Online chemical adsorption studies of Hg, Tl, and Pb on SiO2 and Au surfaces in preparation for chemical investigations on Cn, Nh, and Fl at TASCA

Online gas-solid adsorption studies with single-atom quantities of Hg, Tl, and Pb, the lighter homologs of the superheavy elements (SHE) copernicium (Cn, Z =112), nihonium (Nh, Z =113), and flerovium (Fl, Z =114), were carried out using short-lived radioisotopes. The interaction with Au and SiO 2 surfaces was studied and the overall chemical yield was determined. Suitable radioisotopes were produced in fusion-evaporation reactions, isolated in the gas-filled recoil separator TASCA, and flushed rapidly to an adjacent setup of two gas chromatography detector arrays covered with SiO 2 (first array) and Au (second array). While Tl and Pb adsorbed on the SiO 2 surface, Hg interacts only weakly and reached the Au-covered array. Our results contribute to elucidating the influence of relativistic effects on chemical properties of the heaviest elements by providing experimental data on these lighter homologs

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. The physisorption of the complexes on Au and SiO2 surfaces was studied. We also studied the stability of some of the complexes, showing that these start to decompose at temperatures above 300 ℃ in contact with a quartz surface. Our studies lay a basis for the investigation of such complexes with transactinides.</jats:p

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

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 6d107s2 and 6d107s27p1/22, 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 244Pu(48Ca, 3–4n)288,289Fl and was isolated in-flight from the primary 48Ca 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

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 predictions on the fission-barrier heights of superheavy nuclei in the region of the island of stability