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Journal Articles

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

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 $$^{135}$$Cs, $$^{244}$$Pu, $$^{129}$$I, $$^{126}$$Sn, $$^{93}$$Mo, $$^{107}$$Pd, $$^{236}$$U, $$^{248}$$Cm, and $$^{237}$$Np.

Journal Articles

Fusion reaction $$^{48}$$Ca+$$^{249}$$Bk leading to formation of the element Ts (Z=117)

Khuyagbaatar, J.*; Yakushev, A.*; D$"u$llmann, Ch. E.*; Ackermann, D.*; Andersson, L.-L.*; Asai, Masato; Block, M.*; Boll, R. A.*; Brand, H.*; Cox, D. M.*; et al.

Physical Review C, 99(5), p.054306_1 - 054306_16, 2019/05

We have performed an experiment to synthesize the element 117 (Ts) with the $$^{48}$$Ca+$$^{249}$$Bk fusion reaction. Four $$alpha$$-decay chains attributed to the element 117 were observed. Two of them were long decay chains which can be assigned to the one originating from the $$alpha$$ decay of $$^{294}$$Ts. The other two were short decay chains which are consistent with the one originating from the $$alpha$$ decay of $$^{293}$$Ts. We have compared the present results with the literature data, and found that our present results mostly confirmed the literature data, leading to the firm confirmation of the synthesis of the element 117.

Journal Articles

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

The formation of NbOCl$$_3$$ and TaOCl$$_3$$ 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 ($$Delta H_{rm ads}$$) at zero surface coverage of -$$Delta H_{rm ads}$$(NbOCl$$_3$$) = 102 $$pm$$ 4 kJ/mol and -$$Delta H_{rm ads}$$(TaOCl$$_3$$) = 128 $$pm$$ 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 $$Delta H_{rm ads}$$ values were successively related to the macroscopic standard sublimation enthalpy, $$Delta H^circ _{rm subl}$$, 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 $$Delta H_{rm ads}$$ and $$Delta H^circ _{rm subl}$$ for metal-oxychlorides was updated with the inclusion of the present data. According to the predicted $$Delta H^circ _{rm subl}$$(DbOCl$$_3$$), a $$Delta H_{rm ads}$$(DbOCl$$_3$$) value of 135 $$pm$$ 2 kJ/mol was extrapolated. The future accomplishment of comparative studies with DbOCl$$_3$$ 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.

Journal Articles

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

 Percentile:100(Multidisciplinary Sciences)

Imaging of $$^{95m}$$Tc radioisotope was conducted using an electron tracking-Compton camera (ETCC). $$^{95m}$$Tc emits 204, 582, and 835 keV $$gamma$$ rays, and was produced in the $$^{95}$$Mo(p,n)$$^{95m}$$Tc reaction with a $$^{95}$$Mo-enriched target. The recycling of the $$^{95}$$Mo-enriched molybdenum trioxide was investigated, and the recycled yield of $$^{95}$$Mo was achieved to be 70% - 90%. The images were obtained with each of the three $$gamma$$ rays. Results showed that the spatial resolution increases with increasing $$gamma$$-ray energy, and suggested that the ETCC with high-energy $$gamma$$-ray emitters such as $$^{95m}$$Tc is useful for the medical imaging of deep tissue and organs in the human body.

Journal Articles

Online chemical adsorption studies of Hg, Tl, and Pb on SiO$$_{2}$$ and Au surfaces in preparation for chemical investigations on Cn, Nh, and Fl at TASCA

Lens, L.*; Yakushev, A.*; D$"u$llmann, 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

 Percentile:100(Chemistry, Inorganic & Nuclear)

Online gas-solid adsorption studies with single atom quantities of Hg, Tl, and Pb on SiO$$_{2}$$ 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$$_{2}$$ or Au. The short-lived Tl and Pb were successfully measured by the Si detectors with the SiO$$_{2}$$ surface at room temperature. On the other hand, the Hg did not adsorb on the SiO$$_{2}$$ 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.

Journal Articles

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

 Times Cited Count:4 Percentile:21.13(Chemistry, Multidisciplinary)

The first ionization potential (IP$$_1$$) yields information on valence electronic structure of an atom. IP$$_1$$ 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$$_1$$ 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$$_1$$ among the actinide elements owing to its full-filled 5f and the 7s orbitals. In the present study, we have successfully determined IP$$_1$$ 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$$_1$$ value of heavy actinoids would increase monotonically with filling electrons up in the 5f orbital like heavy lanthanoids.

Journal Articles

Science of heavy and superheavy elements (nuclear physics); Experimental studies on shell structure of superheavy nuclei

Asai, Masato

Radioisotopes, 67(6), p.291 - 298, 2018/06

Stability and limit of existence essentially depend on nuclear shell structure. It is theoretically predicted that stable doubly-closed-shell spherical superheavy nuclei should exist around the region of the proton number 114 to 126 and the neutron number 172 to 184, although their locations and degree of stability have not been established because of large variety of theoretical predictions. On the other hand, recent advances on experimental techniques have made it possible to accumulate experimental data concerning the shell structure of superheavy nuclei, such as half-lives and nuclear masses. In addition, some pioneering experiments have been performed to directly establish the level structure of superheavy nuclei through spectroscopic methods. This paper introduces the current status of experimental studies on nuclear shell structure of superheavy nuclei.

Journal Articles

Determination of fusion barrier distributions from quasielastic scattering cross sections towards superheavy nuclei synthesis

Tanaka, Taiki*; Narikiyo, Yoshihiro*; Morita, Kosuke*; Fujita, Kunihiro*; Kaji, Daiya*; Morimoto, Koji*; Yamaki, Sayaka*; Wakabayashi, Yasuo*; Tanaka, Kengo*; Takeyama, Mirei*; et al.

Journal of the Physical Society of Japan, 87(1), p.014201_1 - 014201_9, 2018/01

 Times Cited Count:3 Percentile:29.91(Physics, Multidisciplinary)

Excitation functions of quasielastic scattering cross sections for the $$^{48}$$Ca + $$^{208}$$Pb, $$^{50}$$Ti + $$^{208}$$Pb, and $$^{48}$$Ca + $$^{248}$$Cm reactions were successfully measured by using the gas-filled recoil-ion separator GARIS. Fusion barrier distributions were extracted from these data, and compared with the coupled-channels calculations. It was found that the peak energies of the barrier distributions for the $$^{48}$$Ca + $$^{208}$$Pb and $$^{50}$$Ti + $$^{208}$$Pb systems coincide with those of the 2n evaporation channel cross sections for the systems, while that of the $$^{48}$$Ca + $$^{248}$$Cm is located slightly below the 4n evaporation ones. This results provide us helpful information to predict the optimum beam energy to synthesize superheavy nuclei.

Journal Articles

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 (Internet), 163, p.00041_1 - 00041_6, 2017/11


Journal Articles

Study of the reaction $$^{48}$$Ca + $$^{248}$$Cm $$rightarrow$$ $$^{296}$$Lv$$^{ast}$$ at RIKEN-GARIS

Kaji, Daiya*; Morita, Kosuke*; Morimoto, Koji*; Haba, Hiromitsu*; Asai, Masato; Fujita, Kunihiro*; Gan, Z.*; Geissel, H.*; Hasebe, Hiroo*; Hofmann, S.*; et al.

Journal of the Physical Society of Japan, 86(3), p.034201_1 - 034201_7, 2017/03

 Times Cited Count:10 Percentile:12.59(Physics, Multidisciplinary)

The fusion reaction of $$^{48}$$Ca + $$^{248}$$Cm $$rightarrow$$ $$^{296}$$Lv$$^{ast}$$ was studied using the gas-filled recoil-ion separator GARIS at RIKEN. A total of seven $$alpha$$ and spontaneous-fission decay chains were observed, which would originate from the reaction products of the element 116, $$^{292}$$Lv and $$^{293}$$Lv. Decay properties observed in the chains are in good agreement with the previously published ones. However, one of the chains showed a discrepancy, indicating the new spontaneous-fission branch in $$^{285}$$Cn or the production of the new isotope $$^{294}$$Lv.

Journal Articles

First ionization potential of the heaviest actinide lawrencium, element 103

Sato, Tetsuya; Asai, Masato; Borschevsky, A.*; Stora, T.*; Sato, Nozomi*; Kaneya, Yusuke; Tsukada, Kazuaki; D$"u$llmann, 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.

Journal Articles

Stability and synthesis of superheavy elements; Fighting the battle against fission - Example of $$^{254}$$No

Lopez-Martens, A.*; Henning, G.*; Khoo, T. L.*; Seweryniak, D.*; Alcorta, M.*; Asai, Masato; Back, B. B.*; Bertone, P. F.*; Boilley, D.*; Carpenter, M. P.*; et al.

EPJ Web of Conferences (Internet), 131, p.03001_1 - 03001_6, 2016/12

 Times Cited Count:1 Percentile:39.82

Fission barrier height and its angular-momentum dependence have been measured for the first time in the nucleus with the atomic number greater than 100. The entry distribution method, which can determine the excitation energy at which fission starts to dominate the decay process, was applied to $$^{254}$$No. The fission barrier of $$^{254}$$No was found to be 6.6 MeV at zero spin, indicating that the $$^{254}$$No is strongly stabilized by the nuclear shell effects.

Journal Articles

Complex chemistry with complex compounds

Eichler, R.*; Asai, Masato; Brand, H.*; Chiera, N. M.*; Di Nitto, A.*; Dressler, R.*; D$"u$llmann, 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)$$_{6}$$. 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)$$_{6}$$, W(CO)$$_{6}$$, and Sg(CO)$$_{6}$$.

Journal Articles

Development of alternative $$^3$$He NDA detector system

Koizumi, Mitsuo; Sakasai, Kaoru; Kureta, Masatoshi; Nakamura, Hironobu

Nippon Genshiryoku Gakkai-Shi, 58(11), p.642 - 646, 2016/11

no abstracts in English

Journal Articles

Vacuum chromatography of Tl on SiO$$_{2}$$ at the single-atom level

Steinegger, P.*; Asai, Masato; Dressler, R.*; Eichler, R.*; Kaneya, Yusuke*; Mitsukai, Akina*; Nagame, Yuichiro; Piguet, D.*; Sato, Tetsuya; Sch$"a$del, M.; et al.

Journal of Physical Chemistry C, 120(13), p.7122 - 7132, 2016/04

 Times Cited Count:8 Percentile:42.61(Chemistry, Physical)

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$$_{2}$$ 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.

Journal Articles

Decomposition studies of group 6 hexacarbonyl complexes, 1; Production and decomposition of Mo(CO)$$_6$$ and W(CO)$$_6$$

Usoltsev, I.*; Eichler, R.*; Wang, Y.*; Even, J.*; Yakushev, A.*; Haba, Hiromitsu*; Asai, Masato; Brand, H.*; Di Nitto, A.*; D$"u$llmann, Ch. E.*; et al.

Radiochimica Acta, 104(3), p.141 - 151, 2016/03

 Times Cited Count:8 Percentile:10.94(Chemistry, Inorganic & Nuclear)

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)$$_6$$. 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)$$_6$$ and W(CO)$$_6$$, indicating that the first bond dissociation energy of Sg(CO)$$_6$$ could be determined with this technique.

Journal Articles

Nuclear structure of elements with $$100 le Z le 109$$ from alpha spectroscopy

Asai, Masato; He${ss}$berger, F. P.*; Lopez-Martens, A.*

Nuclear Physics A, 944, p.308 - 332, 2015/12

 Times Cited Count:24 Percentile:5.74(Physics, Nuclear)

Nuclear structure of Z = 100-109 nuclei studied through $$alpha$$-decay spectroscopy have been reviewed. Experimental techniques and methods concerning separation techniques, summing effects in $$alpha$$ spectra, and the use of digital electronics for $$alpha$$-decay spectroscopy have been described in detail. The presentation of the experimental results and the physics discussion were focused on nuclear structure systematics in even-Z nuclei along the N = 151, 153, and 155 isotonic lines, where most progress has been achieved in the last 10 years.

Journal Articles

Numerical evaluation of the light transport properties of alternative He-3 neutron detectors using ceramic scintillators

Ozu, Akira; Takase, Misao*; Haruyama, Mitsuo; Kurata, Noritaka*; Kobayashi, Nozomi*; Kureta, Masatoshi; Nakamura, Tatsuya; To, Kentaro; Sakasai, Kaoru; Suzuki, Hiroyuki; et al.

Nuclear Instruments and Methods in Physics Research A, 798, p.62 - 69, 2015/10

 Times Cited Count:2 Percentile:66.76(Instruments & Instrumentation)

The light transport properties of scintillator light inside alternative He-3 neutron detector modules using scintillator sheets have been investigated by a ray-tracing simulation code. The detector module consists of a light-reflecting tube, a thin rectangular ceramic scintillator sheet laminated on a glass plate, and two photo-multiplier tubes (PMTs) mounted at both ends of the detector tube. The light induced on the surface of the scintillator sheet via nuclear interaction between the scintillator and neutrons are detected by the two PMTs. The light output of various detector modules in which the scintillator sheets are installed with several different arrangements were examined and evaluated in comparison with experimental results. The results derived from the simulation reveal that the light transport property is strongly dependent on the arrangement of the scintillator sheet inside the tube and the shape of the tube.

Journal Articles

First $$alpha$$-$$gamma$$ spectroscopy using Si-Ge detector array installed at focal plane of GARIS

Kaji, Daiya*; Morimoto, Koji*; Wakabayashi, Yasuo*; Takeyama, Mirei*; Asai, Masato

JPS Conference Proceedings (Internet), 6, p.030106_1 - 030106_4, 2015/06

A Si-Ge detector array was newly installed at the focal plane of the gas-filled recoil ion separator GARIS to perform $$alpha$$-$$gamma$$ (X-rays) spectroscopy for superheavy nuclei. The performance of the array was tested using the $$^{207}$$Pb($$^{48}$$Ca,2n)$$^{253}$$No and $$^{208}$$Pb($$^{48}$$Ca,xn)$$^{256-x}$$No [x=1,2,3] reactions. $$gamma$$ rays originating from the $$alpha$$ decay of $$^{253}$$No and $$^{255}$$No were clearly observed in prompt coincidence with the $$alpha$$ particles.

Journal Articles

Performance of new gas-filled recoil ion separator GARIS-II for asymmetric fusion reaction

Kaji, Daiya*; Morimoto, Koji*; Wakabayashi, Yasuo*; Takeyama, Mirei*; Yamaki, Sayaka*; Tanaka, Kengo*; Haba, Hiromitsu*; Huang, M.*; Murakami, Masashi*; Kanaya, Jumpei*; et al.

JPS Conference Proceedings (Internet), 6, p.030107_1 - 030107_4, 2015/06

Performance of the new gas-filled recoil ion separator GARIS-II was investigated using asymmetric $$^{22}$$Ne-induced fusion reactions. The use of He-H$$_{2}$$ mixture gas for the gas-filled magnet significantly reduced background scattered particles detected at the focal-plane Si detector, and increased a transmission of the asymmetric reaction products. A target-identification system was newly installed for efficient measurements of excitation functions without changing beam energy nor target.

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