Recent major advances in Accelerator Mass Spectrometry (AMS) at the Vienna Environmental Research Accelerator (VERA) regarding detection efficiency and isobar suppression have opened possibilities for the analysis of additional long-lived radionuclides at ultra-low environmental concentrations. These radionuclides, including 233U, 135Cs, 99Tc, and 90Sr, will become important for oceanographic tracer application due to their generally conservative behavior in ocean water. In particular, the isotope ratios 233U/236U and 137Cs/135Cs have proven to be powerful fingerprints for emission source identification as they are not affected by elemental fractionation. Improved detection efficiencies allowed us to analyze all major long-lived actinides, i.e., 236U, 237Np, 239,240Pu, 241Am as well as the very rare 233U, in the same 10 L water samples of a depth profile from the northwest Pacific Ocean. For this purpose, a simplified and very flexible chemical purification procedure based on extraction chromatography (a single UTEVA® column) was implemented which can be extended by a DGA® column for Am purification. The procedure was validated with the reference materials IAEA-381/385. With the additional increase in ionization efficiency expected for the extraction of actinides as fluoride molecules from the AMS ion source, a further reduction of chemical processing may become possible. This method was successfully applied to an exemplary set of air filter samples. In order to determine the quantitative 237Np concentration reliably, a 236Np spike material is being developed in collaboration with the University of Tsukuba, Japan. Ion-Laser Interaction Mass Spectrometry (ILIAMS), a novel technique for the efficient suppression of stable isobaric background, has been developed at VERA and provides unprecedented detection sensitivity for the fission fragments 135Cs, 99Tc, and 90Sr. The corresponding setup is fully operational now and the isobar suppression factors of >105 achieved, in principle, allow for the detection of the mentioned radionuclides in the environment. Especially for 90Sr analysis, this new approach has already been validated for selected reference materials (e.g., IAEA-A-12) and is ready for application in oceanographic studies. We estimate that a sample volume of only (1–3) L ocean water is sufficient for 90Sr as well as for 135Cs analysis, respectively.
Cosmogenic radionuclide 10Be and 26Al targets (BeO and Al2O3) for AMS analysis are produced by a growing number of geochemical laboratories, employing different sample processing methods for the extraction of Be and Al from environmental materials. The reliability of this geochronological tool depends on data reproducibility independent from the preparation steps and the AMS measurements. Our results demonstrate that 10Be and 26Al concentrations of targets processed following different, commonly used protocols and measured at two AMS facilities lead to consistent results. However, insoluble fluoride precipitates, if formed during processing, can cause decreased 26Al results, while 10Be concentrations are unaffected.
The long-lived radioisotope 182Hf (T1/2 = 8.9 Ma) is of high astrophysical interest as its potential abundance in environmental archives would provide insight into recent r-process nucleosynthesis in the vicinity of our solar system. Despite substantial efforts, it could not be measured at natural abundances with conventional AMS so far due to strong isobaric interference from stable 182W. Equally important is an increase in ion source efficiency for the anions of interest. The new Ion Laser InterAction Mass Spectrometry (ILIAMS) technique at VERA tackles the problem of elemental selectivity in AMS with a novel approach. It achieves near-complete suppression of isobar contaminants via selective laser photodetachment of decelerated anion beams in a gas-filled radio-frequency quadrupole (RFQ) ion cooler. The technique exploits differences in electron affinities (EA) within elemental or molecular isobaric systems neutralizing anions with EAs smaller than the photon energy. Alternatively, these differences in EA can also facilitate anion separation via chemical reactions with the buffer gas. We present first results with this approach on AMS-detection of 182Hf. With He +O2 mixtures as buffer gas in the RFQ, suppression of 182WF5− vs 180HfF 5− by >105 has been demonstrated. Mass analysis of the ejected anion beam identified the formation of oxyfluorides as an important reaction channel. The overall Hf-detection efficiency at VERA presently is 1.4% and the W-corrected blank value is 182Hf/180Hf = (3.4 ± 2.1)×10−14. In addition, a survey of different sample materials for highest negative ion yields of HfF 5− with Cs-sputtering has been conducted.
In the past 10 years new and more accurate stellar neutron capture cross section measurements have changed and improved the abundance predictions of the weak s process. Among other elements in the region between iron and strontium, most of the copper abundance observed today in the solar system distribution was produced by the s process in massive stars. However, experimental data for the stellar 63 Ni(n, γ) 64 Ni cross section are still missing, but is strongly required for a reliable prediction of the copper abundances. 63 Ni (t 1/2 =101.2 a) is a branching point and also a bottleneck in the weak s process flow, and behaves differently during core He and shell C burning. During core He burning the reaction flow proceeds via β -decay to 63 Cu, and a change of the 63 Ni(n, γ) 64 Ni cross section would have no influence. However, this behavior changes at higher temperatures and neutron densities during the shell C burning phase. Under these conditions, a significant amount of the s process nucleosynthesis flow is passing through the channel 62 Ni(n, γ) 63 Ni(n, γ) 64 Ni. At present only theoretical estimates are available for the 63 Ni(n, γ) 64 Ni cross section. The corresponding uncertainty affects the production of 63 Cu in present s process nucleosynthesis calculations and propagates to the abundances of the heavier species up to A=70. So far, experimental information is also missing for the inverse 64 Ni(γ, n) channel. We have measured for the first time the 64 Ni(γ, n) 63 Ni cross section and also combined for the first time successfully the photoactivation technique with subsequent Accelerator Mass Spectrometry (AMS). The activations at the ELBE facility in Dresden-Rossendorf were followed by the 63 Ni/ 64 Ni determination with AMS at the MLL accelerator laboratory in Garching. First results indicate that theoretical predictions have overestimated this cross section up to now. If this also holds for the inverse channel 63 Ni(n, γ) 64 Ni, more 63 Ni is accumulated during the high neutron density regime of the C shell that will contribute to the final abundance of 63 Cu by radiogenic decay. In this case, also a lower s process efficiency is expected for the heavier species along the neutron capture path up to the Ga-Ge region.
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