C. Schnabel

Status report of the PSI/ETH AMS facility

The technical and operational details of the Zurich AMS system are discussed and an overview of new developments which have improved efficiency, sensitivity and accuracy of the measurements is given. The numerous applications associated with these measurements will not be covered.

Capabilities of the new SUERC 5MV AMS facility for 14C dating

A new National Electrostatic Corporation (NEC) 5MV accelerator mass spectrometer became operational at the Scottish Universities Environmental Research Centre (SUERC) in July 2002. It has 2 Cs sputter negative ion sources: a 134-sample source (S1) for the routine measurement of all species, and a hybrid source (S2) with 40 spaces for radiocarbon measurements with either graphite or CO (sub 2) samples. A number of performance tests on graphite samples have been carried out on both sources. A precision of better than 0.3% is feasible for modern samples on a routine basis. The (super 14) C background of the machine and the graphite preparation process blank are 0.04+ or -0.01 and 0.16+ or -0.05 pMC, respectively, indicating that (super 14) C dating back to approximately 50 kyr BP is possible. The normalized (super 14) C values for a series of reference materials agree well with the IAEA, TIRI, and FIRI consensus values. Routine measurement of (super 14) C has been underway since May 2003. Preliminary results of performance tests on the CO (sub 2) gas ion source are also reported.

On the analysis of iodine-129 and iodine-127 in environmental materials by accelerator mass spectrometry and ion chromatography.

Based on a review of literature about the abundances of 129I (T1/2 = 15.7 Ma) in the environment we show that there is a severe lack of knowledge, in particular about natural, pre-nuclear levels. Among the two analytical techniques which are sensitive enough to investigate 129I in environmental materials, namely radiochemical neutron activation analysis (RNAA) and accelerator mass spectrometry (AMS), only AMS is capable of covering the natural, pre-nuclear levels. Since such AMS measurements require chemical separation of iodine from the matrix, a wide variety of separation schemes are necessary for environmental analyses. We report here on such schemes for the analysis of soils, plants and soft tissue. They are applied exemplarily to analyses of soils from the vicinity of Chernobyl. For chemical separations prior to analysis, contamination control and blank analyses are essential. Here, we discuss quality control procedures in detail, both for RNAA and AMS. In the case of AMS we use ion-chromatography (IC) for the determination of stable iodine. The IC analysis is included in the separation schemes for environmental materials. First AMS-analyses of terrestrial biospheric materials demonstrate that natural environmental levels of 129I are lower than previously deduced from investigations using RNAA, but higher than expected from model calculations. AMS is capable of providing the missing knowledge about the radioecology of 129I.

Iodine-129: Sample preparation, quality control and analyses of pre-nuclear materials and of natural waters from Lower Saxony, Germany

Sample preparation procedures for AMS measurements of 129I and 127I in environmental materials and some methodological aspects of quality assurance are discussed. Measurements from analyses of some pre-nuclear soil and thyroid gland samples and of a systematic investigation of natural waters in Lower Saxony, Germany, are described. Although the up-to-now lowest 129I/127I ratios in soils and thyroid glands were observed, they are still suspect to contamination since they are significantly higher than the pre-nuclear equilibrium ratio in the marine hydrosphere. A survey on all available 129I/127I isotopic ratios in precipitation shows a dramatic increase until the middle of the 1980s and a stabilization since 1987 at high isotopic ratios of about (3.6–8.3)×10−7. In surface waters, ratios of (57–380)×10−10 are measured while shallow ground waters show with ratios of (1.3–200)×10−10 significantly lower values with a much larger spread. The data for 129I in soils and in precipitation are used to estimate pre-nuclear and modern 129I deposition densities.

On the origin of 129I in rain water near Zürich

129I concentrations in precipitation at Dübendorf/Zürich, Switzerland, have been determined with monthly resolution for almost three years in the mid 1990s. The results confirm that annual mean 129I concentrations in precipitation in central Europe have remained about constant since the late 1980s. Liquid and gaseous emissions from the nuclear fuel reprocessing plants at Sellafield and La Hague are discussed as the only possible sources of 129I in precipitation in central Europe. Based on an upper limit estimate for iodine transferred from the sea to the atmosphere, the gaseous discharges constitute the potentially bigger 129I reservoir for precipitation. Moreover, the time dependence of the annual gaseous 129I releases from Sellafield and La Hague correlates much better with the 129I concentrations in precipitation in central Europe since the late 1980s than does the time dependence of the liquid emissions from these sites. At monthly resolution, the 129I concentrations in the precipitation samples close to Zürich exhibit a large variability. A meteorological transport analysis was carried out for four selected months with particularly low or high observed 129I concentrations. It was found that meteorological transport alone, based upon assimilated wind fields and observed precipitation values, can not directly account for the large month-to-month variability.

14C AMS AT SUERC: IMPROVING QA DATA WITH THE 5MV TANDEM AND 250kV SSAMS

In 2003, a National Electrostatics Corporation (NEC) 5MV tandem accelerator mass spectrometer was installed at SUERC, providing the radiocarbon laboratory with 14C measurements to 4-5‰ repeatability. In 2007, a 250kV single-stage accelerator mass spectrometer (SSAMS) was added to provide additional 14C capability and is now the preferred system for 14C analysis. Changes to the technology and to our operations are evident in our copious quality assurance data: typically, we now use the 134-position MC-SNICS source, which is filled to capacity. Measurement of standards shows that spectrometer running without the complication of on-line δ13C evaluation is a good operational compromise. Currently, 3‰ 14C/13C measurements are routinely achieved for samples up to nearly 3 half-lives old by consistent sample preparation and an automated data acquisition algorithm with sample random access for measurement repeats. Background and known-age standard data are presented for the period 2003-2008 for the 5MV system and 2007-2008 for the SSAMS, to demonstrate the improvements in data quality.

Wet and dry deposition of 129I in Seville (Spain) measured by accelerator mass spectrometry.

Iodine-129 (T1/2 = 1.57 x 10(7) yr) concentrations have been determined by accelerator mass spectrometry in rainwater samples taken at Seville (southwestern Spain) in 1996 and 1997. This technique allows a reduction in the detection limits for this radionuclide in comparison to radiometric counting and other mass spectrometric methods such as ICP-MS. Typical 129I concentrations range from 4.7 x 10(7) 129I atoms/l (19.2%) to 4.97 x 10(9) 129I atoms/l (5.9%), while 129I depositions are normally in the order of 10(8)-10(10) atoms/m2d. These values agree well with other results obtained for recent rainwater samples collected in Europe. Apart from these, the relationship between 129I deposition and some atmospheric factors has been analyzed, showing the importance of the precipitation rate and the concentration of suspended matter in it.

Determination of 129I in atmospheric samples by accelerator mass spectrometry

A method for the radiochemical extraction of 129I from atmospheric charcoal filters and its measurement by accelerator mass spectrometry is presented. Either the 129I concentration or the 129I/127I atom ratio can be determined in the sample. With this method, air filters from Seville, in the Southwest of Spain (37.4 degrees N, 6 degrees W) have been analyzed. Sensitivities in the order of 10(4) atoms/m3 for 129I concentrations and 10(-10) for 129I/127I atom ratios are obtained. AMS measurements are performed with the 6 MV tandem accelerator at the ETH-Hönggerberg in Zurich.

Accelerator mass spectrometry as a powerful tool for the determination of 129I in rainwater

129I is a very long-lived radionuclide (T(1/2) = 15.7 x 10(6) years) that is present in the environment both because of natural and anthropogenic sources. Its environmental interest, for example, as a tracer of geological processes, makes it the research target of a growing scientific community. However, its detection in environmental samples by radiometric methods is very difficult because of its long half-life. In this work, we present the methodology developed for its detection by Accelerator Mass Spectrometry (AMS) in rainwater.

129I/127I ratios and 129I concentrations in a recent sea sediment core and in rainwater from Sevilla (Spain) by AMS

In spite of the environmental relevance of 129I, there is still a scarcity of data about its presence in the different natural compartments. In this work, results are presented on the concentration of 129I in rainwater samples taken in Sevilla (southwestern Spain) and in a sediment core taken near the Ringhals coast (Sweden). Typical concentrations of 108 and 109129I at/l are found in rainwater samples, similar to other values in literature. In the case of the sediment core, our results clearly show the impact of anthropogenic sources, with concentrations in the order of 1013129I at./kg and isotopic ratios 129I/127I in the order of 10−8 in the higher layers.