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Abstract

Many archaeometrical studies aim at identifying the provenance of various archaeological finds. For a large group of objects, e.g. for stone artefacts, the chemical composition might be characteristic for the supposed geological source. In the last 20 years, several projects on different scales have been launched, based on the non-destructive prompt-gamma activation analysis at the Budapest PGAA laboratory. Depending on the type of the raw material (such as obsidian, flint, radiolarite or metamorphic rocks), the success of the various neutron-based studies can be expected at different levels. In this paper, we demonstrate the potentials of the mostly applied neutron-based techniques through case studies.

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... Additionally, both methods can be considered nondestructive, i.e., no visible or invisible modification on the irradiated objects is observed after measurements. Several works on similar pre-historic and historical lithic objects have been reported using these methods for the determination of bulk composition [9][10][11][12][13][14][15], and for the analysis of the surface composition of the artefacts [10,11,[16][17][18][19][20][21]. ...
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... The PGAA facility from BNC had been extensively used to characterize a broad range of archaeological finds, such as lithic materials (Bernardini et al., 2014;Bir o & Kasztovszky, 2018;Kasztovszky, et al., 2008), ceramics (Palamara et al., 2016;Szil agyi et al., 2012), or metallic artefacts (Kasztovszky, Panczyk, et al., 2005;Kiss et al., 2015). The method was also applied to quantify the major constituents and some trace elements of ancient glass (Bugoi, Talmaţchi, et al., 2021;Bugoi, Ţarlea, et al., 2021;Constantinescu et al., 2018;Kasztovszky, Kunicki-Goldfinger, et al., 2005;Moropoulou et al., 2016;Zacharias et al., 2018) and obsidian samples (Kasztovszky et al., 2019). ...
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The Budapest Research Reactor’s Prompt Gamma Activation Analysis (PGAA) and Neutron-Induced Prompt gamma Spectroscopy (NIPS) facilities were significantly upgraded during the last few years. The higher neutron flux, achieved by the partial replacement and realignment of the neutron guides, made feasible the automation and specialization of the two experimental stations. A new neutron flux monitor, computer-controlled beam shutters and a low-level counting chamber have been put into operation to assist with in-beam activation experiments. An automatic sample changer has been installed at the PGAA station, while the NIPS station was redesigned and upgraded with a Compton suppressor to use for the non-destructive analysis of bulky samples. In the near future the latter setup will be completed with a neutron tomograph and a moving table, to turn it into a Neutron Radiography/Tomography-driven PGAA equipment.
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Prompt Gamma Activation Analysis has successfully been applied to provenance research on Carpathian obsidians. The effectiveness of PGAA and a portable XRF device in discriminations of Carpathian, Lipari, Sardinia and Melos origin obsidians was compared on 75 representative geological samples obtained from the Lihotheca Collection of the Hungarian National Museum. Bivariate analyses and Principal Component Analysis have been made based on the individual PGAA and XRF data, as well as on the combination of both data types. Instrumental Neutron Activation Analysis was also applied on a group of 17 samples. The advantages and disadvantages of each method are discussed to determine the best possible way of investigations to fingerprint and characterize long-distance trade items with minimal damage to the samples.
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Using a series of geochemical data from obsidian samples taken from unmodified rocks and prehistoric sites, we investigated the provenance of some obsidian artifacts found in South Korea. By using LA-ICP-MS and SHRIMP methods, we analyzed rare earth elements (REEs) and lead (Pb) isotopic ratios of obsidian samples from the North Korean side of the Baekdusan Mountain (NK) and artifacts from a Neolithic site in Gadeokdo, southeast coast of South Korea (BG). Published accounts on the elemental correlation of previously analyzed samples were re-examined in consideration of their geological compatibility. It appears that the prehistoric artifacts from the middle to northern part of South Korea have a genetic relationship with obsidians from the Baekdusan area, whereas those of the southern part are related to Kyushu, Japan. REE patterns of the BG and the NK samples demonstrate a prominent contrast between them, suggesting their different provenances. Presumably, the BG obsidians are related to the volcanic rocks of Kyushu. Given that Pb isotopic ratios are indicative of the relative contribution of crust versus mantle component to the volcanic magma, they indicate the addition of a crustal component to the volcanic magma for the Baekdusan volcanic rocks and the NK obsidians. The Kyushu volcanics and the BG obsidians have a relative affinity to the mantle component. The geochemical approach adopted in the current research may be regarded as an accurate and effective means to discriminate and isolate obsidian sources, helpful for provenance and other archaeological study of obsidian artifacts.
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Metabasic rocks, particularly greenschists, were very popular raw materials for making polished stone tools by prehistoric man in the Carpathian Basin. The major and trace element compositions of these objects are very helpful in determining the place of origin of the rocks. On the other hand, destruction of the complete object is usually not allowed during the analysis. In this paper we show an application of Prompt Gamma Activation Analyses (PGAA), a relatively new, non-destructive method for investigation of Neolithic stone tools. Twenty-four samples (in the form of greenschist and blueschist polished stone tools from Hungarian Neolithic collections and also greenschists and blueschist from outcrops) were investigated. The aim of this work was to establish a method for distinguishing the different types of greenschists occurring in the Carpathian Basin. PGAA gives reliable data for major and some trace elements of geochemical interest. According to our results, it is possible to distinguish blueschist from macroscopically similar greenschist polished stone tools by PGAA. Three macroscopically different types of greenschist samples form only two groups according to chemical composition, which implies only two different sources of greenschist raw material. We were able to identify one of them as rock from the outcrop of Felsocsatar (Penninic Unit of the Alps in western Hungary). The second source is not yet determined; it requires the study of samples from more outcrops. The investigation of ancient stone tools is only one example of the applicability of PGAA. The advantages of this method can also be exploited in other geochemical research areas.
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The obsidian sources of central Anatolia, the Aegean and central Europe have been studied in detail over the past 50 years. Various analytical techniques have been employed to discriminate artefacts from each of these and to reconstruct their zones of distribution. This paper presents a pXRF method that allows mass sampling of artefacts focusing on three neighbouring regions, particularly where these zones overlap. Successful discrimination of the obsidian source for products could be achieved using three-dimensional scatter plots of trace elements Rb–Sr–Zr. PXRF can thus be appreciated as a powerful tool in the region, enabling non-destructive on-site analyses in contexts where the export of artefacts is often difficult if not impossible. The ability to rapidly process large assemblages also has major implications for generating data-sets of sufficient resolution to transform archaeological interpretation.
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Applying thek 0 standardization method to prompt-gamma activation analysis (PGAA) offers similar benefits as in instrumental neutron activation analysis. It has been demonstrated that under constant flux conditionsk 0-factors obtained by normalizing to a titanium comparator, measured separately, yield consistent analytical sensitivity ratios. The ratio method has been generalized by using stoichiometric compounds for the determination ofk 0-factors. Since chlorine forms compounds with essentially everyelement and it also serves as a detector efficiency standard,k 0 values have been determined relative to chlorine as an internal standard for several analytically important elements in two reactor facilities: the thermal guided beam at the BRR in Budapest and the cold-neutron beams at the NBSR at NIST.
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A complete series of measurements was performed at the Budapest prompt gamma neutron activation analysis (PGAA) facility in order to determine the partial production cross sections of the most suitable neutron capture gamma rays for all naturally occurring elements, excluding noble gases. The values were determined directly, with internal standardisation using stoichiometric compounds and homogeneous mixtures (mainly water solutions) of known composition. A comparison with a recent measurement for 20 elements shows good agreement except for a few non-1/v cross sections. The new data are sufficiently accurate for quantitative multielement determinations in PGAA without the necessity of elemental standards.
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Recently, several archaeometrical projects have been started on the prehistoric collection of the Hungarian National Museum. Among the analytical methods applied, non-destructive prompt gamma activation analysis has a special importance. We have also tested the potential of this method on chipped stone tools, with the aim of determining their exact provenance. On the basis of major and trace element components, characterizations of stone tools and their raw materials—silicites (flint, chert, radiolarite and hornstone) as well as volcanites (felsitic porphyry and obsidian)—were performed. We discuss some important results concerning each group, as case studies. Compiling the data set of different PGAA analysis series, compositions of 110 samples are reported, including 76 archaeological pieces. In the future, we plan to extend the number of investigated objects in each class.
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HYPERMET PC is a user-friendly -ray spectrum analysis software package developed at Budapest, mainly for the purpose of prompt- neutron activation analysis (PGAA). The peak fitting algorithm is an improved version of the well-known HYPERMET code, and contains a partial peak-parameter calibration to describe peak shapes more accurately in the wide energy range typical for prompt- spectra. A nuclide identification routine has also been developed using a new PGAA library, shown in a parallel paper. The new module for quantitative PGAA includes all the features necessary to obtain concentration values for elements.
Prompt gamma activation analysis of some prehistoric stone tools from North-Western Romania
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Transcharpatian influences in the early Neolithic Poland. A case study of Kowalewko and Rudna Wielka sites
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Kabaciński, J., Sobkowiak-Tabaka, I., Kasztovszky, Zs, Pietrzak, S., Langer, J.J., Biró, K.T., Maróti, B., 2015. Transcharpatian influences in the early Neolithic Poland. A case study of Kowalewko and Rudna Wielka sites. Acta Archaeol. Carp. 50, 5-32.
A kárpáti obszidiánok osztályozása prompt gamma aktivációs analízis segítségével: geológiai és régészeti mintákra vonatkozó első eredmények (in Hungarian)
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Kasztovszky, Zs., Biró, K.T., 2004. A kárpáti obszidiánok osztályozása prompt gamma aktivációs analízis segítségével: geológiai és régészeti mintákra vonatkozó első eredmények (in Hungarian). Archeometria Műhely I (1), 9-15.
Előzetes eredmények a magyarországi nagynyomású metaofiolit anyagú csiszolt kőeszközök származási helyének pontosításához
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Váczi, B., Szakmány, Gy, Kasztovszky, Zs, Starnini, E., Nebiacolombo, F.A., 2017. Előzetes eredmények a magyarországi nagynyomású metaofiolit anyagú csiszolt kőeszközök származási helyének pontosításához. Archeometriai Műhely XIV (2), 69-84.
Kora-neolitikus radiolarit és obszidián kőeszközök vizsgálata prompt-gamma aktivációs analízissel
  • Zs Kasztovszky
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Kasztovszky, Zs, Težak-Greg, T., 2009. Kora-neolitikus radiolarit és obszidián kőeszközök vizsgálata prompt-gamma aktivációs analízissel. In: Gábor, Ilon (Ed.), Őskoros Kutatók 6. Összejövetele Konferencia Kötet, pp. 189-195 Szombathely. (in Hungarian).
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K.T. Biró, Z. Kasztovszky Journal of Archaeological Science: Reports 19 (2018) 669-673