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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

 Percentile:100

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

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

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.

Journal Articles

Synthesis and detection of a Seaborgium carbonyl complex

Even, J.*; Yakushev, A.*; D$"u$llmann, 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

 Times Cited Count:35 Percentile:17.05(Multidisciplinary Sciences)

A new superheavy element complex, a seaborgium carbonyl, has been successfully synthesized, and its adsorption property has been studied using a cryo-thermochromatography and $$alpha$$-detection apparatus COMPACT. Nuclear reaction products of short-lived $$^{265}$$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)$$_{6}$$. This is the first synthesis of organometallic compounds of transactinide elements for which only simple inorganic comounds have been synthesized so far.

Journal Articles

Superheavy element flerovium (element 114) is a volatile metal

Yakushev, A.*; Gates, J. M.*; T$"u$rler, A.*; Sch$"a$del, M.; D$"u$llmann, Ch. E.*; Ackermann, D.*; Andersson, L.-L.*; Block, M.*; Br$"u$chle, W.*; Dvorak, J.*; et al.

Inorganic Chemistry, 53(3), p.1624 - 1629, 2014/02

 Times Cited Count:51 Percentile:1.81(Chemistry, Inorganic & Nuclear)

We report on a gas-solid chromatography study of the adsorption of element 114 (flerovium, Fl) on a Au surface. Fl was produced in the nuclear fusion reaction $$^{244}$$Pu($$^{48}$$Ca, 3-4n)$$^{288,289}$$Fl and was isolated in-flight from the primary $$^{48}$$ beam in a physical recoil separator. The adsorption behavior of Fl, its nuclear $$alpha$$-decay product Cn, their lighter homologues in groups 14 and 12, i.e., Pb and Hg, and the noble gas Rn were studied simultaneously by isothermal gas chromatography and thermochromatography. Two Fl atoms were detected. They adsorbed on a Au surface at room temperature, but not as readily as Pb and Hg. The observed adsorption behavior of Fl points to a higher inertness compared to its nearest homologue in the group, Pb. However, the measured lower limit for the adsorption enthalpy of Fl on a Au surface points to the formation of a metal-metal bond of Fl with Au. Fl is the least reactive element in the group, but still a metal.

Journal Articles

Anionic fluoro complex of element 105, Db

Kasamatsu, Yoshitaka*; Toyoshima, Atsushi; Asai, Masato; Tsukada, Kazuaki; Li, Z.; Ishii, Yasuo; Tome, Hayato*; Sato, Tetsuya; Kikuchi, Takahiro; Nishinaka, Ichiro; et al.

Chemistry Letters, 38(11), p.1084 - 1085, 2009/10

 Times Cited Count:13 Percentile:48.46(Chemistry, Multidisciplinary)

We report on the characteristic anion-exchange behavior of the superheavy element dubnium (Db) with atomic number Z = 105 in HF/HNO$$_{3}$$ solution at the fluoride ion concentration [F$$^{-}$$] = 0.003 M. The result clearly demonstrates that the fluoro complex formation of Db is significantly different from that of the group-5 homologue Ta in the 6th period of the periodic table while the behavior of Db is similar to that of the lighter homologue Nb in the 5th period.

Journal Articles

Cross section limits for the $$^{248}$$Cm($$^{25}$$Mg, 4$$n$$-5$$n$$)$$^{268,269}$$Hs reactions

Dvorak, J.*; Br$"u$chle, W.*; D$"u$llmann, Ch. E.*; Dvorakova, Z.*; Eberhardt, K.*; Eichler, R.*; J$"a$ger, E.*; Nagame, Yuichiro; Qin, Z.*; Sch$"a$del, M.*; et al.

Physical Review C, 79(3), p.037602_1 - 037602_4, 2009/05

 Times Cited Count:14 Percentile:28.8(Physics, Nuclear)

no abstracts in English

Journal Articles

Observation of the 3$$n$$ evaporation channel in the complete hot-fusion reaction $$^{26}$$Mg + $$^{248}$$Cm leading to the new superheavy nuclide $$^{271}$$Hs

Dvorak, J.*; Br$"u$chle, W.*; Chelnokov, M.*; D$"u$llmann, Ch. E.*; Dvorakova, Z.*; Eberhardt, K.*; J$"a$ger, E.*; Kr$"u$cken, R.*; Kuznetsov, A.*; Nagame, Yuichiro; et al.

Physical Review Letters, 100(13), p.132503_1 - 132503_4, 2008/04

The analysis of a large body of heavy ion fusion reaction data with medium-heavy projectiles (6$$leq$$Z$$leq$$18) and actinide targets suggests a disappearance of the 3$$n$$ exit channel with increasing atomic number of the projectile. Here, we report a measurement of the excitation function of the reaction $$^{248}$$Cm($$^{26}$$Mg,$$xn$$)$$^{274-x}$$Hs and the observation of the new nuclide $$^{271}$$Hs produced in the 3$$n$$ evaporation channel at a beam energy well below the Bass fusion barrier with a cross section comparable to the maxima of the 4$$n$$ and 5$$n$$ channels. This indicates the possible discovery of new neutron-rich transactinide nuclei using relatively light heavy ion beams of the most neutron-rich stable isotopes and actinide targets.

Journal Articles

Observation of the 3$$n$$ evaporation channel in the complete hot-fusion reaction $$^{26}$$Mg+$$^{248}$$Cm leading to the new superheavy nuclide $$^{271}$$Hs

Dvorak, J.*; Br$"u$chle, W.*; Chelnokov, M.*; D$"u$llmann, Ch. E.*; Dvorakova, Z.*; Eberhardt, K.*; J$"a$ger, E.*; Kr$"u$cken, R.*; Kuznetsov, A.*; Nagame, Yuichiro; et al.

Physical Review Letters, 100(13), p.132503_1 - 132503_4, 2008/04

 Times Cited Count:94 Percentile:5.03(Physics, Multidisciplinary)

Journal Articles

Doubly magic nucleus $$^{270}_{108}$$Hs$$_{162}$$

Dvorak, J.*; Br$"u$chle, W.*; Chelnokov, M.*; Dressler, R.*; D$"u$llmann, Ch. E.*; Eberhardt, K.*; Gorshkov, V.*; J$"a$ger, E.*; Kr$"u$cken, R.*; Kuznetsov, A.*; et al.

Physical Review Letters, 97(24), p.242501_1 - 242501_4, 2006/12

 Times Cited Count:117 Percentile:4.05(Physics, Multidisciplinary)

no abstracts in English

Oral presentation

Anion-exchange behavior of element 105, Db, in HF/HNO$$_{3}$$ media

Kasamatsu, Yoshitaka; Toyoshima, Atsushi; Asai, Masato; Tsukada, Kazuaki; Haba, Hiromitsu*; Ishii, Yasuo; Tome, Hayato; Nishinaka, Ichiro; Akiyama, Kazuhiko*; Kikunaga, Hidetoshi*; et al.

no journal, , 

Dubnium-262 was produced in the $$^{248}$$Cm($$^{19}$$F, 5${it n}$) reaction at the JAEA tandem accelerator. Adsorption of Db on the anion-exchange resin was investigated in 0.89 M HF/0.3 M HNO$$_{3}$$ solution. The anion-exchange behavior of Nb, Ta, and Pa as homologues of Db was also examined in details in HF/HNO$$_{3}$$ solutions. From the comparison of those results, we found that the adsorption of Db on the anion-exchange resin is considerably weaker than that of Ta and is relatively similar to those of Nb and Pa in the studied conditions.

Oral presentation

Chemical behavior of element-105, Db, in mixed HF/HNO$$_{3}$$ solutions

Kasamatsu, Yoshitaka; Tome, Hayato; Toyoshima, Atsushi; Tsukada, Kazuaki; Asai, Masato; Ishii, Yasuo; Nishinaka, Ichiro; Sato, Tetsuya; Shinohara, Nobuo; Nagame, Yuichiro; et al.

no journal, , 

Anion-exchange behavior of $$^{262}$$Db (half-life ${it T$_{1/2}$}$ = 34 s) produced in the $$^{248}$$Cm($$^{19}$$F, 5${it n}$) reaction at the JAEA tandem accelerator was investigated in the mixed 0.89 M HF/0.3 M HNO$$_{3}$$ solution ([F$$^{-}$$] = 3 $$times$$ 10$$^{-3}$$ M) with the automated ion-exchange separation apparatus coupled with the detection system for alpha-spectroscopy (AIDA). Anion-exchange behavior of its lighter homologues, Nb and Ta, was also studied under the same conditions using $$^{88}$$Nb (${it T$_{1/2}$}$ = 14.3 min) and $$^{170}$$Ta (${it T$_{1/2}$}$ = 6.76 min) produced in the $$^{nat}$$Ge($$^{19}$$F, ${it xn}$) and $$^{nat}$$Gd($$^{19}$$F, ${it xn}$) reactions, respectively. It was found that the adsorption probability on the anion-exchange resin is in the order of Ta $$>$$ Nb $$sim$$ Db under the present condition.

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