier elements are briefly discussed.
Cubiss, J.*; Andreyev, A. N.; Mitsuoka, Shinichi*; Nagame, Yuichiro; Nishio, Katsuhisa; Ota, Shuya*; Wakabayashi, Yasuo*; 60 of others*
Physical Review C, 97(5), p.054327_1 - 054327_19, 2018/05
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
Nagame, Yuichiro; Kratz, J. V.*; Schdel, M.*
EPJ Web of Conferences, 131, p.07007_1 - 07007_8, 2016/12