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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

Liquid-phase chemistry of rutherfordium (Rf), dubnium (Db) and seaborgium (Sg)

Nagame, Yuichiro

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.

Journal Articles

Charge radii and electromagnetic moments of $$^{195-211}$$At

Cubiss, J.*; Andreyev, A.; 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

 Times Cited Count:5 Percentile:8.84(Physics, Nuclear)

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

Chemical properties of rutherfordium (Rf) and dubnium (Db) in the aqueous phase

Nagame, Yuichiro; Kratz, J. V.*; Sch$"a$del, M.*

EPJ Web of Conferences (Internet), 131, p.07007_1 - 07007_8, 2016/12


 Times Cited Count:2 Percentile:21.42

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

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

$$beta$$-delayed fission and $$alpha$$ decay of $$^{196}$$At

Truesdale, V. L.*; Andreyev, A.; Ghys, L.*; Huyse, M.*; Van Duppen, P.*; Sels, S.*; Andel, B.*; Antalic, S.*; Barzakh, A.*; Capponi, L.*; et al.

Physical Review C, 94(3), p.034308_1 - 034308_11, 2016/09

 Times Cited Count:5 Percentile:36.63(Physics, Nuclear)

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.

JAEA Reports

Reports on JAEA's Reimei Research Program; April 1, 2013 - March 31, 2015

Nagame, Yuichiro

JAEA-Review 2015-039, 50 Pages, 2016/03


Advanced Science Research Center set out "Reimei (Dawn) Research Program" with the aim to cultivate forefront and frontier researches. This report compiles the summaries of the research subjects carried out in the fiscal year of 2013 and 2014.

Journal Articles

Lawrencium's place at the table

Nagame, Yuichiro

Nature Chemistry, 8(3), P. 282, 2016/03

We summarize the studies of element 103, lawrencium: discovery or synthesis in nuclear reactions, historical argument for recognition as a new element, nuclear and chemical studies of lawrencium isotopes, and recently measured ionization energy. Based on the studies so far performed, we introduce a debate that has emerged over the place in the periodic table.

Journal Articles

Lawrencium's ionization potential, atom by atom (original title)

Nagame, Yuichiro

Pariti, 31(3), p.40 - 41, 2016/03

no abstracts in English

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

Chemical studies of elements with $$Z geq $$ 104 in liquid phase

Nagame, Yuichiro; Kratz, J. V.*; Sch$"a$del, M.

Nuclear Physics A, 944, p.614 - 639, 2015/12


 Times Cited Count:7 Percentile:34.06(Physics, Nuclear)

Journal Articles

Discrepancy in the periodic table appears at element 103; Successful measurement of the first ionization potential of lawrencium, element 103

Sato, Tetsuya; Nagame, Yuichiro; Tsukada, Kazuaki

Kagaku To Kogyo, 68(9), p.824 - 826, 2015/09

We successfully confirmed that lawrencium (Lr, element 103) is the last member of actinide series by a measurement of its first ionization potential. Obtained experimental result suggested that the outermost electronic orbital of Lr atom would have p-orbital similar to elements of group-13. Our result triggered again the discussion of the position of Lr and lutetium, the lanthanide homologue of Lr, on the Periodic Table.

Journal Articles

Measurement of the first ionization potential of lawrencium, element 103

Sato, Tetsuya; Asai, Masato; Borschevsky, A.*; Stora, T.*; Sato, Nozomi; Kaneya, Yusuke; Tsukada, Kazuaki; D$"u$llmann, Ch. E.*; Eberhardt, K.*; Eliav, E.*; et al.

Nature, 520(7546), p.209 - 211, 2015/04

 Times Cited Count:59 Percentile:1.63(Multidisciplinary Sciences)

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, $$Z$$=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.

Journal Articles

In situ synthesis of volatile carbonyl complexes with short-lived nuclides

Even, J.*; Ackermann, D.*; Asai, Masato; Block, M.*; Brand, H.*; Di Nitto, A.*; D$"u$llmann, Ch. E.*; Eichler, R.*; Fan, F.*; Haba, Hiromitsu*; et al.

Journal of Radioanalytical and Nuclear Chemistry, 303(3), p.2457 - 2466, 2015/03

 Times Cited Count:6 Percentile:28.02(Chemistry, Analytical)

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.

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