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…

The new nuclide225U

In the bombardment of a 270μg/cm 2 180Hf target with48 Ca projectiles at a primary beam energy of E/A=4.24 MeV/u the new nuclide225U was produced. The experiment was performed at the velocity filter SHIP. 225U was found to decay by α emission with Eα=(7880 ±20) keV (≈90%), (7830±20) keV (≈10%) and has a half-life ofT 1/2=(80 −20 +40 ms).

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.

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…

Production, isolation and characterization of radiochemically pure 163Ho samples for the ECHo-project

Abstract Several experiments on the study of the electron neutrino mass are based on high-statistics measurements of the energy spectrum following electron capture of the radionuclide 163Ho. They rely on the availability of large, radiochemically pure samples of 163Ho. Here, we describe the production, separation, characterization, and sample production within the Electron Capture in Holmium-163 (ECHo) project. 163Ho has been produced by thermal neutron activation of enriched, prepurified 162Er targets in the high flux reactor of the Institut Laue-Langevin, Grenoble, France, in irradiations lasting up to 54 days. Irradiated targets were chemically processed by means of extraction chromatogr…

Complex chemistry with complex compounds

In recent years gas-phase chemical studies assisted by physical pre-separation allowed for the investigation of fragile single molecular species by gas-phase chromatography. The latest success with the heaviest group 6 transactinide seaborgium is highlighted. The formation of a very volatile hexacarbonyl compound Sg(CO)6 was observed similarly to its lighter homologues molybdenum and tungsten. The interactions of these gaseous carbonyl complex compounds with quartz surfaces were investigated by thermochromatography. Second-generation experiments are under way to investigate the intramolecular bond between the central metal atom of the complexes and the ligands addressing the influence of re…

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…

Production Cross Sections of 261Rf and 262Db in Bombardments of 248Cm with 18O and 19F Ions

Miss Piggy, a californium-252 fission fragment source as a generator of short-lived radionuclides

Abstract Carrier-free short-lived nuclides are employed in many different fields of modern nuclear chemistry. The two main production strategies are either thermal neutron-induced fission of 235U or 239Pu at nuclear reactors or spallation neutron sources or charged particle-induced nuclear reactions at accelerator facilities. An alternative method is to use a spontaneously fissioning nuclide. A facility applying this technique (“Miss Piggy”) was built at the University of Berne (Switzerland). Californium-252 (252Cf), which has a 3% fission branch and a half-life of 2.645 a, is used for the production of short-lived fission products that are stopped in an adjacent recoil chamber. Short-lived…

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 …

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.

A comparison between the chemical behaviour of lead-gold and lead-bismuth eutectics towards 316L stainless steel

Radiochimica acta, 101 (10)

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…

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…

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…

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…

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)…

Direct Measurement of the Mass Difference ofHo163andDy163Solves theQ-Value Puzzle for the Neutrino Mass Determination

The atomic mass difference of (163)Ho and (163)Dy has been directly measured with the Penning-trap mass spectrometer SHIPTRAP applying the novel phase-imaging ion-cyclotron-resonance technique. Our measurement has solved the long-standing problem of large discrepancies in the Q value of the electron capture in (163)Ho determined by different techniques. Our measured mass difference shifts the current Q value of 2555(16) eV evaluated in the Atomic Mass Evaluation 2012 [G. Audi et al., Chin. Phys. C 36, 1157 (2012)] by more than 7σ to 2833(30(stat))(15(sys)) eV/c(2). With the new mass difference it will be possible, e.g., to reach in the first phase of the ECHo experiment a statistical sensit…

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…

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…

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…

Improved column-based radiochemical processing of the generator produced 68Ga.

An improved chemical strategy for processing of the generator produced (68)Ga was developed based on processing of the original (68)Ge/(68)Ga generator eluate on a micro-column. Direct pre-concentration and purification of the eluted (68)Ga is performed on a cation-exchange resin in hydrochloric acid/acetone media. A supplementary step based on a second micro-column filled with a second resin allows direct re-adsorption of (68)Ga eluted from the cation exchanger. (68)Ga is finally striped from the second resin with a small volume of pure water. For this purpose a strong anion exchanger and a novel extraction chromatographic resin based on tetraalkyldiglycolamides are characterized. The stra…

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 …

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…

Total Versus Near-total Thyroidectomy in Graves Disease

Previous data suggest that the incidence of hypoparathyroidism after surgery for Graves disease (GD) is lower after subtotal thyroidectomy compared to total thyroidectomy (TT). The present study evaluated the incidence of postoperative hypoparathyroidism after near-total (NTT) versus TT in GD.In a multicenter prospective randomized controlled clinical trial, patients with GD were randomized intraoperatively to NTT or TT. Primary endpoint was the incidence of transient postoperative hypoparathyroidism. Secondary endpoints were permanent hypoparathyroidism, transient recurrent laryngeal nerve palsy (RLNP), reoperations for bleeding, inadvertently removed parathyroid glands, and recurrent hype…

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…

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…

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.…