lead isotopic analysis for the identification of late...

LEAD ISOTOPIC ANALYSIS FOR THE IDENTIFICATIONOF LATE BRONZE AGE POTTERY FROM HALA SULTAN

TEKKE (CYPRUS)*

V. RENSON,1† J. COENAERTS,2 K. NYS,2 N. MATTIELLI,3 F. VANHAECKE,4 N. FAGEL5

and PH. CLAEYS1

1Earth System Science, Geology Department, Vrije Universiteit Brussel, Pleinlaan 2, 1050 Brussels2Mediterranean Archaeological Research Institute, Vrije Universiteit Brussel, Pleinlaan 2, 1050 Brussels

3Département des Sciences de la Terre et de l’Environnement, Université Libre de Bruxelles,Avenue F. D. Roosevelt 50, 1050 Brussels

4Department of Analytical Chemistry, Ghent University, Krijgslaan 281 – S12, 9000 Ghent5Department of Geology, Université de Liège, Allée du 6–Août B18, 4000 Liège

Lead isotopic compositions were measured for 65 sherds from five pottery wares (Plain White,Coarse, Canaanite, White Slip and Base-ring) excavated from the Late Bronze Age site of HalaSultan Tekke (Cyprus). The elemental composition and isotopic signature of the sherds werecompared with those of 65 clay samples collected in south-east Cyprus, mainly in the sur-roundings (<20 km) of Hala Sultan Tekke. This work shows the effectiveness of using leadisotopic analysis in provenance studies, along with other analytical techniques, such as X-raydiffraction (XRD) and a scanning electron microscope (SEM) equipped with an energydispersive X-ray detection (EDX) facility, to identify the composition of pottery wares and theclay sources used for pottery ware production.

KEYWORDS: LEAD ISOTOPES, POTTERY, CYPRUS, PROVENANCE STUDY, LATE BRONZEAGE, HALA SULTAN TEKKE

INTRODUCTION

For decades, elemental analysis has been widely used in pottery provenance studies (e.g., Knappand Cherry 1994; Hein et al. 2002; Mommsen et al. 2002; Asaro and Adan-Bayewitz 2007;Yellin2007). This approach is often successfully combined with petrographical analysis (e.g., Day et al.1999; Ben-Shlomo et al. 2007) and other analytical techniques (e.g., Tchegg et al. 2008, 2009).Because of the various processes that can be applied to clays before and during pottery produc-tion, as well as the large variety of clays that occur in the vicinity of a production site, mostpottery provenance studies compare pottery samples with a reference group or with pottery ofknown or assumed provenance. Rarely are pottery samples compared with potential clay sources.Nevertheless, several studies have successfully linked pottery to their raw material (e.g., Adan-Bayewitz and Perlman 1985; Gomez et al. 2002; Hein et al. 2004; Tchegg et al. 2009).

Lead isotopic analysis is commonly used to study processes and reveal provenance in geo-sciences (e.g., Allègre 2005; Dickin 2005). In archaeometry, lead isotopic analysis is largely usedto trace sources of different artefacts, such as glasses (e.g., Shortland 2006), glazes (e.g., Wolfet al. 2003) and metals from different periods and origins (e.g., Stos-Gale et al. 1997; Nieder-schlag et al. 2003; Durali-Mueller et al. 2006). So far, lead isotopes have hardly ever been

*Received 9 November 2009; accepted 9 January 2010†Corresponding author: email [email protected]

Archaeometry 53, 1 (2011) 37–57 doi: 10.1111/j.1475-4754.2010.00535.x

© University of Oxford, 2010

applied to characterize the source materials of ceramics (Knacke-Loy et al. 1995; Renson et al.2007). However, original isotopic ratios are unlikely to be strongly affected by the pottery-making process, and consequently the isotopic signature of a pottery sherd should indeed reflectthe isotopic signature of the parent material used to manufacture it. Moreover, the recentimprovements in mass spectrometry techniques make it possible not only to determine Pbisotopic compositions with high precision but also to process large batches of samples efficiently.

A better insight into the use of raw materials selected for pottery-making contributes to theunderstanding of the socio-economic and cultural relations within a given area and period. Thepresent study uses lead isotopic compositions to document the sources of different pottery wares,found at the Late Bronze Age site of Hala Sultan Tekke-Vyzakia, Cyprus. This harbour townrepresents an ideal case study: it was a major polity involved in diverse and international traderelations and its existence spanned from c. 1600 bc to the end of the 12th century bc.

The 207Pb/204Pb and 206Pb/204Pb ratios determined for 65 sherds from Hala Sultan Tekke-Vyzakiawere compared with the values obtained for an extensive set of samples collected from surround-ing geological formations, lithologically well suited for Late Bronze Age ceramic production.This data set is complemented by elemental analysis of selected pottery sherds using a scanningelectron microscope (SEM) equipped with an energy dispersive X-ray detection (EDX) facilityand information on the mineralogy of the sediments using X-Ray diffraction (XRD). Thismulti-proxy study aims: (1) to identify the range of the lead isotopic signatures of the claysavailable in the surroundings of the site and more largely in south-east Cyprus; (2) to define thecharacteristic lead isotopic fingerprint of the pottery production at Hala Sultan Tekke-Vyzakia bycomparing the signature of the sherds with that of the raw material; (3) to identify the leadisotopic composition of four categories of Late Bronze Age pottery found at Hala SultanTekke-Vyzakia and compare it with clay sources; and (4) to show that lead isotopes can success-fully be applied in pottery provenance studies.

SITE DESCRIPTION

The Late Bronze Age settlement of Hala Sultan Tekke-Vyzakia (hereafter HST) lies on the westshore of the Larnaca salt lake in south-east Cyprus (Fig. 1). The oldest indication of humanhabitation at the site dates from the very end of the Middle Cypriot III Period, c. 1600 bc. Thematerial culture indicates that the town flourished from the second half of the 14th century bc tothe first half of the 12th century bc. HST is undoubtedly one of the Cypriot urban polities thatactively participated in the Eastern Mediterranean exchange network, in particular during thetimespan of LC IIC–LC IIIA (c. 1340 to 1110 bc). By the end of the 12th century bc it had beenabandoned (Åström 1986).

MATERIAL

Pottery sherds

Hala Sultan Tekke yielded a large variety of pottery fabrics ranging from the end of MiddleCypriot III until Late Cypriot IIIA2 (c. 1600 to 1110 bc). A representative set (n = 65) of potterywares was selected covering a timespan from LC IIA to LC IIIA2 contexts (c. 1410 to 1110 bc)(Renson et al. 2007, 56–7). Fifty-four samples originated from Areas 8 and 22 in the settlement,while 11 more sherds were collected from the assemblage in Tomb 24 (Åström and Nys 2007).Two samples were taken from misfired Plain White Wheel-made sherds (HST 1a and HST 1b; see

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© University of Oxford, 2010, Archaeometry 53, 1 (2011) 37–57

Table 2). Since it is unlikely that misfired pots would be imported to the site as such, these twosamples must be considered as purely local products. To define the local (HST) fingerprint, thesemisfired fragments were compared with seven other Plain White and two Coarse sherds. Threeother wares were selected to evaluate their relation to the HST composition: 30 White Slip II andfour Base-ring sherds were considered as representative examples of the two most characteristicLate Bronze Age wares in Cyprus, while 20 Canaanite sherds were chosen to test commonassumptions about the potential provenances of this ware within the Eastern Mediterranean.

Sediment and rock samples

A geologically and geographically comprehensive set (n = 65) of fine-grained or clay-rich sedi-ments was collected in south-east Cyprus (Fig. 1). Among these, 42 samples originated from thesurroundings of the site (<20 km). Sampling locations were selected based on geologicalmaps and ‘Memoirs’ published by the Geological Survey of Cyprus (Bagnall 1960; Gass 1960;Pantazis 1967; Gass et al. 1994), to cover the following geological units judged appropriate forpottery production: (1) Holocene alluvium and colluvium (clays); (2) Pleistocene Marine Terracedeposits; (3) Plio-Pleistocene (Apalos-Athalassa Kakkarista formation); (4) Pliocene (Nicosiaformation); (5) Miocene (Pakhna formation); (6) Palaeogene (Lefkara formation) marls and

Upper CretaceousVolcanic sequence

Upper CretaceousIntrusive sequence

PalaeogeneLefkara formation

PleistoceneMarine Terrace

PlioceneNicosia formation

Miocene Pakhna formation

Upper CretaceousMoni formation

Quaternarysediments

Southern Troodos

Transform Fault Zone

5 km N

Figure 1 Location of samples and Hala Sultan Tekke, modified after the Geological Map of Cyprus (GSD, 1995). Somesamples have been collected from the same outcrop; because of the proximity of some outcrops, the circles represent thelocation of one or several samples. The star indicates the location of Hala Sultan Tekke-Vyzakia settlement.

Lead isotopic analysis of Late Bronze Age pottery from Hala Sultan Tekke 39


chalks; (7) Upper Cretaceous clays (Moni formation); (8) Upper Cretaceous umbers (Fe, Mn richclays) and shales (Perapedhi formation); (9) rocks and clays derived from the weathering of therocks from the volcanic sequence of the Troodos Ophiolite; and (10) a soil from the TroodosOphiolite area.

METHODS

Lead isotopic analysis

All the samples were dried at 40°C and crushed in an agate mortar under an extracting hood. Thesurface of the sherds was first cleaned using a diamond-bit micro-drill prior to crushing. Theresulting powders were calcined at 550°C for 4 h. Acid digestions were achieved in a laminar-flow clean-air cabinet. About 200 mg of powder was dissolved in closed Savillex® beakers(125°C, 48 h) using 24M HF sub-boiled and 14M HNO3 sub-boiled in a proportion of 4:1. Afterevaporation, 5 ml of 6.8M HCl sub-boiled was added (125°C, 48 h), and the solutions wereslowly evaporated at 90°C. The dry residues were finally dissolved in 2 ml 0.5M HBr. Leadisolation was accomplished via ion-exchange chromatography (IEC with Dowex AG1–X8 anionexchange resin) and was achieved by successive HBr and HCl additions following the method-ology described in Weis et al. (2006). The eluted pure Pb solution was evaporated and stored.Prior to isotopic analysis, this purified Pb fraction was re-dissolved in 100 ml of 14M HNO3

sub-boiled, evaporated and finally dissolved in 1.5 ml of 0.05M HNO3.Lead isotope ratios were measured using two multicollector – inductively coupled plasma –

mass spectrometers (MC–ICP–MS): a Nu Plasma (Nu Instruments) in operation at the Départe-ment des Sciences de la Terre et de l’Environnement of the Université Libre de Bruxelles,Belgium, and a Thermo Scientific Neptune (Thermo Scientific) in operation at the Department ofAnalytical Chemistry of Ghent University, Belgium. Thirteen pottery samples were previouslymeasured on the two MC–ICP–MS units to control the reproducibility of the measurements (seeTable 2).

A Tl solution was added to each sample and standard to monitor and correct for instrumentalmass discrimination. Lead concentrations varied among the samples; consequently sample solu-tions were prepared to obtain a beam intensity in the axial collector (204Pb) of a minimum of100 mV and a Pb/Tl ratio of ~5, matching the Pb and Tl concentration ratio of the NIST SRM 981‘Common lead’ isotopic standard (150 ng g-1 in Pb, with 50 ng g-1 in Tl). The NIST SRM 981standard was measured several times before each analytical session and between each setof two samples on both devices. In total, 219 analyses of the standard were carried out onthe Nu Plasma and yielded the following mean values: 208Pb/204Pb = 36.714 1 0.006 (2SD),207Pb/204Pb = 15.497 1 0.002 (2SD), 206Pb/204Pb = 16.940 1 0.002 (2SD). Such values agree wellwith the long-term laboratory values [n = 1000, 208Pb/204Pb = 36.713 1 0.012 (2SD), 207Pb/204Pb = 15.495 1 0.004 (2SD), 206Pb/204Pb = 16.939 1 0.004 (2SD)] and the MC–ICP–MS valuesof Weis et al. (2006). These values are also in agreement with thermal ionization mass spectrom-etry (TIMS) triple-spike values previously published by Galer and Abouchami (1998). Thestandard was measured 30 times on the Neptune and yielded the following mean values: 208Pb/204Pb = 36.669 1 0.003 (2SD), 207Pb/204Pb = 15.481 1 0.001 (2SD), 206Pb/204Pb = 16.927 1 0.001(2SD). Although the NIST SRM 981 standard results were within the error of the triple-spikevalues after on-line correction for instrumental mass bias using the bias observed for the addedTl, the sample results were further corrected using the sample-standard bracketing method (asdescribed by White et al. 2000 and Weis et al. 2006) to circumvent any instrumental drift during

40 V. Renson et al.


the analytical session. Ten duplicates (i.e., second total procedure on the same sample) and fivereplicates (i.e., second analysis of the same sample) were measured on the Nu Plasma, and oneduplicate and two replicates were measured on the Neptune to confirm the reproducibility of theanalyses (Tables 1 and 2).

Mineralogy of clay samples and elemental analysis of selected sherds

X-ray diffraction spectrometry (XRD) was used to characterize the mineralogy of the sediments.Samples were dried at 40°C, crushed and the bulk powders were analysed using a Brucker D8Advance diffractometer. The main minerals were identified using their characteristic peaks in theX-ray pattern. Subsequently, the major elements (Si, Ti, Al, Fe, Mn, Mg, Ca, Na, K, P) weredetermined on the matrix of selected Plain White and White Slip sherds using a JEOL-JSM-6400scanning electron microscope (SEM) equipped with an energy dispersive X-ray detection (EDX)facility (Thermo Noran Pioneer with Si-Li detector) at 20 kV and a working distance of 39 mm.Carbon coating of the thin sections was carried out using an EMITECH-Carbon evaporationK450. Several (between two and seven) measurements were performed on the matrix of eachsherd. The measurements were realized on a single point representing the size of the beam(1 mm2) or on scanned areas of variable surface (from 6 ¥ 12 mm to 150 ¥ 170 mm). The majorityof the measurements were realized on surfaces from 20 ¥ 20 mm to 50 ¥ 50 mm. No externalstandard was used, and values were normalized.

RESULTS AND DISCUSSION

Selected sediments and rocks from Cyprus

The bulk mineralogy of the Holocene sediments resembles that of the different chalks and marlsfrom the Miocene to the Palaeogene. They are mainly composed of calcite and clays. Quartz ispresent in most of the samples, and plagioclase and dolomite are frequent components. ThePleistocene sediments display the same mineral assemblage, but some of the samples includetraces of amphibole. The samples from the Moni and Perapedhi formations as well as theweathered products derived from the volcanic sequence of the Troodos Ophiolite are mainlycomposed of clays, and in some of these samples plagioclase, K-feldspar and pyroxene arepresent.

The isotopic field of the Troodos Ophiolite is defined using data from the literature (Galeet al. 1981; Spooner and Gale 1982; Hamelin et al. 1984, 1988). It ranges between 15.48 and15.63 for 207Pb/204Pb and between 17.95 and 18.89 for 206Pb/204Pb ratios. The lead isotopicvalues of the clays and rocks from the volcanic sequence measured in this study fall clearlyinto this isotopic field (Table 1 and Fig. 2). The lead isotopic compositions of the Upper Cre-taceous Peraphedi umbers and shales range from 15.592 to 15.629 for 207Pb/204Pb and from18.516 to 18.724 for 206Pb/204Pb and also plot within the Troodos Ophiolite isotopic field. The207Pb/204Pb and 206Pb/204Pb ratios from the Upper Cretaceous clayey Moni formation range from15.666 to 15.689 and from 18.814 to 18.926, respectively. The field of the Moni formationoverlaps the fields of the Quaternary to Palaeogene marls and sediments (Fig. 2 and Table 1).The field of sedimentary and carbonate rocks (Quaternary to Palaeogene) is located betweenthe more radiogenic Upper Continental Crust values (207Pb/204Pb from 15.71 to 15.78 and206Pb/204Pb from 18.93 to 19.32; see Asmeron and Jacobsen 1993; Hemming and McLennan2001; Millot et al. 2004) and the Troodos Ophiolite field (Fig. 2). A closer look at the isotopic



Table 1 Lead isotope ratios and coordinates of rocks and sediments. Labels in bold refer to samples collected in the surroundings of HST (<20 km). 2se refers to 2standard errors. * duplicate and ** replicate. Formations and age are indicated for each sample. Values in italic refer to measurements carried out using the Neptune at

Ghent University

Sample Formation 208Pb/204Pb 2se 207Pb/204Pb 2se 206Pb/204Pb 2se Lat. N Long. E

Cps05 4 Clay sediment Holocene colluvium and alluvium 38.9530 0.0019 15.6809 0.0007 18.9194 0.0009 34°54′9.36″ 33°35′05.22″Cps05 5 Clay sediment Holocene colluvium and alluvium 38.9614 0.0025 15.6825 0.0009 18.8808 0.0013 34°54′9.36″ 33°35′05.22″Cps05 6 Clay sediment Holocene colluvium and alluvium 38.9559 0.0034 15.6815 0.0013 18.9226 0.0016 34°54′9.36″ 33°35′05.22″Cps05 6 ** Clay sediment Holocene colluvium and alluvium 38.9568 0.0021 15.6846 0.0009 18.9333 0.0010 34°54′9.36″ 33°35′05.22″Cps07 1 Clay sediment Holocene colluvium and alluvium 38.9556 0.0021 15.6852 0.0008 18.9188 0.0009 34°54′9.36″ 33°35′04.98″Cps07 60b Clay sediment Holocene colluvium and alluvium 38.9281 0.0023 15.6765 0.0009 18.8494 0.0009 34°55′44.34″ 33°35′13.98″Cps07 61 Clay sediment Holocene colluvium and alluvium 38.9317 0.0024 15.6775 0.0008 18.8509 0.0008 34°55′44.34″ 33°35′13.98″Cps08 62 Clay sediment Holocene colluvium and alluvium 38.9193 0.0022 15.6821 0.0009 18.8643 0.0011 34°44′22.26″ 33°13′17.22″Cps05 2 Clay sediment Pleistocene Marine Terrace 38.8886 0.0018 15.6615 0.0007 18.8361 0.0008 34°53′24.36″ 33°36′20.04″Cps05 3 Clay sediment Pleistocene Marine Terrace 38.8816 0.0018 15.6596 0.0007 18.8345 0.0009 34°53′24.36″ 33°36′20.04″Cps07 26 Clay sediment Pleistocene Marine Terrace 38.8401 0.0027 15.6536 0.0010 18.8084 0.0011 34°53′23.22″ 33°36′09.30″Cps08 59 Clay sediment Pleistocene Marine Terrace 38.9099 0.0023 15.6682 0.0009 18.8365 0.0010 34°53′38.46″ 33°36′56.76″Cps08 60a Clay sediment Pleistocene Marine Terrace 38.8747 0.0021 15.6580 0.0008 18.8326 0.0010 34°53′56.52″ 33°36′55.56″Cps07 75c Marls and chalks Pleistocene Apalos-A./K.formation 38.9728 0.0019 15.6856 0.0007 18.9173 0.0009 35°01′6.54″ 33°41′45.84″Cps07 59 Marls and chalks Pliocene Nicosia formation 38.8991 0.0027 15.6722 0.0009 18.8549 0.0009 34°54′25.74″ 33°36′23.28″Cps08 39 Marls and chalks Pliocene Nicosia formation 38.9763 0.0020 15.6849 0.0007 18.9129 0.0009 34°53′25.02″ 33°37′54.36″Cps08 39 * Marls and chalks Pliocene Nicosia formation 38.9784 0.0023 15.6857 0.0009 18.9135 0.0010 34°53′25.02″ 33°37′54.36″Cps08 39 ** Marls and chalks Pliocene Nicosia formation 38.9770 0.0025 15.6864 0.0009 18.9111 0.0011 34°53′25.02″ 33°37′54.36″Cps08 39 ** Marls and chalks Pliocene Nicosia formation 38.9694 0.0023 15.6841 0.0008 18.9106 0.0009 34°53′25.02″ 33°37′54.36″Cps08 40 Marls and chalks Pliocene Nicosia formation 38.9837 0.0019 15.6864 0.0008 18.9182 0.0009 34°53′21.6″ 33°37′46.86″Cps07 65a Marls and chalks Miocene Pakhna formation 38.8745 0.0022 15.6614 0.0008 18.8085 0.0008 34°43′58.98″ 32°59′16.20″Cps07 65c Marls and chalks Miocene Pakhna formation 38.8997 0.0027 15.6705 0.0010 18.8382 0.0011 34°43′58.98″ 32°59′16.20″Cps07 69a Marls and chalks Miocene Pakhna formation 38.9480 0.0019 15.6946 0.0007 18.9813 0.0008 34°45′29.64″ 32°55′49.44″Cps07 69b Marls and chalks Miocene Pakhna formation 38.9625 0.0019 15.6871 0.0006 18.8821 0.0007 34°45′29.64″ 32°55′49.44″Cps07 70a Marls and chalks Miocene Pakhna formation 38.9446 0.0025 15.6911 0.0009 18.9449 0.0010 34°45′43.56″ 32°55′23.32″Cps07 70b Marls and chalks Miocene Pakhna formation 38.9455 0.0019 15.6926 0.0007 18.9658 0.0008 34°45′43.56″ 32°55′23.32″Cps08 12a Marls and chalks Miocene Pakhna formation 38.9938 0.0024 15.6972 0.0009 19.0038 0.0010 34°53′6.66″ 33°33′04.56″Cps08 12b Marls and chalks Miocene Pakhna formation 38.9328 0.0027 15.6830 0.0010 18.8873 0.0012 34°53′6.66″ 33°33′04.56″Cps08 32a Marls and chalks Miocene Pakhna formation 39.0078 0.0011 15.7024 0.0004 19.0467 0.0005 34°42′45.84″ 33°07′36.30″Cps08 32b Marls and chalks Miocene Pakhna formation 38.8900 0.0014 15.6708 0.0005 18.9131 0.0006 34°42′45.84″ 33°07′36.30″Cps08 32c Marls and chalks Miocene Pakhna formation 38.9701 0.0015 15.6957 0.0005 19.0658 0.0006 34°42′45.84″ 33°07′36.30″Cps08 48b Marls and chalks Miocene Pakhna formation 38.9151 0.0012 15.6734 0.0005 18.8522 0.0006 34°42′53.82″ 33°08′48.72″Cps08 48c Marls and chalks Miocene Pakhna formation 38.9150 0.0013 15.6726 0.0004 18.8397 0.0005 34°42′53.82″ 33°08′48.72″Cps08 49 Marls and chalks Miocene Pakhna formation 38.8868 0.0010 15.6810 0.0004 18.8234 0.0004 34°43′17.52″ 33°08′35.94″Cps07 19a Marls and chalks Palaeogene Lefkara formation 38.9383 0.0028 15.6829 0.0010 18.9463 0.0012 34°53′46.26″ 33°32′41.04″Cps07 22 Marls and chalks Palaeogene Lefkara formation 38.9332 0.0032 15.6801 0.0011 18.8972 0.0012 34°53′46.26″ 33°32′41.04″

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Cps07 23 Marls and chalks Palaeogene Lefkara formation 39.0188 0.0025 15.6989 0.0010 18.9890 0.0010 34°53′46.26″ 33°32′41.04″Cps07 23 * Marls and chalks Palaeogene Lefkara formation 39.0123 0.0021 15.6967 0.0008 18.9860 0.0009 34°53′46.26″ 33°32′41.04″Cps 07 21b Marls and chalks Palaeogene Lefkara formation 38.9972 0.0018 15.7000 0.0006 19.0095 0.0007 34°53′46.26″ 33°32′41.04″Cps07 21b * Marls and chalks Palaeogene Lefkara formation 38.9961 0.0025 15.6996 0.0010 19.0100 0.0011 34°53′46.26″ 33°32′41.04″Cps05 7 Marls and chalks Palaeogene Lefkara formation 38.9054 0.0023 15.6786 0.0009 18.8484 0.0011 34°53′32.28″ 33°32′14.28″Cps05 8 Marls and chalks Palaeogene Lefkara formation 38.9037 0.0021 15.6823 0.0008 18.8634 0.0011 / /Cps05 9 Marls and chalks Palaeogene Lefkara formation 38.8872 0.0023 15.6808 0.0007 18.8743 0.0010 34°53′22.86″ 33°32′14.70″Cps05 10 Marls and chalks Palaeogene Lefkara formation 38.9168 0.0018 15.6902 0.0007 18.8545 0.0009 34°53′22.86″ 33°32′14.70″Cps05 13 Marls and chalks Palaeogene Lefkara formation 38.8345 0.0021 15.6493 0.0009 18.7228 0.0012 34°58′32.28″ 33°31′39.96″Cps07 3 Marls and chalks Palaeogene Lefkara formation 38.8855 0.0023 15.6807 0.0008 18.8443 0.0008 34°53′23.04″ 33°32′14.82″Cps07 6 Marls and chalks Palaeogene Lefkara formation 38.8934 0.0033 15.6780 0.0012 18.8429 0.0013 34°53′14.04″ 33°32′26.46″Cps07 27 Marls and chalks Palaeogene Lefkara formation 38.9043 0.0032 15.6712 0.0011 18.7425 0.0012 34°59′55.92″ 33°25′43.62″Cps07 31 Marls and chalks Palaeogene Lefkara formation 38.8806 0.0019 15.6659 0.0007 18.7382 0.0007 34°59′36.24″ 33°28′36.78″Cps07 34 Marls and chalks Palaeogene Lefkara formation 38.9562 0.0031 15.6979 0.0011 19.0620 0.0010 34°59′51.48″ 33°30′18.66″Cps07 35 Marls and chalks Palaeogene Lefkara formation 38.9382 0.0024 15.6838 0.0009 18.8893 0.0010 34°59′51.48″ 33°30′18.66″Cps 07 4 Marls and chalks Palaeogene Lefkara formation 38.8840 0.0024 15.6786 0.0009 18.8449 0.0009 34°53′17.46″ 33°32′23.88″Cps 07 16 Marls and chalks Palaeogene Lefkara formation 38.9250 0.0021 15.6808 0.0008 18.8157 0.0008 34°52′19.98″ 33°30′39.90″Cps07 49 Marls and chalks Palaeogene Lefkara formation 38.8984 0.0029 15.6791 0.0010 18.8370 0.0012 34°45′52.08″ 33°18′03.78″Cps07 53 Marls and chalks Palaeogene Lefkara formation 38.9542 0.0024 15.6834 0.0009 18.8767 0.0010 34°45′52.08″ 33°18′03.78″Cps08 61b Marls and chalks Palaeogene Lefkara formation 38.8897 0.0018 15.6790 0.0007 18.8366 0.0009 34°53′16.62″ 33°32′01.02″Cps08 61d Marls and chalks Palaeogene Lefkara formation 38.9103 0.0023 15.6799 0.0009 18.8419 0.0010 34°53′16.2″ 33°31′58.74″Cps07 63 Clay Upper Cretaceous Moni formation 39.0638 0.0025 15.6812 0.0009 18.9258 0.0011 34°44′23.94″ 33°13′51.24″Cps08 34 Clay Upper Cretaceous Moni formation 38.8761 0.0010 15.6658 0.0004 18.8476 0.0004 34°44′35.52″ 33°07′42.36″Cps08 35a Clay Upper Cretaceous Moni formation 38.9315 0.0011 15.6840 0.0004 18.8249 0.0005 34°44′15.24″ 33°07′41.64″Cps08 35a* Clay Upper Cretaceous Moni formation 38.9326 0.0010 15.6842 0.0004 18.8254 0.0004 34°44′15.24″ 33°07′41.64″Cps08 35a** Clay Upper Cretaceous Moni formation 38.9308 0.0010 15.6840 0.0004 18.8247 0.0004 34°44′15.24″ 33°07′41.64″Cps08 35a** Clay Upper Cretaceous Moni formation 38.9293 0.0011 15.6837 0.0004 18.8249 0.0005 34°44′15.24″ 33°07′41.64″Cps08 35b Clay Upper Cretaceous Moni formation 38.9858 0.0009 15.6890 0.0003 18.8139 0.0004 34°44′15.24″ 33°07′41.64″Cps08 63a Umber Upper Cretaceous Perapedhi formation 38.7387 0.0011 15.6292 0.0004 18.7241 0.0005 34°48′0.42″ 33°16′47.28″Cps08 63b Shale Upper Cretaceous Perapedhi formation 38.6792 0.0011 15.6160 0.0004 18.6610 0.0005 34°48′0.42″ 33°16′47.28″Cps08 76b Shale Upper Cretaceous Perapedhi formation 38.5202 0.0010 15.5918 0.0004 18.5157 0.0004 34°46′32.46″ 33°15′41.10″Cps08 76a Umber Upper Cretaceous Perapedhi formation 38.6417 0.0011 15.6123 0.0004 18.6368 0.0005 34°46′32.46″ 33°15′41.10″Cps07 Oph 12 Clay Upper Cretaceous Volcanic sequence 38.8791 0.0018 15.6124 0.0007 18.8294 0.0008 34°55′47.94″ 33°23′48.36″Cps07 Oph 2 Alt Clay Upper Cretaceous Volcanic sequence 38.9039 0.0043 15.6007 0.0012 18.8910 0.0014 34°55′38.46″ 33°23′34.74″Cps07 Oph 2 Alt ** Clay Upper Cretaceous Volcanic sequence 38.9193 0.0031 15.6022 0.0012 18.9042 0.0014 34°55′38.46″ 33°23′34.74″Cps07 Oph 2 Rock Rock Upper Cretaceous Volcanic sequence 38.9415 0.0052 15.6065 0.0021 18.8841 0.0023 34°55′38.46″ 33°23′34.74″Cps07 Oph 20a Clay Upper Cretaceous Volcanic sequence 38.8180 0.0081 15.5899 0.0030 18.7703 0.0029 35°01′35.58″ 33°36′58.02″Cps07 Oph 20b Clay Upper Cretaceous Volcanic sequence 38.7845 0.0022 15.5821 0.0008 18.7092 0.0008 35°01′35.58″ 33°36′58.02″Cps08 69a Clay soil Upper Cretaceous Intrusive sequence 38.9611 0.0012 15.6529 0.0004 18.8775 0.0005 34°51′16.14″ 33°12′29.10″

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Table 2 Lead isotopic ratios of pottery sherds. 2se refers to 2 standard errors. * duplicate and** replicate. Pottery ware is indicated for each sample. Values in italic refer to measurements carried out using the

Neptune at Ghent University

Sample 208Pb/204Pb 2se 207Pb/204Pb 2se 206Pb/204Pb 2se

HST 2 Plain White Wheel-made II 38.9492 0.0022 15.6823 0.0008 18.8806 0.0010HST 6b Plain White Wheel-made II 38.9422 0.0021 15.6776 0.0008 18.8756 0.0009HST 6b ** 38.9517 0.0023 15.6796 0.0009 18.8791 0.0011HST 6f Plain White Wheel-made 38.9210 0.0023 15.6844 0.0008 18.9311 0.0010HST 6g Plain White Wheel-made II 38.9368 0.0024 15.6827 0.0008 18.8497 0.0008HST 6h Plain White Wheel-made II 38.9391 0.0022 15.6849 0.0008 18.8707 0.0009HST 32 Plain White Wheel-made 39.0250 0.0021 15.6840 0.0008 19.0295 0.0010HST 32 * 39.0257 0.0027 15.6837 0.0010 19.0305 0.0012HST 32 ** 39.0381 0.0025 15.6837 0.0010 19.0260 0.0011HST 33 Plain White Wheel-made 38.8012 0.0022 15.6754 0.0008 18.8226 0.0009HST 1a Plain White misfired 38.9791 0.0020 15.6869 0.0008 18.9080 0.0009HST 1b Plain White misfired 38.9606 0.0023 15.6803 0.0008 18.9054 0.0010HST 6c Coarse Wheel-made 38.9693 0.0022 15.6821 0.0008 18.8893 0.0009HST 6d Coarse Hand-made 38.9355 0.0026 15.6710 0.0009 18.8741 0.0010HST 4d White Slip II 38.9910 0.0034 15.6784 0.0012 18.9219 0.0009HST 13 White Slip IIA 38.9177 0.0030 15.6764 0.0012 18.8278 0.0013

38.9075 0.0009 15.6728 0.0009 18.8238 0.0011HST 16 White Slip II 38.9943 0.0031 15.6659 0.0011 18.9383 0.0013

38.9948 0.0011 15.6662 0.0011 18.9384 0.0014HST 17 White Slip II 38.9338 0.0029 15.6661 0.0010 18.8717 0.0012

38.9171 0.0010 15.6616 0.0010 18.8673 0.0013WS 14 White Slip II 39.0186 0.0023 15.6842 0.0009 18.9260 0.0010WS 17 White Slip II 39.0181 0.0031 15.6738 0.0012 18.9354 0.0015WS 27 White Slip II 39.0058 0.0029 15.6809 0.0011 18.9266 0.0012WS 28 White Slip II 39.0321 0.0023 15.6815 0.0008 18.9126 0.0010WS 29 White Slip II 39.0392 0.0019 15.6837 0.0008 18.9475 0.0009WS 33 White Slip II 38.0075 0.0026 15.6129 0.0010 18.1089 0.0010WS 33 * 38.0067 0.0024 15.6127 0.0009 18.1092 0.0010WS 35 White Slip II 38.8039 0.0025 15.6357 0.0009 18.8197 0.0011WS 36 White Slip II 38.7882 0.0018 15.6666 0.0007 18.7369 0.0008WS 37 White Slip II 39.0118 0.0023 15.6780 0.0009 18.9376 0.0010WS 38 White Slip II 39.0101 0.0027 15.6798 0.0010 18.9223 0.0011WS 39 White Slip II 38.9845 0.0017 15.6787 0.0006 18.9144 0.0007WS 40 White Slip II 39.0170 0.0018 15.6821 0.0007 18.9383 0.0007WS 43 White Slip II 39.0355 0.0021 15.6809 0.0008 18.9342 0.0009WS 51 White Slip II 39.0486 0.0021 15.6842 0.0008 18.9491 0.0010WS 53 White Slip II 39.0322 0.0022 15.6821 0.0008 18.9444 0.0009WS 58 White Slip II 39.0312 0.0025 15.6776 0.0009 18.9386 0.0010WS 59 White Slip II 39.0125 0.0020 15.6747 0.0007 18.9324 0.0009WS 60 White Slip II 38.9204 0.0021 15.6739 0.0008 18.8496 0.0009WS 61 White Slip II 39.0430 0.0024 15.6823 0.0009 18.9350 0.0011WS 62 White Slip II 39.0305 0.0023 15.6835 0.0008 18.9341 0.0009WS 63 White Slip II 39.0071 0.0027 15.6800 0.0010 18.9206 0.0013WS 65 White Slip II 38.9574 0.0023 15.6765 0.0009 18.8749 0.0011WS 66 White Slip II 39.0551 0.0019 15.6822 0.0007 18.9563 0.0008WS 69 White Slip II 39.0411 0.0025 15.6832 0.0009 18.9809 0.0012WS 70 White Slip II 39.0020 0.0026 15.6703 0.0010 18.9421 0.0011WS 70 ** 39.0053 0.0020 15.6700 0.0007 18.9439 0.0008

44 V. Renson et al.


field of the sedimentary rocks makes it possible to differentiate each formation (Fig. 3). Thelead isotopic composition of the Pleistocene terrace deposits ranges between 15.654 and15.668 and between 18.808 and 18.836 for 207Pb/204Pb and 206Pb/204Pb, respectively (Table 1).The carbonate-rich Holocene sediments present a lead isotopic composition similar to thesignature of the surrounding marls from the Pleistocene, Pliocene, Miocene and Palaeogene,which are overlapping. They range from 15.649 to 15.702 and from 18.723 to 19.066 for207Pb/204Pb and 206Pb/204Pb, respectively (Table 1). The lead isotopic composition of the soilsample collected in the Troodos Ophiolite area is clearly more radiogenic than the TroodosOphiolite signature (Table 1).

Table 2 (Continued)

Sample 208Pb/204Pb 2se 207Pb/204Pb 2se 206Pb/204Pb 2se

WS 74 White Slip II 39.0043 0.0024 15.6702 0.0009 18.9457 0.0011HST 4c Canaanite 38.6802 0.0019 15.6426 0.0007 18.8006 0.0008HST 21 Canaanite 38.9609 0.0026 15.6909 0.0009 19.0483 0.0010

38.9597 0.0012 15.6900 0.0012 19.0474 0.0014HST 22 Canaanite 39.0705 0.0026 15.7185 0.0011 18.9567 0.0011

39.0703 0.0010 15.7183 0.0010 18.9560 0.0012HST 22 ** 39.0683 0.0028 15.7164 0.0011 18.9567 0.0012HST 23 Canaanite 38.9866 0.0022 15.6795 0.0008 19.0884 0.0009

38.9866 0.0010 15.6800 0.0010 19.0874 0.0012HST 24 Canaanite 39.0212 0.0022 15.7045 0.0008 19.3279 0.0011

39.0193 0.0014 15.7038 0.0014 19.3271 0.0017HST 25 Canaanite 38.9611 0.0028 15.6873 0.0011 18.9864 0.0012

38.9563 0.0009 15.6860 0.0009 18.9840 0.0009HST 26 Canaanite 38.8782 0.0024 15.6794 0.0009 18.9871 0.0010

38.8738 0.0007 15.6780 0.0007 18.9849 0.0007HST 27 Canaanite 38.9692 0.0028 15.6933 0.0010 19.1728 0.0012

38.9730 0.0008 15.6948 0.0008 19.1741 0.0009HST 35 Canaanite 38.8758 0.0021 15.6754 0.0007 18.7952 0.0008HST 35 ** 38.8846 0.0024 15.6747 0.0010 18.7711 0.0011HST 38 Canaanite 38.9920 0.0023 15.7070 0.0008 19.3152 0.0010HST 39 Canaanite 38.6881 0.0021 15.6402 0.0008 18.7677 0.0009HST 42 Canaanite 39.0140 0.0022 15.6976 0.0010 19.0606 0.0012HST 43 Canaanite 38.9658 0.0017 15.6998 0.0006 19.2814 0.0006HST 44 Canaanite 39.0875 0.0029 15.7250 0.0010 18.9356 0.0014HST 47 Canaanite 38.9939 0.0025 15.6812 0.0010 19.0871 0.0011HST 51 Canaanite 38.6122 0.0026 15.6382 0.0011 18.6919 0.0011HST 54 Canaanite 38.9318 0.0024 15.6883 0.0007 19.0104 0.0008HST 56 Canaanite 38.9608 0.0021 15.6896 0.0008 19.0617 0.0008HST 57 Canaanite 38.9349 0.0018 15.7181 0.0007 19.7184 0.0008HST 60 Canaanite 38.9696 0.0018 15.6900 0.0007 19.0647 0.0008HST 3a Base-ring I 39.0846 0.0021 15.7104 0.0008 18.8081 0.0009HST 3a ** 39.0876 0.0195 15.7116 0.0007 18.8092 0.0008HST 10 Base-ring I-II 39.0897 0.0025 15.7102 0.0010 18.7964 0.0011

39.0930 0.0006 15.7117 0.0006 18.7977 0.0007HST 14 Base-ring II 39.0874 0.0027 15.7079 0.0011 18.7984 0.0012

39.0817 0.0010 15.7061 0.0010 18.7958 0.0011HST 15 Base-ring II 39.0775 0.0022 15.7081 0.0008 18.8031 0.0009

39.0639 0.0010 15.7031 0.0010 18.7966 0.0011



Pottery wares

Plain White Wheel-made and Coarse wares To define the elemental chemistry of the localproduction in HST, the clay matrix of three Plain White samples (HST 1b, HST 33 and HST 32)was analysed by SEM-EDX. In sample HST 1b (misfired) and sample HST 33, the CaO contentis high and varies between 11.9 and 40.1 wt%, while the SiO2 and Al2O3 contents range between36.2 and 70.4 and between 8.9 and 16 wt% respectively (Table 3). Sample HST 32 presents alower CaO content (between 4.8 and 8.7 wt%) than the two other Plain White analysed. There isa clear negative correlation between CaO and SiO2+Al2O3+K2O, which are the major constituents

T.O.

Perapedhi Ft.umbers + shales

19.00 19.5018.5018.0015.50

15.55

15.60

15.65

15.70

15.75

207 P

b/20

4 Pb

206Pb/204Pb

C.T.S.

Volcanic sequence+ weathering products

Figure 2 207Pb/204Pb versus 206Pb/204Pb three-isotope plot for selected sediments and rocks (n = 65). T.O. field representsTroodos Ophiolite rocks, sulphides and umbers (Gale et al., 1981; Spooner and Gale, 1982; Hamelin et al., 1984, 1988).Grey areas within the Troodos Ophiolite represent four samples of shales and umbers collected in the PerapedhiFormation and five rocks and clays collected in the volcanic sequence measured in this study, respectively. C.T.S. fieldrepresents Circum Troodos Sediments: the soil collected in the T.O., samples from the Moni, Lefkara, Pakhna, Nicosia,Apalos-Athalassa Kakkarista Formations, from the Pleistocene Marine Terrace and the Holocene.

1

2

3

4

6

15.64

15.66

15.70

19.2019.0018.60 18.80

15.68

206Pb/204Pb

207 P

b/20

4 Pb

5

Figure 3 207Pb/204Pb versus 206Pb/204Pb three-isotope plot for Plain White, Coarse and misfired sherds and the sedimentscollected within 20 km around the site (samples from the Troodos Ophiolite have been removed for clarity). Fields: (1)Lefkara formation; (2) Holocene sediments; (3) Pleistocene Marine Terrace; (4) Nicosia formation; (5) Apalos-AthalassaKakkarista formation; (6) Pakhna formation. White circles represent Plain White, Coarse and misfired sherds.

46 V. Renson et al.


Table 3 Major element composition as obtained by SEM-EDX analysis of selected Plain White and White Slip sherds from HST. Total iron as FeO. Values in wt%. Tracesof Cu2O, ZrO2 and BaO have been detected in some samples and are reported as they were above the detection limits (0.15 wt% for elements above Na)

SiO2 TiO2 Al2O3 FeO MnO MgO CaO Na2O K2O P2O5 Cu2O ZrO2 BaO Total

PW SH 1b 49.8 0.9 14.5 4.1 0.0 4.7 22.6 2.1 1.0 0.0 0.20 0.0 0.0 100.0PW SH 1b 52.0 1.5 12.8 4.5 0.0 6.8 19.5 1.9 1.1 0.0 0.00 0.0 0.0 100.0PW SH 1b 45.6 1.6 12.7 5.8 0.0 8.8 25.0 0.5 0.0 0.0 0.00 0.0 0.0 100.0PW SH 1b 36.2 0.5 8.9 2.3 0.0 6.9 40.1 1.6 0.0 3.6 0.00 0.0 0.0 100.0PW SH 1b 43.8 0.8 13.4 3.9 0.0 3.8 29.3 2.4 1.0 1.7 0.00 0.0 0.0 100.0

PW HST 32 63.2 1.3 19.1 4.3 0.0 2.4 6.6 0.6 2.1 0.0 0.0 0.4 0.0 100.0PW HST 32 65.5 1.4 17.6 2.8 0.0 2.0 7.6 1.6 1.6 0.0 0.0 0.0 0.0 100.0PW HST 32 67.3 1.3 15.0 3.2 0.0 2.5 8.1 0.5 1.4 0.0 0.0 0.7 0.0 100.0PW HST 32 69.7 0.8 13.2 2.7 0.0 1.9 8.7 0.8 1.3 0.0 0.0 0.6 0.0 100.0PW HST 32 64.5 1.1 16.6 5.9 0.0 2.2 7.8 0.6 1.2 0.0 0.0 0.0 0.0 100.0PW HST 32 72.0 1.3 13.9 2.4 0.3 1.4 6.3 1.1 1.3 0.0 0.0 0.0 0.0 100.0PW HST 32 79.8 0.8 10.0 1.9 0.0 1.2 4.8 0.4 0.8 0.0 0.0 0.4 0.0 100.0

PW HST 33 54.3 0.4 11.3 1.3 0.0 1.3 29.8 0.0 0.9 0.0 0.0 0.0 0.6 100.0PW HST 33 52.1 0.0 16.0 5.0 0.0 3.1 20.7 0.4 1.8 1.0 0.0 0.0 0.0 100.0PW HST 33 64.9 0.0 14.3 4.2 0.0 2.6 11.9 0.5 1.5 0.0 0.0 0.0 0.0 100.0PW HST 33 55.8 0.0 14.7 3.6 0.0 2.7 20.5 1.1 1.6 0.0 0.0 0.0 0.0 100.0PW HST 33 59.2 0.0 15.7 4.5 0.0 2.8 15.2 0.6 2.1 0.0 0.0 0.0 0.0 100.0PW HST 33 70.4 0.0 10.5 2.7 0.0 1.8 12.7 0.0 1.3 0.6 0.0 0.0 0.0 100.0

WS 33 60.6 0.0 16.9 4.8 0.0 13.2 2.5 1.1 0.9 0.0 0.0 0.0 0.0 100.0WS 33 67.2 0.0 17.8 4.1 0.0 5.8 3.3 1.1 0.7 0.0 0.0 0.0 0.0 100.0WS 33 64.4 0.0 20.7 0.6 0.0 3.0 2.7 7.6 1.0 0.0 0.0 0.0 0.0 100.0WS 33 59.9 0.4 23.9 3.8 0.0 4.8 4.1 2.4 0.8 0.0 0.0 0.0 0.0 100.0WS 33 59.7 0.0 22.0 4.8 0.0 8.5 3.4 0.9 0.7 0.0 0.0 0.0 0.0 100.0

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Table 3 (Continued)

SiO2 TiO2 Al2O3 FeO MnO MgO CaO Na2O K2O P2O5 Cu2O ZrO2 BaO Total

WS 35 60.6 0.7 21.0 6.8 0.0 4.7 2.6 3.2 0.4 0.0 0.0 0.0 0.0 100.0WS 35 67.6 0.0 20.7 0.3 0.0 0.4 0.9 8.7 1.3 0.0 0.0 0.0 0.0 100.0WS 35 58.3 2.1 21.2 6.2 0.0 4.1 3.1 4.6 0.4 0.0 0.0 0.0 0.0 100.0WS 35 76.5 0.0 14.7 0.2 0.0 0.0 2.3 6.1 0.1 0.0 0.0 0.0 0.0 100.0WS 35 53.5 0.5 23.8 11.1 0.0 7.1 3.2 0.5 0.3 0.0 0.0 0.0 0.0 100.0WS 35 49.7 1.1 21.3 11.0 0.5 12.0 2.9 0.7 0.8 0.0 0.0 0.0 0.0 100.0

WS 36 58.7 0.3 25.9 4.9 0.0 5.7 2.9 0.8 0.8 0.0 0.0 0.0 0.0 100.0WS 36 56.7 0.0 27.4 1.4 0.0 1.7 9.7 3.1 0.1 0.0 0.0 0.0 0.0 100.0WS 36 62.1 0.2 23.1 3.4 0.0 3.1 3.2 4.1 0.8 0.0 0.0 0.0 0.0 100.0WS 36 60.3 0.0 25.0 0.4 0.0 0.6 7.0 5.7 1.0 0.0 0.0 0.0 0.0 100.0WS 36 66.2 0.0 21.6 2.5 0.0 2.3 3.0 2.6 1.6 0.0 0.0 0.0 0.0 100.0

WS 58 59.1 0.6 24.1 5.7 0.0 5.0 3.4 1.3 0.8 0.0 0.0 0.0 0.0 100.0WS 58 56.2 0.3 24.7 6.6 0.0 8.7 1.7 0.8 1.1 0.0 0.0 0.0 0.0 100.0

WS 62 57.2 0.8 26.4 7.7 0.0 4.0 1.9 1.2 0.9 0.0 0.0 0.0 0.0 100.0WS 62 60.6 0.0 26.3 4.3 0.0 1.9 3.4 3.5 0.0 0.0 0.0 0.0 0.0 100.0WS 62 52.6 0.0 31.6 7.8 0.0 6.7 0.6 0.7 0.0 0.0 0.0 0.0 0.0 100.0WS 62 59.9 0.0 25.3 0.5 0.0 0.0 8.4 5.9 0.0 0.0 0.0 0.0 0.0 100.0WS 62 65.6 0.0 24.0 1.2 0.0 0.7 2.0 6.6 0.0 0.0 0.0 0.0 0.0 100.0

WS 74 69.7 0.0 20.1 0.6 0.0 0.4 3.1 3.6 2.6 0.0 0.0 0.0 0.0 100.0WS 74 64.1 0.6 20.8 5.8 0.0 1.9 2.7 3.1 0.9 0.0 0.0 0.0 0.0 100.0

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of clay minerals in the matrix of the three sherds (Fig. 4). Moreover, in these three samples (HST1b, HST 32 and HST 33), the elemental mapping shows that Ca is distributed in the matrix andalso appears to be concentrated in areas depleted in Si and Al (Fig. 5 (a)). This indicates thatthe clay used for their production was a mixture between a calcareous and an alumino-silicatecomponent.

The misfired sherds, the Plain White ware and the Coarse ware have been selected to define thelead isotopic composition of the local production in HST. The two misfired Plain White sherdspresent a similar isotopic composition and fall within the field of the Plain White and Coarsewares (Fig. 6). The lead isotopic composition of this assemblage displays values ranging from15.671 to 15.687 for 207Pb/204Pb and from 18.823 to 19.029 for 206Pb/204Pb (Table 2). This verynarrow range of variability forms a cluster within the population of 66 sherds (Fig. 6), probablyindicating a similar source material for these pottery wares.

It is commonly admitted that potters did not generally collect clays far from the production site(Rice 1987). The composition of the Plain White and the Coarse wares matches the isotopicsignature of the marls from different formations (Apalos-Athalassa Kakkarista Ft., Nicosia Ft.,Pakhna Ft. and Lefkara Ft.) and Holocene sediments, readily available in the surroundings of theHST site (Fig. 3). The mineralogy of these sediments fits the chemistry of the Plain White sherdsanalysed in this paper. Consequently, we infer: (1) that local carbonate clays were used forcommon pottery production in HST during the Late Bronze Age; and (2) that no foreign clayseems to have been added. Therefore the cluster of the Plain White and the Coarse wares definesthe characteristic lead isotopic fingerprint of the HST production. This local (HST) fingerprintcan be compared with other sherd assemblages, such as Canaanite, White Slip and Base-ringwares.

The Canaanite ware Petrographical studies and elemental analysis show that Canaanite jarscould originate from many different regions (Israel, Syria, Lebanon, Turkey, Cyprus) in theEastern Mediterranean (Åstrom 1991; Serpico 2008). Among the numerous Canaanite waresexcavated at HST, different fabrics have been identified (Åstrom 1991; Eriksson 1995). Sherds

0

5

10

15

20

25

30

35

40

45

40 50 60 70 80 90 100

CaO

(w

t%)

SiO2+Al2O3+K2O (wt%)

Figure 4 CaO versus SiO2+Al2O3+K2O biplot showing the different trends between sherds displaying analumino-silicated matrix (White Slip sherds, shown here as black dots) and those characterized by a more calcareousmatrix (Plain White sherds, shown here as black crosses).



from HST were previously analysed by neutron activation analysis, and it was suggested thatthese sherds came from pottery partly made in Cyprus and partly imported from Ugarit andCilicia (Raban 1980; Åström 1991). The lead isotopic composition of the 20 Canaanite sherdsdisplays a large variability for 207Pb/204Pb and 206Pb/204Pb ratios (Fig. 6). The values range from15.638 to 15.725 and from 18.692 to 19.718, respectively (Table 2), and most of the Canaanitesherd values plot out of the cluster drawn by the local HST production (Fig. 6). The observed leadisotopic variability probably reflects different origins for the Canaanite sherds excavated at HST.However, as the lead isotopic composition of four Canaanite sherds (HST 25, HST 26, HST 35and HST 54) plots relatively close to the cluster of local pottery, the possibility that they were partof locally made Canaanite pots cannot be excluded. A closer petrographical and mineralogicalexamination of the 20 Canaanite sherds is in progress and will be combined with lead isotopicanalysis to further assess whether a specific fabric can be associated with a specific lead isotopiccomposition. In addition, more lead isotope analyses of Canaanite samples from localities withinCyprus and the Eastern Mediterranean region could shed light on the exact provenance of theforeign Canaanite pottery recovered at HST.

The White Slip ware Previous studies suggested that the basaltic clays used to produce WhiteSlip differed from the clays used to make the other Cypriot pottery wares and probably originatedfrom the surroundings of the Troodos Ophiolite (Courtois 1970; Artzy et al. 1981). The elementalcomposition showed that, although White Slip represented a consistent group, some chemicalvariability could appear within this pottery ware (Knapp and Cherry 1994 and references therein).

Figure 5 (a) Ca, Si and Al elemental mapping of a Plain White sherd (HST 1b); (b) Ca, Si and Al elemental mappingof a White Slip sherd (WS 58). Data obtained using SEM-EDX.

50 V. Renson et al.


Archaeological evidence has led to the proposal of Sanidha, a site located in the southern foothillsof the Troodos Ophiolite, as a production site of White Slip pottery (Todd and Hadjicosti 1991;Todd et al. 1992; Todd and Pilides 1993). Previous elemental analysis and mineralogical studiesshowed that the composition of White Slip II sherds from Sanidha corresponds to that of claysources collected in the Troodos and its periphery: namely, highly weathered gabbros collectedin the surroundings of Sanidha and an alluvial clay from the nearby Vasilikos valley (Rautmanet al. 1993; Gomez et al. 1995).

A set of 30 White Slip sherds excavated at HST were analysed to identify their lead isotopiccomposition and compare it with the composition of different clay sources. Moreover, the claymatrix of six White Slip samples has been analysed by SEM-EDX.

These chemical analyses show that the White Slip sherds from HST present an alumino-silicatematrix (Fig. 5 (b) and Table 3). The White Slip samples display a low to intermediate CaOcontent (0.6%–9.7%) and relatively high SiO2 and Al2O3 contents (49.7–76.5wt% and 14.7–31.6wt%, respectively). Large variations in FeO, MgO and Na2O are also present, between 0.2and 11.1wt%, 0 and 13.2wt%, and 0.5 and 8.7wt%, respectively. In White Slip sherds, CaO doesnot correlate with SiO2+Al2O3+K2O (Fig. 4). A weak correlation coefficient was calculated(R2 = 0.0003). The elemental mapping shows that most of the Ca content appears to be concen-trated in the alumino-silicate clay matrix (Fig. 5 (b)). The elemental composition of these sherdsis compatible with that of basaltic rocks and clays derived from their weathering (smectitegroup). The large elemental variations could reflect the presence of fresh minerals in the matrixand in the clay used for the White Slip production.

15.60

15.62

15.64

15.66

15.68

15.70

15.72

15.74

18.00 18.20 18.40 18.60 18.80 19.00 19.20 19.40 19.60 19.80

Plain White Wheel-made

Plain White Misfired

Coarse

White Slip

Canaanite

Base-ring

206Pb/204Pb

207 Pb/2

04Pb

Figure 6 207Pb/204Pb versus 206Pb/204Pb three-isotope plot for the 65 sherds from HST.



Most of the White Slip sherds analysed (28/30) plot in the same part of the diagram and displayvalues ranging from 15.666 to 15.684 for 207Pb/204Pb ratio and from 18.737 to 18.981 for206Pb/204Pb ratio (Fig. 6 and Table 2). Two samples show a clearly different lead isotopic com-position, displaying lower values for both the 207Pb/204Pb and 206Pb/204Pb ratios (WS 33) or for207Pb/204Pb ratio only (WS 35). This implies that the majority of the White Slip found at HSTcould originate from a common source presenting some internal variability (Fig. 6). The WhiteSlip field partly overlaps the lead isotopic signature of different marls and Holocene sedimentsand the clays from the Moni formation (Fig. 7). Considering that the White Slip sherds are clearlydominated by alumino-silicate material, it is unlikely that the CaCO3-rich marls and Holocenesediments provided the clay used for the White Slip production. Moreover, the lead isotopiccomposition of most of the White Slip sherds analysed is clearly more radiogenic than theTroodos Ophiolite field, including several gabbros (Fig. 7). If the clay source used in White Slipproduction is a weathered gabbro, as proposed in Gomez et al. (1995), it implies that either thereis an isotopic fractionation between the rock and its weathering product or it has been mixed withanother type of clay presenting a significantly more radiogenic isotopic signature. An isotopicfractionation linked to the weathering is likely, as already shown by leaching experiments inbasalts (e.g., Hanano et al. 2009). The fractionation between the gabbros and their derived clayswill be analysed in a follow-up study that will compare the lead isotopic composition of the WhiteSlip sherds with the composition of clays outcropping in the surroundings of Sanidha, includingthe alteration products of the gabbros. Gomez et al. (1995) also proposed the alluvial clay fromthe Vasilikos valley as a potential source. It does represent a natural mix of different materials thatcould provide a lead isotopic signature divergent from that of the Troodos Ophiolite, but itremains to be confirmed. Finally, according to lead isotope ratios, the Moni formation provides

15.60

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19.2019.0018.60 18.80

15.64

15.68

206Pb/204Pb

207 P

b/20

4 Pb

TROODOSOPHIOLITE

Figure 7 207Pb/204Pb versus 206Pb/204Pb three-isotope plot for White Slip and Base-ring sherds and sediments. Blacksquares, Lefkara, Pakhna, Nicosia, Apalos-Athalassa Kakkarista formations, Pleistocene Marine Terrace and Holocenesediments; white diamonds, Moni formation; white circle, soil from the Troodos Ophiolite area; black cross, White Slipsherds; plus sign, Base-ring sherds.

52 V. Renson et al.


another potential clay source. Its precise mineralogy and geochemistry will be compared withthat of the White Slip to confirm or refute this possibility.

The Base-ring ware Elemental analysis and petrographical studies proposed a single, but stillunidentified, clay source for Base-ring production (Artzy et al. 1981; Courtois 1981; Vaughan1994). Vaughan (1994) suggested three potential source areas: (1) the Kythrea Flysh (located inthe Kyrenia Range in northern Cyprus); (2) the Pakhna formation and the Moni formation;and (3) the Mamonia Complex and the Kannaviou Formation (south-west Cyprus). By usingpetrography and elemental analysis, Courtois (1981) also proposed the Kyrenia Range and theMamonia complex as potential source areas and suggested that the Troodos Ophiolite and itsderived sediments were unlikely to be the source of Base-ring ware.

The four Base-ring sherds analysed in this study show similar isotopic compositions (from15.708 to 15.710 and 18.796 and 18.808 for 207Pb/204Pb and 206Pb/204Pb ratios, respectively),corroborating the results of geochemical and petrographical studies pointing to a unique rawmaterial source for Base-ring ware (Table 2 and Fig. 6). The 207Pb/204Pb values measured inBase-ring ware are more radiogenic than the values obtained for the local HST fingerprint and forthe marls and Holocene sediments in the HST surroundings (Fig. 7). This range of values forBase-ring ware does not correspond to the lead isotopic composition of any clay analysed so farin south-east Cyprus, despite the broad selection investigated in this study. Since both the Pakhnaand Moni sediments, and even a mix of the two sources, display a much lower 207Pb/204Pb ratiothan the Base-ring sherds, it is unlikely that these sediments provided the raw clay used forBase-ring production. The composition of the Mamonia Complex and the Kyrenia Range,proposed as potential source areas by Courtois (1981), differ from each other, from the TroodosOphiolite and from its surrounding rocks and sediments. The Mamonia complex is an assemblageof sedimentary, metamorphic and igneous rocks from the Middle Triassic to the Upper Creta-ceous that was tectonically ‘attached’ to the Troodos Ophiolite during the Maastrichtian (GSD2009a). The Kyrenia Range is an assemblage of Permian to recent sedimentary rocks, and morerarely of metamorphic and igneous rocks, that was emplaced in the northern part of the TroodosOphiolite during the end of the Miocene (GSD 2009b). Part of their constitutive rocks issignificantly older than the Ophiolite. Thus, although these lithologies have not yet been analysedfor their lead isotopic composition, they are compatible as a source since they are likely to yieldmore radiogenic values that those of the Troodos Ophiolite.

The homogeneous lead isotopic composition of the Base-ring makes it possible to furtherrefine the source of the Base-ring. It eliminates the Troodos Ophiolite and circum TroodosOphiolite sediments as potential clays source for Base-ring production. Further analyses willhopefully provide a good tool to distinguish between the two other sources proposed in theliterature (Courtois 1981; Vaughan 1994). This will require detailed clay sampling in theMamonia Complex and the Kyrenia Range areas and a comparison with the Base-ring compo-sition. As the Base-ring composition is homogeneous, it should fit precisely with a unique claysource composition.

CONCLUSIONS

The local (HST) production was identified by first comparing the lead isotope values of twomisfired Plain White Wheel-made sherds with those of seven other Plain White sherds and twoCoarse samples. As all 11 sherds form a cluster within the population of 65 sherds, it may beinferred that a similar source material was used for the production of these pots. Second, by



comparing the lead isotope values of these sherds with those of local clay sources such as themarls and the Holocene sediments available in the surroundings of the site, the local (HST)fingerprint could be defined.

The lead isotopic composition of Canaanite sherds presents a large variability that reflectsdifferent origins, as expected from the literature. Nevertheless, the lead isotopic composition offour Canaanite sherds, which plot relatively close to the local (HST) fingerprint, could indicatethat these Canaanite pots were locally produced in HST.

The lead isotope ratios reflect the common clay source used for White Slip production andpropose the Moni formation as a potential raw material. Further investigations coupling leadisotopes, mineralogy and elemental analysis should allow refining hypotheses on the provenanceof clay sources of White Slip ware.

Lead isotopic analysis can be successfully applied to identify the unique and homogeneouscomposition of Base-ring ware and to eliminate any source within the Troodos Ophiolite and thecircum Troodos Ophiolite sediments. Planned isotopic analysis of clays from the MamoniaComplex and the Kyrenia Range should enable identification of the sources used for Base-ringproduction

The above investigation of four pottery wares found at HST demonstrates that using leadisotope analyses is a useful additional tool in pottery provenance studies. As several sherds and/orparent material can have similar mineralogical, elemental and/or lead isotopic compositions, amultiproxy approach on pottery and parental material should be used as much as possible infuture provenance studies. In our case, future investigations will be focused on White Slip sherdsfrom various sites and further potential clay sources, in order to refine its composition and origin.Ideally, as the application of lead isotope analysis to ceramics becomes more and more common,a broad database of Mediterranean pottery and potential raw material should documentexchanges of this commodity within the Eastern Mediterranean.

ACKNOWLEDGEMENTS

This study is supported by the Research Foundation Flanders (FWO grants KN137 to KarinNys and G.0585.06 to Philippe Claeys and Frank Vanhaecke) and the Research Council of theVrije Universiteit Brussel (grant HOA11 to Karin Nys and Philippe Claeys). We are verygrateful to the late Professor Paul Åström for his unremitting enthusiastic support. We alsowarmly thank the following: Dr Flourentzos, Director of the Department of Antiquities,Cyprus, for granting export permission for the sherds from Hala Sultan Tekke-Vyzakia; Pro-fessor Niceas Schamp, Permanent Secretary of the Royal Flemish Academy of Belgium forScience and the Arts, for providing the facilities used for writing the first draft of this manu-script; Claude Maerschalk and Jeroen DeJonghe (Université Libre de Bruxelles), for their help,explanations and advice during the laboratory work and the measurements on the MC–ICP–MS; Kris Latruwe and Ellen Dewaele (Ghent University), for the measurements on theNeptune; Oscar Steenhaut and Kamal Kolo (Vrije Universiteit Brussel), for the time they spentexplaining and helping during the measurements on the SEM-EDX; Frédéric Hatert (Univer-sity of Liège), for help with the interpretation of some of the XRD spectra and for providingcomplementary analyses; and François De Vleeschouwer (University of Liège), for his help inthe realization and presentation of some figures and his advice and support during the writing.Comments from the managing editor, Mark Pollard, and two anonymous reviewers greatlyimproved this manuscript.

54 V. Renson et al.


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