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G
tz, M.*; Yakushev, A.*; Gtz, S.*; Di Nitto, A.*; D
llmann, Ch. E.*; Asai, Masato; Kindler, B.*; Krier, J.*; Lommel, B.*; Nagame, Yuichiro*; et al.
Radiochimica Acta, 110(2), p.75 - 86, 2022/02
Times Cited Count：2 Percentile：16.03(Chemistry, Inorganic & Nuclear)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
Times Cited Count：5 Percentile：20.14(Chemistry, Multidisciplinary)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.
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
Times Cited Count：2 Percentile：15.49(Chemistry, Analytical)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).
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
Times Cited Count：6 Percentile：28.92(Chemistry, Inorganic & Nuclear)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.
Eichler, R.*; Asai, Masato; Brand, H.*; Chiera, N. M.*; Di Nitto, A.*; Dressler, R.*; Dllmann, Ch. E.*; Even, J.*; Fangli, F.*; Goetz, M.*; et al.
EPJ Web of Conferences, 131, p.07005_1 - 07005_7, 2016/12
Times Cited Count：3 Percentile：69.95(Chemistry, Inorganic & Nuclear)In recent years gas-phase chemical studies assisted by physical pre-separation allowed for the productions and investigations of fragile single molecular species of superheavy elements. The latest highlight is the formation of very volatile hexacarbonyl compound of element 106, Sg(CO)
. Following this success, second-generation experiments were performed to measure the first bond dissociation energy between the central metal atom and the surrounding ligand. The method using a tubular decomposition reactor was developed and successfully applied to short-lived Mo(CO), W(CO), and Sg(CO).
LrAsai, Masato; Kamada, Hiroki*; Shigekawa, Yudai*; Tsukada, Kazuaki; Sato, Tetsuya; Toyoshima, Atsushi; Mitsukai, Akina; Nagame, Yuichiro; Nishio, Katsuhisa; Hirose, Kentaro; et al.
no journal, ,
To clarify the fission mechanism of mass-symmetric spontaneous fissions observed around the neutron-rich Fm region, we have measured kinetic energies and mass distribution of spontaneous-fission fragments in this nuclear region precisely. The experiment was performed at the JAEA tandem accelerator facility using an on-line isotope separator (ISOL). The mass-separated Lr nuclei were implanted into thin foil, and two fragments of their spontaneous fission were coincidently measured with two Si detectors. The spontaneous fission of Lr was found to show a narrow symmetric mass distribution. On the other hand, their total kinetic energy TKE was found to be low, which is apparently different from the high-TKE symmetric fissions observed in the Fm isotopes. This indicates that the fission mechanisms of these two symmetric fissions are different.
Kaneya, Yusuke*; Tomitsuka, Tomohiro; Sato, Tetsuya; Asai, Masato; Tsukada, Kazuaki; Toyoshima, Atsushi; Mitsukai, Akina; Makii, Hiroyuki; Hirose, Kentaro; Osa, Akihiko; et al.
no journal, ,
Tomitsuka, Tomohiro; Kaneya, Yusuke*; Sato, Tetsuya; Asai, Masato; Tsukada, Kazuaki; Toyoshima, Atsushi; Mitsukai, Akina; Osa, Akihiko; Nishio, Katsuhisa; Nagame, Yuichiro; et al.
no journal, ,
In order to investigate the adsorption behavior of Lawrencium (Lr, Z = 103) on a Tantalum (Ta) surface, we measured ionization efficiencies of Lr under several temperature conditions of the surface ionization. We observed ionization efficiencies of Lr which were lower than those calculated by the Saha-Langmuir equation in lower temperature region. Based on a temperature dependence of the obtained ionization efficiencies, we discuss the adsorption behavior of Lr on the Ta surface.
Kaneya, Yusuke*; Asai, Masato; Sato, Tetsuya; Tomitsuka, Tomohiro; Tsukada, Kazuaki; Toyoshima, Atsushi; Mitsukai, Akina; Makii, Hiroyuki; Hirose, Kentaro; Osa, Akihiko; et al.
no journal, ,
To study the influence of the valence 7p
electronic orbital on chemical properties of lawrencium, a measurement of the adsorption enthalpy of lawrencium was carried out. A new method using a surface ionization technique coupled to an on-line isotope separator was developed, which enabled one to measure temperature dependence of lawrencium surface adsorption on a metallic tantalum surface at high temperature up to 2800 K. The temperature dependences of adsorption of lawrencium as well as various lanthanide elements were investigated with this method, and the adsorption enthalpy of lawrencium was successfully extracted.
Sato, Tetsuya; Kaneya, Yusuke*; Asai, Masato; Tsukada, Kazuaki; Toyoshima, Atsushi; Mitsukai, Akina*; Osa, Akihiko; Makii, Hiroyuki; Hirose, Kentaro; Nagame, Yuichiro; et al.
no journal, ,
Our experimental results on the first ionization potential measurement of lawrencium (Lr, element 103) have strongly suggested that the Lr atom has a [Rn]
configuration as a result of the influence of strong relativistic effects. The configuration is different from that expected from the lanthanide homologue, lutetium (Lu). According to a semi-empirical consideration, it is expected that the change of the electronic configuration leads higher volatility of Lr than that of Lu. In this work, adsorption behaviors of Lr and various short-lived rare earth isotopes on a tantalum surface were investigated via observation of their surface ionization efficiencies. It was found that Lr would behave like low volatile rare earth elements such as Lu contrary to the semi-empirical expectation.
Chiera, N. M.; Sato, Tetsuya; Asai, Masato; Suzuki, Hayato*; Tokoi, Katsuyuki; Tomitsuka, Tomohiro; Toyoshima, Atsushi; Tsukada, Kazuaki; Nagame, Yuichiro
no journal, ,
Es targetAsai, Masato; Tsukada, Kazuaki; Hirose, Kentaro; Toyoshima, Atsushi; Tomitsuka, Tomohiro; Chiera, N. M.; Ito, Yuta; Makii, Hiroyuki; Nagame, Yuichiro; Nishio, Katsuhisa; et al.
no journal, ,
Spontaneous fissions of neutron-rich heavy actinide isotopes 
Fm, 
Fm, and Lr have been measured at the JAEA Tandem accelerator facility. Fm and Fm were produced in a multinucleon transfer reaction with an 
O beam and an extremely rare Es target with a half-life of 276 days. Reaction products were mass-separated with an on-line isotope separator (ISOL). A transition between the typical asymmetric mass distribution and a very sharp symmetric one was clearly observed between Fm and Fm, while the spontaneous fission of Lr was found to exhibit mixture of three different fission modes.
Md produced in the 
He+Es reactionNishio, Katsuhisa; Hirose, Kentaro; Makii, Hiroyuki; Orlandi, R.; Kean, K. R.*; Tsukada, Kazuaki; Asai, Masato; Toyoshima, Atsushi*; Sato, Tetsuya; Ito, Yuta; et al.
no journal, ,
no abstracts in English
Np isomerAsai, Masato; Suekawa, Yoshihide*; Higashi, Masato*; Kamada, Hiroki*; Tobe, Teruhisa*; Andreyev, A. N.; Hirose, Kentaro; Ito, Yuta; Makii, Hiroyuki; Nishio, Katsuhisa; et al.
no journal, ,
We have carried out experiments to study nuclear structure of the new isomer 
Np which we discovered recently. The Np was produced in the reaction of 
U target with 
Li beam at JAEA tandem accelerator, and was mass-separated with an on-line isotope separator (ISOL). The half-life was determined accurately through LX-ray measurements. The 
transition emitted by following the isomeric transition was successfully observed through LX- coincidence measurements. Moreover, the multipolarities of the transitions were determined with internal-conversion electron measurements. On the basis of these experimental results, We have clarified excitation energy, spin-parity, and nuclear structure of Np.
Sato, Tetsuya; Chiera, N. M.*; Tomitsuka, Tomohiro; Tokoi, Katsuyuki*; Suzuki, Hayato*; Ito, Yuta; Asai, Masato; Shirai, Kaori*; Inoue, Hiroki*; Adachi, Sadia*; et al.
no journal, ,
The influence of strong relativistic effects on chemical properties has been interesting in the superheavy element region. Their chemical properties, however, have not been investigated sufficiently because of experimental difficulties owing to their low production rates and short half-lives. In order to elucidate the chemical properties of dubnium (Db, Z = 105), we have conducted on-line isothermal gas chromatographic experiments of oxychloride of group-5 elements. We confirmed the formation of volatile oxychlorides of Db and its lighter homologs Nb and Ta by using Db (half-life, 
= 33.8 s), 
Nb ( = 14.5 min.), and 
Ta ( = 6.76 min.), respectively. We successfully determined the adsorption enthalpies of the oxychlorides of each element on the quartz surface from their isothermal gas chromatographic behavior. The obtained volatility sequence of the group-5 elements is found to be Nb 
Ta 
Db.
Md produced in the He + Es reactionNishio, Katsuhisa; Hirose, Kentaro; Makii, Hiroyuki; Orlandi, R.; Kean, K. R.*; Tsukada, Kazuaki; Toyoshima, Atsushi*; Asai, Masato; Sato, Tetsuya; Chiera, N. M.*; et al.
no journal, ,
no abstracts in English
Tomitsuka, Tomohiro; Tokoi, Katsuyuki*; Sato, Tetsuya; Asai, Masato; Tsukada, Kazuaki; Toyoshima, Atsushi; Chiera, N. M.; Kamada, Hiroki; Nagame, Yuichiro; Goto, Shinichi*
no journal, ,
no abstracts in English
Tomitsuka, Tomohiro*; Tokoi, Katsuyuki*; Sato, Tetsuya; Asai, Masato; Chiera, N. M.; Goto, Shinichi*; Osa, Akihiko; Toyoshima, Atsushi; Tsukada, Kazuaki; Nagame, Yuichiro
no journal, ,
Tokoi, Katsuyuki; Sato, Tetsuya; Eichler, R.*; Ito, Yuta; Tomitsuka, Tomohiro; Suzuki, Hayato*; Asai, Masato; Tsukada, Kazuaki; Toyoshima, Atsushi*; Chiera, N. M.; et al.
no journal, ,
We developed a new experimental method combining vacuum chromatography and surface ionization, and applied this to investigate adsorption behavior of lawrencium (Lr, Z =103) on a surface of high temperature metallic tantalum. The adsorption behavior of Lr was similar to that of lutetium having low volatility among lanthanide elements. In this work, a Monte Carlo simulation code has been newly developed to study ionization and chromatographic behavior of short-lived atoms. In the presentation, we will report the details of a developed simulation code and calculation results.
Es targetAsai, Masato; Tsukada, Kazuaki; Hirose, Kentaro; Toyoshima, Atsushi; Tomitsuka, Tomohiro; Chiera, N. M.; Ito, Yuta; Makii, Hiroyuki; Nagame, Yuichiro; Nishio, Katsuhisa; et al.
no journal, ,
Spontaneous fissions of Fm, Fm, and Lr have been measured using an Es target at the JAEA Tandem Accelerator Facility. These three nuclei show different fission properties: the asymmetric fission, the high total-kinetic-energy (TKE) symmetric fission, and the low TKE symmetric fission, and the mechanisms of these three fissions should be very different. It is of great interest to elucidate how these differences occur. We have produced 
Fm in multinucleon-transfer reactions with a Es target and O projectiles, and produced Lr in the 
Cm(
N,4n) fusion-evaporation reaction. The reaction products were mass-separated with a gas-jet-coupled on-line isotope separator, and were delivered into a rotating wheel alpha- and fission-fragment detection system. By comparing the mass and TKE distributions deduced from the present experimental data, we will discuss the differences in fission mechanism among Fm, Fm, and Lr.
