A NEW METHOD FOR THE DETERMINATION OF THE PROVENANCE OF WHITE MARBLES BY CHEMICAL ANALYSIS OF INCLUSION FLUIDS: THE MARBLES OF THE MAUSOLEUM OF BELEVI/TURKEY*

A new method is presented in this paper to pinpoint the origin of white marbles using the chemical analysis of fluids occurring as micro-inclusions in calcitic or dolomitic marbles. Beside the conventional methods usually applied for this purpose, the analyses of significant anions and cations in fluids extracted from white marbles were used to characterize different types of marbles. Using this new approach it is possible to distinguish different groups of marbles which cannot be separated isotopically. A case study was performed on the mausoleum of Belevi, close to Ephesus in Turkey, and the quarries in the area of the mausoleum. The marbles used for the architecture of the mausoleum cannot be distinguished isotopically but were split into two groups when using fluid inclusion analysis. The corresponding quarry for the high-quality marble (cella walls, columns etc.) turned out to be the Kentli Çiftliği quarry, which also supplied the marbles for the classical Artemision. According to the chemical and fluid data it can be shown, however, that neither the adjacent famous antique quarry of Belevi nor the underground mine of Kusini, some 5 km away from the mausoleum, are the sources for the marbles used for the construction or decoration of the mausoleum.     

CATHODOLUMINESCENCE OF WHITE MARBLES: AN OVERVIEW*

Identifying the source area of white marbles has long been a problem in archaeology. To address this problem, about 1000 samples from known Classical quarrying areas in Greece, Italy and Turkey were analysed using cathodoluminescence. Twenty-one cathodomicrofacies were recognized, each of which generally characterizes a given area. In cases where the cathodomicrofacies is common to more than one area, δ¹³C and δ¹⁸O signatures provide an effective complementary dataset which allows additional distinctions. Determination keys for the 21 cathodomicrofacies observed are proposed based upon their principal cathodoluminescence colour, and their stable isotopic signature.     

COMPOSITIONAL CHARACTERIZATION OF FRENCH LIMESTONE: A NEW TOOL FOR ART HISTORIANS*

Limestone from quarries known to medieval craftsmen and from the monuments they built and embellished, as well as from carvings now in museum collections, has been characterized by neutron activation analysis. Specimens from 38 quarries in the Lutetian and Jurassic limestone formations of France and from sculptures in American and French museums have been tested, and the results have been compiled in a data base to which art historians may refer when attempting to determine provenance for sculptures. Multivariate statistical analysis of concentration data shows stone from a particular quarry in the Paris basin to be compositionally homogeneous and distinguishable from other quarries in the same formation. The same approach to data related to quarries near the Burgundian abbey of Cluny finds general agreement between classifications based on compositional and on petrographic data, but the number of samples available for analysis at the time of writing was insufficient to achieve the finer distinctions reported for the Paris basin.     

A SCULPTURAL MARBLE OF PRIME QUALITY IN ANTIQUITY—THE DOLOMITIC MARBLE OF THE SIVEC MOUNTAINS IN MACEDONIA

This paper presents analytical data on a major occurrence of fine‐grained dolomitic marble in the Sivec Mountains, close to the city of Prilep in today's former Yugoslavian Republic of Macedonia. This is the first presentation of an analytical database of a large‐scale source of fine‐grained dolomitic marble, whose ancient use can be demonstrated by tool marks and archaeological evidence. Many traces of ancient mining have fallen victim to a big modern quarrying operation in this area, which for decades has produced high‐quality blocks of marble (‘Macedonian Carrara’) and exported them all over the world. A combination of different analytical methods is used to characterize the marbles and to present a database for investigating ancient artefacts made of fine‐grained dolomites. Petrographic investigations revealed the very homogeneous micro‐fabric of this marble, which is of high purity with very low silicate contamination and has a maximum grain‐size of 1 mm. In addition to analysis of the stable isotopes, trace element analyses of carbonate lattice elements (Mg, Fe, Mn and Sr) were performed. An alternative method, the analysis of the chemical composition of the inclusion fluids, was also employed. On the basis of these techniques, a multivariate discrimination analysis was performed, and a clear separation of the different dolomitic marbles (Thasos, Ephesos, Proconnesos and Karacasu) was obtained. Finds of artefacts of high artistic quality made from this dolomite prove the existence of a significant workshop in the neighbourhood of the Sivec quarries. Because of its vulnerability to weathering, this fine‐grained dolomitic marble was used preferentially for indoor applications. Sculptures of prime artistic quality made of Sivec marble have so far been found in several locations of the Republic of Macedonia.     

A PROVENANCE STUDY OF FRENCH LIMESTONE BASED ON VARIABLE SELECTION FROM COMPOSITIONAL PROFILES

The present study shows how multivariate analysis and variable selection techniques can be used in archaeological provenances studies to improve classification performances. Neutron activation analysis (NAA), in combination with stepwise linear discrimination analysis (SLDA) (capable of simultaneously performing variable selection and classification), was applied to differentiate among limestone samples from different quarries across the north of France based on their compositional fingerprint. A hierarchical classification approach was followed, aimed at progressively assigning limestone samples to more specific sources of origin, from the broadest classification units (French regions) to the narrowest ones (individual quarries). The application of the stepwise variable selection procedure to extract the most discriminating compositional variables prior to each classification development allowed us to obtain a perfect separation between the limestone categories considered at every classification stage (all samples were correctly classified and predicted in all cases). The high‐quality results obtained were even more remarkable considering the relatively small number of significant variables selected in each case using the SLDA method. An illustrative example was provided in order to demonstrate that the classification strategy proposed can actually allocate an unknown sculpture to a particular quarry of origin.     

SCIENTIFIC CHARACTERIZATION OF THE POHORJE MARBLES,SLOVENIA

As a former part of the great Roman Empire, Slovenia has many archaeological sites featuring buildings and objects entirely or partly constructed from marble whose provenance is doubtful. In Slovenia, the most probable source of such marble is the Pohorje Mountains. For the purpose of supporting further provenance studies, these marbles are fully scientifically characterized. The techniques used are petrographic and geochemical analysis, stable isotope ratio analysis and EPR spectroscopy. The results show that the Pohorje marbles are highly heterogeneous in both their isotopic and geochemical parameters as well as grain sizes. The parameters of the different Pohorje marble outcrops are compared between themselves and with the parameters of known ancient quarries in the Mediterranean and Austria. The use of a multi‐technique approach with combined parameters allows the best possible discrimination.     

AN UPDATED,MULTI‐METHOD DATABASE OF EPHESOS MARBLES,INCLUDING WHITE,GRECO SCRITTO AND BIGIO VARIETIES*

An updated database of Ephesos marbles including 244 samples from 16 quarrying districts is reported. The unknown Greco Scritto quarries near Hasançavuslar and the Bigio marbles from the quarries of Belevi and of Mt Panayir are also presented. The paper, however, is mostly devoted to the identification of the Ephesos white marbles, whereas the problems posed by the Bigio and Greco Scritto varieties are deferred to future work. The samples have been characterized by isotopic analysis, EPR spectroscopy and additional petrographic and optical properties. Owing to the complex geology of the region, the white marbles of Ephesos exhibit rather inhomogeneous properties and are conveniently classified into four marble groups, which can be almost completely discriminated. The problem of distinguishing the Ephesos white marbles from other similar varieties has been dealt with by statistically comparing the Ephesos samples with all the similar, medium‐grained varieties present in the marble database. Although some of the four Ephesos groups can be reliably identified, general solution of the discriminant problem is difficult. Historical archaeological information is needed to reduce the complexity of the problem by eliminating unlikely provenances. In this way relevant problems, such as the discrimination between Ephesos and Proconnesos marbles, can be solved.     

In the Steps of William the Conqueror: Neutron Activation Analysis of Caen Stone*

Quarries in the Bathonian stone formation surrounding Caen produced high‐quality limestone for medieval churches in northern France and southern England and for their sculptural decoration. To investigate compositional differences among proximate stone sources, 103 samples collected from five separate quarries were analysed by NAA. The results show Caen stone to be essentially pure calcite and relatively homogeneous, but distinction among quarries is possible by discriminant analysis. Comparing compositions of quarry samples with data in the Brookhaven Limestone Database identified the origin of stone used in masonry and sculpture at Saint‐Étienne and La Trinité, Caen, and in several museum objects.     

Roman lava quarries in the Eifel region (Germany): geochemical data for millstone provenance studies

Roman millstones of assumed Eifel origin were produced and exported in huge quantities to many parts of Roman Europe and can be used as tracers for trade patterns in Roman times. This study presents for the first time a raw-material centred geochemical definition of the 13 well-known Roman basaltic lava quarries in the Quaternary East and West Eifel volcanic fields. The aim is to find a way to characterize the individual exploitation sites precisely by means of their geochemical composition and to recommend a standard procedure for further millstone provenance analysis. Based on major and trace element composition analyses by XRF, a differentiation of each quarry is achieved by using a combination of geochemical discrimination and cluster and discriminant analysis. Therefore, for provenance analysis of a unknown millstone sample the following procedure is recommended: (1) geochemical discrimination to check if it actually belongs to the volcanic Eifel quarries; (2) cluster analysis to check to which quarry or cluster of quarries the millstone can be affiliated; and (3) discriminant analysis to assign the sample to its quarry of origin with a certain confidence.     

MARBLE PROVENANCE INVESTIGATION OF ROMAN SARCOPHAGI FROM THESSALONIKI*

The provenance question of the marbles used for making the sarcophagi of local production of Thessaloniki in the Roman period had been posed by archaeologists in the past. The hypothesis was that the material came mainly from the quarries of Thassos Island. This paper presents the scientific analysis of 23 characteristic samples from selected sarcophagi at the Museum of Thessaloniki, using three different techniques: electron paramagnetic resonance (EPR) spectroscopy, stable isotope analysis and maximum grain size measurements, plus in-situ examination. New combinations of parameters were used in order to resolve fully the provenance of all samples. The results showed that the vast majority of the objects were indeed made in Thassian marble but from three different quarries, namely Vathy/Saliara (dolomitic marble), Aliki (calcitic marble) and Acropolis/Phanari (calcitic marble). The calcitic marbles from Aliki and to a lesser degree from Acropolis/Phanari are met in all the basic types of sarcophagi (framed type, plain type, garland sarcophagi). The use of the better quality and snow-white dolomitic marble from Vathy/Saliara quarries is relatively restricted and is often found in works that are above the average regarding the quality of their workmanship. In addition, two sarcophagi were made in Pentlelic marble and one in Proconnesian. The scientific analysis results provide a good confirmation of the archaeological estimates and, furthermore, the conclusions constitute henceforth a secure basis for the study of the entire sculptured works of Thessaloniki.     

THE PROPERTIES AND IDENTIFICATION OF MARBLE FROM PROCONNESOS (MARMARA ISLAND,TURKEY): A NEW DATABASE INCLUDING ISOTOPIC,EPR AND PETROGRAPHIC DATA*

This paper reports an updated and enlarged archaeometric database of Proconnesos marbles with the aim of attaining more reliable inter‐ and intra‐site identification. Quarry and artefact samples (n = 397) from 23 different quarrying areas were characterized using petrographic, isotopic and EPR results. The most distinct property of Proconnesos marbles is their extremely weak EPR intensity, associated with the low concentration of Mn²⁺impurities. This feature, supported by the contribution of other important isotopic and petrographic variables, forms the basis for the correct identification of Proconnesos marbles. Within the site the distribution of properties is relatively homogeneous; only limited intra‐site discrimination is possible. All the experimental results, as well as the quarry samples are made available to other researchers willing to measure additional experimental properties, thus increasing the rate of within the site discrimination. Extensive survey has proved that, although about 10% of the samples exhibit maximum grain size below 1.0 mm, no locations exist where fine grained marbles could be intentionally quarried. The historical aspects of Proconnesos marble quarrying and usage are also discussed.     

INAA of pre-contact basalt quarries on the Samoan Island of Tutuila: a preliminary baseline for an artifact-centered provenance study

This project presents a material-centered instrumental neutron activation analysis (INAA) characterization of 120 geologic samples selected from four fine-grained basalt quarries on the Samoan Island of Tutuila. Previous attempts at definitive differentiation of these Tutuilan quarries have utilized x-ray fluorescence (XRF). In this study, clear differentiation of each analyzed quarry was achieved using INAA. Biplots of canonical discriminant analysis (CDA) scores for the INAA data illustrate clear separation based on the variation in chemical composition between each quarry. The samples analyzed not only define quarry separation, but also provide the “core group” for a preliminary baseline necessary for future artifact-centered provenance studies. Inclusion of these “core group” samples in the baseline was confirmed by stepwise discriminant analysis. These findings suggest the ability to determine artifact quarry of origin on the island of Tutuila, which can elucidate the importance of individual Tutuilan quarries in the production, distribution and consumption of fine-grained basalt artifacts in Polynesia.     

Assessing XRF for the geochemical characterization of radiolarian chert artifacts from northeastern North America

The purpose of this paper is to emphasize the benefits of adopting non-destructive energy dispersive X-ray fluorescence (ED-XRF) as a first-order technique to determine chert whole-rock geochemistry for archaeological sourcing. Chemical signatures for the Touladi and La Martre prehistoric quarries from the lower St. Lawrence and Gaspé Peninsula region of Quebec, Canada, are determined and serve as references to test the provenance of regional chert artifacts. Chert experimental flakes, created from quarry geological hand samples, are analyzed and used to validate the method. Archaeological flakes and tools recovered from three archaeological sites are analyzed and tested against quarry samples. Geochemical diagrams and Principal Component Analysis are used to establish artifact-quarry relationships. The effects of surface weathering on the geochemical analysis of archaeological chert artifacts are presented. Sample restoration and research avenues are discussed and proposed to further enhance the robustness of future chert geochemical data sets.     

A New Methodology for the Provenance of Marble Based on EPR Spectroscopy

Fifteen years of research in investigating the characteristics of the EPR spectra of different types of white marble from several quarries in the Eastern Mediterranean has produced an accumulation of a large number of data, and much experience. Statistical treatment of these EPR data (statistical distributions and parameter correlations), has led to the selection of 10 parameters that are useful for quarry discrimination. Apart from the EPR parameters, the maximum grain size, measured with a stereomicroscope, has been found very useful. Boxplots have been found to be very useful as a first easy visual tool for evaluating the discrimination capacity of each parameter. On the basis of these results, a new methodology for determining the provenance of an archaeological sample was developed in stages, using a different pair or combination of parameters each time. In the first stage, the Penteli, Naxos, Hymettus and Proconnessus quarries are completely separated from each other. However, overlapping occurs between the parameter fields of Paros and Proconnessus, Paros and Hymettus and between the two archaic quarries of Melanes and Apollon on Naxos. If the sample is located in a non‐overlapping area, its provenance is obvious and easily determined. If the sample lies in one of the above three overlapping areas, an additional stage is necessary, in which other parameters are used to eliminate or decrease the overlap. Despite the partial overlapping of Paros with other quarries, the famous Lychnites marble of Paros, which was quarried underground, is clearly distinguished.     

New data of 87Sr/86Sr ratio in classical marble: an initial database for marble provenance determination

⁸⁷Sr/⁸⁶Sr ratios are presented for white marbles collected from some of the most famous classical quarry areas of the Mediterranean: Carrara, Paros, Naxos, Pentelikon, Dokimeion, Hymettus, Thasos, and Proconnesus. These ratios range from 0.7071 to 0.7092. The ranges of the different quarry areas are notably superimposed; this prevents a common adoption of this parameter in distinguishing the quarry locations for the classification of the provenance of marbles used during classical times for architectural and sculptural artefacts. However some quarry areas show peculiar distributions of their isotopic values, which could help to assign the provenance to an unknown marble artefact.Adding these new data to the scarce number of strontium isotopic compositions measured on white marbles and available in the relevant literature, permits the creation of an initial database of 11 classical quarry locations. This database confirms that the strontium isotope ratio could be used in marble provenance determination, together with petrographic and geochemical methods, as an ancillary technique.     

Sampling for Provenance: Tailings from Prehistoric Stone Quarries in the South Pacific

Stone is a principal component in archaeological assemblages across the Pacific. It provided a major element in architecture, used as trade goods, and was fashioned into implements and ornaments, monolithic monuments, statues, money, and emblematic symbols of victory, status and ethnicity. In short, stone is a pervasive element in the economic, social, and political fabric of Pacific cultural traditions. However, provenance of rock quarries, the source of this raw material, has received limited attention in Oceania. Provenance studies have been sidestepped or short-changed in the rush to analyse artifactual materials. Here we establish a foundation for more robust provenance studies and field sampling strategies through a discussion of (1) quarry identification and (2) sampling within prospective sources. A model of quarry identification, sampling, and characterization is drawn from work on Rapa Nui (Easter Island), and the fundamental precepts are outlined for future sampling experiments and provenance work in stone quarries generally.     

A Multi‐Method Database of the Black and White Marbles of Göktepe (Aphrodisias), Including Isotopic,EPR, Trace and Petrographic Data

A database of the ancient marbles of Göktepe near Aphrodisias is reported, and includes 160 white, black and bichrome samples from 13 quarries and two waste deposits. The quarries are grouped into four districts. Districts 1 and 2, to the north, produced exclusively black or dark grey marbles (nero antico). Districts 3 and 4 produced white statuary marble. Nero antico and a black and white stone were also quarried in district 4, where the black marble surfaces again. The samples were characterized using petrography, isotopic analysis, EPR spectroscopy and trace analysis. The Göktepe white exhibits an unparalleled combination of fine grain, low EPR intensity and high strontium concentration that often allows easy identification. The isotopic values are less distinctive and similar to those for Carrara. In most cases, however, they are tightly grouped and also quite indicative. The black marbles exhibit a much weaker metamorphic overprint. With respect to the white marbles, they show analytical similarities but also notable differences. Therefore, establishing their provenance can be more difficult and may require the support of petrographic analysis. The results suggest that the Göktepe marbles were among the most prized and widespread statuary marbles used in Roman times, particularly from the early second century ad onwards.     

The marbles of two early Christian churches at Latrun (Cyrenaica,Libya)

The provenance of twenty-seven architectural marbles from the two 6th century AD Christian churches of Latrun (Cyrenaica, Libya) has been established by discriminant function analysis of twelve isotopic, EPR and petrographic/morphological variables. Sixteen samples (59%) originate from Proconnesos, while 8 samples (30%) are assigned to the calcitic quarries of Thasos and 1 to the Docimium quarries near Afyon. The last two samples are of uncertain provenance and might be Proconnesian as well. These results demonstrate that the suggestion made long ago by Ward-Perkins that the presence on non-Proconnesian, possibly Thasian, marbles at Latrun was well founded. Particularly interesting is the strong correlation found between provenance and type of the architectural element sampled. Thasian marbles at Latrun were used exclusively for the manufacture of chancel screens. Seven out of nine screens sampled have this provenance, suggesting that the use of different materials is related to issues of work organisation and specialisation in different marble production centres.     

PROVENANCE OF MARBLES FROM NAXOS BASED ON MICROSTRUCTURAL AND GEOCHEMICAL CHARACTERIZATION

A detailed quantitative microstructural study coupled with cathodoluminescence and geochemical analyses on marbles from Naxos demonstrates that the analysis of microstructures is the most sensitive method to define the origin of marbles within, and between, different regions. Microstructure examination can only be used as an accurate provenance tool if a correction for the second‐phase content is considered. If second phases are not considered, a large spread of different microstructures occurs within sample sites, making a separation between neighbouring outcrops difficult or impossible. Moreover, this study shows that the origin of a marble is defined more precisely if the microstructural observations are coupled with cathodoluminescence data.     

CARBON AND OXYGEN ISOTOPIC RATIOS: A DATA BASE FOR CLASSICAL GREEK AND ROMAN MARBLE

An isotopic data base of δ¹³C and δ¹⁸O analyses of 528 samples collected from 39 classical Greek and Roman quarries of Turkey, Greece, Italy and Tunisia has been accumulated. The discriminative possibilities of the data base vary from quarry to quarry. Most quarries have a distinctive pattern for either or both variables, but some have more than one grouping. The data also overlap for many quarries preventing a unique provenance assignment. If the alternatives are known so that the total pool of possible sources is reduced, the data base can then discriminate and assign a provenance for most classical marble artifacts.