Christof Vockenhuber

Accelerator mass spectrometry of heavy long-lived radionuclides

Abstract This paper describes the upgrade of the Vienna Environmental Research Accelerator (VERA) to a universal facility for accelerator mass spectrometry (AMS). As a result, it is now possible to measure many long-lived radionuclides at natural abundances across the nuclear chart, from the lightest ( 10 Be ) to the heaviest ( 244 Pu ). Particular emphasis is placed on measurements to understand the ion optics and the origin of background ions, which ultimately limit the sensitivity. VERA is now ready to venture into the realm of actinides (e.g., 236 U , 244 Pu ), and other heavy radionuclides (e.g., 182 Hf ), which promise interesting applications in astrophysics and other fields.

Extension of the measuring capabilities at VERA

Our standard setup used for accelerator mass spectrometry (AMS) with 14C was modified for measuring various other radionuclides. The injection and detection systems were modified to suit the particular isotope investigated. 10B, the stable isobar of 10Be, is stopped in a gas absorber in front of a surface barrier detector. 26Al is measured similar to 14C, except for a modification of the timing for the sequential isotope injection. For 129I, a time-of-flight setup was built to separate 129I from 127I. For heavier rare radionuclides, the mass resolution of the injector system was improved. We also improved our capabilities in measuring carbon samples having very low mass. We describe two different methods to prepare and to measure sub-milligram 14C samples.

Reconstruction of the 236U input function for the Northeast Atlantic Ocean: Implications for 129I/236U and 236U/238U‐based tracer ages

A reconstruction of historical discharges of 236U into the Northeast Atlantic Ocean by nuclear installations is presented. The nuclear reprocessing facilities Sellafield (SF), Great Britain (GB) and La Hague (LH), France and potentially also the nuclear fuel processing installation Springfields (SP), GB represent the main contributors of 236U in the Northeast Atlantic Ocean. Because data on 236U releases is lacking, 236U discharges from SP and SF are estimated based on the U-isotopic systematics found in the discharges from LH. The resulting reconstruction of 236U releases indicates that, until 2013, a total of (95±32) kg of 236U was discharged from SF, SP, and LH. In a second step, the reconstructed 236U releases are combined with 129I data from literature and oceanic and atmospheric box models are used to derive the 129I/236U and 236U/238U input functions that, for example, can be used to calculate tracer ages of Atlantic Waters in the Arctic Ocean. Our conceptual results show that the combination of 129I/236U and 236U/238U generally allows the estimation of tracer ages over the past approximately 25 yr if contributions of 236U from global fallout are considered. Finally, as a proof of concept, the new method is applied to calculate tracer ages of Arctic Ocean surface samples (collected in 2011/12) and the results are in good agreement with literature data. We conclude that the combination of 129I/236U with 236U/238U in a dual tracer approach provides a sensitive tool for the calculation of tracer ages and ventilation rates in the North Atlantic region. This article is protected by copyright. All rights reserved.

ARE COMPACT AMS FACILITIES A COMPETITIVE ALTERNATIVE TO LARGER TANDEM ACCELERATORS

In the last decade, small and compact accelerator mass spectrometry (AMS) systems became available oper- ating at terminal voltages of 1 MV and below. This new category of instruments has become competitive for radiocarbon detection to larger tandem accelerators and many of these instruments are successfully used for 14C dating or biomedical applications. The AMS group at ETH Zurich has demonstrated that small instruments can be built, which allow measurements also of other radionuclides such as 10Be, 26Al, 129I, and the actinides. 41Ca measurements can be performed with sufficient sen- sitivity for biomedical applications. A summary of recent developments made at the 500kV Pelletron in Zurich is given and its performance is compared with that of a commercial compact instrument from the company High Voltage Engineering Europe (HVEE) in Amersfoort, the Netherlands, operating at 1MV at CNA in Seville, Spain, as well as with that of larger AMS facilities. It turns out that the ion optics, stripper design, and the detection system are critical for the performance.

Lifetimes of states in 19Ne above the 15O+α breakup threshold

The 15 O(α, γ) 19 Ne reaction plays a role in the ignition of type I x-ray bursts on accreting neutron stars. The lifetimes of states in 19 Ne above the 15 O+α threshold of 3.53 MeV are important inputs to calculations of the astrophysical reaction rate. These levels in 19 Ne were populated in the 3 He( 20 Ne , α) 19 Ne reaction at a 20 Ne beam energy of 34 MeV. The lifetimes of six states above the threshold were measured with the Doppler-shift attenuation method. The present measurements agree with previous determinations of the lifetimes of these states and in some cases are considerably more precise.

Potential Releases of 129I, 236U, and Pu Isotopes from the Fukushima Dai-ichi Nuclear Power Plants to the Ocean from 2013 to 2015

After the Fukushima Dai-ichi nuclear accident, many efforts were put into the determination of the presence of 137Cs, 134Cs, 131I, and other gamma-emitting radionuclides in the ocean, but minor work was done regarding the monitoring of less volatile radionuclides, pure beta-ray emitters or simply radionuclides with very long half-lives. In this study we document the temporal evolution of 129I, 236U, and Pu isotopes (239Pu and 240Pu) in seawater sampled during four different cruises performed 2, 3, and 4 years after the accident, and we compare the results to 137Cs collected at the same stations and depths. Our results show that concentrations of 129I are systematically above the nuclear weapon test levels at stations located close to the FDNPP, with a maximum value of 790 × 107 at·kg-1, that exceeds all previously reported 129I concentrations in the Pacific Ocean. Yet, the total amount of 129I released after the accident in the time 2011-2015 was calculated from the 129I/137Cs ratio of the ongoing 137Cs releases and estimated to be about 100 g (which adds to the 1 kg released during the accident in 2011). No clear evidence of Fukushima-derived 236U and Pu isotopes has been found in this study, although further monitoring is encouraged to elucidate the origin of the highest 240Pu/239Pu atom ratio of 0.293 ± 0.028 we found close to FDNPP.

Anthropogenic 236U and 129I in the Mediterranean Sea: First comprehensive distribution and constrain of their sources

The first basin-wide distribution of 236U/238U atom ratios and 129I concentrations is presented for the Mediterranean Sea. During the GEOTRACES GA04S-MedSeA expedition in 2013 seawater was collected from 10 vertical profiles covering the principal sub-basins of the Mediterranean Sea. The main objective was to understand the distributions of 236U and 129I in relation to the water masses, and to constrain their sources in this region. The 236U/238U atom ratios and the 129I concentrations ranged from (710±40)×10-12 to (2220±60)×10-12 and from (4.0±0.1)×107 to (13.8±0.3)×107at·kg-1, respectively. The results show that radionuclide-poor Atlantic Water is entering at the surface through the Strait of Gibraltar whereas comparably radionuclide-enriched Levantine Intermediate Water is sinking in the Eastern Basin and flowing westward at intermediate depths. Low radionuclide levels were found in the oldest water masses at about 1000-2000m depth in the Eastern Basin. At greater depths, waters were relatively enriched in 236U and 129I due to dense water formation occurring in both, the Eastern and Western Basins. The inventories of 236U and 129I cannot be explained only by global fallout from atmospheric nuclear bomb testings carried out in the 1950s and 1960s. We estimate that the liquid input of 236U from the nuclear reprocessing facility of Marcoule (France), via the Rhône river, was of the same order of magnitude than the contribution from global fallout, whereas liquid and gaseous releases of 129I from Marcoule were up to two orders of magnitude higher than global fallout. For both radionuclides, the contribution from the Chernobyl accident is found to be minor.

Constraining nova observables: direct measurements of resonance strengths in 33S(p,\gamma)34Cl

The 33S(p,\gamma)34Cl reaction is important for constraining predictions of certain isotopic abundances in oxygen-neon novae. Models currently predict as much as 150 times the solar abundance of 33S in oxygen-neon nova ejecta. This overproduction factor may, however, vary by orders of magnitude due to uncertainties in the 33S(p,\gamma)34Cl reaction rate at nova peak temperatures. Depending on this rate, 33S could potentially be used as a diagnostic tool for classifying certain types of presolar grains. Better knowledge of the 33S(p,\gamma)34Cl rate would also aid in interpreting nova observations over the S-Ca mass region and contribute to the firm establishment of the maximum endpoint of nova nucleosynthesis. Additionally, the total S elemental abundance which is affected by this reaction has been proposed as a thermometer to study the peak temperatures of novae. Previously, the 33S(p,\gamma)34Cl reaction rate had only been studied directly down to resonance energies of 432 keV. However, for nova peak temperatures of 0.2-0.4 GK there are 7 known states in 34Cl both below the 432 keV resonance and within the Gamow window that could play a dominant role. Direct measurements of the resonance strengths of these states were performed using the DRAGON recoil separator at TRIUMF. Additionally two new states within this energy region are reported. Several hydrodynamic simulations have been performed, using all available experimental information for the 33S(p,\gamma)34Cl rate, to explore the impact of the remaining uncertainty in this rate on nucleosynthesis in nova explosions. These calculations give a range of ~ 20-150 for the expected 33S overproduction factor, and a range of ~ 100-450 for the 32S/33S ratio expected in ONe novae.

Concentrations of iodine isotopes (129I and 127I) and their isotopic ratios in aerosol samples from Northern Germany

New data about (129)I, (127)I concentrations and their isotopic ratios in aerosol samples from the trace survey station of the Physikalisch-Technische Bundesanstalt (PTB) in Braunschweig, Northern Germany, are presented and discussed in this paper. The investigated samples were collected on a weekly basis during the years 2011 to 2013. Iodine was extracted from aerosol filters using a strong basic solution and was separated from the matrix elements with chloroform and was analysed by accelerator mass spectrometry (AMS) for (129)I and by inductively coupled plasma mass spectrometry (ICP-MS) for (127)I. The concentrations of (127)I and (129)I in aerosol filters ranged from 0.31 to 3.71 ng m(-3) and from 0.06 to 0.75 fg m(-3), respectively. The results of (129)I/(127)I isotopic ratios were in the order 10(-8) to 10(-7). The (129)I originated directly from gaseous emissions and indirectly from liquid emissions (via sea spray) from the reprocessing plants in Sellafield and La Hague. In comparison with the results of (131)I after the Fukushima accident, no contribution of (129)I from this accident was detectable in Central Europe due to the high background originating from the (129)I releases of the European reprocessing plants. (129)I atmospheric activity concentrations were compared with those of an anthropogenic radionuclide ((85)Kr). We did not find any correlation between (129)I and (85)Kr, both having nuclear reprocessing plant as the main source.

Calorimetric low temperature detectors for low-energetic heavy ions and their application in accelerator mass spectrometry

The energy-sensitive detection of heavy ions with calorimetric low temperature detectors was investigated in the energy range of E=0.1-1 MeV/amu, commonly used for accelerator mass spectrometry (AMS). The detectors used consist of sapphire absorbers and superconducting aluminum transition edge thermometers operated at T approximately 1.5 K. They were irradiated with various ion beams (13C, 197Au, 238U) provided by the VERA tandem accelerator in Vienna, Austria. The relative energy resolution obtained was DeltaE/E=(5-9) x 10(-3), even for the heaviest ions such as 238U. In addition, no evidence for a pulse height defect was observed. This performance allowed for the first time to apply a calorimetric low temperature detector in an AMS experiment. The aim was to precisely determine the isotope ratio of 236U/238U for several samples of natural uranium, 236U being known as a sensitive monitor for neutron fluxes. Replacing a conventionally used detection system at VERA by the calorimetric detector enabled to substantially reduce background from neighboring isotopes and to increase the detection efficiency. Due to the high sensitivity achieved, a value of 236U/238U=6.1 x 10(-12) could be obtained, representing the smallest 236U/238U ratio measured at the time. In addition, we contributed to establishing an improved material standard of 236U/238U, which can be used as a reference for future AMS measurements.