Synthesis and detection of a seaborgium carbonyl complex

A carbonyl compound that tips the scales Life is short for the heaviest elements. They emerge from high-energy nuclear collisions with scant time for detection before they break up into lighter atoms. Even et al. report that even a few seconds is long enough for carbon to bond to the 106th element, seaborgium (see the Perspective by Loveland). The authors used a custom apparatus to direct the freshly made atoms out of the hot collision environment and through a stream of carbon monoxide and helium. They compared the detected products with theoretical modeling results and conclude that hexacarbonyl Sg(CO) 6 was the most likely structural formula. Science , this issue p. 1491 ; see also p. 14…

Lawrencium chemistry: no evidence for oxidation states lower than 3+ in aqueous solution

Lawrencium (3-min 260Lr) together with other actinides, was produced in the bombardment of a 249Bk target with 18O ions. There was no sign of a reduction of Lr3+ in dilute hydrochloric acid by V2+ or Cr2+, although in the same experiments, Md3+ was reduced to Md2+ (E°=−0.2 V). The resulting limit for the reduction potential of the Lr3+/Lr1(2)+ couple is E° < −0.44 V.

Extraction behavior of rutherfordium into tributylphosphate from hydrochloric acid

The extraction behavior of rutherfordium (Rf) into tributylphosphate (TBP) from hydrochloric acid (HCl) has been studied together with those of the lighter group-4 elements Zr and Hf. The extractability of261Rf,169Hf, and85Zr into TBP was investigated under identical conditions in 7.2–8.0 M HCl by on-line reversed-phase extraction chromatography. The percent extractions of Rf, Hf, and Zr into the TBP resin increase steeply with increasing HCl concentration, and the order of extraction is Zr &gt; Hf ≈ Rf. By considering the order of chloride complexation among these elements, it is suggested that the stability of the TBP complex of Rf tetrachloride is lower than those of Zr and Hf.

An EC-branch in the decay of 27-s 263Db: Evidence for the isotope 263Rf

Summary 27-s 263Db was produced in the 249Bk ( 18O, 4n) reaction at 93 MeV. The activity was transported by a He/KCl-jet to the laboratory where it was collected for 15 min and then subjected to a chemical separation specific for group-4 elements. The activity was dissolved in 0.5 M unbuffered α-HiB and eluted from a cation-exchange column. The effluent was made 9 M in HCl and group-4 tetrachlorides were extracted into TBP/Cyclohexane which was evaporated to dryness on a Ta disc. The Ta discs were assayed for α and SF activity. A SF activity with a half life on the order of 20 min was observed and assigned to the nuclide 263Rf. It is formed by electron-capture decay of 263Db with a decay br…

The recoil transfer chamber—An interface to connect the physical preseparator TASCA with chemistry and counting setups

Performing experiments with transactinide elements demands highly sensitive detection methods due to the extremely low production rates (one-atom-at-a-time conditions). Preseparation with a physical recoil separator is a powerful method to significantly reduce the background in experiments with sufficiently long-lived isotopes (t1/2≥0.5 s). In the last years, the new gas-filled TransActinide Separator and Chemistry Apparatus (TASCA) was installed and successfully commissioned at GSI. Here, we report on the design and performance of a Recoil Transfer Chamber (RTC) for TASCA—an interface to connect various chemistry and counting setups with the separator. Nuclear reaction products recoiling o…

Alpha-Photon Coincidence Spectroscopy Along Element 115 Decay Chains

Produced in the reaction 48Ca+243Am, thirty correlated α-decay chains were observed in an experiment conducted at the GSI Helmholzzentrum fur Schwerionenforschung, Darmstadt, Germany. The decay chains are basically consistent with previous findings and are considered to originate from isotopes of element 115 with mass numbers 287, 288, and 289. A set-up aiming specifically for high-resolution charged particle and photon coincidence spectroscopy was placed behind the gas-filled separator TASCA. For the first time, γ rays as well as X-ray candidates were observed in prompt coincidence with the α-decay chains of element 115.

Chemical studies of elements with Z≥ 104 in liquid phase

Abstract 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, is also given. A newly developed experimental approach to investigate single atoms of the heaviest elements with an electrochemical method is introduced. Perspectives for liquid-phase chemistry experiments on heavier elements are briefly discussed.

First Aqueous Chemistry with Seaborgium (Element 106)

Fluoride Complexation of Element 104, Rutherfordium (Rf), Investigated by Cation-exchange Chromatography

We report on new and much more precise cation-exchange data of element 104, rutherfordium (Rf), in the fluoride ion concentration [F−] range of 5.29×10−5−1.04×10−3 M. The result based on one-atom-a...

Recoil-α-fission and recoil-α–α-fission events observed in the reaction 48Ca + 243Am

Products of the fusion-evaporation reaction 48Ca + 243Am were studied with the TASISpec set-up at the gas-filled separator TASCA at the GSI Helmholtzzentrum für Schwerionenforschung, Darmstadt, Germany. Amongst the detected thirty correlated α-decay chains associated with the production of element Z=115, two recoil-α-fission and five recoil-α-α-fission events were observed. The latter five chains are similar to four such events reported from experiments performed at the Dubna gas-filled separator, and three such events reported from an experiment at the Berkeley gas-filled separator. The four chains observed at the Dubna gas-filled separator were assigned to start from the 2n-evaporation ch…

First ionization potential of the heaviest actinide lawrencium, element 103

The first ionization potential (IP1 ) of element 103, lawrencium (Lr), has been successfully determined for the first time by using a newly developed method based on a surface ionization process. The measured IP 1 value is 4.9630.08 0.07 eV. This value is the smallest among those of actinide elements and is in excellent agreement with the value of 4.963(15) eV predicted by state-of-the-art relativistic calculations also performed in this work. Our results strongly support that the Lr atom has an electronic configuration of [Rn]7s 2 5f 14 7p 1 1/2 , which is influenced by strong relativistic effects. The present work provides a reliable benchmark for theoretical calculations and also opens t…

Extraction of the fluoride-, chloride- and bromide complexes of the elements Nb, Ta, Pa, and 105 into aliphatic amines

Abstract Previous studies of the halide complex formation of element 105 in HCl–HF mixtures and extractions into triisooctyl amine (TIOA) have been performed with the Automated Rapid Chemistry Apparatus, ARCA II. Element 105 was shown to be absorbed on the column from 12 M HCl–0.02 M HF together with its lighter homologues Nb, Ta and the pseudohomologue Pa. In elutions with 10 M HCl–0.025 M HF, 4 M HCl–0.02 M HF, and 0.5 M HCl–0.01 M HF, the extraction sequence Ta>Nb>105>Pa was observed and element 105 behaved very differently from its closest homologue Ta. As it is not possible within reasonable effort to model the many presumably mixed fluoride–chloride complexes involved in these studies…

Cross section limits for theCm248(Mg25,4n−5n)Hs268,269reactions

We report on an attempt to produce and detect $^{268}\mathrm{Hs}$ and $^{269}\mathrm{Hs}$ in the nuclear fusion reaction $^{25}\mathrm{Mg}+^{248}\mathrm{Cm}$ using the gas phase chemistry apparatus COMPACT. No decay chains attributable to the decay of hassium isotopes were observed during the course of this experiment. From the nonobservation of $^{269}\mathrm{Hs}$ we derive a cross section limit of 0.4 pb (63% confidence limit) for the reaction $^{248}\mathrm{Cm}(^{25}\mathrm{Mg},4n)^{269}\mathrm{Hs}$ at a center-of-target beam energy of 140 MeV. The evaluated cross section limit for the $^{248}\mathrm{Cm}(^{25}\mathrm{Mg},5n)^{268}\mathrm{Hs}$ reaction depends on the assumed half-life of …

Production and Decay of Element 114: High Cross Sections and the New NucleusHs277

The fusion-evaporation reaction Pu-244(Ca-48, 3-4n)(288,289)114 was studied at the new gas-filled recoil separator TASCA. Thirteen correlated decay chains were observed and assigned to the production and decay of (288, 289)114. At a compound nucleus excitation energy of E* = 39.8-43.9 MeV, the 4n evaporation channel cross section was 9.8(-3.1)(+3.9) pb. At E* = 36.1-39.5 MeV, that of the 3n evaporation channel was 8.0-(+7.4)(4.5) pb. In one of the 3n evaporation channel decay chains, a previously unobserved alpha branch in (281)Ds was observed ( probability to be of random origin from background: 0.1%). This alpha decay populated the new nucleus (277)Hs, which decayed by spontaneous fission…

Search for Superheavy Elements in theU238+U238Reaction

A search was made for spontaneously fissioning superheavy elements in damped collisions of two uranium nuclei. Different techniques were applied covering the elements 108 to 118 and approx. =126, and a half-life range from 1 ms to more than 1 yr. No evidence for superheavy elements was found at upper cross-section limits of 10/sup -32/, 10/sup -33/, and 10/sup -35/ cm/sup 2/ for half-lives from 1 to 100 ms, 100 ms to 1 d, and 1 d to 1 yr, respectively.

Isotope Distributions in the Reaction ofU238withU238

Radiochemically determined cross sections $\ensuremath{\sigma}(Z, A)$ were used to construct charge and mass distributions for the reaction of 1785-MeV $^{238}\mathrm{U}$ ions with thick $^{238}\mathrm{U}$ targets. Fission of the colliding nuclei is found to dominate. For the surviving uraniumlike fragments an enhancement of yields compared to the Kr + U and Xe + U reactions is observed. The formation of heavy actinides is shown to be associated with the low-energy tails of the broad excitation energy distributions in damped collisions.

First Ionization Potentials of Fm, Md, No, and Lr

We report the first ionization potentials (IP1) of the heavy actinides, fermium (Fm, atomic number Z = 100), mendelevium (Md, Z = 101), nobelium (No, Z = 102), and lawrencium (Lr, Z = 103), determined using a method based on a surface ionization process coupled to an online mass separation technique in an atom-at-a-time regime. The measured IP1 values agree well with those predicted by state-of-the-art relativistic calculations performed alongside the present measurements. Similar to the well-established behavior for the lanthanides, the IP1 values of the heavy actinides up to No increase with filling up the 5f orbital, while that of Lr is the lowest among the actinides. These results clear…

Anionic Fluoro Complex of Element 105, Db

We report on the characteristic anion-exchange behavior of the superheavy element dubnium (Db) with atomic number Z=105 in HF/HNO3 solution at the fluoride ion concentration [F−]=0.003 M. The resul...

Low-lying states in Ra219 and Rn215 : Sampling microsecond α -decaying nuclei

Short-lived α-decaying nuclei "northeast" of 208Pb in the chart of nuclides were studied using the reaction 48Ca+243Am with the decay station TASISpec at TASCA, GSI Darmstadt. Decay energies and times from pile-up events were extracted with a tailor-made pulse-shape analysis routine and specific α-decay chains were identified in a correlation analysis. Decay chains starting with the even-even 220Ra and its odd-A neighbors, 219Fr, and 219,221Ra, with a focus on the 219Ra→215Rn decay, were studied by means of α-γ spectroscopy. A revised α-decay scheme of 219Ra is proposed, including a new decay branch from a previously not considered isomeric state at 17 keV excitation energy. Conclusions on …

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

Recent experimental studies of the chemical characterization of the first two transactinide elements, rutherfordium (Rf) and dubnium (Db), conducted atom-at-a-time in aqueous phases are reviewed. A short description on experimental techniques based on partition methods, specifically automated rapid chemical separation systems, is also given. Perspectives for aqueous-phase chemistry experiments on heavier elements are briefly discussed.

Decomposition studies of group 6 hexacarbonyl complexes. Part 1: Production and decomposition of Mo(CO)6 and W(CO)6

Abstract Chemical studies of superheavy elements require fast and efficient techniques, due to short half-lives and low production rates of the investigated nuclides. Here, we advocate for using a tubular flow reactor for assessing the thermal stability of the Sg carbonyl complex – Sg(CO)6. The experimental setup was tested with Mo and W carbonyl complexes, as their properties are established and supported by theoretical predictions. The suggested approach proved to be effective in discriminating between the thermal stabilities of Mo(CO)6 and W(CO)6. Therefore, an experimental verification of the predicted Sg–CO bond dissociation energy seems to be feasible by applying this technique. By in…

Determination of the partial electron capture- and spontaneous-fission half-lives of254No

The isotope254No was produced in the fusion reaction48Ca +208Pb. Using the velocity filter SHIP and radiochemical techniques it was found that the nuclide254No with a half-life of 55 s decays byα, EC, and spontaneous-fission. Deduced partial half-lives are (61±2) s forα-decay, (550−160+370) s for EC and [2.2−1.0+2.0]×104 s for spontaneous fission.

Backings and targets for chemical and nuclear studies of transactinides with TASCA

Abstract At GSI the gas-filled separator TASCA (TransActinide Separator and Chemistry Apparatus) was set up to investigate the chemical and physical properties of the heaviest elements making use of the highest beam intensities available [ www.gsi.de/tasca ; M. Schadel, D. Ackermann, A. Semchenkov, A. Turler, GSI Scientific Report 2005, GSI Report 2006-1, p. 262]. Appropriate backings and targets have to be developed. Conceivable backing materials are aluminium, titanium, and carbon. Aluminium backings and titanium backings in different thickness and from different companies are produced by cold rolling. Deposition by resistance heating is applied for carbon backings. For experiments in a c…

Superheavy element flerovium (element 114) is a volatile metal.

The electron shell structure of superheavy elements, i.e., elements with atomic number Z ≥ 104, is influenced by strong relativistic effects caused by the high Z. Early atomic calculations on element 112 (copernicium, Cn) and element 114 (flerovium, Fl) having closed and quasi-closed electron shell configurations of 6d(10)7s(2) and 6d(10)7s(2)7p1/2(2), respectively, predicted them to be noble-gas-like due to very strong relativistic effects on the 7s and 7p1/2 valence orbitals. Recent fully relativistic calculations studying Cn and Fl in different environments suggest them to be less reactive compared to their lighter homologues in the groups, but still exhibiting a metallic character. Expe…

Actinide Production in Collisions ofU238withCm248

Cross sections for the production of heavy actinides in damped collisions of $^{238}\mathrm{U}$ ions with $^{248}\mathrm{Cm}$ targets are reported and compared with similar data for other projectiles. The relatively small differences in the formation rates of a given isotope made by different projectiles indicate a balance between increased mass transfer probability with increasing projectile mass and a concurrent decrease in survivability because of an increase in excitation energy.

Preparation of targets for the gas-filled recoil separator TASCA by electrochemical deposition and design of the TASCA target wheel assembly

Abstract The Transactinide Separator and Chemistry Apparatus (TASCA) is a recoil separator with maximized transmission designed for performing advanced chemical studies as well as nuclear reaction and structure investigations of the transactinide elements ( Z >103) on a one-atom-at-a-time basis. TASCA will provide a very clean transactinide fraction with negligible contamination of lighter elements from nuclear side reactions in the target. For TASCA a new target chamber was designed and built at GSI including the rotating target wheel assembly ARTESIA for beam intensities up to 2 μA (particle). For the production of longer-lived isotopes of neutron-rich heavier actinide and transactinide e…

Fission in the landscape of heaviest elements: Some recent examples

The fission process still remains a main factor that determines the stability of the atomic nucleus of heaviest elements. Fission half-lives vary over a wide range, 10^−19 to 10^24 s. Present experimental techniques for the synthesis of the superheavy elements that usually measure α-decay chains are sensitive only in a limited range of half-lives, often 10^5 to 10^3 s. In the past years, measurement techniques for very short-lived and very long-lived nuclei were significantly improved at the gas-filled recoil separator TASCA at GSI Darmstadt. Recently, several experimental studies of fission-related phenomena have successfully been performed. In this paper, results on 254−256Rf and 266Lr ar…

Unusual excitation-energy division in quasi-fission reactions between50Ti,54Cr and58Fe with207,208Pb at the barrier

IRiS—Exploring new frontiers in neutron-rich isotopes of the heaviest elements with a new Inelastic Reaction Isotope Separator

Abstract A dedicated Inelastic Reaction Isotope Separator (IRiS) for multi-nucleon transfer products will be designed and installed at GSI. Research at IRiS will focus on the investigation of new neutron-rich isotopes of the heaviest elements, study of which will advance various research fields, such as nuclear chemistry, nuclear and atomic physics, as well as nuclear astrophysics. The scientific motivation for this project and the alternative design options for the separator and its main components are discussed.

Chemical studies on rutherfordium (Rf) at JAERI

SummaryChemical studies on element 104, rutherfordium (Rf), at JAERI (Japan Atomic Energy Research Institute) are reviewed. The transactinide nuclide261Rf has been produced in the reaction248Cm(18O, 5n) at the JAERI tandem accelerator with the production cross section of about 13 nb. On-line anion-exchange experiments on Rf together with the lighter homologues, group-4 elements Zr and Hf, in acidic solutions have been conducted with a rapid ion-exchange separation apparatus. From the systematic study of the anion-exchange behavior of Rf, it has been found that the properties of Rf in HCl and HNO3solutions are quite similar to those of Zr and Hf, definitely confirming that Rf is a member of …

First successful ionization of Lr (Z = 103) by a surface-ionization technique.

We have developed a surface ionization ion-source as part of the JAEA-ISOL (Isotope Separator On-Line) setup, which is coupled to a He/CdI2 gas-jet transport system to determine the first ionization potential of the heaviest actinide lawrencium (Lr, Z = 103). The new ion-source is an improved version of the previous source that provided good ionization efficiencies for lanthanides. An additional filament was newly installed to give better control over its operation. We report, here, on the development of the new gas-jet coupled surface ion-source and on the first successful ionization and mass separation of 27-s (256)Lr produced in the (249)Cf + (11)B reaction.

Continuous separation and identification of neutronrich neptunium isotopes from heavy-ion reactions by means of the centrifuge system “sisak”

Abstract Neutron-rich neptunium isotopes formed in direct transfer reactions between 136 Xe projectiles and targets of 244 Pu have been separated from other reaction products with the on-line liquid-liquid extraction system SISAK. A four-detector delay method was used to determine the half-lives of the previously unknown isotopes 243 Np and 244 Np. From the decay of the 287.4 keV γ-line a half-life of 1.8 ± 0.3 min was determined for 243 Np. From the decay curves of the γ-lines at 162.7 and 216.7 keV, which fit into the known level scheme of 244 Pu, a half-life of 2.5 ± 0.3 min results for 244 Np.

Ca48+Bk249Fusion Reaction Leading to ElementZ=117: Long-Livedα-DecayingDb270and Discovery ofLr266

The superheavy element with atomic number Z=117 was produced as an evaporation residue in the 48Ca+249Bk fusion reaction at the gas-filled recoil separator TASCA at GSI Darmstadt, Germany. The radioactive decay of evaporation residues and their α-decay products was studied using a detection setup that allowed measuring decays of single atomic nuclei with half-lives between sub-μs and a few days. Two decay chains comprising seven α decays and a spontaneous fission each were identified and are assigned to the isotope 294-117 and its decay products. A hitherto unknown α-decay branch in 270Db (Z=105) was observed, which populated the new isotope 266Lr (Z=103). The identification of the long-liv…

Anion-exchange Behavior of Rf in HCl and HNO3 Solutions

H. Haba,∗,a K. Tsukada,a M. Asai,a S. Goto,a,b A. Toyoshima,a,c I. Nishinaka,a K. Akiyama,a M. Hirata,a S. Ichikawa,a Y. Nagame,a Y. Shoji,c M. Shigekawa,c T. Koike,c M. Iwasaki,c A. Shinohara,c T. Kaneko,b T. Maruyama,b S. Ono,b H. Kudo,b Y. Oura,d K. Sueki,d H. Nakahara,a,d M. Sakama,e A. Yokoyama,f J. V. Kratz,g M. Schadel,h and W. Bruchleh Advanced Science Research Center, Japan Atomic Energy Research Institute, Tokai-mura, Ibaraki 3191195, Japan Department of Chemistry, Faculty of Science, Niigata University, Niigata-shi, Niigata 950-2181, Japan Department of Chemistry, Graduate School of Science, Osaka University, Toyonaka-shi, Osaka 5600043, Japan Department of Chemistry, Graduate Sc…

Measurement of the Md3+/Md2+ Reduction Potential Studied with Flow Electrolytic Chromatography

The reduction behavior of mendelevium (Md) was studied using a flow electrolytic chromatography apparatus. By application of the appropriate potentials on the chromatography column, the more stable Md(3+) is reduced to Md(2+). The reduction potential of the Md(3+) + e(-) → Md(2+) couple was determined to be -0.16 ± 0.05 V versus a normal hydrogen electrode.

Search for superheavy elements in damped collisions betweenU238andCm248

Negative results for the production of superheavy elements in damped collisions between $^{238}\mathrm{U}$ projectiles and $^{248}\mathrm{Cm}$ targets are reported. This reaction was believed to permit a closer and more widespread approach to the predicted island of stability near Z=114 and N=184 than any practical fusion reaction. Aqueous and gas phase chemistry techniques were used to isolate superheavy element fractions. The fractions were counted for spontaneous fission activity, fragment kinetic energies, and neutron multiplicities. Cross-section limits for half-lives from hours to several years are g4\ifmmode\times\else\texttimes\fi{}${10}^{\mathrm{\ensuremath{-}}35}$ ${\mathrm{cm}}^{…

Excitation functions for production of heavy actinides from interactions ofCa40andCa48ions withCm248

Excitation functions have been measured for production of isotopes of Bk through Fm in bombardments of /sup 248/Cm with 234- to 294-MeV /sup 40/Ca ions and with 239- to 318-MeV /sup 48/Ca ions. The maxima of the isotopic distributions for these elements occur at only 2 to 3 mass numbers larger for /sup 48/Ca than for /sup 40/Ca reactions. The shapes of the distributions and the half-widths of about 2.5 mass numbers are quite similar to those observed previously for reactions of /sup 16/O, /sup 18/O, /sup 20/Ne, and /sup 22/Ne with /sup 248/Cm. In general, the excitation functions for /sup 40/Ca show maxima near the Coulomb barrier while those for /sup 48/Ca are about 20 MeV above the barrie…

Chemical investigation of hassium (element 108).

The periodic table provides a classification of the chemical properties of the elements. But for the heaviest elements, the transactinides, this role of the periodic table reaches its limits because increasingly strong relativistic effects on the valence electron shells can induce deviations from known trends in chemical properties. In the case of the first two transactinides, elements 104 and 105, relativistic effects do indeed influence their chemical properties, whereas elements 106 and 107 both behave as expected from their position within the periodic table. Here we report the chemical separation and characterization of only seven detected atoms of element 108 (hassium, Hs), which were…

Measurement of the first ionization potential of lawrencium (element 103)

Lawrencium, with atomic number 103, has an isotope with a half-life of 27 seconds; even so, its first ionization potential has now been measured on an atom-at-a-time scale and agrees well with state-of-the-art theoretical calculations that include relativistic effects. The most dramatic modern revision of Mendeleev's periodic table of elements came in 1944 when Glenn T. Seaborg placed a new series of elements, the actinides (atomic numbers 89–103), below the lanthanides. In this issue of Nature, Yuichiro Nagame and colleagues report the first measurement of one of the basic atomic properties of element 103 (lawrencium), namely its first ionization potential. Lawrencium is only accessible vi…

First superheavy element experiments at the GSI recoil separator TASCA: The production and decay of element 114 in thePu244(Ca48,3-4n) reaction

Experiments with the new recoil separator, Transactinide Separator and Chemistry Apparatus (TASCA), at the GSI were performed by using beams of Ca-48 to irradiate targets of Pb206-208, which led to the production of No252-254 isotopes. These studies allowed for evaluation of the performance of TASCA when coupled to a new detector and electronics system. By following these studies, the isotopes of element 114 ((288-291)114) were produced in irradiations of Pu-244 targets with Ca-48 beams at compound nucleus excitation energies around 41.7 and 37.5 MeV, demonstrating TASCA's ability to perform experiments with picobarn-level cross sections. A total of 15 decay chains were observed and were as…

Rapid Synthesis of Radioactive Transition-Metal Carbonyl Complexes at Ambient Conditions

Carbonyl complexes of radioactive transition metals can be easily synthesized with high yields by stopping nuclear fission or fusion products in a gas volume containing CO. Here, we focus on Mo, W, and Os complexes. The reaction takes place at pressures of around 1 bar at room temperature, i.e., at conditions that are easy to accommodate. The formed complexes are highly volatile. They can thus be transported within a gas stream without major losses to setups for their further investigation or direct use. The rapid synthesis holds promise for radiochemical purposes and will be useful for studying, e.g., chemical properties of superheavy elements.

Attempts to chemically investigate element 112

Summary Two experiments aiming at the chemical investigation of element 112 produced in the heavy ion induced nuclear fusion reaction of 48Ca with 238U were performed at the Gesellschaft für Schwerionenforschung (GSI), Darmstadt, Germany. Both experiments were designed to determine the adsorption enthalpy of element 112 on a gold surface using a thermochromatography setup. The temperature range covered in the thermochromatography experiments allowed the adsorption of Hg at about 35 °C and of Rn at about -180 °C. Reports from the Flerov Laboratory for Nuclear Reactions (FLNR), Dubna, Russia claim production of a 5-min spontaneous fission (SF) activity assigned to 283112 for the 238U(48Ca,3n)…

Adsorption of Db and its homologues Nb and Ta, and the pseudo-homologue Pa on anion-exchange resin in HF solution

Anion-exchange chromatography of element 105, dubnim (Db), produced in the 206 Cm( 19 F, 5n) 262 Db reaction is investigated together with the homologues Nb and Ta, and the pseudo-homologue Pa in 13.9 M hydrofluoric acid (HF) solution. The distribution coefficient (K d ) of Db on an anion-exchange resin is successfully determined by running cycles of 1702 chromatographic column separations. The result clearly indicates that the adsorption of Db on the resin is significantly different from that of the homologues and that the adsorption of anionic fluoro complexes of these elements decreases in the sequence of Ta ≈ Nb > Db > Pa.

Fluoride Complexation of Element 104, Rutherfordium

Fluoride complexation of element 104, rutherfordium (Rf), produced in the 248Cm(18O,5n)261Rf reaction has been studied by anion-exchange chromatography on an atom-at-a-time scale. The anion-exchange chromatographic behavior of Rf was investigated in 1.9-13.9 M hydrofluoric acid together with those of the group-4 elements Zr and Hf produced in the 18O-induced reactions on Ge and Gd targets, respectively. It was found that the adsorption behavior of Rf on anion-exchange resin is quite different from those of Zr and Hf, suggesting the influence of relativistic effects on the fluoride complexation of Rf.

New nuclideHa263

A new nuclide $^{263}\mathrm{Ha}$ was produced in the bombardment of a $^{249}\mathrm{Bk}$ target with 93-MeV $^{18}\mathrm{O}$ ions. It was detected via spontaneous fission counting and was shown to have a half-life of about 0.5 min. This activity was also separated from the reaction products by automated rapid chemical separations using cation-exchange chromatography in 0.05M \ensuremath{\alpha}-hydroxyisobutyric acid. After chemical separation, $^{263}\mathrm{Ha}$ was found to decay by spontaneous fission (${57}_{\mathrm{\ensuremath{-}}15}^{+13}$%) and by \ensuremath{\alpha} emission (${\mathit{E}}_{\mathrm{\ensuremath{\alpha}}}$=8.35 MeV, 43%) with a half-life of ${27}_{\mathrm{\ensurem…

Search for elements 119 and 120

A search for production of the superheavy elements with atomic numbers 119 and 120 was performed in the 50Ti+249Bk and 50Ti+249Cf fusion-evaporation reactions, respectively, at the gas-filled recoil separator TASCA at GSI Darmstadt, Germany. Over four months of irradiation, the 249Bk target partially decayed into 249Cf, which allowed for a simultaneous search for both elements. Neither was detected at cross-section sensitivity levels of 65 and 200 fb for the 50Ti+249Bk and 50Ti+249Cf reactions, respectively, at a midtarget beam energy of Elab=281.5 MeV. The nonobservation of elements 119 and 120 is discussed within the concept of fusion-evaporation reactions including various theoretical pr…

Gas phase chromatography of halides of elements 104 and 105

On-line isothermal gas phase chromatography was used to study halides of261104 (T1/2=65 s) and262,263105 (T1/2=34 s and 27 s) produced an atom-at-a time via the reactions248Cm(18O, 5n) and249Bk(18O, 5n, 4n), respectively. Using HBr and HCl gas as halogenating agents, we were able to produce volatile bromides and chlorides of the above mentioned elements and study their behavior compared to their lighter homologs in Groups 4 or 5 of the periodic table. Element 104 formed more volatile bromide than its homolog Hf. In contrast, element 105 bromides were found to be less volatile than the bromides of the group 5 elements Nb and Ta. Both 104 and Hf chlorides were observed to be more volatile tha…

Electrodeposition methods in superheavy element chemistry

To prepare electrodeposition experiments with superheavy elements (SHE), their homologs were investigated. In the experiments, various electrode materials and electrolytes were used. Critical potentials (E crit ) where the electrodeposition starts and potentials for the deposition of 50% of the atoms in solution (E 50% ) were determined. Underpotential deposition was observed in most cases. An electrolytic cell for a fast electrochemical deposition was developed and the time for the deposition of 50% of the atoms in solution (t 50% ) was determined. Short lived α-emitting isotopes were produced at Gesellschaft fur Schwerionenforschung (GSI), Darmstadt, transferred to the aqueous phase with …

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

Abstract The kinematics of multi-nucleon transfer reactions in 48Ca + 248Cm collisions at 262 MeV (center of target) was investigated by using a stacked-foil technique and radiochemical separations of trans-curium elements. Trans-curium isotopes were identified by α-particle spectroscopy. For Fm isotopes, by comparing the centroids of the measured post-neutron emission isotope distributions with the most probable primary mass number predicted by Volkov's generalized Q g g systematics, the missing mass (number of evaporated neutrons) is estimated. The latter is compared with that deduced from the measured centroid of the laboratory angular distribution peaked closely to the grazing angle and…

Competition between binary reactions and fusion in heavy-ion collisions at the Coulomb barrier

Mass and charge distributions for binary reaction channels have been measured for the reactions86Kr with76Ge,104Ru and130Te at the Coulomb barrier using chemical separations andγ-ray spectroscopy. These systems span the region where dynamical hindrance to complete fusion sets in. The binary reactions can be subdivided into two components associated withi) reflection from the outer potential barrier (quasielastic), andii) reseparation after passing the barrier (complex reactions). The sum of complex-reaction channels and evaporation residues from complete fusion can be reproduced by a barrier passing calculation. The fraction of the barrier passing flux leading to reseparation increases from…

Hexafluoro complex of rutherfordium in mixed HF/HNO3 solutions

Formation of anionic fluoride-complexes of element 104, rutherfordium, produced in the 248 Cm( 18 O, 5n) 261 Rf reaction was studied by anion-exchange on an atom-at-a-time scale. It was found that the hexafluoro complex of Rf, [RfF 6 ] 2- , was formed in the studied fluoride ion concentrations of 0.0005-0.013 M. Formation of [RfF 6 ] 2- was significantly different from that of the homologues Zr and Hf, [ZrF 6 ] 2- and [HfF 6 ] 2- ; the evaluated formation constant of [RfF 6 ] 2- is at least one-order of magnitude smaller than those of [ZrF 6 ] 2- and [HfF 6 ] 2- .

New Short-Lived IsotopeU221and the Mass Surface NearN=126

Two short-lived isotopes ^{221}U and ^{222}U were produced as evaporation residues in the fusion reaction ^{50}Ti+^{176}Yb at the gas-filled recoil separator TASCA. An α decay with an energy of E_{α}=9.31(5)  MeV and half-life T_{1/2}=4.7(7)  μs was attributed to ^{222}U. The new isotope ^{221}U was identified in α-decay chains starting with E_{α}=9.71(5)  MeV and T_{1/2}=0.66(14)  μs leading to known daughters. Synthesis and detection of these unstable heavy nuclei and their descendants were achieved thanks to a fast data readout system. The evolution of the N=126 shell closure and its influence on the stability of uranium isotopes are discussed within the framework of α-decay reduced widt…

Fluorido Complex Formation of Element 104, Rutherfordium (Rf)

We have investigated the cation-exchange behavior of element 104, rutherfordium (Rf), together with its lighter group-4 homologs Zr and Hf, and the tetravalent pseudo-homolog Th in HF/HNO3 mixed so...

Decay properties of265Sg(Z=106)and266Sg(Z=106)

The presently known most neutron-rich isotopes of element 106 (seaborgium, Sg), {sup 265}Sg and {sup 266}Sg, were produced in the fusion reaction {sup 22}Ne+{sup 248}Cm at beam energies of 121 and 123 MeV. Using the On-Line Gas chemistry Apparatus OLGA, a continuous separation of Sg was achieved within a few seconds. Final products were assayed by {alpha}-particle and spontaneous fission (SF) spectrometry. {sup 265}Sg and {sup 266}Sg were identified by observing time correlated {alpha}-{alpha}-({alpha}) and {alpha}-SF decay chains. A total of 13 correlated decay chains of {sup 265}Sg (with an estimated number of 2.8 random correlations) and 3 decay chains of {sup 266}Sg (0.6 random correlat…

Extraction Chromatographic Behavior of Rf, Zr, and Hf in HCl Solution with Styrenedivinylbenzene Copolymer Resin Modified by TOPO (trioctylphosphine oxide)

It is of great interest to study chemical properties of the transactinide elements with atomic numbers (Z) ≥ 104. One of the most important subjects is to establish the position of the elements at the extreme end of the periodic table. To this end we perform studies of chemical properties of these transactinides and compare them with those of their lighter homologues and with the ones expected from extrapolations in the periodic table. So far, chromatographic studies of the transactinides have provided experimental proof of placing rutherfordium (Rf, Z = 104) through hassium (Hs, Z = 108) into groups 4 to 8, respectively. 1-10 Quite recently, copernicium (Cn, Z = 112) has been shown to be a…

Preparation of targets by electrodeposition for heavy element studies

Abstract For heavy element studies at GSI, lanthanide and actinide targets have been prepared by molecular plating. The deposition occurs from an isopropanolic solution at 1000–1200 V with current densities of a few mA/cm 2 . Several lanthanide targets have been prepared for test experiments. With nat Gd deposited on a 10 μm thick Be backing foil a target density of 1100 μg/cm 2 could be achieved. Gd-targets were used for the production of α-emitting isotopes of Os, the homologue of hassium (Hs; Z =108), in order to develop a chemical separation procedure for Hs. 248 Cm targets with densities up to 730 μg/cm 2 have been produced for recent experiments to investigate the chemical behaviour o…

Doubly Magic NucleusHs162108270

Theoretical calculations predict $^{270}\mathrm{Hs}$ ($Z=108$, $N=162$) to be a doubly magic deformed nucleus, decaying mainly by $\ensuremath{\alpha}$-particle emission. In this work, based on a rapid chemical isolation of Hs isotopes produced in the $^{26}\mathrm{Mg}+^{248}\mathrm{Cm}$ reaction, we observed 15 genetically linked nuclear decay chains. Four chains were attributed to the new nuclide $^{270}\mathrm{Hs}$, which decays by $\ensuremath{\alpha}$-particle emission with ${Q}_{\ensuremath{\alpha}}=9.02\ifmmode\pm\else\textpm\fi{}0.03\text{ }\text{ }\mathrm{MeV}$ to $^{266}\mathrm{Sg}$ which undergoes spontaneous fission with a half-life of ${444}_{\ensuremath{-}148}^{+444}\text{ }\t…

Evidence for the formation of sodium hassate(VIII)

SummaryHassium, element 108, was produced in the fusion reaction between26Mg and248Cm. The hassium recoils were oxidizedin-situto a highly volatile oxide, presumably HsO4, and were transported in a mixture of He and O2to a deposition and detection system. The latter consisted of 16 silicon PIN-photodiodes facing a layer of NaOH, which served, in the presence of a certain partial pressure of water in the transport gas, as reactive surface for the deposition of the volatile tetroxides. Six correlated α-decay chains of Hs were detected in the first 5 detectors centred around detection position 3. In analogy to OsO4, which forms Na2[OsO4(OH)2], an osmate(VIII), with aqueous NaOH, HsO4presumably…

Status of the SHIPTRAP Project: A Capture and Storage Facility for Heavy Radionuclides from SHIP

The ion trap facility SHIPTRAP is being set up to deliver very clean and cool beams of singly-charged recoil ions produced at the SHIP velocity filter at GSI Darmstadt. SHIPTRAP consists of a gas cell for stopping and thermalizing high-energy recoil ions from SHIP, an rf ion guide for extraction of the ions from the gas cell, a linear rf trap for accumulation and bunching of the ions, and a Penning trap for isobaric purification. The progress in testing the rf ion guide is reported. A transmission of about 93(5)% was achieved.

Fluoride complexation of rutherfordium (Rf, element 104)

The fluoride complexation of the group-4 elements Zr, Hf and Rf, and of the pseudo-homolog Th, has been investigated in mixed HNO3/HF solutions by studying Kd values on both cation exchange resins (CIX) and anion exchange resins (AIX) using the automated rapid chemistry apparatus ARCA. On the CIX, the four elements are strongly retained as cations below 10-3M HF. For Zr and Hf, the decrease of the Kd values due to the formation of fluoride complexes occurs between 10-3M HF and 10-2M HF. For Rf and Th, this decrease is observed at one order of magnitude higher HF concentrations. On the AIX, for Zr and Hf, a rise of the Kd values due to the formation of anionic fluoride complexes is observed …

The hydration enthalpies of Md3+ and Lr3+

Lawrencium (3-min 260Lr) and lighter actinides were produced in the bombardment of a 249Bk target with 18O ions and loaded onto a cation exchange column in 0.05 M α-hydroxyisobutyrate solution at pH=4.85, together with the radioactive lanthanide tracers 166Ho, 171Er and 171Tm. In elutions with 0.12 M α=hydroxyisobutyrate solution (pH=4.85), trivalent Lr was eluted exactly together with the Er tracer and Md was eluted close to Ho. Lr elutes much later than expected based on the known elution positions of the lighter actinides and the expected analogy to the elution positions of the homologous lanthanides. From the measured elution positions, ionic radii were calculated for Lr3+ and Md3+. Sem…

Observation of the3nEvaporation Channel in the Complete Hot-Fusion ReactionMg26+Cm248Leading to the New Superheavy NuclideHs271

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

Chemical Properties of Element 105 in Aqueous Solution: Halide Complex Formation and Anion Exchange into Triisoctyl Amine

Studies of the halide complexation of element 105 in aqueous solution were performed on 34-s 262Ha produced in the 249Bk(18-O,5n) reaction. The 262Ha was detected by measuring the fission and alpha activities associated with its decay and the alpha decays of its daughter, 4.3-s 258Lr. Time-correlated pairs of parent and daughter alpha particles provided a unique identification of the presence of 262Ha. About 1600 anion exchange separations of 262Ha from HCl and mixed HC1/HF solutions were performed on a one-minute time scale. Reversed-phase micro-chromatographic columns incorporating triisooctyl amine (TIOA) on an inert support were used in the computer-controlled liquid chromatography appa…

Fusion reaction Ca48+Bk249 leading to formation of the element Ts ( Z=117 )

The heaviest currently known nuclei, which have up to 118 protons, have been produced in 48Ca induced reactions with actinide targets. Among them, the element tennessine (Ts), which has 117 protons, has been synthesized by fusing 48Ca with the radioactive target 249Bk, which has a half-life of 327 d. The experiment was performed at the gas-filled recoil separator TASCA. Two long and two short α decay chains were observed. The long chains were attributed to the decay of 294Ts. The possible origin of the short-decay chains is discussed in comparison with the known experimental data. They are found to fit with the decay chain patterns attributed to 293Ts. The present experimental results confi…

The application of neutron activation analysis, scanning electron microscope, and radiographic imaging for the characterization of electrochemically deposited layers of lanthanide and actinide elements

Lanthanide and actinide targets are prepared at the University of Mainz by molecular plating, an electrochemical deposition from an organic solvent, for heavy-ion reaction studies at GSI. To acquire information about deposition yield, target thickness, and target homogeneity, the following analysis methods are applied. With neutron activation analysis (NAA) the deposition yield and the average thickness of the deposited material is determined. We report on the analytical procedure of NAA performed subsequent to the molecular plating process. Scanning electron microscope (SEM) is used to determine the morphology of the target surfaces. In combination with energy dispersive X-ray spectrometer…

Study of non-fusion products in the Ti50+Cf249 reaction

The isotopic distribution of nuclei produced in the 50Ti + 249Cf reaction has been studied at the gas-filled recoil separator TASCA at GSI Darmstadt, which separates ions according to differences in magnetic rigidity. The bombardment was performed at an energy around the Bass barrier and with the TASCA magnetic fields set for collecting fusion-evaporation reaction products. Fifty-three isotopes located “north-east” of 208Pb were identified as recoiling products formed in non-fusion channels of the reaction. These recoils were implanted with energies in two distinct ranges; besides one with higher energy, a significant low-energy contribution was identified. The latter observation was not ex…

Charge-Asymmetry Equilibration in the Reaction ofXe129,132,136withAu197near the Interaction Barrier

Neutron-proton population ratios for quasielastic and inelastic processes in the reactions of 761-MeV $^{129}\mathrm{Xe}$, 769-MeV $^{132}\mathrm{Xe}$, and 795-MeV $^{136}\mathrm{Xe}$ ions with thick $^{197}\mathrm{Au}$ targets were determined radiochemically. Completely relaxed $\frac{N}{Z}$ ratios are observed for damped collisions involving the transfer of $\ensuremath{\Delta}Zg~1$ charge units. The limiting condition $\ensuremath{\Delta}Z\ensuremath{\approx}1$ corresponds to a characteristic time of the order of ${10}^{\ensuremath{-}22}$ sec which indicates the absence of dissipative forces in the equilibration of the charge-asymmetry mode.

Spectroscopy along Flerovium Decay Chains: Discovery ofDs280and an Excited State inCn282

A nuclear spectroscopy experiment was conducted to study α-decay chains stemming from isotopes of flerovium (element Z=114). An upgraded TASISpec decay station was placed behind the gas-filled separator TASCA at the GSI Helmholtzzentrum fur Schwerionenforschung in Darmstadt, Germany. The fusion-evaporation reactions ^{48}Ca+^{242}Pu and ^{48}Ca+^{244}Pu provided a total of 32 flerovium-candidate decay chains, of which two and eleven were firmly assigned to ^{286}Fl and ^{288}Fl, respectively. A prompt coincidence between a 9.60(1)-MeV α particle event and a 0.36(1)-MeV conversion electron marked the first observation of an excited state in an even-even isotope of the heaviest man-made eleme…

Attempts to Produce Superheavy Elements by Fusion ofCa48withCm248in the Bombarding Energy Range of 4.5-5.2 MeV/u

A search for superheavy elements was made in bombardments of $^{248}\mathrm{Cm}$ with $^{48}\mathrm{Ca}$ ions performed at projectile energies close to the interaction barrier in order to keep the excitation energy of the compound nucleus $Z=116$, $A=296$ as low as possible. No evidence for superheavy nuclei was obtained in a half-life region from 1 \ensuremath{\mu}s to 10 yr with a production cross section greater than ${10}^{\ensuremath{-}34}$ to ${10}^{\ensuremath{-}35}$ ${\mathrm{cm}}^{2}$.

To identify the atomic number of superheavy nuclei produced in Ca-48-induced fusion-evaporation reactions, an experiment aiming at measuring characteristic X-rays is being prepared at GSI, Darmstadt, Germany. The gas-filled separator TASCA will be employed, sending the residues towards the multi-coincidence detector setup TASISpec. Two ion-optical modes relying on differing magnetic polarities of the quadrupole magnets can be used at TASCA. New simulations and experimental tests of transmission and background suppression for these two focusing modes into TASISpec are presented.

TASCAを用いたCn, Nh, Fl化学実験のためのHg, Tl, PbのSiO2及びAu表面に対するオンライン化学吸着研究

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 no…

In-situ formation, thermal decomposition, and adsorption studies of transition metal carbonyl complexes with short-lived radioisotopes

Abstract We report on the in-situ synthesis of metal carbonyl complexes with short-lived isotopes of transition metals. Complexes of molybdenum, technetium, ruthenium and rhodium were synthesized by thermalisation of products of neutron-induced fission of 249Cf in a carbon monoxide-nitrogen mixture. Complexes of tungsten, rhenium, osmium, and iridium were synthesized by thermalizing short-lived isotopes produced in 24Mg-induced fusion evaporation reactions in a carbon monoxide containing atmosphere. The chemical reactions took place at ambient temperature and pressure conditions. The complexes were rapidly transported in a gas stream to collection setups or gas phase chromatography devices.…