Claudio Tuniz

Accelerator mass spectrometry: ultra-sensitive analysis for global science

Accelerator mass spectrometry (AMS) is the analytical technique of choice for the detection of long-lived radionuclides that cannot be practically analysed with decay counting or conventional mass spectrometry. AMS has been used for the analysis of 14 C, 10 Be, 36 Cl and other cosmogenic radionuclides in archaeology, geology and environmental science. In addition, the ultrasensitivity of AMS is being applied in biomedicine to study the exposure of human tissues to chemicals and biomolecules at attomole levels. AMS is also being considered for the detection of anthropogenic radionuclides, such as 129 I and 236 U, in environmental samples for the verification of the nuclear non- proliferation agreements. The state of the art of AMS is reviewed with examples from some recent applications. r 2001 Elsevier Science Ltd. All rights reserved.

Luminescence dating of rock art and past environments using mud-wasp nests in northern Australia

Mud-nesting wasps are found in all of the main biogeographical regions of the world, and construct nests that become petrified after abandonment. Nests built by mud-dauber and potter wasps in rock shelters in northern Australia, often overlie, and occasionally underlie, prehistoric rock paintings. Mud nests contain pollen, spores and phytoliths from which information about local palaeovegetation can be gleaned. Here we report a new application of optical dating, using optically stimulated luminescence (OSL), and accelerator mass spectrometry (AMS) 14C dating of pollen to determine the ages of mud-wasp nests associated with rock paintings in the Kimberley region of Western Australia,. Optical dating of quartz sand (including the analysis of individual grains) embedded in the mud of fossilized nests shows that some anthropomorphic paintings are more than 17,000 years old. Reconstructions of past local environments are also possible from the range of pollen and phytolith types identified. This approach should have widespread application to studies of rock-art dating and late Quaternary environmental change on continents where mud-wasps once lived and other sources of palaeoecological information are absent.

Measurement of 236U in environmental media

The long-lived uranium isotope 236U (T1/2=23.4 Ma) is produced by 235U neutron capture and builds up to high levels in nuclear fuel. It has been distributed in the environment as a result of nuclear activities including nuclear explosions, accidents at nuclear plants, dumping of nuclear waste and releases from nuclear facilities. 236U is a potentially useful tracer of irradiated uranium for nuclear safeguards or other applications, due to its virtual absence in natural samples (236U:238U ratio ∼10−10 in uranium ore). We have measured 236U in soil and sediment reference materials (IAEA 375, 135 and 300) by accelerator mass spectrometry (AMS). The AMS system on the ANTARES accelerator has been upgraded to make such measurements possible. The system, including sample preparation procedures, is described and the results discussed.

AMS at ANTARES – The first 10 years

Abstract The status and capabilities of the ANTARES AMS facility after 10 years are reviewed. The common AMS radioisotopes, 10 Be, 14 C, 26 Al, 36 Cl and 129 I, are routinely analysed. A capability for the detection of 236 U and other actinide isotopes has been developed. The measurement program includes support to Quaternary science projects at Australian universities and to ANSTO projects in global climate change and nuclear safeguards.

New optical and radiocarbon dates from Ngarrabullgan Cave, a Pleistocene archaeological site in Australia : implications for the comparability of time clocks and for the human colonization of Australia

The human settlement of Australia falls into that period where dating is hard because it is near or beyond the reliable limit of radiocarbon study; instead a range of luminescence methods are being turned to (such as thermoluminescence at Jinmium: December 1996 ANTIQUITY). Ngarrabullgan Cave, a rock-shelter in Queensland, now offers a good suite of radiocarbon determinations which match well a pair of optically stimulated luminescence (OSL) dates - encouraging sign that OSL determinations can be relied on.

Beeswax as dental filling on a Neolithic human tooth

Evidence of prehistoric dentistry has been limited to a few cases, the most ancient dating back to the Neolithic. Here we report a 6500-year-old human mandible from Slovenia whose left canine crown bears the traces of a filling with beeswax. The use of different analytical techniques, including synchrotron radiation computed micro-tomography (micro-CT), Accelerator Mass Spectrometry (AMS) radiocarbon dating, Infrared (IR) Spectroscopy and Scanning Electron Microscopy (SEM), has shown that the exposed area of dentine resulting from occlusal wear and the upper part of a vertical crack affecting enamel and dentin tissues were filled with beeswax shortly before or after the individual’s death. If the filling was done when the person was still alive, the intervention was likely aimed to relieve tooth sensitivity derived from either exposed dentine and/or the pain resulting from chewing on a cracked tooth: this would provide the earliest known direct evidence of therapeutic-palliative dental filling.

Accelerator mass spectrometry analyses of environmental radionuclides: sensitivity, precision and standardisation

Accelerator Mass Spectrometry (AMS) is the analytical technique of choice for the detection of long-lived radionuclides which cannot be practically analysed with decay counting or conventional mass spectrometry. AMS allows an isotopic sensitivity as low as one part in 10(15) for 14C (5.73 ka), 10Be (1.6 Ma), 26Al (720 ka), 36Cl (301 ka), 41Ca (104 ka), 129I (16 Ma) and other long-lived radionuclides occurring in nature at ultra-trace levels. These radionuclides can be used as tracers and chronometers in many disciplines: geology, archaeology, astrophysics, biomedicine and materials science. Low-level decay counting techniques have been developed in the last 40-50 years to detect the concentration of cosmogenic, radiogenic and anthropogenic radionuclides in a variety of specimens. Radioactivity measurements for long-lived radionuclides are made difficult by low counting rates and in some cases the need for complicated radiochemistry procedures and efficient detectors of soft beta-particles and low energy x-rays. The sensitivity of AMS is unaffected by the half-life of the isotope being measured, since the atoms not the radiations that result from their decay, are counted directly. Hence, the efficiency of AMS in the detection of long-lived radionuclides is 10(6)-10(9) times higher than decay counting and the size of the sample required for analysis is reduced accordingly. For example, 14C is being analysed in samples containing as little as 20 microg carbon. There is also a world-wide effort to use AMS for the analysis of rare nuclides of heavy mass, such as actinides, with important applications in safeguards and nuclear waste disposal. Finally, AMS microprobes are being developed for the in-situ analysis of stable isotopes in geological samples, semiconductors and other materials. Unfortunately, the use of AMS is limited by the expensive accelerator technology required, but there are several attempts to develop compact AMS spectrometers at low (< or = 0.5 MV) terminal voltages. Recent advances in AMS will be reviewed with highlights from the scientific programs at Lucas Heights and other AMS centres.

Micro-biomechanics of the Kebara 2 hyoid and its implications for speech in Neanderthals.

The description of a Neanderthal hyoid from Kebara Cave (Israel) in 1989 fuelled scientific debate on the evolution of speech and complex language. Gross anatomy of the Kebara 2 hyoid differs little from that of modern humans. However, whether Homo neanderthalensis could use speech or complex language remains controversial. Similarity in overall shape does not necessarily demonstrate that the Kebara 2 hyoid was used in the same way as that of Homo sapiens. The mechanical performance of whole bones is partly controlled by internal trabecular geometries, regulated by bone-remodelling in response to the forces applied. Here we show that the Neanderthal and modern human hyoids also present very similar internal architectures and micro-biomechanical behaviours. Our study incorporates detailed analysis of histology, meticulous reconstruction of musculature, and computational biomechanical analysis with models incorporating internal micro-geometry. Because internal architecture reflects the loadings to which a bone is routinely subjected, our findings are consistent with a capacity for speech in the Neanderthals.

Measurements of the 14CO2 bomb pulse in firn and ice at Law Dome, Antarctica

Abstract 14CO2 produced in the atmosphere by nuclear weapons testing in the 1960s is now incorporated in the air bubbles of Antarctic ice. The high atmospheric radiocarbon growth rates through the period of tests and subsequent decline provide a unique and independent test for the smoothing of atmospheric CO2 signals due to firn diffusion and bubble close off. The level of smoothing quantifies the time resolution with which atmospheric trace gas histories can be reconstructed from ice cores. In this paper, the methodologies for the preparation and AMS measurements of ice core and firn 14CO2 from high accumulation sites at Law Dome are detailed. The results are compared with predictions of a numerical model incorporating firn air diffusion and bubble close-off. The sample sizes, precision of measurements and sources of contamination are discussed for both firn and ice samples.

Sherlock Holmes counts the atoms

Modern forensic science has to deal not only with homicides and other traditional crimes but also with more global threats such as smuggling of nuclear materials, clandestine production of weapons of mass destruction, stockpiling of illicit drugs by state-controlled groups and war crimes. Forensic applications have always benefited from the use of advanced analytical tools that can characterise materials found at crime scenes. In this paper we will discuss the use of accelerator mass spectrometry as an ultra sensitive tool for the crime labs of the third millennium.