Chemical characterization of a volatile dubnium compound, DbOCl

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

https://doi.org/10.1002/anie.202102808

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.

Measurement of fission-fragment mass distributions in the multinucleon transfer channels of the O+Np reaction

Vermeulen, M. J.; Nishio, Katsuhisa; Hirose, Kentaro; Kean, K. R.; Makii, Hiroyuki; Orlandi, R.; Tsukada, Kazuaki; Tsekhanovich, I.*; Andreyev, A. N.; Ishizaki, Shoma*; et al.

Physical Review C, 102(5), p.054610_1 - 054610_11, 2020/11

https://doi.org/10.1103/PhysRevC.102.054610

First online operation of TRIGA-TRAP

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

https://doi.org/10.1016/j.nima.2020.164013

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.

Anomalous radioisotope production for ZnO using polyethylene by accelerator neutrons

Tsukada, Kazuaki; Nagai, Yasuki*; Hashimoto, Shintaro; Minato, Futoshi; Kawabata, Masako*; Hatsukawa, Yuichi*; Hashimoto, Kazuyuki*; Watanabe, Satoshi*; Saeki, Hideya*; Motoishi, Shoji*

Journal of the Physical Society of Japan, 89(3), p.034201_1 - 034201_7, 2020/03

https://doi.org/10.7566/JPSJ.89.034201

We found anomalously large yields of Ga, Ga, Zn and Cu by neutron irradiation on a ZnO sample in a polyethylene shield. Neutron beams are generated from the Be() reaction for 50 MeV deuterons. The yields obtained were more than 20 times larger than those in the unshielded sample. On the other hand, the yields of Ga, Ga, Zn and Cu from a metallic Zn sample and the yields of Cu, Ni and Zn from the ZnO and Zn samples were almost insensitive to the shield conditions. This finding would provide us a unique capability of accelerator neutrons to simultaneously produce a large amount of several radioisotopes, including proton induced reaction products, by using a single sample. The experimental data were compared with the yields estimated by using the Particle and Heavy Ion Transport code System and the result was discussed.

Sensitivity of charged particle activation analysis for long-lived radioactive nuclide determination

Oshima, Masumi*; Yamaguchi, Yurie*; Asai, Masato; Tsukada, Kazuaki; Goto, Jun*; Bamba, Shigeru*; Bi, C.*; Morimoto, Takao*

Journal of Nuclear Science and Technology, 56(9-10), p.866 - 872, 2019/09

https://doi.org/10.1080/00223131.2019.1593892

Sensitivity of charged particle activation analysis with 8 MeV proton beam was studied for determination of 35 long-lived radioactive nuclides. Reaction cross sections for those nuclides were estimated with ALICE-91 code and isomer yield ratios were estimated from those of neighboring isotopes by taking into account their spins and parities. It was found that the proposed charged particle activation analysis should show high sensitivity for the determination of several hardly measurable nuclides with long half-lives such as Cs, Pu, I, Sn, Mo, Pd, U, Cm, and Np.

Validation of the multinucleon transfer method for the determination of the fission barrier height

Kean, K. R.; Nishio, Katsuhisa; Hirose, Kentaro; Vermeulen, M. J.; Makii, Hiroyuki; Orlandi, R.; Tsukada, Kazuaki; Andreyev, A. N.; Tsekhanovich, I.*; Chiba, Satoshi*

Physical Review C, 100(1), p.014611_1 - 014611_6, 2019/07

https://doi.org/10.1103/PhysRevC.100.014611

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.

Electron-tracking Compton camera imaging of technetium-95m

Hatsukawa, Yuichi*; Hayakawa, Takehito*; Tsukada, Kazuaki; Hashimoto, Kazuyuki*; Sato, Tetsuya; Asai, Masato; Toyoshima, Atsushi; Tanimori, Toru*; Sonoda, Shinya*; Kabuki, Shigeto*; et al.

PLOS ONE (Internet), 13(12), p.e0208909_1 - e0208909_12, 2018/12

https://doi.org/10.1371/journal.pone.0208909

Imaging of Tc radioisotope was conducted using an electron tracking-Compton camera (ETCC). Tc emits 204, 582, and 835 keV rays, and was produced in the Mo(p,n)Tc reaction with a Mo-enriched target. The recycling of the Mo-enriched molybdenum trioxide was investigated, and the recycled yield of Mo was achieved to be 70% - 90%. The images were obtained with each of the three rays. Results showed that the spatial resolution increases with increasing -ray energy, and suggested that the ETCC with high-energy -ray emitters such as Tc is useful for the medical imaging of deep tissue and organs in the human body.

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.

Role of multichance fission in the description of fission-fragment mass distributions at high energies

Hirose, Kentaro; Nishio, Katsuhisa; Tanaka, Shoya*; Lguillon, R.*; Makii, Hiroyuki; Nishinaka, Ichiro*; Orlandi, R.; Tsukada, Kazuaki; Smallcombe, J.*; Vermeulen, M. J.; et al.

Physical Review Letters, 119(22), p.222501_1 - 222501_6, 2017/12

https://doi.org/10.1103/PhysRevLett.119.222501

Fission-fragment mass distributions were measured for U, Np and Pu populated in the excitation-energy range from 10 to 60 MeV by multi-nucleon transfer channels in the reaction O + U at the JAEA tandem facility. Among them, the data for U and Np were observed for the first time. It was found that the mass distributions for all the studied nuclides maintain a double-humped shape up to the highest measured energy in contrast to expectations of predominantly symmetric fission due to the washing out of nuclear shell effects. From a comparison with the dynamical calculation based on the fluctuation-dissipation model, this behavior of the mass distributions was unambiguously attributed to the effect of multi-chance fission.