D. Schumann

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.

First Aqueous Chemistry with Seaborgium (Element 106)

For the first time, chemical separations of element 106 (Seaborgium, Sg) were performed in aqueous solutions. The isotopes Sg and Sg were produced in the Cm + Ne reaction at a beam energy of 121 MeV. The reaction products were continuously transported by a He(KCl)-jet to the computer-controlled liquid chromatography system ARCA. In 0.1 M HNO3/5 X ΙΟ -4 M HF, Sg was found to be eluted within 10 s from 1.6X8 mm cation-exchange columns (Aminex A6, 17.5±2 μπι) together with the hexavalent Moand W-ions, while hexavalent U-ions and tetravalent Zr-, Hf-, and element 104 ions were strongly retained on the column. Element 106 was detected by measuring correlated α-decays of the daughter isotopes 78-s 104 and 26-s 102. For the isotope Sg, we have evidence for a spontaneous fission branch. It yields a partial spontaneousfission half-life which is in agreement with recent theoretical predictions. The chemical results show that the most stable oxidation state of Sg in aqueous solution is +6, and that like its homologs Mo and W, Sg forms neutral or anionic oxoor oxohalide-compounds under the present condition. In these first experiments, Sg exhibits properties very characteristic of group 6 elements, and does not show U-like properties.

New Measurement of the {sup 60}Fe Half-Life

We have made a new determination of the half-life of the radioactive isotope 60Fe using high precision measurements of the number of 60Fe atoms and their activity in a sample containing over 10(15) 60Fe atoms. Our new value for the half-life of 60Fe is (2.62+/-0.04) x 10(6) yr, significantly above the previously reported value of (1.49+/-0.27) x 10(6) yr. Our new measurement for the lifetime of 60Fe has significant implications for interpretations of galactic nucleosynthesis, for determinations of formation time scales of solids in the early Solar System, and for the interpretation of live 60Fe measurements from supernova-ejecta deposits on Earth.

Neutron capture cross section of unstable 63Ni: implications for stellar nucleosynthesis.

The 63Ni(n,γ) cross section has been measured for the first time at the neutron time-of-flight facility n_TOF at CERN from thermal neutron energies up to 200 keV. In total, capture kernels of 12 (new) resonances were determined. Maxwellian averaged cross sections were calculated for thermal energies from   kT=5-100  keV with uncertainties around 20%. Stellar model calculations for a 25M⊙ star show that the new data have a significant effect on the s-process production of 63Cu, 64Ni, and 64Zn in massive stars, allowing stronger constraints on the Cu yields from explosive nucleosynthesis in the subsequent supernova.

Chromatographic Study of Rutherfordium (Element 104) in the System HCl/Tributylphosphate (TBP)

Liquid-liquid extractions of Zr and Hf from various concentrations of HCl were conducted using tributylphosphate (TBP) in toluene (benzene), and undiluted TBP. Quantitative extraction of both Zr and Hf into TBP in toluene (benzene) was observed from > 8 M HCl and into undiluted TBP from > 10M HCl. Extraction from 8 M HCl into undiluted TBP was 80% for Zr and 20% for Hf. Based on these results, a chromatographic separation of Hf from Zr with the Automated Rapid Chemistry Apparatus ARCA II was performed on 1.6X8 mm columns containing undiluted TBP on an inert support. This separation was also studied on-line with short-lived Hf produced in the Gd(0,xn) reaction and with 78-s Rf produced in the Cm(O,5n) reaction at the Philips Cyclotron of the Paul Scherrer Institute. From the distribution of α-decays of Rf between the Hfand Zr-fraction, the R v a l u e for Rf in 8 M HCl was determined, and the following extraction trend was established: Zr > Rf > Hf. This is at variance with earlier results where Rf seemingly did not extract as well as Hf which was tentatively attributed to increased hydrolysis of Rf.

Measurement of the 60Fe(n, gamma)61Fe Cross Section at Stellar Temperatures.

Observations of galactic gamma-ray activity have challenged the current understanding of nucleosynthesis in massive stars. Recent measurements of (60)Fe abundances relative to ;{26}Al;{g} have underscored the need for accurate nuclear information concerning the stellar production of (60)Fe. In light of this motivation, a first measurement of the stellar (60)Fe(n, gamma)(61)Fe cross section, the predominant destruction mechanism of (60)Fe, has been performed by activation at the Karlsruhe Van de Graaff accelerator. Results show a Maxwellian averaged cross section at kT = 25 keV of 9.9 +/-_{1.4(stat)};{2.8(syst)}mbarn, a significant reduction in uncertainty with respect to existing theoretical discrepancies. This result will serve to significantly constrain models of (60)Fe nucleosynthesis in massive stars.

Chemical procedure applied for the identification of Rf/Db produced in the 48Ca +243Am reaction

Summary A chemical separation procedure for Rf/Db is described which was applied to a long-lived decay product from the nuclear fusion reaction 48Ca+ 243Am. A 1.2 mg thick 243Am target was bombarded by 247 MeV 48Ca particles. The recoiling products were collected in a thick Cu catcher for about one day and then subjected to a chemical separation procedure that included an ion exchange from dilute HF solutions. Final samples were prepared on 30 μg/cm2 thick polyethylene (PE) foils and counted in 4π-geometry for α-particles and spontaneous fission (SF) coincidences. The detector arrays were surrounded by 3He detectors to also assay prompt neutrons. Decontamination factors from actinides of about 105 were achieved. Group 6 (W) to 14 (Pb) elements as models for their heavier homologues were shown to be separated from the Rf/Db fraction with more than 90%. In eight final samples, representing a total beam dose of 3.4 × 1018 particles, 15 SF events were detected. The decay pattern points to a single component with a half-life of ≈32h, which shows a chemical behavior similar to the lighter homologues of group 4 and 5 elements.

Accelerator waste as a source for exotic radionuclides

With the development of advanced large-scale accelerator facilities, considerable quantities of activated material are now being produced. From both a scientific and a technological viewpoint, many of these nuclides are of great interest for future research, and in fact cannot be obtained through other means. The Paul Scherrer Institute—operating one of the most powerful proton accelerators in Europe—is able to provide considerable amounts of several exotic long-lived radionuclides. The present report is focused on the separation and application of radionuclides with a special interest on nuclear astrophysics topics.

44Ti, 26Al and 53Mn samples for nuclear astrophysics: the needs, the possibilities and the sources

Exploration of the physics involved in the production of cosmogenic radionuclides requires experiments using the same rare, radioactive nuclei in sufficient quantities. For this work, such exotic radionuclides have been extracted from previously proton-irradiated stainless steel samples using wet chemistry separation techniques. The irradiated construction material has arisen from an extended material research programme at the Paul Scherrer Institute, called STIP (SINQ Target Irradiation Program), where several thousand samples of different materials were irradiated with protons and neutrons of energies up to 570 MeV. In total, 8 × 1017 atoms of 44Ti, ∼1016 atoms of 26Al and ∼1019 atoms of 53Mn are available from selected samples. These materials may now be used to produce targets or radioactive beams for nuclear reaction studies with protons, neutrons and α-particles. The work is part of the ERAWAST initiative (Exotic Radionuclides from Accelerator Waste for Science and Technology), aimed at facilitating new collaborations between the isotope producers and users from different scientific fields including nuclear astrophysics.

Radiochemical analysis of a copper beam dump irradiated with high-energetic protons

Abstract The radionuclide inventory of a copper beam dump from the 590 MeV proton accelerator of the Paul Scherrer Institute in Switzerland was determined, focusing on radioisotopes with half-lives of more than 60 d, and in particular, of long-lived isotopes with T1/2=104−107 years, which are important regarding radioactive waste management. The measurements were carried out using high resolution γ-measurement without sample destruction, as well as liquid scintillation counting (LSC) and accelerator mass spectrometry (AMS) after chemical separation. For the first time, a beam dump from a high power accelerator facility was completely characterized concerning the depth and radial distribution profile of the most hazardous and/or long-lived radionuclides. Moreover, it turned out that some of the investigated radionuclides, like for instance 26Al, 44Ti or 60Fe represent valuable material for application in several scientific fields like nuclear astrophysics, basic nuclear physics research, radiopharmacy and many others. Therefore, based on the analytical results, a special research and development program has been started at PSI objecting on specific preparative extraction of long-lived radioisotopes (ERAWAST — exotic radionuclides from accelerator waste for science and technology).