Kenneth E. Gregorich

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 generated as isotopes 269Hs (refs 8, 9) and 270Hs (ref. 10) in the fusion reaction between 26Mg and 248Cm. The hassium atoms are immediately oxidized to a highly volatile oxide, presumably HsO4, for which we determine an enthalpy of adsorption on our detector surface that is comparable to the adsorption enthalpy determined under identical conditions for the osmium oxide OsO4. These results provide evidence that the chemical properties of hassium and its lighter homologue osmium are similar, thus confirming that hassium exhibits properties as expected from its position in group 8 of the periodic table.

Chemical properties of element 106 (seaborgium)

The synthesis, via nuclear fusion reactions, of elements heavier than the actinides, allows one to probe the limits of the periodic table as a means of classifying the elements. In particular, deviations in the periodicity of chemical properties for the heaviest elements are predicted as a consequence of increasingly strong relativistic effects on the electronic shell structure. The transactinide elements have now been extended up to element 112 (ref. 8), but the chemical properties have been investigated only for the first two of the transactinide elements, 104 and 105 (refs 9,10,11,12,13,14,15,16,17,18,19). Those studies showed that relativistic effect render these two elements chemically different from their lighter homologues in the same columns of the periodic table (Fig. 1). Here we report the chemical separation of element 106 (seaborgium, Sg) and investigations of its chemical behaviour in the gas phase and in aqueous solution. The methods that we use are able to probe the reactivity of individual atoms, and based on the detection of just seven atoms of seaborgium we find that it exhibits properties characteristic of the group 6 homologues molybdenum and tungsten. Thus seaborgium appears to restore the trends of the periodic table disrupted by relativistic effects in elements 104 and 105.

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. Experimental gas-solid chromatography studies on Cn have, indeed, revealed a metal-metal bond formation with Au. In contrast to this, for Fl, the formation of a weak bond upon physisorption on a Au surface was inferred from first experiments. Here, we report on a gas-solid chromatography study of the adsorption of Fl on a Au surface. Fl was produced in the nuclear fusion reaction (244)Pu((48)Ca, 3-4n)(288,289)Fl and was isolated in-flight from the primary (48)Ca beam in a physical recoil separator. The adsorption behavior of Fl, its nuclear α-decay product Cn, their lighter homologues in groups 14 and 12, i.e., Pb and Hg, and the noble gas Rn were studied simultaneously by isothermal gas chromatography and thermochromatography. Two Fl atoms were detected. They adsorbed on a Au surface at room temperature in the first, isothermal part, but not as readily as Pb and Hg. The observed adsorption behavior of Fl points to a higher inertness compared to its nearest homologue in the group, Pb. However, the measured lower limit for the adsorption enthalpy of Fl on a Au surface points to the formation of a metal-metal bond of Fl with Au. Fl is the least reactive element in the group, but still a metal.

New cold and ultra hot binary and cold ternary spontaneous fission modes for 252Cf and new band structures with gammasphere

Abstract Prompt γ-γ-γ and x-γ-γ coincidence studies following the spontaneous fission of 252Cf were carried out first at Oak Ridge then at Gammasphere first with 36 and later with 72 Ge and two x-ray detectors and a long x-ray-γ coincidence experiment at Idaho. Many new cases of correlated pairs in cold (zero neutron emission) binary fission are observed and for the first time the heavier correlated pairs are identified in ternary fission where the third partners are α, 6He (or α2n), 10Be and, tentatively, 14C. Theoretical calculations were carried out of the relative yields of cold binary and ternary fission. There is reasonable agreement between the relative theoretical and experimental yields. New level structures and isotopes include new octupole deformations, identical bands and other structures. Stable octupole deformation is now observed in N=86, 140Xe, 142Ba and 144Ba and 143Ba, 148Ba and to higher spin in 144Ba. The 142–146Ba data provide the first evidence for the predicted disappearance of stable octupole deformation at high spins from band crossings. Identical yrast bands are observed with widely different neutron and proton numbers in 98,100Sr, 108,110Ru, 112,116Pd, 144,146Ba, 152,154,156Nd, 156Sm, 160Gd and a new type of shifted identical bands in 156,158,160Sm as well as the first identical octupole bands in 142,144Ba. Other new level structures are found. Yields and neutron multiplicities were measured directly for SrNd, ZrCe, MoBa, RuXe, and PdTe correlated pairs. A new ultra hot fission mode was discovered going via only 108Mo144Ba, 107Mo145Ba, and/or 106Mo146Ba pairs where one or more of 44,145,146Ba are hyperdeformed at scission with 3:1 axis ratio.

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) 283112 reaction. Hence, Experiment I was designed to detect spontaneously fissioning (SF) isotopes of element 112 with half-lives (t1/2) longer than about 20 s. 11 high-energy events were detected. 7 events exhibit a deposition pattern resembling a chromatographic peak in the vicinity of Rn deposition. However, the energy of the events observed in Experiment I was lower than expected for a SF-decay of 283112. Therefore, these events could not be unambiguously attributed to the decay of 283112. In contradiction with earlier publications newer reports from FLNR Dubna claim that 283112 decays by α-particle emission (Eα = 9.5 MeV) with t1/2 = 4 s followed by a SF-decay of 279Ds (t1/2 = 0.2 s). Therefore, Experiment II was designed to be sensitive to both claimed decay properties of 283112. However, during this experiment neither short α-SF correlations nor SF coincidences were detected. The conclusion is that 283112 was not unambiguously detected, neither in Experiment I nor in Experiment II.

Evidence for the possible synthesis of element 110 produced by the {sup 59}Co+{sup 209}Bi reaction

An experiment to synthesize element 110 by the {sup 59}Co+{sup 209}Bi reaction has been performed at the SuperHILAC at the Lawrence Berkeley Laboratory. One event with many of the expected characteristics of a successful synthesis of {sup 267}110 was observed. This event corresponds to a production cross section of about one picobarn.

First Measurement of a Thermochemical Property of a Seaborgium Compound.

With only a few atoms of seaborgium (Sg, element 106), in the form of volatile SgO(2)Cl(2), it was possible to determine the sublimation enthalpy of this compound using gas chromatography. Furthermore, it was demonstrated that in Group 6 Sg is chemically more similar to W than to Mo.

Octupole deformation in 142,143Ba and 144Ce: new band structures in neutron-rich Ba-isotopes

Abstract New, high spin band structures are established for the neutron-rich nuclei 142,143,145,147Ba, and 144Ce, and levels of 144,146Ba extended to higher spins from the study of γ-γ and γ-γ-γ coincidence studies in spontaneous fission. Alternating parity sequences connected by strong electric dipole transitions are identified in 142,143Ba and 144Ce but not in 145,147Ba to confirm theoretical predictions of stable octupole deformation for N = 86.

Alpha decay properties of light einsteinium isotopes

Abstract The light einsteinium isotopes, with mass numbers 249, 248, 247, 246, 245 and 243, were produced by irradiating 249Cf with protons, 238U with 14N, 237Np with 12C and 233U with 14N, and have been studied by means of α-ray spectroscopy. An analysis of the complex α-peaks of the einsteinium isotopes gave new α-branchings. The tentative assignments of 7 2 + → 7 2 + , 9 2 + ) in the α-decay of 249Es, ( 7 2 + → 7 2 + , 9 2 + , 11 2 + ) in 247Es, ( 3 2 − → 7 2 + , 3 2 − , 5 2 − , 7 2 − ) in 245Es, and ( 3 2 − → 7 2 + , 3 2 − ) in 243Es were made.

Evidence for the synthesis of 267110 produced by the 59Co+209Bi reaction

Abstract An experiment to synthesize element 110 by the 59 Co+ 209 Bi reaction has been performed at the SuperHILAC at the Lawrence Berkeley Laboratory. One event with many of the expected characteristics of a successful synthesis of 267 110 was observed. This event corresponds to a production cross section of about one picobarn.