Yokoyama, Akihiko*; Kitayama, Yuta*; Fukuda, Yoshiki*; Kikunaga, Hidetoshi*; Murakami, Masashi*; Komori, Yukiko*; Yano, Shinya*; Haba, Hiromitsu*; Tsukada, Kazuaki; Toyoshima, Atsushi*
Radiochimica Acta, 107(1), p.27 - 32, 2019/01
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
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.
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.
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 (Internet), 163, p.00041_1 - 00041_6, 2017/11
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 (Internet), 131, p.05001_1 - 05001_6, 2016/12
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.
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 (Internet), 131, p.07005_1 - 07005_7, 2016/12
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).
Steinegger, P.*; Asai, Masato; Dressler, R.*; Eichler, R.*; Kaneya, Yusuke*; Mitsukai, Akina*; Nagame, Yuichiro; Piguet, D.*; Sato, Tetsuya; Schdel, M.; et al.
Journal of Physical Chemistry C, 120(13), p.7122 - 7132, 2016/04
A new experimental method "vacuum chromatography" has been developed to measure adsorption enthalpy of superheavy elements, and its feasibility has been examined using short-lived thallium isotopes. The short-lived thallium isotopes were produced at the JAEA tandem accelerator. The thallium ion beam prepared with an on-line isotope separator which ionized and mass-separated the thallium isotopes was injected into an isothermal vacuum chromatography apparatus. A temperature-dependent adsorption property of thallium atom on SiO surface were measured. The adsorption enthalpy of thallium was determined to be 158 kJ/mol. The thallium is a homolog of element 113. Thus, the vacuum chromatography developed in this study enables us to perform chemical experiments for short-lived superheavy elements with half-lives of a order of one second.
Usoltsev, I.*; Eichler, R.*; Wang, Y.*; Even, J.*; Yakushev, A.*; Haba, Hiromitsu*; Asai, Masato; Brand, H.*; Di Nitto, A.*; Dllmann, Ch. E.*; et al.
Radiochimica Acta, 104(3), p.141 - 151, 2016/03
Conditions of the production and decomposition of hexacarbonyl complexes of short-lived Mo and W isotopes were investigated to study thermal stability of the heaviest group 6 hexacarbonyl complex Sg(CO). A tubular flow reactor was tested to decompose the hexacarbonyl complexes and to extract the first bond dissociation energies. A silver was found to be the most appropriate reaction surface to study the decomposition of the group 6 hexacarbonyl. It was found that the surface temperature at which the decomposition occurred was correlated to the first bond dissociation energy of Mo(CO) and W(CO), indicating that the first bond dissociation energy of Sg(CO) could be determined with this technique.
Nishinaka, Ichiro; Yokoyama, Akihiko*; Washiyama, Koshin*; Maeda, Eita*; Watanabe, Shigeki; Hashimoto, Kazuyuki; Ishioka, Noriko; Makii, Hiroyuki; Toyoshima, Atsushi; Yamada, Norihiro*; et al.
Journal of Radioanalytical and Nuclear Chemistry, 304(3), p.1077 - 1083, 2015/06
Production cross sections of astatine isotopes At in the 29-57 MeV Li induced reaction with Pb target have been measured by - and -ray spectrometry. Excitation functions of production cross sections have been compared with a statistical model calculation to study the reaction mechanism of Li + Pb. Considerably small experimental cross sections of At and At compared with the calculation were clearly observed at incident energies higher than 44 MeV, indicating that the effects of breakup reaction play a role. A chemical separation of astatine from an irradiated lead target has been studied with a dry-distillation method. A complementary way to produce astatine isotopes has been developed.
Huang, M.*; Haba, Hiromitsu*; Murakami, Masashi*; Asai, Masato; Kaji, Daiya*; Kanaya, Jumpei*; Kasamatsu, Yoshitaka*; Kikunaga, Hidetoshi*; Kikutani, Yuki*; Komori, Yukiko*; et al.
Journal of Radioanalytical and Nuclear Chemistry, 304(2), p.845 - 849, 2015/05
A technique to utilize radioisotopes of Nb and Ta was developed for chemical studies of element 105, Db, by coupling a gas-jet transport system to the RIKEN gas-filled recoil ion separator (GARIS). The short-lived Nb and Ta were produced with nuclear reactions using a F beam whose energy was the same as that to produce Db. Then, they were separated with GARIS and extracted to a chemistry laboratory with the gas-jet transport system. By changing only magnetic field of GARIS and inserting an energy degrader and a shutter for recoil ions, we could deliver the Nb and Ta to a chemistry device for Db without changing other experimental conditions.
Sato, Tetsuya; Asai, Masato; Borschevsky, A.*; Stora, T.*; Sato, Nozomi; Kaneya, Yusuke; Tsukada, Kazuaki; Dllmann, Ch. E.*; Eberhardt, K.*; Eliav, E.*; et al.
Nature, 520(7546), p.209 - 211, 2015/04
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 successfully measured ionization efficiencies of lawrencium (Lr, =103) using a gas-jet coupled surface ion-source. The ionization potential of Lr has not been determined owing to its low production rate and its short half-life. Based on a relationship between the ionization efficiency and the ionization potential obtained via measurements of short-lived lanthanide isotopes, the ionization potential of Lr was determined.
Even, J.*; Ackermann, D.*; Asai, Masato; Block, M.*; Brand, H.*; Di Nitto, A.*; Dllmann, Ch. E.*; Eichler, R.*; Fan, F.*; Haba, Hiromitsu*; et al.
Journal of Radioanalytical and Nuclear Chemistry, 303(3), p.2457 - 2466, 2015/03
Rapid In situ synthesis of metal carbonyl complexes has been demonstrated using short-lived isotopes produced in nuclear fission and fusion reactions. The short-lived isotopes with high recoil energy directly react with carbon-monoxides and form carbonyl complexes. Only highly volatile complexes were fast transported in a gas stream to counting and chemistry devices. Short-lived Mo, Tc, Ru, Rh, W, Re, Os, and Ir were found to form volatile carbonyl complexes, while no volataile complex of Hf and Ta were detected. This technique has been applied to a chemical investigation of the superheavy element Sg (atomic number 106), and will be applicable to various fields of nuclear science with short-lived transition metal isotopes.
Hatsukawa, Yuichi; Hashimoto, Kazuyuki; Tsukada, Kazuaki; Sato, Tetsuya; Asai, Masato; Toyoshima, Atsushi; Nagai, Yasuki; Tanimori, Toru*; Sonoda, Shinya*; Kabuki, Shigeto*; et al.
Journal of Radioanalytical and Nuclear Chemistry, 303(2), p.1283 - 1285, 2015/02
Technetium-99m (Tc) is used in radioactive medical diagonostic tests, for example as a radioactive tracer that medical equipment can detect in the human body. It is well suited to the role because it emits readily detectable 141 keV rays, and its half-life is 6.01 hours (meaning that about 94% of it decays to technetium-99 in 24 hours). There are at least 31 commonly used radiopharmaceuticals based on technetium-99m for imaging and functional studies of the brain, myocardium, thyroid, lungs, liver, gallbladder, kidneys, skeleton, blood, and tumors. Recent years, with the develop-ment of the Compton camera which can realize high position resolution, technetium isotopes emitting high energy -rays are required. In this study, technetium-95m which emits some rays around 800 keV was produced by the Mo(p,n)Tc reaction.
Sato, Tetsuya; Asai, Masato; Sato, Nozomi; Tsukada, Kazuaki; Toyoshima, Atsushi; Oe, Kazuhiro*; Miyashita, Sunao*; Kaneya, Yusuke; Osa, Akihiko; Schdel, M.; et al.
Journal of Radioanalytical and Nuclear Chemistry, 303(2), p.1253 - 1257, 2015/02
We have developed a surface-ionization ion-source coupled to the He/CdI gas-jet transport system for the Isotope Separator On-Line (ISOL) at the JAEA tandem accelerator for experimental determination of the first ionization potential of lawrencium (Lr, ). We performed to ionize a short-lived Lr isotope and various lanthanide isotopes. We successfully observed mass-separated ions of Lr by using our present system at the first time. The first ionization potential of Lr was evaluated based on a correlation between of effective ionization potential and ionization efficiency of short-lived lanthanide isotopes in our system.
Even, J.*; Yakushev, A.*; Dllmann, Ch. E.*; Haba, Hiromitsu*; Asai, Masato; Sato, Tetsuya; Brand, H.*; Di Nitto, A.*; Eichler, R.*; Fan, F. L.*; et al.
Science, 345(6203), p.1491 - 1493, 2014/09
A new superheavy element complex, a seaborgium carbonyl, has been successfully synthesized, and its adsorption property has been studied using a cryo-thermochromatography and -detection apparatus COMPACT. Nuclear reaction products of short-lived Sg preseparated with a gas-filled recoil ion separator GARIS at RIKEN were directly injected into a gas cell filled with He/CO mixture gas, and chemical reaction products of volatile carbonyl complexes were trasported to COMPACT. The Sg carbonyl complex detected with COMPACT was found to be very volatile with adsorption enthalpy of 50 kJ/mol, from which we have concluded that this complex should be a Sg hexacarbonyl Sg(CO). This is the first synthesis of organometallic compounds of transactinide elements for which only simple inorganic comounds have been synthesized so far.
Nagame, Yuichiro; Toyoshima, Atsushi; Tsukada, Kazuaki; Asai, Masato; Sato, Tetsuya; Schdel, M.
Journal of Radioanalytical and Nuclear Chemistry, 300(1), p.77 - 88, 2014/04
Sato, Nozomi; Sato, Tetsuya; Asai, Masato; Toyoshima, Atsushi; Tsukada, Kazuaki; Li, Z.*; Nishio, Katsuhisa; Nagame, Yuichiro; Schdel, M.; Haba, Hiromitsu*; et al.
Radiochimica Acta, 102(3), p.211 - 219, 2014/03
Production cross-sections of the isotope Lr in the Cf + B, Am + O, and Cm + N reactions were measured using a He/KCl gas-jet transport system and a rotating wheel -particle detection apparatus. The -particle energy of Lr was distributed from 8.3 to 8.7 MeV and its half-life, , was measured to be s. The maximum cross sections in the Cf(B, 4)Lr and Am(O, 5)Lr reactions were determined to be nb at the beam energy of 63 MeV and nb at 96 MeV, respectively. In the Cm(N, 6)Lr reaction, the cross section was measured to be nb at 91 MeV.
Haba, Hiromitsu*; Huang, M.*; Kaji, Daiya*; Kanaya, Jumpei*; Kudo, Yuki*; Morimoto, Koji*; Morita, Kosuke*; Murakami, Masashi*; Ozeki, Kazutaka*; Sakai, Ryutaro*; et al.
Physical Review C, 89(2), p.024618_1 - 024618_11, 2014/02
Toyoshima, Atsushi; Li, Z.*; Asai, Masato; Sato, Nozomi; Sato, Tetsuya; Kikuchi, Takahiro; Kaneya, Yusuke; Kitatsuji, Yoshihiro; Tsukada, Kazuaki; Nagame, Yuichiro; et al.
Inorganic Chemistry, 52(21), p.12311 - 12313, 2013/11
The reduction behavior of mendelevium (Md) was studied using a flow electrolytic chromatography apparatus. By applying appropriate potentials on the chromatography column, the more stable Md is reduced to Md. The reduction potential of the Md + e Md couple was determined to be -0.160.05 V vs. a normal hydrogen electrode.
Kasamatsu, Yoshitaka*; Toyoshima, Atsushi; Tome, Hayato*; Tsukada, Kazuaki; Asai, Masato; Haba, Hiromitsu*; Nagame, Yuichiro
Journal of Nuclear and Radiochemical Sciences (Internet), 13(1), p.9 - 12, 2013/06
Adsorption behavior of the group-5 elements, Nb and Ta, on cation-exchange resin was studied in mixed solution of HF and HNO as a model experiment of their heavier homologue, element 105 (dubnium, Db). Chemical reactions of these elements in the cation exchange rapidly reached the equilibrium. It was found that distribution coefficients of Nb and Ta decrease with increasing the fluoride ion concentration in the studied range of 10 - 10 M. Clear difference between Nb and Ta was observed in the variations of the distribution coefficients against the fluoride ion concentration. This would originate from their different chemical species of fluoride complexes. We propose the cation-exchange experiment of Db based on the present experimental results to understand its fluoride complex formation.