Neutron Activation Analysis and Provenance Research in Archaeology
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Measurement Science and Technology Related content - Physical studies of archaeological Neutron activation analysis and provenance materials Z Goffer research in archaeology - PIXE studies of turquoise artefacts from Salado Platform Mound sites inArizona Jangsuk Kim, Arleyn W Simon, Vincent To cite this article: Michael D Glascock and Hector Neff 2003 Meas. Sci. Technol. 14 1516 Ripoche et al. - Uses of neutrons in engineering and technology J. Walker View the article online for updates and enhancements. Recent citations - Destructive and nondestructive geochemical analysis of vesicular basalt from bedrock outcrops in the Salt-Gila Basin, Arizona: Evaluating the potential of nondestructive portable X-ray fluorescence spectroscopy for archaeological provenance analyses Craig Fertelmes and Michael D. Glascock - Late Pleistocene Lithic Procurement and Geochemical Characterization of the Cerro Kaskio Obsidian Source in South-western Bolivia J. M. Capriles et al - Iron oxide geochemistry in the Great Lakes Region (North America): Implications for ochre provenance studies Brandi Lee MacDonald et al This content was downloaded from IP address 128.194.172.218 on 10/07/2018 at 17:46 INSTITUTE OF PHYSICS PUBLISHING MEASUREMENT SCIENCE AND TECHNOLOGY Meas.Sci.Technol. 14 (2003) 1516–1526 PII: S0957-0233(03)56714-5 Neutron activation analysis and provenance research in archaeology Michael D Glascock1,3 and Hector Neff2 1 Research Reactor Center, University of Missouri, Columbia, MO 65211, USA 2 Department of Anthropology, California State University, Long Beach, CA 90840, USA E-mail: [email protected] and [email protected] Received 27 November 2002, accepted for publication 7 April 2003 Published 29 July 2003 Online at stacks.iop.org/MST/14/1516 Abstract Neutron activation analysis is a powerful quantitative analytical technique with application in a broad range of disciplines such as agriculture, archaeology, geochemistry, health and human nutrition, environmental monitoring and semiconductor technology. Due to its excellent sensitivity, great accuracy and precision, and versatility, the technique is a suitable method for analysing many different types of samples. Archaeologists, in particular, have made extensive use of neutron activation analysis for the purpose of characterizing archaeological materials and determining their provenance. This paper presents a brief history of the technique and its application to archaeology, describes the physics behind the analytical method, and explains how the method is generally employed to determine the sources of archaeological materials. Keywords: neutron activation analysis, nuclear reactions, cross-sections, thermal neutrons, gamma-ray spectra, provenance, ceramics, clays, obsidian, chert, multivariate statistics 1. Introduction mass spectrometry (ICP-MS) on liquid samples, NAA offers sensitivities that are superior to those possible by all other The application of chemical analytical methods to archaeo- analytical methods. Moreover, the accuracy and precision logical materials in support of provenance research has grown of the technique are such that NAA is still one of the rapidly over the past few decades. Provenance research en- primary methods employed by the National Institute of tails the use of compositional profiles of artefacts and source Standards and Technology to certify the concentrations of materials to trace individual artefacts from their find spot to elements in standard reference materials. Applications of their place of origin. The information obtained is used by NAA are by no means limited to archaeology, but include a archaeologists to investigate questions regarding the location broad range of disciplines such as agriculture, geochemistry, of prehistoric production areas, the identification of routes of health and human nutrition, environmental monitoring and trade and exchange of raw materials and artefacts, and the mo- semiconductors. bility patterns of prehistoric peoples. Although a number of The NAA technique involves the irradiation of a sample techniques have been employed to characterize archaeologi- by neutrons to make the sample radioactive. After irradiation, cal materials, the analytical method with one of the longest the gamma rays emitted from the radioactive sample are and most successful histories of application for provenance measured to determine the amounts of different elements research has been neutron activation analysis (NAA). present in the sample. As a result, NAA has a number Neutron activation analysis isasensitive technique useful of advantages over most other analytical methods when for qualitative and quantitative multi-element analysis of investigating archaeological specimens. First, it is nearly free major, minor, and trace elements present in many sample of any matrix interference effects because the vast majority matrices. With the exception of inductively coupled plasma- of archaeological samples are transparent to the probe, the neutron, and the emitted analytical signal, the gamma ray. 3 http://www.missouri.edu/∼glascock/archlab.htm Second, because NAA can be applied instrumentally (without 0957-0233/03/091516+11$30.00 © 2003 IOP Publishing Ltd Printed in the UK 1516 Neutron activation analysis and provenance research in archaeology sample digestion or dissolution), there is little opportunity for Perlman and Asaro (1969) provided a description of the reagent or laboratory contamination. Third, the preparation standard-comparator method of NAA as applied to provenance of samples from most matrices (especially geological sample determination at the Lawrence Berkeley Laboratory (LBL). types) for analysis by NAA is extremely easy—in most Archaeologists turned more frequently to NAA during the instances a portion of the sample need only be weighed and 1970s and 1980s to determine the sources of pottery, obsidian, place in an appropriate container. In contrast, the difficulty chertand other materials (Hughes et al 1991, Kuleff and of achieving complete digestion of geological samples for Djingova 1990, Neff and Glascock 1995). The NAA analysis by ICP-MS can be challenging and the labour costs are laboratories at BNL and LBL were joined by laboratories at much greater. Finally, although nuclear reactors are becoming the University of Michigan, University of Toronto, Hebrew less available while ICP-MS instruments are becoming University, National Institute of Standards and Technology, more widely available, many reactors offer competitive low- University of Missouri, and a number of smaller university cost analyses on projects involving collaborative academic research reactors. By the early 1990s, NAA was regarded as research. the technique of choice for provenance research (Bishop et al This paper presents a brief history of NAA and its 1990, Gilmore 1991). application to archaeology, describes the physics behind the Although the late 1980s and 1990s, saw reactor NAA technique, and explains how the method is generally decommissioning and retirements of key personnel which employed to determine the provenance of archaeological concluded a number of the major programmes (i.e. BNL, materials. The finalsection presents a few examples of NAA LBL, the University of Toronto and Hebrew University), the applied to recent archaeological studies. demand for NAA has not decreased. Fortunately, although there are fewer places to perform NAA today, the remaining 2. A brief history programmes have been able to increase their capacity such that access to NAA is still readily available. The notion that nuclear reactions might be used for quantitative analysis first occurred to Georg Hevesy and Hilde Levy in 3. Theory 1936 when they exposed rare-earth salts to a naturally emitting Ra(Be) neutron source (Ehmann and Vance 1991). They found 3.1. Nuclearreactions that many of the rare-earth elements became highly radioactive Nuclear reactions occupy a central role in all methods of upon bombardment with neutrons,and the radiation emitted activation analysis. In a nuclear reaction, an incident particle from the different elements decreased according to different (e.g. neutron, proton or alpha particle) interacts with a target timeconstants. From this discovery, they recognized the nucleus either by scattering or by absorption. The diagram potential for identifying elements present in mixtures of shown in figure 1 illustrates a typical nuclear reaction involving samples through measurement of different radiations and half- absorption of the incident particle followed by the emission lives of the radioactive elements. of both particles and prompt gamma rays and by production The 1950s and 1960s saw the construction of nuclear of a radioactive nucleus. If the incident particle is a thermal reactors with neutron fluxes sufficient to allow sensitivities for neutron, a prompt particle is rarely emitted. If the reaction NAA at levels of interest to solving real analytical problems. involves an incident fast neutron or a charged particle, a prompt In addition, there were improvements in the sophistication particle is always emitted. In either case, prompt gamma rays and sensitivity of instrumentation used to make nuclear will always occur. The reaction can also be described by the measurements, and hundreds of experiments were performed expression to measure the basic nuclear parameters (i.e. reaction cross- a + A → [X] → b + B + Q (1) sections, half-lives, gamma-ray abundances and branching ratios) associated with nuclear reactions. or in shorthand notation A(a, b)B.Wherethesymbol