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Spontaneous and photo-induced decay processes of HfF5− and WF5− molecular anions were investigated in the Double ElectroStatic Ion Ring ExpEriment (DESIREE). The observation of these reactions over long time scales (several tens of ms) was possible due to the cryogenic temperatures (13 K) and the extremely low residual gas pressure (∼10−14 mbar) of DESIREE. For photo-induced reactions, laser wavelengths in the range 240 to 450 nm were employed. Both anion species were found to undergo spontaneous decay via electron detachment or fragmentation. After some ms, radiative cooling processes were observed to lower the probability for further decay through these processes. Photo-induced reactions indicate the existence of an energy threshold for WF5− anions at about 3.5 eV, above which the neutralization yield increases strongly. By contrast, HfF5− ions exhibit essentially no enhanced production of neutrals upon photon interaction, even for the highest photon energy used in this experiment (∼5.2 eV). This suppression will be highly beneficial for the efficient detection, in accelerator mass spectrometry, of the extremely rare isotope 182Hf using the 182HfF5− anion while effectively reducing the interfering stable isobar 182W in the analyte ion 182WF5−. The radionuclide 182Hf is of great relevance in astrophysical environments as it constitutes a potential candidate to study the events of nucleosynthesis that may have taken place in the vicinity of the solar system several million years ago. [ABSTRACT FROM AUTHOR]

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.

A setup for ion-laser interaction was coupled to the state-of-the-art AMS facility VERA five years ago and its potential and applicability as a new means of isobar suppression in accelerator mass spectrometry (AMS) has since been explored. Laser photodetachment and molecular dissociation processes of anions provide unprecedented isobar suppression factors of >1010 for several established AMS isotopes like 36Cl or 26Al and give access to new AMS isotopes like 90Sr, 135Cs or 182Hf at a 3-MV-tandem facility. Furthermore, Ion-Laser InterAction Mass Spectrometry has been proven to meet AMS requirements regarding reliability and robustness with a typical reproducibility of results of 3%. The benefits of the technique are in principle available to any AMS machine, irrespective of attainable ion beam energy. Since isobar suppression via this technique is so efficient, there often is no need for any additional element separation in the detection setup and selected nuclides may even become accessible without accelerator at all. [ABSTRACT FROM AUTHOR]

Abstract: Recent progress with compact ionization chambers has opened new possibilities for isobar suppression in accelerator mass spectrometry (AMS). Separation of 36Cl (t 1/2 =0.30Ma) at natural isotopic levels from its stable isobar 36S became feasible at particle energies of 24MeV, which are also accessible for medium-sized tandem accelerators with 3MV terminal voltage like VERA (Vienna Environmental Research Accelerator). Investigations with an ionization chamber revealed how physics favors isobar separation even at energies below the maximum of the Bragg curve. The strong energy focusing effect at high energy losses reduces energy straggling significantly and isobar separation steadily increases up to almost full energy loss. With an optimized detection setup, sulfur suppression factors of 2×104 have been achieved. Refraining from the additional use of degrader foils has the benefit of high transmission to the detector (∼16%), but requires a low sulfur output from the ion source. Therefore several backing materials have been screened for sulfur content. The dependence of the sulfur output on the AgCl sample size has been investigated as well. Precision and accuracy have been thoroughly assessed over the last two years. Since drifts in the spectra are efficiently corrected by monitoring the position of the 36S peak, the reproducibility for high ratio samples (36Cl/Cl>10−12) is better than 2%. Our blank value of 36Cl/Cl≈(5±5)×10−16 is competitive to other labs. 36Cl has become a routine AMS-isotope at VERA. Recently we also explored novel techniques for additional sulfur suppression already in the ion source. While results with a small gas reaction cell in front of the sputter target were discouraging, a decrease in the sulfur/chlorine ratio by one order of magnitude was achieved by directing 300mW continuous wave laser beam at 445nm towards the cathode in the ion source. [Copyright &y& Elsevier]

Abstract: Accelerator mass spectrometry (AMS) of 36Cl (t 1/2 =0.30Ma) at natural isotopic concentrations requires high particle energies for the separation from the stable isobar 36S and was so far the exclusive domain of tandem accelerators with at least 5MV terminal voltage. Using terminal foil stripping and a detection setup consisting of a split-anode ionization chamber and an additional energy signal from a silicon strip detector, a 36S suppression of >104 at 3MV terminal voltage was achieved. To further increase the 36S suppression energy loss straggling in various counter gases (C4H10, Ar–CH4 and C4H10–Ar) and the effect of “energy focusing” below the maximum of the Bragg curve was investigated. The comparison of experimental data with simulations and published data yielded interesting insights into the physics underlying the detectors. Energy loss, energy straggling and angular scattering determine the 36S suppression. In addition, we improved ion source conditions, target backing materials and the cathode design with respect to sulfur output and cross contamination. These changes allow higher currents during measurement (35Cl− current≈5μA) and also increased the reproducibility. An injector to detector efficiency for 36Cl ions of 8% (16% stripping yield for the 7+ charge state in the accelerator, 50% 36Cl detection efficiency) was achieved, which can favorably be compared to other facilities. The memory effect in our ion source was also thoroughly investigated. Currently our measured blank value is 36Cl/Cl≈3×10−15 when samples with a ratio of 10−11 are used in the same sample wheel and 36Cl/Cl≈5×10−16 if measured together with samples with a ratio of 10−12 or below. This is in good agreement with the lowest so far published isotope ratios around 5×10−16 and demonstrates that 3MV tandems can achieve the same sensitivity for 36Cl as larger machines. [Copyright &y& Elsevier]

In 1889 the German poet and novelist Theodor Fontane wrote the popular literary ballad “Herr von Ribbeck auf Ribbeck im Havelland.” The Squire von Ribbeck is described as a gentle and generous person, who often gives away pears from his pear trees to children passing by and continued donating pears after his death. Now, 135 years later the rock called Ribbeck is giving us insight into processes that happened 4.5 billion years ago. The meteorite Ribbeck (official find location: 52°37′15″N, 12°45′40″E) fell January 21, 2024, and has been classified as a brecciated aubrite. This meteoroid actually entered the Earth's atmosphere at 00:32:38 UTC over Brandenburg, west of Berlin, and the corresponding fireball was recorded by professional all sky and video cameras. More than 200 pieces (two proved by radionuclide analysis to belong to this fresh fall) were recovered totaling about 1.8 kg. Long‐lived radionuclide and noble gas data are consistent with long cosmic ray exposure (55–62 Ma) and a preatmospheric radius of Ribbeck between 20 and 30 cm. The heavily brecciated aubrite consists of major (76 ± 3 vol%) coarse‐grained FeO‐free enstatite (En99.1Fs<0.04Wo0.9), with a significant abundance (15.0 ± 2.5 vol%) of albitic plagioclase (Ab95.3 An2.0Or2.7), minor forsterite (5.5 ± 1.5 vol%; Fo99.9) and 3.5 ± 1.0 vol% of opaque phases (mainly sulfides and metals) with traces of nearly FeO‐free diopside (En53.2Wo46.8) and K‐feldspar (Ab4.6Or95.4). The rock has a shock degree of S3 (U‐S3), and terrestrial weathering has affected metals and sulfides, resulting in the brownish appearance of rock pieces and the partial destruction of certain sulfides already within days after the fall. The bulk chemical data confirm the feldspar‐bearing aubritic composition. Ribbeck is closely related to the aubrite Bishopville. Ribbeck does not contain solar wind implanted gases and is a fragmental breccia. Concerning the Ti‐ and O‐isotope compositions, the data are similar to those of other aubrites. They are also similar to E chondrites and fall close to the data point for the bulk silicate Earth (BSE). Before the Ribbeck meteoroid entered Earth's atmosphere, it was observed in space as asteroid 2024 BX1. The aphelion distance of 2024 BX1's orbit lies in the innermost region of the asteroid belt, which is populated by the Hungaria family of minor planets characterized by their E/X‐type taxonomy and considered as the likely source of aubrites. The spectral comparison of an average large‐scale emission spectrum of Mercury converted into reflectance and of the Ribbeck meteorite spectrum does not show any meaningful similarities. [ABSTRACT FROM AUTHOR]

The nuclide 35Cl can act as a minor "neutron poison" in the stellar slow neutron capture process. Neutron activation combined with accelerator mass spectrometry (AMS) was applied to measure the (n,γ) cross section of 35Cl for neutron spectra simulating Maxwell-Boltzmann distributions of kT≈30 and 40 keV. The neutron activations were performed at the Karlsruhe Van de Graaff accelerator and at the superconducting linear accelerator of the Soreq Applied Research Accelerator Facility utilizing the 7Li(p,n)7Be reaction. AMS measurements of the irradiated samples were performed at the 3 MV Vienna Environmental Research Accelerator, the 6 MV tandem accelerator at the Dresden AMS facility, and the 14 UD tandem accelerator of the Australian National University in Canberra. Our method is independent of previous measurements. For an energy of kT=30keV, we report a Maxwellian averaged cross section of 8.33(32) mb. Using this new value in stellar isotopic abundance calculations, minor changes for the abundances of 35Cl, 36Cl, and 36S are derived. [ABSTRACT FROM AUTHOR]

Highlights: [•] Long-term memory effect in negative ion sources investigated for chlorine isotopes. [•] Interlaboratory comparison of four up-to date negative ion sources. [•] Ion source improvement at DREAMS for minimization of long-term memory effect. [•] Long-term memory effect is the limitation for precise AMS data of volatile elements. [•] Findings to be considered for samples with highly variable ratios of 36Cl/Cl &129I/I. [Copyright &y& Elsevier]

Abstract: The possibility of detecting 36Cl for geological exposure dating has been explored for several years at VERA (the Vienna Environmental Research Accelerator). First results on real samples were obtained with an ionization chamber (developed at the ETH/PSI, Zürich, Switzerland) with two anodes. To improve the suppression of 36S, we equipped the ionization chamber with an exit window and added a Time-of-Flight (TOF) system with a double-sided silicon strip detector (50×50mm2) as stop detector. We optimized the TOF setup by using silicon nitride foils to reduce scattering tails in the energy spectra. At 3MV terminal voltage, corresponding to a particle energy of 24MeV of 36Cl7+, we achieved a 36S7+-suppression of 21,500 (50% 36Cl-detector-efficiency). [Copyright &y& Elsevier]

Abstract: 36Cl AMS measurements at natural isotopic concentrations have yet been performed only at tandem accelerators with 5MV terminal voltage or beyond. We have developed a method to detect 36Cl at natural terrestrial isotopic concentrations with a 3-MV system, operated above specifications at 3.5MV. An effective separation was obtained with an optimized split-anode ionization chamber design (adopted from the ETH/PSI Zurich AMS group), providing a suppression factor of up to 30,000 for the interfering isobar 36S. Despite the good separation, a relatively high sulfur output from the ion source (36S−/35Cl− ≈4×10−10 for samples prepared from chemically pure reagents), and a possibly cross contamination resulted in a background corresponding to 36Cl/Cl≈3×10−14. The method was applied to samples containing between 105 and 106 atoms 36Cl/g rock from sites in Italy and Iran, which were already investigated by other laboratories for surface exposure dating. The 36Cl/Cl ratios in the range from 2×10−13 to 5×10−12 show a generally good agreement with the previous results. These first measurements demonstrate that also 3-MV tandems, constituting the majority of dedicated AMS facilities, are capable of 36Cl exposure dating, which is presently the domain of larger facilities. [Copyright &y& Elsevier]

The sensitive analysis of 90 Sr with accelerator mass spectrometry (AMS) was developed to advance environmental radiology. One advantage of AMS is the ability to analyze environmental samples with 90 Sr/ 88 Sr atomic ratios of 10 -14 in following a simple chemical separation. Three different IAEA samples with known 90 Sr concentrations (moss-soil, animal bone, Syrian soil: 1 g each) were analyzed to assess the validity of the chemical separation and the AMS measurement. The 90 Sr measurements were conducted on the AMS system VERA combined with the Ion Laser InterAction Mass Spectrometry (ILIAMS) setup at the University of Vienna, which has excellent isobaric separation performance. The isobaric interference of 90 Zr in the 90 Sr AMS was first largely removed by chemical separation. The separation factor of Zr in two-step column chromatography with Sr resin and anion exchange resin was 10 6 . The 90 Zr remaining in the sample was effectively suppressed by ILIAMS. This procedure achieved a limit of detection <0.1 mBq in the 90 Sr AMS, which is lower than typical β-ray detection. The agreement between AMS measurements and nominal values for the 90 Sr concentrations of IAEA samples indicated that the new highly-sensitive 90 Sr analysis in the environmental samples with AMS is reliable.