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.

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…

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…

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…

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 …

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…

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…

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)…

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…

Liquid-scintillation detection of preseparated 257Rf with the SISAK-system

Abstract The fast liquid–liquid extraction system SISAK with continuous liquid scintillation detection was coupled to the Berkeley Gas-filled Separator to enable studies of the chemical properties of α -decaying transactinide elements. The preseparated transactinide 257Rf (4.7 s), was transported via a He/KCl-jet directly into the scintillation solution. This permitted the first unambiguous detection of transactinide atoms by the means of the α -liquid scintillation detectors of the SISAK-system. During the experiment, 89 257Rf atoms were observed. The type of events observed correspond well with the expectations based on half-lives, decay branches and transport- and hold-up times. The succ…

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…

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…

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…

Decay and Fission Hindrance of Two- and Four-QuasiparticleKIsomers inRf254

Two isomers decaying by electromagnetic transitions with half-lives of 4.7(1.1) and 247(73) μs have been discovered in the heavy ^{254}Rf nucleus. The observation of the shorter-lived isomer was made possible by a novel application of a digital data acquisition system. The isomers were interpreted as the K^{π}=8^{-}, ν^{2}(7/2^{+}[624],9/2^{-}[734]) two-quasineutron and the K^{π}=16^{+}, 8^{-}ν^{2}(7/2^{+}[624],9/2^{-}[734])⊗8^{-}π^{2}(7/2^{-}[514],9/2^{+}[624]) four-quasiparticle configurations, respectively. Surprisingly, the lifetime of the two-quasiparticle isomer is more than 4 orders of magnitude shorter than what has been observed for analogous isomers in the lighter N=150 isotones. …

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.