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Journal Articles

On the adsorption and reactivity of element 114, flerovium

Yakushev, A.*; Lens, L.*; D$"u$llmann, Ch. E.*; Khuyagbaatar, J.*; J$"a$ger, E.*; Krier, J.*; Runke, J.*; Albers, H. M.*; Asai, Masato; Block, M.*; et al.

Frontiers in Chemistry (Internet), 10, p.976635_1 - 976635_11, 2022/08

 Times Cited Count:8 Percentile:81.08(Chemistry, Multidisciplinary)

Flerovium (Fl, element 114) is the heaviest element chemically studied so far. The first chemical experiment on Fl suggested that Fl is a noble-gas-like element, while the second studies suggested that Fl has a volatile-metal-like character. To obtain more reliable conclusion, we performed further experimental studies on Fl adsorption behavior on Si oxide and gold surfaces. The present results suggest that Fl is highly volatile and less reactive than the volatile metal, Hg, but has higher reactivity than the noble gas, Rn.

Journal Articles

Gas phase synthesis of 4d transition metal carbonyl complexes with thermalized fission fragments in single-atom reactions

G$"o$tz, M.*; G$"o$tz, S.*; Kratz, J.-V.*; Ballof, J.*; D$"u$llmann, Ch. E.*; Eberhardt, K.*; Mokry, C.*; Renisch, D.*; Runke, J.*; Sato, Tetsuya; et al.

Radiochimica Acta, 109(3), p.153 - 165, 2021/03

 Times Cited Count:3 Percentile:47.54(Chemistry, Inorganic & Nuclear)

We report on a novel two-chamber approach for the synthesis of volatile complexes that allows spatial decoupling of thermalization and gas-phase carbonyl complex synthesis. Neutron induced fission on $$^{235}$$U and spontaneous fission of $$^{248}$$Cm were employed for the production of the fission products. These were stopped inside a gas volume behind the target and flushed with an inert-gas flow into a second chamber. This was flushed with carbon monoxide to allow the gas-phase synthesis of carbonyl complexes. Parameter studies of the transfer from the first into the second chamber as well as on the carbonyl complex formation and transport processes have been performed. High overall efficiencies of more than 50% were reached rendering this approach interesting for studies of superheavy elements. Our results show that carbonyl complex formation of thermalized fission products is a single-atom reaction, and not a hot-atom reaction.

Journal Articles

Search for elements 119 and 120

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, 102(6), p.064602_1 - 064602_9, 2020/12

 Times Cited Count:30 Percentile:97.96(Physics, Nuclear)

A search for production of the superheavy elements with atomic numbers 119 and 120 was performed in the $$^{50}$$Ti+$$^{249}$$Bk and $$^{50}$$Ti+$$^{249}$$Cf fusion-evaporation reactions, respectively, at the gas-filled recoil separator TASCA. Over four months of irradiation, neither was detected at cross-section sensitivity levels of 65 and 200 fb, respectively. The non-observation of elements 119 and 120 is discussed within the concept of fusion-evaporation reactions including various theoretical predictions on the fission-barrier heights of superheavy nuclei in the region of the island of stability.

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

AA2019-0039.pdf:5.03MB

 Times Cited Count:21 Percentile:90.63(Physics, Nuclear)

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

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

AA2018-0417.pdf:0.99MB

 Times Cited Count:6 Percentile:63.44(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

Radiochemical study of the kinematics of multi-nucleon transfer reactions in $$^{48}$$Ca + $$^{248}$$Cm collisions 10% above the Coulomb barrier

G$"o$tz, M.*; G$"o$tz, S.*; Kratz, J. V.*; D$"u$llmann, Ch. E.*; Mokry, Ch.*; Runke, J.*; Th$"o$rle-Pospiech, P.*; Wiehl, N.*; Sch$"a$del, M.; Ballof, J.*; et al.

Nuclear Physics A, 961, p.1 - 21, 2017/05

 Times Cited Count:6 Percentile:47.32(Physics, Nuclear)

The kinematics of multi-nucleon transfer reactions in the $$^{48}$$Ca + $$^{248}$$Cm collisions were investigated using a stacked-foil technique and radiochemical separations. In previous studies, isotopic distributions of the products of below-target isotopes were found to be broader than those of above-target isotopes, which had been interpreted as larger contributions of strongly dumped collisions in the productions of below-target isotopes than above-target ones. However, in the present study, the average total kinetic energy loss (TKEL), and thus, the average excitation energies were determined for both below-target and above-target isotopes, and they were found to be similar. This contradicts the previous interpretation, and thus, a new interpretation has been proposed; highly excited above-target products are lost by fission.

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, 131, p.05001_1 - 05001_6, 2016/12

 Times Cited Count:0 Percentile:0.9

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

Recoil-$$alpha$$-fission and recoil-$$alpha$$-$$alpha$$-fission events observed in the reaction $$^{48}$$Ca + $$^{243}$$Am

Forsberg, U.*; Rudolph, D.*; Andersson, L.-L.*; Di Nitto, A.*; D$"u$llmann, Ch. E.*; Fahlander, C.*; Gates, J. M.*; Golubev, P.*; Gregorich, K. E.*; Gross, C. J.*; et al.

Nuclear Physics A, 953, p.117 - 138, 2016/09

 Times Cited Count:45 Percentile:94.66(Physics, Nuclear)

Alpha-decay chains observed in the element-115 production reactions of $$^{48}$$Ca + $$^{243}$$Am were investigated using a new data set consisting of our recently reported data obtained at GSI and previously reported ones at Dubna and LBNL. Short decay chains of recoil-$$alpha$$-($$alpha$$)-fission type, fourteen of which were observed, and some of which were interpreted as the 2-neutron evaporation products $$^{289}$$Mc, have been reassigned. It is plausible that most of them were assigned to the 3-neutron evaporation products $$^{288}$$Mc whose decay chain would on the way have branches of EC decays followed by fission.

Journal Articles

Review of even element super-heavy nuclei and search for element 120

Hofmann, S.*; Heinz, S.*; Mann, R.*; Maurer, J.*; M$"u$nzenberg, G.*; Antalic, S.*; Barth, W.*; Burkhard, K. G.*; Dahl, L.*; Eberhardt, K.*; et al.

European Physical Journal A, 52(6), p.180_1 - 180_34, 2016/06

 Times Cited Count:155 Percentile:93.43(Physics, Nuclear)

Journal Articles

Remarks on the fission barriers of super-heavy nuclei

Hofmann, S.*; Heinz, S.*; Mann, R.*; Maurer, J.*; M$"u$nzenberg, G.*; Antalic, S.*; Barth, W.*; Dahl, L.*; Eberhardt, K.*; Grzywacz, R.*; et al.

European Physical Journal A, 52(4), p.116_1 - 116_12, 2016/04

 Times Cited Count:28 Percentile:87.4(Physics, Nuclear)

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:104 Percentile:97.57(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

Selected spectroscopic results on element 115 decay chains

Rudolph, D.*; Forsberg, U.*; Golubev, P.*; Sarmiento, L. G.*; Yakushev, A.*; Andersson, L.-L.*; Di Nitto, A.*; D$"u$llmann, Ch. E.*; Gates, J. M.*; Gregorich, K. E.*; et al.

Journal of Radioanalytical and Nuclear Chemistry, 303(2), p.1185 - 1190, 2015/02

 Times Cited Count:7 Percentile:51.55(Chemistry, Analytical)

Thirty correlated $$alpha$$-decay chains of element 115 were observed, which were consistent with previous observations interpreted as the decay chain of $$^{288}$$115. GEANT4 Monte-Carlo simulations were performed to reproduce high-resolution $$alpha$$-photon coincidence results, which allows one to propose Q$$_{alpha}$$ values and excitation schemes of the superheavy nuclei with unprecedented precision.

Journal Articles

$$^{48}$$Ca + $$^{249}$$Bk fusion reaction leading to element Z = 117; Long-lived $$alpha$$-decaying $$^{270}$$Db and discovery of $$^{266}$$Lr

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 Letters, 112(17), p.172501_1 - 172501_5, 2014/05

 Times Cited Count:201 Percentile:98.44(Physics, Multidisciplinary)

The superheavy element with atomic number 117 was produced in the $$^{48}$$Ca + $$^{249}$$Bk fusion reaction using the gas-filled recoil separator TASCA at GSI in Germany. This result verified the previous result of the discovery of new element 117 reported by Flerov Laboratory of Nuclear Reactions in Russia, which makes certain the synthesis and discovery of element 117 in human history. On the other hand, the last nucleus in the $$alpha$$ decay chain from the element 117 was assigned to be the unknown nucleus $$^{266}$$Lr instead of the previously reported $$^{270}$$Db, and $$^{270}$$Db was found to be the $$alpha$$-decaying nucleus with very long half-life.

Journal Articles

Spectroscopic tools applied to element Z = 115 decay chains

Forsberg, U.*; Rudolph, D.*; Golubev, P.*; Sarmiento, L. G.*; Yakushev, A.*; Andersson, L.-L.*; Di Nitto, A.*; D$"u$llmann, Ch. E.*; Gates, J. M.*; Gregorich, K. E.*; et al.

EPJ Web of Conferences, 66, p.02036_1 - 02036_4, 2014/03

 Times Cited Count:7 Percentile:88.88

A focal-plane Si detector setup applied to the spectroscopy of the element 115 $$alpha$$-decay chains was reported. Results of the digital signal analysis for preamplifier signals and of the event-by-event $$alpha$$-energy loss correction analysis were presented. The detectors consist of five double-sided Si strip detectors (DSSSD) arranged as a box, and signals from one side of the detector at the bottom of the box were digitally processed. Energy losses of $$alpha$$ particles detected by two Si detectors at the bottom and a side differs event-by-event, because each $$alpha$$ particle passed through two dead layers with a certain tilted angle. By correcting for the energy loss of each $$alpha$$ event using the angle of the $$alpha$$-particle emission extracted from the detected positions, we succeeded in improving the $$alpha$$ energy resolution significantly.

Journal Articles

Alpha-photon coincidence spectroscopy along element 115 decay chains

Rudolph, D.*; Forsberg, U.*; Golubev, P.*; Sarmiento, L. G.*; Yakushev, A.*; Andersson, L.-L.*; Di Nitto, A.*; D$"u$llmann, Ch. E.*; Gates, J. M.*; Gregorich, K. E.*; et al.

Acta Physica Polonica B, 45(2), p.263 - 272, 2014/02

 Times Cited Count:22 Percentile:75.45(Physics, Multidisciplinary)

Produced in the reaction of $$^{48}$$Ca beam with an $$^{243}$$Am target, thirty correlated $$alpha$$-decay chains were observed. Observed decay chains are consistent with a previously reported decay chain, which confirms the identification of the element 115. In addition, an $$alpha$$-photon coincidence measurement was performed, and $$gamma$$ rays as well as X-ray candidates were observed in this decay chain. The $$gamma$$-ray observation in the heaviest region of superheavy nuclei brings a big progress in the superheavy nuclear structure studies.

Journal Articles

Ion-track membranes of fluoropolymers; Toward controlling the pore size and shape

Yamaki, Tetsuya; Nuryanthi, N.*; Koshikawa, Hiroshi; Asano, Masaharu; Sawada, Shinichi; Hakoda, Teruyuki; Maekawa, Yasunari; Voss, K.-O.*; Severin, D.*; Seidl, T.*; et al.

Nuclear Instruments and Methods in Physics Research B, 314, p.77 - 81, 2013/11

 Times Cited Count:3 Percentile:26.8(Instruments & Instrumentation)

Ion-track membranes of poly(vinylidene fluoride) (PVDF), a type of fluoropolymer, could find wide applications due to its superior chemical and mechanical properties. In order to produce track-etched pores in PVDF films, we have independently employed much milder etching conditions without any oxidant additives in the alkaline etching solution. The goal of this work is to pursue the possibility of varying beam parameters and applying the effect of the etching pretreatment to control the pore size and shape. Ongoing in-situ/on-line analyses at the M-branch of the UNILAC would shed light on the detailed chemistry of not only ion-induced degradation but also the post-irradiation reactivity.

Journal Articles

Spectroscopy of element 115 decay chains

Rudolph, D.*; Forsberg, U.*; Golubev, P.*; Sarmiento, L. G.*; Yakushev, A.*; Andersson, L. L.*; Di Nitto, A.*; D$"u$llmann, Ch. E.*; Gates, J. M.*; Gregorich, K. E.*; et al.

Physical Review Letters, 111(11), p.112502_1 - 112502_5, 2013/09

 Times Cited Count:123 Percentile:96.32(Physics, Multidisciplinary)

Journal Articles

Investigation of nanopore evolution in track-etched poly(vinylidene fluoride) membranes

Yamaki, Tetsuya; Nuryanthi, N.*; Koshikawa, Hiroshi; Asano, Masaharu; Sawada, Shinichi; Hasegawa, Shin; Maekawa, Yasunari; Voss, K.-O.*; Trautmann, C.*; Neumann, R.*

Transactions of the Materials Research Society of Japan, 37(2), p.223 - 226, 2012/06

The aim of this study is to investigate the formation of the poly(vinylidene fluoride) (PVDF) track membranes in detail by electrolytic conductometry. A PVDF film was irradiated with a 450 MeV $$^{129}$$Xe or 2.2 GeV $$^{197}$$Au ion beam, and then the latent tracks were etched in a 9 mol dm$$^{-3}$$ aqueous KOH solution at 80$$^{circ}$$C that had been poured into a conductometric cell. At the same time, the evolution of cylindrical nanopores was monitored by measuring the conductance through the membrane. The etching kinetics significantly depended on the deposited energy within each track, which is represented by the LET. Interestingly, applying a higher voltage to the cell promoted track etching up to the breakthrough probably because the electrophoretic migration of dissolved products occurred out of each pore.

Journal Articles

Conductometric analysis for the formation of poly(vinylidene fluoride)-based ion track membranes

Yamaki, Tetsuya; Nuryanthi, N.*; Koshikawa, Hiroshi; Asano, Masaharu; Sawada, Shinichi; Hasegawa, Shin; Maekawa, Yasunari; Voss, K.-O.*; Trautmann, C.*; Neumann, R.*

ECS Transactions, 35(24), p.1 - 12, 2011/05

 Times Cited Count:7 Percentile:94.1

Our focus has been placed on ion track membranes of poly(vinylidene fluoride) (PVDF), a type of fluoropolymer, because of their superior chemical, mechanical and ferro-electric properties. The aim of this study is to investigate the formation of the PVDF track membranes in more detail by electrolytic conductometry. Interestingly, application of a higher voltage to the conductometry cell as well as irradiation with a higher-LET beam promoted track etching up to breakthrough probably because electrophoretic migration of dissolved products occurred out of each pore.

Journal Articles

Poly(vinylidene fluoride)-based ion track membranes with different pore diameters and shapes; SEM observations and conductometric analysis

Nuryanthi, N.*; Yamaki, Tetsuya; Koshikawa, Hiroshi; Asano, Masaharu; Enomoto, Kazuyuki; Sawada, Shinichi; Maekawa, Yasunari; Voss, K.-O.*; Trautmann, C.*; Neumann, R.*

Denki Kagaku Oyobi Kogyo Butsuri Kagaku, 78(2), p.146 - 149, 2010/02

 Times Cited Count:6 Percentile:13.75(Electrochemistry)

Poly(vinylidene fluoride) (PVDF) membranes with conical and cylindrical nanopores were prepared in a controlled manner by the ion-track technique, which involved heavy ion beam irradiation and the subsequent alkaline etching. Etching behavior mainly depended on energy deposition of ion beams, and thus its depth distribution, estimated by theoretical simulation, was successfully applied to control the shapes and diameters of the etched pores. Scanning electron microscopy (SEM) and electrolytic conductometry then gave an insight into critical experimental parameters. Interestingly, applying a higher voltage to the conductometry cell promoted track etching up to breakthrough probably because electrophoretic migration of dissolved products occurred out of each pore.

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