36Cl production rate from K-spallation in the European Alps (Chironico landslide, Switzerland)

The abundant production of in situ cosmogenic 36Cl from potassium renders 36Cl measurements in K-rich rocks or minerals, such as K-feldspars, potentially useful for precisely dating rock surfaces, either in single-nuclide or in multi-nuclide studies, for example combined with 10Be measurements in quartz. However, significant discrepancies in experimentally calibrated 36Cl production rates from spallation of potassium (36PK-sp), referenced to sea-level/high-latitude (SLHL), limit the accuracy of 36Cl dating from K-rich lithologies. We present a new 36Cl calibration using K-feldspars, in which K-spallation is the most dominant 36Cl production pathway (>92% of total 36Cl), thus minimizing uncertainties from the complex multi-pathway 36Cl production systematics. The samples are derived from boulders of an ∼13.4 ka-old landslide in the Swiss Alps (∼820 m, 46.43°N, 8.85°E). We obtain a local 36PK-sp of 306 ± 16 atoms 36Cl (g K)−1 a−1 and an SLHL 36PK-sp of 145.5 ± 7.7 atoms 36Cl (g K)−1 a−1, when scaled with a standard scaling protocol (‘Lm’). Applying this SLHL 36PK-sp to determine 36Cl exposure ages of K-feldspars from 10Be-dated moraine boulders yields excellent agreement, confirming the validity of the new SLHL 36PK-sp for surface exposure studies, involving 36Cl in K-feldspars, in the Alps.

Radiochemical determination of 129I and 36Cl in MEGAPIE, a proton irradiated lead-bismuth eutectic spallation target

The concentrations of the long-lived nuclear reaction products 129I and 36Cl have been measured in samples from the MEGAPIE liquid metal spallation target. Samples from the bulk target material (lead-bismuth eutectic, LBE), from the interface of the metal free surface with the cover gas, from LBE/steel interfaces and from noble metal absorber foils installed in the cover gas system were analysed using Accelerator Mass Spectrometry at the Laboratory of Ion beam Physics at ETH Zürich. The major part of 129I and 36Cl was found accumulated on the interfaces, particularly at the interface of LBE and the steel walls of the target container, while bulk LBE samples contain only a minor fraction of these nuclides. Both nuclides were also detected on the absorber foils to a certain extent (≪ 1% of the total amount). The latter number is negligible concerning the radio-hazard of the irradiated target material; however it indicates a certain affinity of the absorber foils for halogens, thus proving the principle of using noble metal foils for catching these volatile radionuclides. The total amounts of 129I and 36Cl in the target were estimated from the analytical data by averaging within the different groups of samples and summing up these averages over the total target. This estimation could account for about half of the amount of 129I and 36Cl predicted to be produced using nuclear physics modelling codes for both nuclides. The significance of the results and the associated uncertainties are discussed.

Characterisation and optimisation of the new Prompt Gamma-ray Activation Analysis (PGAA) facility at FRM II

At the research reactor Forschungs-Neutronenquelle Heinz Maier-Leibnitz (FRM II) a new Prompt Gamma-ray Activation Analysis (PGAA) facility was installed. The instrument was originally built and operating at the spallation source at the Paul Scherrer Institute in Switzerland. After a careful re-design in 2004–2006, the new PGAA instrument was ready for operation at FRM II. In this paper the main characteristics and the current operation conditions of the facility are described. The neutron flux at the sample position can reach up 6.07×1010 [cm−2 s−1], thus the optimisation of some parameters, e.g. the beam background, was necessary in order to achieve a satisfactory analytical sensitivity for routine measurements. Once the optimal conditions were reached, detection limits and sensitivities for some elements, like for example H, B, C, Si, or Pb, were calculated and compared with other PGAA facilities. A standard reference material was also measured in order to show the reliability of the analysis under different conditions at this instrument.

Analysis of the 207Bi, 194Hg/Au and 173Lu distribution in the irradiated MEGAPIE target

Samples obtained from different locations within the prototype liquid metal spallation target MEGAPIE irradiated in 2006 at PSI were analysed using γ-spectrometry. A variety of radionuclides formed by reaction of the target material, lead–bismuth eutectic (LBE), with the proton beam and secondary particles were identified. While nuclides representing the target material itself (207Bi) and nuclides of noble metals were found in LBE samples throughout the target, nuclides of electropositive metals were found to be quantitatively deposited on free surfaces and material interfaces within the target system. This behaviour is analysed in more detail based on results obtained for three nuclides representing groups of elements with distinct chemical behaviour, namely 207Bi, 194Hg/Au and 173Lu. Quantitative analysis results are given and compared with predictions obtained using nuclear physics calculations for those nuclides showing rather homogeneous distribution within the target. Possible reasons for the separation of radionuclides from the liquid metal and their deposition on surfaces are given, and consequences arising for nuclear facilities utilizing liquid metals are discussed.

A comparison between the chemical behaviour of lead-gold and lead-bismuth eutectics towards 316L stainless steel

Lead-gold eutectic (LGE) has been recently proposed as an alternative target material for high power spallation sources. In order to compare the corrosive properties of LGE to the better-studied eutectic of lead-bismuth (LBE), an isothermal twin-loop made of SS 316L was built and operated at the Institute of Physics of the University of Latvia. We have measured the concentration of steel alloying elements dissolved in both alloys at the end of two test campaigns via ICP-OES. In case of LGE, a pronounced concentration increase of Fe, Ni, Mn and Cr is found in the liquid metal, which is significantly higher compared to LBE. Similar results were obtained during complementary investigations on material samples exposed to both alloys in this twin-loop at 400 ◦C and 450 ◦C. These findings indicate that in contact with LGE, SS 316L steel suffers from substantial chemical attack. Detailed investigations using structure materials other than SS 316L have to be undertaken before qualifying LGE as a serious alternative to LBE.

Coupled W–Os–Pt isotope systematics in IVB iron meteorites: In situ neutron dosimetry for W isotope chronology

Tungsten isotope compositions of magmatic iron meteorites yield ages of differentiation that are within ±2 Ma of the formation of CAIs, with the exception of IVB irons that plot to systematically less radiogenic compositions yielding erroneously old ages. Secondary neutron capture due to galactic cosmic ray (GCR) irradiation is known to lower the ε182W of iron meteorites, adequate correction of which requires a measure of neutron dosage which has not been available, thus far. The W, Os and Pt isotope systematics of 12 of the 13 known IVB iron meteorites were determined by MC-ICP-MS (W, Os, Pt) and TIMS (Os). On the same dissolutions that yield precise ε182W, stable Os and Pt isotopes were determined as in situ neutron dosimeters for empirical correction of the ubiquitous cosmic-ray induced burn-out of 182W in iron meteorites. The W isotope data reveal a main cluster with ε182W of ∼−3.6, but a much larger range than observed in previous studies including irons (Weaver Mountains and Warburton Range) that show essentially no cosmogenic effect on their ε182W. The IVB data exhibits resolvable negative anomalies in ε189Os (−0.6ε) and complementary ε190Os anomalies (+0.4ε) in Tlacotepec due to neutron capture on 189Os which has approximately the same neutron capture cross section as 182W, and captures neutrons to produce 190Os. The least irradiated IVB iron, Warburton Range, has ε189Os and ε190Os identical to terrestrial values. Similarly, Pt isotopes, which are presented as ε192Pt, ε194Pt and ε196Pt range from +4.4ε to +53ε, +1.54ε to −0.32ε and +0.73ε to −0.20ε, respectively, also identify Tlacotepec and Dumont as the most GCR-damaged samples. In W–Os and W–Pt isotope space, the correlated isotope data back-project toward a 0-epsilon value of ε192Pt, ε189Os and ε190Os from which a pre-GCR irradiation ε182W of −3.42±0.09 (2σ) is derived. This pre-GCR irradiation ε182W is within uncertainty of the currently accepted CAI initial ε182W. The Pt and Os isotope correlations in the IVB irons are in good agreement with a nuclear model for spherical irons undergoing GCR spallation, although this model over-predicts the change of ε182W by ∼2×, indicating a need for better W neutron capture cross section determinations. A nucleosynthetic effect in ε184W in these irons of −0.14±0.08 is confirmed, consistent with the presence of Mo and Ru isotope anomalies in IVB irons. The lack of a non-GCR Os isotope anomaly in these irons requires more complex explanations for the production of W, Ru and Mo anomalies than nebular heterogeneity in the distribution of s-process to r-process nuclides.

Cosmogenic 180W variations in meteorites and re-assessment of a possible 184Os–180W decay system

We measured tungsten (W) isotopes in 23 iron meteorites and the metal phase of the CB chondrite Gujba in order to ascertain if there is evidence for a large-scale nucleosynthetic heterogeneity in the p-process isotope 180W in the solar nebula as recently suggested by Schulz et al. (2013). We observed large excesses in 180W (up to ≈ 6 ε) in some irons. However, significant within-group variations in magmatic IIAB and IVB irons are not consistent with a nucleosynthetic origin, and the collateral effects on 180W from an s-deficit in IVB irons cannot explain the total variation. We present a new model for the combined effects of spallation and neutron capture reactions on 180W in iron meteorites and show that at least some of the observed within-group variability is explained by cosmic ray effects. Neutron capture causes burnout of 180W, whereas spallation reactions lead to positive shifts in 180W. These effects depend on the target composition and cosmic-ray exposure duration; spallation effects increase with Re/W and Os/W ratios in the target and with exposure age. The correlation of 180W/184W with Os/W ratios in iron meteorites results in part from spallogenic production of 180W rather than from 184Os decay, contrary to a recent study by Peters et al. (2014). Residual ε180W excesses after correction for an s-deficit and for cosmic ray effects may be due to ingrowth of 180W from 184Os decay, but the magnitude of this ingrowth is at least a factor of ≈2 smaller than previously suggested. These much smaller effects strongly limit the applicability of the putative 184Os-180W system to investigate geological problems.

Radiochemical Determination of Rare Earth Elements in Proton-Irradiated Lead–Bismuth Eutectic

Various types of proton-irradiated lead–bismuth eutectic (LBE) samples from the MEGAPIE prototype spallation target were analyzed concerning their content of 148Gd, 173Lu, and 146Pm by use of α- and γ-spectrometry. A radiochemical separation procedure was developed to isolate the lanthanide fraction and to prepare thin samples for α-ray measurement. The results prove a substantial depletion of these three elements in bulk samples, whereas accumulation on the LBE/steel-interfaces was observed. The amount of material accumulated on surfaces was roughly estimated by relating the values measured on the sample surfaces to the total surface of the inner target walls. The amount of 148Gd, 173Lu, and 146Pm was then quantified by summing up the contributions from every sample type. The results show a reasonable agreement with theoretical predictions. The obtained results are of utmost importance for the evaluation of the performance of high-power spallation targets, especially concerning the residual nuclide production, the physicochemical behavior of the produced radionuclides during operation, and in terms of an intermediate or final disposal.

Enseignement et recherche

Le vote du 9 février sur l'immigration a eu des répercussions sur les programmes de formation et de recherche académique, Eramsus+ et Horizon 2020. - L'initiative « Protection contre la sexualisation à l'école maternelle et primaire » a récolté le nombre de signatures requises. - La question de l'équivalence des diplômes de la formation professionnelle supérieure a fait débat. - La loi sur la formation continue a abouti. - Le contre-projet indirect à l'initative sur les bourses d'étude propose une réforme de la loi sur les aides à la formation. - La participation de la Suisse à la « Source européenne de spallation ESS » à passer le cap du premier Conseil.