Niko Kivel

Variable aperture extraction lens for ion beam investigation in inductively coupled plasma-mass spectrometry

A variable aperture was introduced into a commercially available sector field multicollector inductively coupled plasma-mass spectrometer. A diameter-variable aperture allows an in situ study of the radial isotopic composition within the ion beam. Additional information on the intensity distribution could be gained. The elements boron, cadmium and lead, covering a wide mass range, were investigated. In contrast to earlier experiments [Kivel et al., Spectrochimica Acta Part B: Atomic Spectroscopy, 2012, 76, 126–132], the current setup allows for lower element concentration levels in the samples and a drastically reduced measurement time. A significant radial dependence of the isotopic composition within the ion beam was observed for cadmium and lead, whereas for boron, such dependence could not be detected. The beam profiles however show a systematic trend towards smaller beam diameters for higher masses. Even though the beam diameter is dependent upon the mass of the ion, the transmission into the mass spectrometer can be considered almost complete. Thus, a contribution to mass discrimination by space-charge induced beam broadening and energy-selective ion transmission, at least within the boundaries studied here, can be excluded.

Analysis of xenon gas inclusions in nuclear fuel using laser ablation ICP-MS

Analysis of fluid and gaseous inclusions in solids have been a major interest in various fields and have been carried out at different pressures, temperatures, and phase conditions. In nuclear fuel, approximately 20% of the fission products (FPs) are gaseous with isotopes of Xe contributing up to 90% to the product gases. However, previous to this work quantitative analysis of Xe inclusions in nuclear fuel samples have not been performed systematically. The method used must incorporate simple sample handling procedures in a shielded environment. This study is the development of a method for the direct determination of the fission gas (FG) products in micro inclusions contained in nuclear fuels using LA-ICP-MS. To determine the concentration of Xe in nuclear fuel, two calibration strategies were investigated. The first strategy was based on the direct injection of a known quantity of a reference gas into the LA-ICP-MS carrier gas system. Further, the ablation of a ‘matrix-matched’ standard of a non-irradiated UO2 sample, implanted with a known amount of 129Xe was also applied. Using these quantification methods, quantitative LA-ICP-MS measurements were performed on high burnup nuclear fuel. This study demonstrates that direct gas injection is most suitable for the quantification of fission gas in micron-sized inclusions. The direct gas addition is simple and linear calibration curves were obtained. Good reproducibility was obtained and matrix effects were within the uncertainty of the measurements. For the quantification of fission gases in nuclear fuel, aerosol particles were filtered before entering the ICP to remove interferences on the Xe isotopes from the solid FP matrix. The first quantitative determinations of the amount of gas in nuclear fuel using the direct injection method for calibration led to sample pressure calculations which were in good agreement with pressures estimated from computer simulations.

Production, separation and target preparation of 171Tm and 147Pm for neutron cross section measurements

Abstract The knowledge of the neutron capture cross sections of s-process branching point isotopes represents a basic requirement for the understanding of star evolution. Since such branching point isotopes are by definition radioactive, the measurement of their cross sections from thermal to stellar energies becomes a challenging task. Considerable amounts of material have to be produced, representing a significant radioactive hazard. We report here on the production and separation of 3.5 mg 171Tm from 240 mg 170Er2O3 and 72 μg 147Pm from 100 mg 146Nd2O3 irradiated at the ILL high flux reactor. Thin targets were prepared with high chemical and radioisotopic purity suitable for neutron capture measurements at n_TOF CERN and the SARAF-LiLiT facility.

Quantification of 60Fe atoms by MC-ICP-MS for the redetermination of the half-life

In many scientific fields, the half-life of radionuclides plays an important role. The accurate knowledge of this parameter has direct impact on, e.g., age determination of archeological artifacts and of the elemental synthesis in the universe. In order to derive the half-life of a long-lived radionuclide, the activity and the absolute number of atoms have to be analyzed. Whereas conventional radiation measurement methods are typically applied for activity determinations, the latter can be determined with high accuracy by mass spectrometric techniques. Over the past years, the half-lives of several radionuclides have been specified by means of multiple-collector inductively coupled plasma mass spectrometry (MC-ICP-MS) complementary to the earlier reported values mainly derived by accelerator mass spectrometry. The present paper discusses all critical aspects (amount of material, radiochemical sample preparation, interference correction, isotope dilution mass spectrometry, calculation of measurement uncertainty) for a precise analysis of the number of atoms by MC-ICP-MS exemplified for the recently published half-life determination of

Nucleosynthesis Reactions With The High-intensity Saraf-lilit Neutron Source

^{60}

Separation of weighable amounts of 10Be from proton irradiated graphite

Fe (Rugel et al, Phys Rev Lett 103:072502, 2009).

Characterization of nuclear fuels by ICP mass-spectrometric techniques

We present a status report of recent neutron capture experiments performed with the mA-proton beam (1.92 MeV, 3 kW) of the Soreq Applied Research Accelerator Facility (SARAF) and the Liquid-Lithium Target (LiLiT). Experiments and preliminary results for (n,gamma) reactions on 36,38Ar, studied for the first time with 30-keV neutrons, on natKr, natCe and on radioactive targets 147Pm and 171Tm are described.

Isotope fractionation during ion beam formation in multi-collector inductively coupled plasma mass spectrometry

Large amounts of 10Be are produced at the PSI muon production facility by high-energy proton spallation in polycrystalline graphite. For the extraction of 10Be out of large amounts of carbon, pyrolysis followed by chemical purification has been performed. Approx. 270g of graphite from Target E92, which had received a total proton charge of 29 Ah between 2002 and 2005, have been burned at 1000°C in a stream of oxygen. The volatile radioactive oxidation product 3H2O was trapped in 3 water bubblers connected in series. The remainder, a white hygroscopic solid material mainly consisting of 7Li2O, 9/10BeO and 10/11B2O3, was dissolved in HF and subsequently purified by ion exchange chromatography. Radioactive impurities such as 22Na, 44Ti, 54Mn, 60Co, 101Rh, 133Ba and 172Hf have been separated from the final product. The purified material represents a mixture of approx. 6.5mg 9Be and 3.5mg (3.3MBq) 10Be. It is ready to be used for scientific investigations requiring large amounts of this precious isotope.