Vienna Environmental Research Accelerator Research Articles

Cosmic rays, radiocarbon and the beginning of high-energy particle physics: Marietta Blau and the “disintegration stars”

Abstract This brief review describes the discovery of cosmic rays by Victor Hess from the Vienna Radium Institute and the later contribution of Marietta Blau through her observation of “disintegration stars” in photographic emulsion plates exposed to cosmic-ray bombardment. Marietta Blau, a nearly forgotten cosmic-ray pioneer from the Vienna Radium Institute, developed the nuclear emulsion technique for studying nuclear reactions, eventually discovering the disintegration of nuclei through high-energy cosmic rays. Blau survived the Holocaust by escaping to Mexico City from 1939 to 1944. Starting in 1948 at Columbia University, later as a staff member of Brookhaven National Laboratory and then University of Miami, she performed fundamental and original research with nuclear emulsions exposed to 3-GeV protons at the Brookhaven Cosmotron and to 6-GeV protons at the Berkeley Bevatron. Blau returned to Vienna in 1960, where at the Radium Institute a classical β-decay counting facility for radiocarbon dating had been installed, which was finally superseded by the Vienna Environmental Research Accelerator (VERA), a modern versatile accelerator mass spectrometry facility.

Detection of 135Cs &137Cs in environmental samples by AMS

The detection of low abundances of 135Cs in environmental samples is of significant interest in different fields of environmental sciences, especially in combination with its shorter-lived sister isotope 137Cs. The method of Ion–Laser InterAction Mass Spectrometry (ILIAMS) for barium separation at the Vienna Environmental Research Accelerator (VERA) was investigated and further improved for low abundance cesium detection. The difluorides BaF2− and CsF2− differ in their electron detachment energies and make isobar suppression with ILIAMS by more than 7 orders of magnitude possible. By this method, samples with ratios down to the order of 135,137Cs/133Cs ≈10−11 are measurable and the 135Cs/137Cs ratios of first environmental samples were determined by AMS.

Relative formation probabilities for fluoride and oxyfluoride anions of U, Np, Pu and Am in accelerator mass spectrometry measurements at VERA

Fluoride molecular anions have emerged as a potential alternative to oxides for the analysis of actinides in AMS. Research at the Vienna Environmental Research Accelerator (VERA) has focused on mixing samples prepared in an Fe2O3 matrix with PbF2 for in situ fluoridation during the sputter process. The relative formation probabilities for a range of (oxy-)fluoride molecular anions of uranium, neptunium, plutonium, and americium have been found to be characteristic for each of the actinides investigated. These data can help to identify isobaric interference for the mentioned actinides. A first application is monitoring of the 236U co-production with 236Np during Th irradiation. Extracting these actinides in the form of tetrafluoride anions allows the suppression of U by an order of magnitude relative to Np.

Developing Accelerator Mass Spectrometry Capabilities for Anthropogenic Radionuclide Analysis to Extend the Set of Oceanographic Tracers

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.

Highly sensitive 26Al measurements by Ion-Laser-InterAction Mass Spectrometry

The method of Ion-Laser InterAction Mass Spectrometry (ILIAMS) offers new options for the determination of 26Al by Accelerator Mass Spectrometry (AMS) and improves the sensitivity and efficiency for the detection of this isotope in artificial and environmental samples. In ILIAMS, a laser is overlapped with the ion beam during its passage through a radiofrequency quadrupole ion cooler. Those ions with electron affinity lower than the energy of the photons are selectively neutralized in a photodetachment process. Because the electron affinity of MgO is lower than that of AlO, ILIAMS can suppress the isobar 26Mg by 14 orders of magnitude. No further isobar suppression on the high-energy side of the spectrometer is necessary, so that the more prolific AlO− beam can now also be used at facilities with terminal voltages < 5 MV. At the 3 MV Vienna Environmental Research Accelerator (VERA) routine 26Al AMS measurements assisted by ILIAMS are performed utilizing AlO− extracted from the ion source and charge states 2+ and 3+ for the Al ions after the accelerator on the high-energy side of the spectrometer. The most efficient generation of AlO− currents (in the range of several μA) is realized when mixing the Al2O3 sample material with Fe powder. Blank materials are measured down to 26Al/27Al ratios of 5⋅10−16. The efficiency relative to the use of Al− extraction is improved typically by a factor 3–5 and thus the new method is useful for measurements with highest sensitivity and down to very low 26Al/27Al ratios.

Comparison of methods for the detection of 10Be with AMS and a new approach based on a silicon nitride foil stack

Natural 10Be (t1/2 = 1.387 ± 0.012 Ma) is produced by cosmic rays and is present on Earth's surface only at ultratrace concentrations (typically 104 to 1010 atoms/g). Its cosmogenic origin makes it an important tracer for many applications in Earth and environmental sciences. An improved accelerator mass spectrometry (AMS) method has been developed at the Vienna Environmental Research Accelerator (VERA) at the University of Vienna to detect the long-lived radionuclide 10Be and separate it from its isobar 10B. Recently installed and projected AMS facilities mainly apply a degrader foil followed by an electrostatic or magnetic separator to remove 10B from the ion beam. This provides the highest suppression of 10B, but suffers from significant transmission losses of 10Be ions. The new technique described here achieves comparable 10B suppression with a passive absorber, consisting of a stack of silicon nitride foils. Compared to a gas absorber, the smaller energy straggling in foils allows separation at lower energies. For a tandem accelerator operated at 3 MV, the charge state 2 + instead of 3 + can be used, with a stripping yield as high as 55%. This way, a high overall efficiency is gained. The setup is simple to operate, and provides good precision and accuracy. We compare this new approach with other methods used at VERA and at other AMS facilities. The foil stack setup was fully characterized with artificial samples from chemically and isotopically well-defined reagents, and is now routinely applied to real samples in various research projects at VERA. The new method is straightforward to be implemented, and was already adopted at another AMS facility with higher terminal voltage, the potential use at tandem accelerators with lower terminal voltage is under exploration.

36Cl in a new light: AMS measurements assisted by ion-laser interaction

The experimental setup at the Vienna Environmental Research Accelerator (VERA) was extended with an ion beam cooler and a 18 W laser to perform Ion-Laser InterAction Mass Spectrometry (ILIAMS). Gas collisions of the decelerated negative ion beam with He buffer gas inside a radio-frequency quadrupole slow down the ions, which facilitates element selective photodetachment to remove isobaric interferences. Here we present the first successful implementation of a suppression of the isobar of 36Cl via laser-photodetachment into an AMS measurement. Whereas conventional AMS measurements require separation of the isobar 36S at high beam energy, ILIAMS takes advantage of the higher electron affinities of Cl− (3.6 eV) compared to S− (2.1 eV). Using 532 nm photons (Eph = 2.3 eV) the isobar 36S is suppressed by 10 orders of magnitude. A high transmission of the Cl− beam through the ion cooler (up to 80%) and a quantitative suppression of the isobaric interference allows for competitive measurements at low accelerator voltages and with lower charge states. This results in high yields for 36Cl transport to the detector. The ILIAMS system is stable over several days of beamtime and blank levels below 36Cl/Cl = 10−15 are reached. The accomplishment of a 36Cl AMS measurement at a final beam energy as low as 5.4 MeV with full separation of isobars and m/q interferences shows the potential of the new isobar suppression method to widen the capabilities of smaller and middle-sized AMS facilities.

Precise measurement of the thermal and stellar Fe54(n,γ)Fe55 cross sections via accelerator mass spectrometry

The detection of long-lived radionuclides through ultra-sensitive single atom counting via accelerator mass spectrometry (AMS) offers opportunities for precise measurements of neutron capture cross sections, e.g. for nuclear astrophysics. The technique represents a truly complementary approach, completely independent of previous experimental methods. The potential of this technique is highlighted at the example of the $^{54}$Fe($n, \gamma$)$^{55}$Fe reaction. Following a series of irradiations with neutrons from cold and thermal to keV energies, the produced long-lived $^{55}$Fe nuclei ($t_{1/2}=2.744(9)$ yr) were analyzed at the Vienna Environmental Research Accelerator (VERA). A reproducibility of about 1% could be achieved for the detection of $^{55}$Fe, yielding cross section uncertainties of less than 3%. Thus, the new data can serve as anchor points to time-of-flight experiments. We report significantly improved neutron capture cross sections at thermal energy ($\sigma_{th}=2.30\pm0.07$ b) as well as for a quasi-Maxwellian spectrum of $kT=25$ keV ($\sigma=30.3\pm1.2$ mb) and for $E_n=481\pm53$ keV ($\sigma= 6.01\pm0.23$ mb). The new experimental cross sections have been used to deduce improved Maxwellian average cross sections in the temperature regime of the common $s$-process scenarios. The astrophysical impact is discussed using stellar models for low-mass AGB stars.

D-REAMS: A New Compact AMS System for Radiocarbon Measurements at the Weizmann Institute of Science, Rehovot, Israel

AbstractThe Dangoor REsearch Accelerator Mass Spectrometer (D-REAMS) is a dedicated carbon-only AMS system, built by National Electrostatics Corporation (NEC). It is based on the 1.5SDH Pelletron, operating at 460 keV. The machine was installed at the Weizmann Institute of Science, Rehovot, Israel, in January–February 2013, and passed the acceptance test on March 2013. Since then, over 4500 samples have been successfully measured. Here, we present the results of an intercomparison experiment, done in collaboration with the Vienna Environmental Research Accelerator (VERA), and some typical operation parameters and measurement values of the new AMS system.

Selective laser photodetachment of intense atomic and molecular negative ion beams with the ILIAS RFQ ion beam cooler

The Ion Laser InterAction Setup (ILIAS) project at the University of Vienna aims at the exploration of negative ion beam filtering by selective laser photodetachment for applications in accelerator mass spectrometry (AMS). A gas-filled radio frequency quadrupole (RFQ) is used to decelerate and cool negative atomic and molecular ion beams with intensities of up to several hundred nA, and overlap them collinearly with a continuous wave (cw) laser beam. Ion-laser interaction times ranging from 500 μs to several ms allow for highly efficient, selective photodetachment depletion of disturbing ion species within these beams. The elemental selectivity of this technique is based on the differences in electron affinities, and therefore does not depend on relative differences in atomic numbers. It may therefore provide sufficient isobar suppression for new trace isotopes, which are not accessible with existing AMS techniques.The ILIAS RFQ cooler was characterized at a purpose-built test bench with respect to ion beam transmission, ion cooling capabilities and ion residence times as a function of injected ion current to assess its suitability for future AMS use. A 63Cu− test beam of 600nA was photodetached with more than 99.999% efficiency with a 532nm laser at 10.8 W power. At the same time, ions of interest having electron affinities higher than the photon energy passed the cooler unaffected. Total ion losses were thus found to be below 50% of the sputter source output. Finally, first photodetachment experiments in connection with 26Al detection demonstrated selective isobar suppression of MgO− vs. AlO− by more than 4 orders of magnitude.Currently, the RFQ cooler is moved to a new injector beamline at the Vienna Environmental Research Accelerator (VERA) for first applications of this novel technique at a state-of-the-art AMS facility.

Forefoot diseases in art

Silverpoint drawings from the Renaissance are among the most precious and rarest treasures of graphical art. Our research group is particularly interested in the analysis of silverpoint drawings by Albrecht Dürer (1471–1528). A very sensitive and non-destructive analytical method, either spatially resolved synchrotron-radiation induced X-ray fluorescence (SY-XRF) or proton-induced X-ray emission (PIXE), is needed to determine the chemical composition of the very faint silver marks on such drawings. Dürer drawings from the collection of the Albertina, Vienna, were analyzed to amend existing data on Dürer drawings. For this purpose an external-beam PIXE setup was installed at the Vienna Environmental Research Accelerator (VERA). It allows to analyze a spot of ∼0.15 mm on the object in air with 3 MeV protons, and to detect the emitted X-rays that are characteristic for the chemical composition with very good sensitivity and without harming the precious objects. After successful measurements on artificial test samples, four original silverpoint drawings were investigated: two portraits from Albrecht Dürer’s very early period (self-portrait and portrait of his father) and two drawings from Dürer’s sketch book of his travel to the Netherlands 1520/21.

Using the nuclear activation AMS method for determining chlorine in solids at ppb-levels and below

Neutron activation analysis using decay counting of the activated element is a well-established method in elemental analysis. However, for chlorine there is a better alternative to measuring decay of the short-lived activation product chlorine-38 (t1/2=37.24min) – accelerator mass spectrometry (AMS) of 36Cl: the relatively high neutron capture cross section of chlorine-35 for thermal neutrons (43.7b) and combined the AMS technique for chlorine-36 (t1/2=301ka) allow for determination of chlorine down to ppb-levels using practical sample sizes and common exposure durations. The combination of neutron activation and AMS can be employed for a few other elements (nitrogen, thorium, and uranium) as well.For bulk solid samples an advantage of the method is that lab contamination can be rendered irrelevant. The chlorine-35 in the sample is activated to chlorine-36, and surface chlorine can be removed after the irradiation. Subsequent laboratory contamination, however, will not carry a prominent chlorine-36 signature. After sample dissolution and addition of sufficient amounts of stable chlorine carrier the produced chlorine-36 and thus the original chlorine-35 of the sample can be determined using AMS.We have developed and applied the method for analysis of chlorine in steel samples. The chlorine content of steel is of interest to nuclear industry, precisely because of above mentioned high neutron capture cross section for chlorine-35, which leads to accumulation of chlorine-36 as long-term nuclear waste. The samples were irradiated at the TRIGA Mark II reactor of the Atominstitut in Vienna and the 36Cl-AMS setup at the Vienna Environmental Research Accelerator (VERA) was used for 36Cl/Cl analysis.

Accelerator Mass Spectrometry of Actinides in Ground- and Seawater: An Innovative Method Allowing for the Simultaneous Analysis of U, Np, Pu, Am, and Cm Isotopes below ppq Levels.

(236)U, (237)Np, and Pu isotopes and (243)Am were determined in ground- and seawater samples at levels below ppq (fg/g) with a maximum sample size of 250 g. Such high sensitivity was possible by using accelerator mass spectrometry (AMS) at the Vienna Environmental Research Accelerator (VERA) with extreme selectivity and recently improved efficiency and a significantly simplified separation chemistry. The use of nonisotopic tracers was investigated in order to allow for the determination of (237)Np and (243)Am, for which isotopic tracers either are rarely available or suffer from various isobaric mass interferences. In the present study, actinides were concentrated from the sample matrix via iron hydroxide coprecipitation and measured sequentially without previous chemical separation from each other. The analytical method was validated by the analysis of the Reference Material IAEA 443 and was applied to groundwater samples from the Colloid Formation and Migration (CFM) project at the deep underground rock laboratory of the Grimsel Test Site (GTS) and to natural water samples affected solely by global fallout. While the precision of the presented analytical method is somewhat limited by the use of nonisotopic spikes, the sensitivity allows for the determination of ∼10(5) atoms in a sample. This provides, e.g., the capability to study the long-term release and retention of actinide tracers in field experiments as well as the transport of actinides in a variety of environmental systems by tracing contamination from global fallout.

Isobar separation of 93Zr and 93Nb at 24 MeV with a new multi-anode ionization chamber

93Zr with a half-life of 1.6Ma is produced with high yield in nuclear fission, and thus should be present as a natural or anthropogenic trace isotope in all compartments of the general environment. Sensitive measurements of this isotope would immediately find numerous applications, however, its detection at sufficiently low levels has not yet been achieved. AMS measurements of 93Zr suffer from the interference of the stable isobar 93Nb. At the Vienna Environmental Research Accelerator VERA a new multi-anode ionization chamber was built. It is optimized for isobar separation in the medium mass range and is based on the experience from AMS experiments of 36Cl at our 3-MV tandem accelerator facility. The design provides high flexibility in anode configuration and detector geometry. After validating the excellent energy resolution of the detector with 36S, it was recently used to study iron–nickel and zirconium–niobium–molybdenum isobar separation. To our surprise, the separation of 94Zr (Z=40) from 94Mo (Z=42) was found to be much better than that of 58Fe (Z=26) from 58Ni (Z=28), despite the significantly larger ΔZ/Z of the latter pair. This clearly contradicts results from SRIM-simulations and suggests that differences in the stopping behavior may unexpectedly favor identification of 93Zr. At 24MeV particle energy, a 93Nb (Z=41) suppression factor of 1000 is expected based on a synthetic 93Zr spectrum obtained by interpolation between experimental spectra from the two neighboring stable isotopes 92Zr and 94Zr. Assuming realistic numbers for chemical niobium reduction, a detection level of 93Zr/Zr below 10−9 seems feasible.

Interlaboratory study of the ion source memory effect in 36Cl accelerator mass spectrometry

Understanding and minimization of contaminations in the ion source due to cross-contamination and long-term memory effect is one of the key issues for accurate accelerator mass spectrometry (AMS) measurements of volatile elements. The focus of this work is on the investigation of the long-term memory effect for the volatile element chlorine, and the minimization of this effect in the ion source of the Dresden accelerator mass spectrometry facility (DREAMS). For this purpose, one of the two original HVE ion sources at the DREAMS facility was modified, allowing the use of larger sample holders having individual target apertures. Additionally, a more open geometry was used to improve the vacuum level. To evaluate this improvement in comparison to other up-to-date ion sources, an interlaboratory comparison had been initiated. The long-term memory effect of the four Cs sputter ion sources at DREAMS (two sources: original and modified), ASTER (Accélérateur pour les Sciences de la Terre, Environnement, Risques) and VERA (Vienna Environmental Research Accelerator) had been investigated by measuring samples of natural 35Cl/37Cl-ratio and samples highly-enriched in 35Cl (35Cl/37Cl∼999). Besides investigating and comparing the individual levels of long-term memory, recovery time constants could be calculated. The tests show that all four sources suffer from long-term memory, but the modified DREAMS ion source showed the lowest level of contamination. The recovery times of the four ion sources were widely spread between 61 and 1390s, where the modified DREAMS ion source with values between 156 and 262s showed the fastest recovery in 80% of the measurements.

AMS of the Minor Plutonium Isotopes

VERA, the Vienna Environmental Research Accelerator, is especially equipped for the measurement of actinides, and performs a growing number of measurements on environmental samples. While AMS is not the optimum method for each particular plutonium isotope, the possibility to measure 239Pu, 240Pu, 241Pu, 242Pu and 244Pu on the same AMS sputter target is a great simplification. We have obtained a first result on the global fallout value of 244Pu/239Pu=(5.7±1.0)×10−5 based on soil samples from Salzburg prefecture, Austria. Furthermore, we suggest using the 242Pu/240Pu ratio as an estimate of the initial 241Pu/239Pu ratio, which allows dating of the time of irradiation based solely on Pu isotopes. We have checked the validity of this estimate using literature data, simulations, and environmental samples from soil from the Salzburg prefecture (Austria), from the shut down Garigliano Nuclear Power Plant (Sessa Aurunca, Italy) and from the Irish Sea near the Sellafield nuclear facility. The maximum deviation of the estimated dates from the expected ages is 6years, while relative dating of material from the same source seems to be possible with a precision of less than 2years. Additional information carried by the minor plutonium isotopes may allow further improvements of the precision of the method.

The Age of Olfactory Bulb Neurons in Humans

Continuous turnover of neurons in the olfactory bulb is implicated in several key aspects of olfaction. There is a dramatic decline postnatally in the number of migratory neuroblasts en route to the olfactory bulb in humans, and it has been unclear to what extent the small number of neuroblasts at later stages contributes new neurons to the olfactory bulb. We have assessed the age of olfactory bulb neurons in humans by measuring the levels of nuclear bomb test-derived (14)C in genomic DNA. We report that (14)C concentrations correspond to the atmospheric levels at the time of birth of the individuals, establishing that there is very limited, if any, postnatal neurogenesis in the human olfactory bulb. This identifies a fundamental difference in the plasticity of the human brain compared to other mammals.

AMS of 36Cl with the VERA 3 MV tandem accelerator

Recent progress with compact ionization chambers has opened new possibilities for isobar suppression in accelerator mass spectrometry (AMS). Separation of 36Cl (t1/2=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.

AMS Applications in Nuclear Astrophysics: New Results for 13C(n,γ) 14C and 14N(n,p) 14C

AbstractThe technique of accelerator mass spectrometry (AMS) offers a complementary tool for studying long-lived radionuclides in nuclear astrophysics: (1) as a tool for investigating nucleosynthesis in the laboratory; and (2) via a direct search of live long-lived radionuclides in terrestrial archives as signatures of recent nearby supernova-events. A key ingredient to our understanding of nucleosynthesis is accurate cross-section data. AMS was applied for measurements of the neutron-induced cross sections 13C(n,γ) and 14N(n,p), both leading to the long-lived radionuclide 14C. Solid samples were irradiated at Karlsruhe Institute of Technology with neutrons closely resembling a Maxwell–Boltzmann distribution for kT = 25 keV, and with neutrons of energies between 123 and 178 keV. After neutron activation the amount of 14C nuclides in the samples was measured by AMS at the VERA (Vienna Environmental Research Accelerator) facility. Both reactions, 13C(n,γ)14C and 14N(n,p)14C, act as neutron poisons in s-process nucleosynthesis. However, previous experimental data are discordant. The new data for both reactions tend to be slightly lower than previous measurements for the 25 keV Maxwell–Boltzmann energy distribution. For the higher neutron energies no previous data did exist for 13C(n,γ), but model calculations indicated a strong resonance structure between 100 and 300 keV which is confirmed by our results. Very limited information is available for 14N(n,p) at these energies. Our new data at 123 and 178 keV suggest lower cross sections than expected from previous experiments and data evaluations.

Ultrasensitive search for long-lived superheavy nuclides in the mass rangeA=288toA=300in natural Pt, Pb, and Bi

Theoretical models of superheavy elements (SHEs) predict a region of increased stability around the proton and neutron shell closures of $Z$ $=$ 114 and $N$ $=$ 184. Therefore a sensitive search for nuclides in the mass range from $A$ $=$ 288 to $A$ $=$ 300 was performed in natural platinum, lead, and bismuth, covering long-lived isotopes of Eka-Pt (Ds, $Z$ $=$ 110), Eka-Pb ($Z$ $=$ 114), and Eka-Bi ($Z$ $=$ 115). Measurements with accelerator mass spectrometry (AMS) at the Vienna Environmental Research Accelerator (VERA) established upper limits for these SHE isotopes in Pt, Pb, and Bi with abundances of 2\ifmmode\times\else\texttimes\fi{}10${}^{\ensuremath{-}15}$, 5\ifmmode\times\else\texttimes\fi{}10${}^{\ensuremath{-}14}$, and 5\ifmmode\times\else\texttimes\fi{}10${}^{\ensuremath{-}13}$, respectively. These results complement earlier searches for SHEs with AMS at VERA in natural thorium and gold, which now amounts to a total number of 37 SHE nuclides having been explored with AMS. In none of our measurements was evidence found for the existence of SHEs in nature at the reported sensitivity level. Even though a few events were observed in the window for $^{293}\mathrm{Ek}$a-Bi, a particularly strong pileup background did not allow a definite SHE isotope identification. The present result sets limits on nuclides around the center of the island of stability, essentially ruling out the existence of SHE nuclides with half-lives longer than \ensuremath{\sim}150 million years.