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1 Lead Isotope Ratios of Lead Objects Excavated from Kaman-Kalehöyük Junko ENOMOTO and Yoshimitsu HIRAO Tokyo Oita INTRODUCTION In this study, lead isotope analysis was applied to lead artifacts excavated from Kaman-Kalehöyük. The purposes of this study are to understand the nature of these metal products and how they were processed, to determine which mines the raw materials originated from, and to propose trading systems of these materials. Lead isotope analysis has proved to be a useful tool for provenance studies of archaeological copper and lead objects. Lead isotope ratios in copper and lead ores are influenced by the geologic history of each ore deposit, such as ore forming processes or crust forming processes. Therefore, lead isotope ratios of ores from different copper or lead mines will differ from each other according to the different geologic history of each mine. In addition, as lead isotope ratios do not change by heating, oxidation and reduction, the values in processed copper products will suggest the mine from which the raw material originated. The Kaman-Kalehöyük site is divided into four main stratigraphic sequences. In previous studies, copper objects from the different levels were sampled for lead isotope analysis, and a hypothetical diagram was postulated from the results (Fig.1: Hirao and Enomoto 1993). Since that time, as excavation has proceeded and more data of lead isotope ratios has been accumulated (Fig.2), data distribution has become too complicated to understand. Therefore, in order to better understand the data trends, we decided to measure lead isotope ratios of only the lead artifacts from the site, as a precursor to the study of copper products. Analysis of the lead items is somewhat more straightforward than analysis of the copper artifacts: (1) Only a small sample size is required (less than 1mg) for the analysis. (2) There is little risk that the lead isotope value will be changed by contamination from soil and other materials. (3) The different lead isotope ratios reflect different Fig.1 Generalized lead isotope diagram for the distribution of copper objects excavated from Kaman-Kalehöyük ( A type figure). Fig.2 Distribution of lead isotope ratios of copper, bronze, and lead objects excavated from Kaman-Kalehöyük between 1986 and 2002 ( A type figure).

2 224 J. ENOMOTO and Y. HIRAO AAS XV Map 1 Map 2

3 2006 Lead Isotope Ratios of Lead Objects 225 mine proveniences. In other words, only the ores that have experienced the same geologic history show similar values. Different geological sites are unlikely to show the same isotope ratios. (4) The lead samples do not require pre-treatment in the chemical analysis process, such as removal of other elements, which takes hours and may cause errors. The present paper includes new results, and the results from previous studies (Enomoto and Hirao 1992; 1999; 2001). ratios were measured with a Thermo-Electron MAT262 surface ionization mass spectrometer equipped with multiple collectors. The rhenium filament with the lead sample was placed in the machine and evacuated to high vacuum. The filament was gradually heated passing current through it. At a temperature of approximately 1200 degrees C, the beam conditions settled, 20 lead isotope ratios were measured three times, and all the ratios were calculated for the averages. The isotope ratios obtained were normalized to the lead standard NBS-SRM-981 for each run (Hirao and Mabuchi 1989). SAMPLES All samples are from lead artifacts excavated at Kaman-Kalehöyük. A small sample was removed from each object and brought to Japan with permission from the Turkish government. Previous analysis includes: 24 samples in 1997 (Enomoto and Hirao 1999), 25 samples in 1998 (Enomoto and Hirao 2001), and 1 sample in 1989 (Hirao et al. 1992). ANALYSIS Measurement of lead isotope ratios Lead isotope ratios of the samples excavated from Kaman-Kalehöyük were measured using a surface ionization mass spectrometer after the lead was purified by the following chemical procedure (Hirao et al. 1992). A small part of each sample was dissolved with 5 to 6 drops of nitric acid and then diluted to 5 to 10 ml. Lead in the solution was separated by an electro-deposition method using 2V and approximately 10 ma of direct current and using platinum electrodes. Lead accumulated on the platinum plate anode as lead peroxide in a few hours, then was dissolved with a few drops of nitric acid and hydrogen peroxide in a different bottle. The lead solution was diluted to 2 to 10 ml and the lead concentration was measured with a graphite furnace atomic absorption spectrometer. Then about 0.1 microgram of lead was taken out and placed on a rhenium filament for mass spectrometry with a phosphoric acid - silica gel method. Lead isotope RESULTS AND DISCUSSION Lead isotope ratio values of the 97 new samples and 50 previously published samples are listed in Table 1. The first two numbers of each sample number indicate the year in which the sample was excavated; L signifies a lead product. Maps 1 and 2 show lead ore sample locations. Photos 001 through 096 show the unpublished samples. In this study, the lead isotope ratio values are plotted in A and B type figures: in an A type figure, the horizontal axis is 207 Pb/ 206 Pb and the vertical axis is 208 Pb/ 206 Pb, and in a B type figure, the horizontal axis is 206 Pb/ 204 Pb and the vertical axis is 207 Pb/ 204 Pb. These two types of figures show the relationship between four lead isotopes. All of the lead isotope ratio values of the samples analyzed are plotted in Fig. 3 in an A type figure. In this figure, the samples mainly concentrate in four groups. However, in a B type figure, Fig. 4, five to seven groups can be identified. Therefore, it is proposed that in the Kaman-Kalehöyük sample set there are five to seven distinct lead material types. These seven groups are labeled areas A to G in Fig. 5 and in all the other A type figures, corresponding to areas A to G in Figure 4 and in all the other B type figures in this report. In the first series of figures in this report, areas A (A ) to G (G ) are compared to published values of lead ore (e.g., galena, sphalerite) and slag from Turkey, in order to estimate the sources of the Kaman-Kalehöyük lead materials. Hirao et al. (1995), Enomoto et al. (1999) and Yener et al. (1991) have

4 226 J. ENOMOTO and Y. HIRAO AAS XV Fig.3 Distribution of lead isotope ratios of lead objects excavated from Kaman-Kalehöyük between 1986 and 2000 ( A type figure). reported on the lead isotope values of slag and ore samples from mines in Turkey. As these mine samples were collected from only a few areas of Turkey, it will be difficult to conclude the origins of the Kaman-Kalehöyük samples with certainty, but some possibilities can be proposed. Lead isotope ratios of the lead ores and slag examined for this study are shown in Fig. 6 (type A) and Fig. 7 (type B). Table 2 indicates how many samples were obtained from each area. In an A type figure plotting lead ore samples, ores from Çanakkale in western Turkey, the North Anatolian Mountains, and the area from Kozan to Tufanbeyli east of the Ala Mountains (Alada lar ) have a 207 Pb/ 206 Pb value higher than None of the lead Fig.4 Distribution of lead isotope ratios of lead objects excavated from Kaman-Kalehöyük between 1986 and 2000 ( B type figure). Five to seven groups are indicated (areas A ~G ). Fig.6 Distribution of lead isotope ratios of lead minerals in Turkey ( A type figure). The values of are from Yener et al. (1991). T.B.K. () are obtained by our measurements (1999). Fig.5 Distribution of lead isotope ratios of lead objects excavated from Kaman-Kalehöyük between 1986 and 2000 ( A type figure). Groups A - G correspond to areas A - G in Fig. 4. Fig.7 Distribution of lead isotope ratios of lead minerals in Turkey ( B type figure). The values of are from Yener et al. (1991). T.B.K. () are obtained by our measurements (1999).

5 2006 Lead Isotope Ratios of Lead Objects 227 items from Kaman-Kalehöyük have these high values, so it is thought that Kaman-Kalehöyük did not have a deep relationship with the North Anatolian Mountains and areas over the Ala Mountains. The lead samples excavated from Kaman-Kalehöyük are distributed mainly in the range of to in the 207 Pb/ 206 Pb of a type A figure, so this range was looked at in detail. In the second series of figures, the relationship between lead isotope ratio and date was examined by plotting the samples according to the excavation stratum in which they were found. The site of Kaman-Kalehöyük has four main stratigraphic levels. From the top, Stratum IisOttoman period, Stratum II is Phrygian period, Stratum III is Hittite period and Stratum IV is the period before the Hittites. The number of samples from Stratum I was so small that those samples are excluded from the discussion in this article. In the figures, or indicates ores or slag, indicates samples from Stratum II, indicates samples from Stratum III, indicates samples from Stratum IV and indicates samples whose classification is still unclear. Kaman-Kalehöyük Samples Compared to Ore Samples Area A in Fig. 5 (area A in Fig. 4) Area A in Fig. 5 (area A in Fig. 4) is enlarged in Fig. 8 (Fig. 9). Samples from Kaman-Kalehöyük (solid line) are closely distributed within the range of ore samples from the Bolkar Mountains (Bolkarda lar ) (dotted line) which is called Taurus 1A by Yener. Samples indicated with a black square, gray and white square in Fig. 8 and Fig. 9 include the Taurus 1A group and ores and slag from Ulk flla/madenköy and the Bolkar Mountains (Yener et al. 1991; Hirao et al. 1995). This may indicate that Kaman-Kalehöyük received raw lead materials from an area in the Bolkar Mountains. Yener et al. (1991) reported that four samples in their analysis were slag samples found at ancient metal working sites near Ulk flla. In Fig. 8 and 9, these slag samples are indicated with a white square. Onthe other hand, ores from Ulk flla/madenköy analyzed by TBK (Tokyo Bunkazai Kenkyujo (in Japanese) or Tokyo National Research Institute of Cultural Properties) are indicated with a gray Hirao,Y., J. Enomoto and H.Tachikawa The isotope ratios of ores near Madenköy coincide with those of slag collected from the metal working sites and of samples excavated from Strata between IIa and IIIb at Kaman-Kalehöyük. Fig.8 Area A of Fig. 5 is enlarged ( A type figure).,, and indicate samples excavated from Stratum II, III, and undecided, respectively. white square indicates minerals obtained from a metalworking site by Yener et al. (1991). (gray square) indicates minerals obtained from Ulk flla by T.B.K. (black square) indicates the other minerals. The dotted line area indicates Taurus 1A reported by Yener et al. (1991). The solid line area indicates excavated samples from Kaman-Kalehöyük. Fig.9 Area A of Fig. 4 is enlarged ( B type figure)., and indicate samples excavated from Stratum II, III, and undecided, respectively. white square indicates minerals obtained from a metalworking site by Yener et al. (1991). (gray square) indicates minerals obtained from Ulk flla by T.B.K. (black square) indicates the other minerals. The dotted line area indicates Taurus 1A reported by Yener et al. (1991). The solid line area indicates samples excavated from Kaman-Kalehöyük.

6 228 J. ENOMOTO and Y. HIRAO AAS XV Area B in Fig. 5 (area B in Fig. 4) Area B in Fig. 5 (area B in Fig. 4) is enlarged in Fig. 10 (Fig. 11). In Fig. 5, area B is included in a larger unit with areas C, D, and E, but in Fig. 4, area B is clearly different from the other areas. Area B is made up of 27 samples closely clustered together, and as Table 2 shows, 22 of the samples were excavated from early periods, Strata between IV and IIIb. It is not yet clear where these lead materials originated. However a piece of slag obtained from Fig.10 Areas B - E of Fig. 5 are enlarged ( A type figure).,,, indicate samples excavated from Stratum II, III, IV, and undecided, respectively. indicates minerals. The dotted line area indicates Taurus 1B from Yener et al. (1991). Fig.11 Areas B - E of Fig. 4 are enlarged ( B type figure).,,, indicate samples excavated from Stratum II, III, IV and undecided, respectively. indicates minerals. The dotted line area indicates Taurus 1B from Yener et al. (1991). Kültepe included in this area was observed in a report by Hirao,Y., J. Enomoto and H.Tachikawa (1995). This may indicate that the lead of this isotope composition (area B) reached Kaman-Kalehöyük through a relationship with Kültepe, a major site not far from Kaman-Kalehöyük. The Kaman-Kalehöyük samples are mainly between Stratum IV and IIIb. Only a few samples were excavated from the later level, raising the question as to why the supply of this lead material stopped after the Stratum IIIb period. Analysis of more samples from Kültepe may provide further information on the trade relationships between Kaman-Kalehöyük and Kültepe. Area C in Fig. 5 (area C in Fig. 4) Area C in Fig. 5 (area C in Fig. 4) is enlarged in Fig. 10 (Fig. 11). In Fig. 5, it is difficult to delineate area C, because the sample distribution forms a relatively large domain together with areas B, D, and E. However, when Fig. 5 is enlarged to Fig. 10 and area B is excluded, it becomes clear that area C distributes to the left of area B, and in Fig. 11, a clear grouping is apparent. In Fig. 10, area C partially overlaps the area reported as Taurus lb by Yener, while in Fig. 11, area C is distinct from Taurus lb, so the samples are not included in Yener s classification. In other words, none of the analyzed ores match this group of samples. The Kaman-Kalehöyük samples of this group are mainly from Stratum IIa. In general, area C samples are from a later period than area B samples. Area D in Fig. 5 (area D in Fig. 4) Area D in Fig. 5 (area D in Fig. 4) was enlarged in Fig. 10 (Fig. 11). In Fig. 5 (Fig.10), area D is not clear enough to judge it to be a distinct area because it seems to overlap areas B and C. In Fig. 11, area D is to the left of area C. At first sight, it seems that this area partly overlaps with Taurus lb of Yener, but the plotted values of each ore in both Fig. 10 and Fig. 11 (Fig. 4 and Fig. 5) do not coincide with the Kaman-Kalehöyük samples. Two ore samples from Akda madeni fall near the area D samples. Most of the area D samples are from Stratum IIIb and Stratum IV. There was a transportation

7 2006 Lead Isotope Ratios of Lead Objects 229 network from the Akda madeni area to the Kayseri (Kültepe) area during those periods and lead materials from near Akda madeni may have been brought to Kaman-Kalehöyük through Kültepe. Areas C and D are close to each other in Fig. 4 and Fig. 5, and may be from the same system of ores. Area E in Fig. 5 (area E in Fig. 4) Area E in Fig. 5 (area E in Fig. 4) is enlarged in Fig. 10 (Fig. 11). In Fig. 5 (Fig. 10), area E distributes on a straight line somewhat below areas C and D. In Fig. 4 (Fig. 11), it distributes on a straight line above areas C and D. Although none of the ores correspond to this distribution, some ore samples that are distributed on the extension of this line will be explained in the discussion of area G. Area F in Fig. 5 (area F in Fig. 4) Area F in Fig. 5 (area F in Fig. 4) was enlarged in Fig. 12 (Fig. 13)). In Fig. 5, area F centers around a 207 Pb/ 206 Pb value of 0.84 and a 208 Pb/ 206 Pb value of In Fig. 12 (Fig. 6), this area corresponds to the lower part of the Taurus 2A field distinguished by Yener et al. (1991). However, in area F and the left of area F there are ore samples from Alada (shown as ) and samples from Kaman-Kalehöyük Stratum IV distribute among these ore samples. Therefore, it is possible that area F extends further to the left. In Fig. 13, the ore samples from Alada and samples from Kaman-Kalehöyük Stratum IV are in the lower part of area F, and it is possible that the lower part of area F should also be wider. This area includes many ores from the Ala Mountains and many excavated samples from Kaman-Kalehöyük Stratum IIIc; this is a characteristic feature of this stratum. These results are discussed in more detail below. Area G in Fig. 5 (area G in Fig. 4) Area G in Fig. 5 (area G in Fig. 4) is enlarged in Fig. 12 (Fig. 13. InFig. 5, area G is a relatively small cluster. An ore sample from Galena mine in Alada /Yahyal analyzed by Yener et al. (1991) corresponds to this area. This ore was collected northeast of Fig.12 Areas F and G of Fig. 5 are enlarged ( A type figure).,,, indicate samples excavated from Stratum II, III, IV and undecided, respectively. indicates minerals obtain from Alada and Yahyal near Alad. indicates the other minerals. The dotted line area indicates Taurus 2A reported by Yener et al. (1991). The solid line area indicates areas F and G. The slender line area may indicate area F in the future. Fig.13 Areas F and G of Fig. 4 are enlarged ( B type figure).,,, indicate samples excavated from Stratum II, III, IV and undecided, respectively. indicates minerals obtained from Alada and Yahyal near Alada. indicates the other minerals. Yahyal, approximately 30 km from the other ores in the Taurus 2A group, which are from the south and southwest of Yahyal. Area G samples are mainly from Kaman-Kalehöyük Stratum III and Stratum IV, with only one sample from Stratum II. As seen in Fig.14, some samples from Kaman-Kalehöyük are on the straight line which connects L9606 (indicated with a black square ), slag obtained at Çamard by Yener (indicated with a black square ) and ore belonging to area G (indicated with

8 230 J. ENOMOTO and Y. HIRAO AAS XV Fig.14 Distribution of samples on a straight line ( A type figure). indicates samples excavated from Kaman-Kalehöyük. indicates minerals obtained from Alada and Yahyal near Alada. indicates slag obtained form Çamard and L9606 excavated from Kaman-Kalehöyük. Fig.15 Samples excavated from Kaman-Kalehöyük and ores obtained from Yahyal ( B type figure). indicates samples excavated from Kaman-Kalehöyük. indicates minerals obtained from Alada and Yahyal near Alada. indicates slag obtained form Çamard and L9606 excavated from Kaman-Kalehöyük Stratum IV. Fig.16 Distribution of lead isotope ratios of lead objects excavated from Stratum IV ( A type figure). indicates samples excavated from Stratum IV. indicates minerals. Fig.17 Distribution of lead isotope ratios of lead objects excavated from Stratum IV ( B type figure). indicates samples excavated from Stratum IV. indicates minerals. Fig.18 Distribution of lead isotope ratios of lead objects excavated from Stratum III ( A type figure). indicates samples excavated from Stratum IIIc. indicates slag from Çamard. indicates the other minerals. indicates sample L9606 excavated from Stratum IV. Fig.19 Distribution of lead isotope ratios of lead objects excavated from Stratum IIIc. ( type figure). indicates samples excavated from Stratum IIIc. indicates slag from Çamard. indicates the other minerals. indicates sample L9606 excavated from Stratum IV.

9 2006 Lead Isotope Ratios of Lead Objects 231 a white square ). All ore samples from Alada are indicated with white squares. This straight line is an extension of area/line E mentioned above. The lead isotope ratios of area E, F, and G (E, F and G ) samples are distributed along the lead evolution curve of Dalrymple (1991). Therefore, it is possible that the original source rocks that produced the lead in areas E, F, and G are related to each other through the evolution of a single rock system. Since ores obtained at Alada and Yahyal (indicated with a white square ) coincide with samples from Kaman-Kalehöyük, the relationship between them was investigated. As seen in Fig. 15 (the B type counterpart of Fig. 14), there is a distribution of Kaman-Kalehöyük samples on the solid line which connects black squares and area G, but as the dotted line shows, many of the ores obtained at Yahyal are on a line with a different slope. It is possible to propose that samples in areas C and D (C and D ) also situate on a lead evolution curve, but a different one from that of areas E, F and G. Kaman-Kalehöyük Samples Grouped by Stratum Samples from Stratum IV (19 samples) (Fig. 16 and Fig. 17) Samples from Stratum IV are mainly concentrated in areas B, D and G in Fig. 16 (see Table 2). There is only one sample (L9606) which is apart from others, to the upper right of area A; the lead isotope ratio of this sample agrees with that of a sample from Çamard area (Yener et al. 1991). Ore from a mine in Yahyal is included in area G. Ore samples from mines situated around the Ala Mountains about 200 km southeast of Kaman-Kalehöyük are included in area F. Area D values are similar to those of ores from Akda madeni about 200 km east of Kaman-Kalehöyük. Most of the samples of this period are distributed in area B. It is not yet clear where the ore of area B samples originated, but slag from Kültepe plots in area B. It appears that the people in Kaman-Kalehöyük obtained lead materials from relatively near places, possibly by way of Kültepe or other cities, in this period. Samples from Stratum IIIc (19 samples) (Fig. 18 and Fig. 19) The characteristic of this stratum is that there are no samples in areas A, C, and D. Most of the samples of this period distribute on a line that connects L9606 (indicated with a black diamond ) and slag (indicated with a white square ) toarea G. This straight-line distribution of the samples is not seen in the other periods. As shown in Fig. 18, a group of lead ores (indicated with a black square ) from near Yahyal distributes near this line. However, as Fig. 19 shows, the distribution slopes of the ores and the Kaman-Kalehöyük samples differ from each other, so it is unlikely that the Stratum IIIc samples are from Yahyal. The straight line distribution of the samples can be explained by at Fig.20 Distribution of lead isotope ratios of lead objects excavated from Stratum IIIb ( A type figure) indicates samples excavated from Stratum IIIb. The dotted line area indicates Taurus 1A reported by Yener et al. (1991). Fig.21 Distribution of lead isotope ratios of lead objects from Stratum IIIb ( B type figure).

10 232 J. ENOMOTO and Y. HIRAO AAS XV stratum that 11 of the 31 samples are in area B, similar to the case for Stratum IV; it is supposed that there was a certain relationship with Kültepe. The distribution of the Stratum IIIb samples is wider than that of Stratum IIIc samples, which may indicate that the exchange of materials took place across a wider geographic range in this period. Fig.22 Distribution of lead isotope ratios of lead objects from Stratum IIIa ( A type figure). Fig.23 Distribution of lead isotope ratios of lead objects from Stratum IIIa ( B type figure). least two possible factors. One is that lead isotope ratios of ores in the same mine can have different values due to the different influence of geological diastrophism that formed the ore system. The second is that lead originating from more than one mine may have been mixed together when objects were manufactured. In this case, the lead isotope ratios of the objects would be plotted between those of the constituent ores. Samples from Stratum IIIb (31 samples) (Fig. 20 and Fig. 21) Samples from this layer are plotted in areas A and A in Fig. 20 and Fig. 21. The samples in area A in Fig. 20 are the same as Galena ore minerals from the Bolkar Mountains. The most notable feature of this Samples from Stratum IIIa (9 samples) (Fig. 22 and Fig. 23) In Fig. 22, samples are somewhat concentrated in area G. There are no samples from this period in areas B, C and F. The sample size is too small to provide valuable information. Samples from Stratum IId (9 samples) (Fig. 24 and Fig. 25) There are no Stratum IId samples in areas E, F, and G, and after this period no samples can be observed in areas E and G, but the number of samples from this stratum is too small to provide any conclusions. Of the nine samples, four are outside of our seven main groupings. Some of the samples are near area D, and may belong to that area. Samples from Stratum IIc (8 samples) (Fig. 26 and Fig. 27) There are no Stratum IIc samples in areas A, B, E, F, and G. The number of samples is too small to provide valuable information. Samples from Stratum IIb There are no analyzed samples from Stratum IIb. Samples from Stratum IIa (19 samples) (Fig. 28 and Fig. 29) Samples from this period are mainly distributed in area C in Fig. 28 (Fig. 29). Some are situated between areas B and D in Fig. 29. Ore corresponding to these samples has not been found yet. There are two samples in area B. Many samples from Stratum IV through IIIb belong to area B, and may share a similar origin with these two Stratum IIa samples. In this study, 147 lead samples excavated at Kaman-Kalehöyük were summarized according to the

11 2006 Lead Isotope Ratios of Lead Objects 233 Fig.24 Distribution of lead isotope ratios of lead objects from Stratum IId ( A type figure). Fig.25 Distribution of lead isotope ratios of lead objects from Stratum IId ( B type figure). Fig.26 Distribution of lead isotope ratios of lead objects from Stratum IIc ( A type figure). Fig.27 Distribution of lead isotope ratios of lead objects from Stratum IIc ( B type figure). Fig.28 Distribution of lead isotope ratios of lead objects from Stratum IIa ( A type figure). Fig.29 Distribution of lead isotope ratios of lead objects from Stratum IIa ( B type figure).

12 234 J. ENOMOTO and Y. HIRAO AAS XV results of lead isotope ratio analysis. Isotope ratios of lead ore from Turkey were compared with those of the excavated samples in order to determine provenance, but there are too few mine samples analyzed to allow definitive conclusions. Therefore, it will be necessary to analyze much more ore samples from Turkey. With lead isotope ratio measurements from many other sites, it will become possible to better understand the ore sources of the artifacts, and the processing sites, trade routes, and perhaps the movement of people and their technological skills. ACKNOWLEDGMENTS Throughout this study, Dr. S. Omura and members of the Kaman-Kalehöyük excavation team and the Middle Eastern Culture Centre in Japan assisted us. Dr. K. Matsumura checked the stratigraphy and Ms. M. Watanabe translated this paper. We would like to express our thanks to them. BIBLIOGRAPHY Brill, R. H. and J. M. Wampler Isotope ratios in archaeological objects of lead, Application of Science in Examination of Works of Art, Museum of Fine Arts, Boston, pp Brill, R. H. et al Lead Isotopes in some Japanese and Chinese glasses, Ars Orientalis 11, pp Dalrymple, G. B Modern Radiometric Methods: How They Work, The Age of the EARTH, Stanford University Press, pp Enomoto, J. and Y. Hirao 1998 Chemical study of copper objects excavated by the 10th (1995) expedition of Kaman-Kalehöyük, AAS VII, pp (in Japanese) Lead isotope ratios of lead objects excavated from the 12th (1997) expedition of Kaman-Kalehöyük, AAS VIII, pp (in Japanese) Lead isotope ratios of excavated lead objects from Kaman-Kalehöyük in Turkey, AAS X, pp Hirao, Y Provenance study using lead isotope ratios, S. Matsuura, Y. Uesugi and T. Warashina (eds.), Archaeology and Science 4, Doseisha, Tokyo, pp Hirao, Y. and J. Enomoto 1993 Chemical study of copper objects excavated by the fifth (1990) excavation expedition of Kaman-Kalehöyük, AAS II, pp (in Japanese) Lead isotope ratio of copper objects excavated by the sixth (1991) and seventh (1992) expeditions of Kaman-Kalehöyük, AAS III, pp (in Japanese) Chemical study of copper objects excavated in the 8th (1993) and 9th (1994) expeditions of Kaman-Kalehöyk, AAS VI, pp (in Japanese). Hirao, Y., J. Enomoto and H. Tachikawa 1995 Lead isotope ratios of copper, zinc and lead minerals in Turkey - In relation to the provenance study of artifacts, BMECCJ VIII, pp Hirao, Y. and H. Mabuchi 1989 Fractionation collection factor for the surface ionization mass - spectrometer of VG Sector, Conservation Science 28, pp Hirao, Y. et al Lead isotope study of copper objects excavated from Kaman-Kalehöyük, AAS I, pp Yener, K. A. et al Stable Lead Isotope Studies of Central Taurus Ore Sources and Related Artifacts from Eastern Mediterranean Chalcolithic and Bronze Age Sites, Journal of Archaeological Science 18, pp

13 2006 Lead Isotope Ratios of Lead Objects 235 Junko Enomoto and Yoshimitsu Hirao Faculty of Humanities Beppu University 82 Kita-ishigaki, Beppu, Ooita Japan

14 236 J. ENOMOTO and Y. HIRAO AAS XV Table I Lead isotope ratios of lead objects excavated from Kaman-Kalehöyük Sample No. Sector Grid Stratum Provisional Layer (PL) Note Year No. Date L8601 North (N) III XL-54 IIa1!3 No L8701 N IV XXXIX-55 IIa t-u P88, No L8702 N IV XXXIX-55 IIa t-u P68, No L8703 N IV XXXVIII-55 IIa e-ra!8 No L8704 N III XL-54 IIa No L8705 N III XL-55 IIa No L8706 N V XXXVII-54 IIa No L8834 N IV XXXVIII-55 IIa L8835 N V XXXVI-54 IIc # L8836 N VII XXXII-54 Surface q L8924 N IV XXXVIII-54 III $5b L8938 N VII XXXIII-54 Ib t L8939 N VII XXXII-54 Surface q L9126 N III XLI-54 IIIc % L9127 N IV XXXIX-54 IIIc %7 R66, No L9128 N III XL-55 IIIc %5e No L9129 N IV XXXIX-54 IIIc %7b R76, No L9130 N IV XXXIX-55 IIIc $8b No L9131 N III XL-54 IIIc %0a No L9132 N IX XXVIII-55 Surface w No L9133 N III XL-54 IIIc %0a kurtz L9134 N III XLI-54 IIIc % L9251 N V XXXVI-54 IIIb %2g No.17ring L9252 N V XXXVI-55 IIIb $7d No L9253 N VI XXXV-55 IIIc %9j No.39ring L9254 N VII XXXIII-55 IId w!2a No L9255 N V XXXVI-54 IIIb %2g No L9256 N VI XXXIV-55 IId q-e %1 No L9257 N IV XXXIX-55 IIIc %1 No.15P L9258 N V XXXVI-54 IIIb %3g No L9259 N V XXXVI-55 IIIb $9e No L9339 N XIII XL-52 I e No L9340 N II XLIII-54 No L9341 N I XLIV-55 IIIc!5 No L9465 N II XLIII-55 No L9466 N II XLII-55 No L9467 N VII XXXIII-55 IId No L9468 N VII XXXII-54 IId y L9469 N VII XXXIII-55 No L9470 N VI XXXV-55 IIIb ^0 No L9471 N II XLII-55 No L9472 N V XXXVI-55 IId(?) W2take out, No L9473 N II XLII L9474 N VI XXXV-55 IIIb ^1 No L9475 N VII XXXIII-54 IId e!6 No L9476 N II XLII-54 IIIb P L9539 N VI XXXIV-54 IIIb ^2 No L9540 N VI XXXV-55 IIIb %9 No L9541 N VI XXXIV-55 IId t^1a L9542 N VI XXXV-55 IIIb ^2 No L9543 N VII XXXIII L9544 N VII XXXIII L9545 N II XLII-55 No L9546 N II XLII L9547 N VI XXXIII-55 IId No L9548 N II XLII L9549 N VI XXXIV-55 IId t^2 No L9550 N II XLIX-54 IIIb # L9601 N III XL-54 IVa % L9602 N V XXXVI-55 IIIb %3 No L9603 N III XLI-55 IV &2 No L9604 N V XXXVI-54 IV %6b R217, No L9605 N V XXXVII-55 No L9606 N III XL-55 IV %9b L9607 N IV XXXVLLL-55 IIIc % L9608 N III XL-55 IV %8a L9609 N III XLI-54 IV ^1 No L9610 N III XL-55 IV %8 No.3, P L9611 N III XL-54 IV % L9612 N III XLI-54 IV ^ L9701 N XXX XLIX L9702 N XXX XLVIII-51 R L9703 N XV XXXVI-52 IIa!0 No L9704 N XIV XXXVIII-52 IIa!

15 2006 Lead Isotope Ratios of Lead Objects Pb/ 206 Pb 208 Pb/ 206 Pb 206 Pb/ 204 Pb 207 Pb/ 204 Pb 208 Pb/ 204 Pb Photo No. AASVol. Sample No. Analysis No new data KP new data KP new data KP new data KP new data KP new data KP new data KP new data KP new data KP new data KP Vol.1, 8924 CP new data KP new data KP new data KP new data KP new data KP new data KP new data KP new data KP new data KP new data KP new data KP new data KP new data KP new data KP new data KP new data KP new data KP new data KP new data KP new data KP new data KP new data KP new data KP new data KP new data KP new data KP new data KP new data KP new data KP new data KP new data KP new data KP new data KP new data KP new data KP new data KP new data KP new data KP new data KP new data KP new data KP new data KP new data KP new data KP new data KP new data KP new data KP new data KP new data KP new data KP new data KP new data KP new data KP new data KP new data KP new data KP new data KP new data KP new data KP Vol.8, L9701 KP Vol.8, L9702 KP Vol.8, L9703 KP Vol.8, L9704 KP1114

16 238 J. ENOMOTO and Y. HIRAO AAS XV Table I Lead isotope ratios of lead objects excavated from Kaman-Kalehöyük Sample No. Sector Grid Stratum PL Note Year No. Date L9705 N XIV XXXVIII-52!3 W L9706 N XIV XXXIX-53 IIa i No L9707 N XIV XXXVIII-53 IIc oa L9708 N V XXXVII-54 IIIb< ^ L9709 N V XXXVII-54 IIIc ^ L9710 N V XXXVII-54 IIIb< ^ L9711 N VII XXXII L9712 N IV XXXVIII-54 IVa %4a L9713 N III XL-54 IV % L9714 N III XLI-54 IV ^ L9715 N III XLI-54 IV ^3b L9716 N XIV XXXVIII-53 IIa ob No L9717 N III XL-55 IId P1829No L9718 N XV XXXVI-53 IIa i No L9719 N XV XXXVI-52 IIc>! L9720 N XIV XXXVIII-53 IIa y No L9721 N XIII XLI-52 IIa<! L9722 N XIII XLI-52! L9723 N XV XXXVI-53 IIa i No L9724 N XXVI XLVII-53 W L9725 N XXX L9726 N XXX XLIX-50 No L9727 N XXX XLIX-50 No L9728 N XXX XLVIII-51!9b L9729 N XXX XLVIII-51 IIIa!9b L9730 N XXX XLVIII-51 IIIc!9b No L9731 N XXX XLVIII-51!9b No L9801 N IV XXXVIII-55 IVa %8 P L9802 N VI XXXIV-55 IIIb &0a L9803 N VI XXXIV-55 IIIb ^ L9804 N VI XXXV-55 IIIc &1b L9805 N VII XXXII L9806 N VII XXXII-55 No L9807 N XXI XLVII L9808 N XXIV XLVIII-57 No L9809 N XXV XLIII-52 IIc?!3b L9810 N XXVI XLIV-52!1a No L9811 N XXVI L9812 N XXVI L9813 N XXX XLIX-50 IIIa # L9814 N XXX XLIX-50 IIIa # L9815 N XXX XLIX-50 IIIa # L9816 N XXX XLIX-51 # L9817 N XXX XLIX-51 IIIa #0 No L9818 N XXX XLIX-51 No L9901 N VII XXXII-55 IIIb #1b No L9902 N XVII XLI L9903 N VII XXXII-55 IIIb # L9904 N I,XXII XLV-55,56 border u No L9905 N XV XXXVI-52 IIc!4 P2100, No L9906 N XLIII-52,53 unknown kuzey kesit temizleme L9907 N III XL-55 IV & L9908 N XIV XXXIX L9910 N XXIV XLIV L9912 N VII XXXIII-54 IIIc ^ L9913 N XXVI XLV-53 IIa! L9914 N VII XXXIII-54 IIIb $6 No L9915 N XXVII XLVI-52 IIIb # L9916 N XXIII XLIII-56 IIIb t L9917 N XXIII,XLIV-57 IIIa!3a L9918 N III XLI-54 IV ^8a L9919 N XVIII XXXVIII L9920 N XXVI XLV-52 No L9921 N VII XXXIII-54 IIIb ^1 P2201,No L9922 N XV XXXVII-52 P2192,No L9924 N VII XXXIII-54 IIIb ^1 P2201,No L9925 N XXVII XLVI-52 IIIb< #1 No L9926 N XXVIII XLIX-52 IIIc $7 No L9927 N XVI XXXV-52 IIa! L9928 N XV XXXVI L9929 N XV XXXVII-52 IIc #8 No L9930 N III XL-54 IV L0005 N III XL-54 IV &0 No

17 2006 Lead Isotope Ratios of Lead Objects Pb/ 206 Pb 208 Pb/ 206 Pb 206 Pb/ 204 Pb 207 Pb/ 204 Pb 208 Pb/ 204 Pb Photo No. AASVol. Sample No. Analysis No Vol.8, L9705 KP Vol.8, L9706 KP Vol.8, L9707 KP Vol.8, L9708 KP Vol.8, L9709 KP Vol.8, L9710 KP Vol.8, L9711 KP Vol.8, L9712 KP Vol.8, L9713 KP Vol.8, L9714 KP Vol.8, L9715 KP Vol.8, L9716 KP Vol.8, L9717 KP Vol.8, L9718 KP Vol.8, L9719 KP Vol.8, L9720 KP Vol.8, L9721 KP Vol.8, L9722 KP Vol.8, L9723 KP Vol.8, L9724 KP Vol.10, L9725 KP Vol.10, L9726 KP Vol.10, L9727 KP Vol.10, L9728 KP Vol.10, L9729 KP Vol.10, L9730 KP Vol.10, L9731 KP Vol.10, L9801 KP Vol.10, L9802 KP Vol.10, L9803 KP Vol.10, L9804 KP Vol.10, L9805 KP Vol.10, L9806 KP Vol.10, L9807 KP Vol.10, L9808 KP Vol.10, L9809 KP Vol.10, L9810 KP Vol.10, L9811 KP Vol.10, L9812 KP1431B Vol.10, L9813 KP Vol.10, L9814 KP Vol.10, L9815 KP Vol.10, L9816 KP Vol.10, L9817 KP Vol.10, L9818 KP new data KP new data KP new data KP new data KP new data KP new data KP new data KP new data KP new data KP new data KP new data KP new data KP new data KP new data KP new data KP new data KP new data KP new data KP new data KP new data KP new data KP new data KP new data KP new data KP new data KP new data KP new data KP new data KP2214

18 240 J. ENOMOTO and Y. HIRAO AAS XV Table II Numbers of samples excavated from each stratum and area in Kaman-Kalehöyük Stratum Area A and A' B and B' C and C' D and D' E and E' F and F' G and G' Subtotal Outlier Total IV IIIc IIIb IIIa IId IIc IIa Surface or I Undecided Total

19 2006 Lead Isotope Ratios of Lead Objects 241 Photo 1 L8601 Photo 2 L8701 Photo 3 L8702 Photo 4 L8703 Photo 5 L8704 Photo 6 L8705 Photo 7 L8706 Photo 8 L8834 Photo 9 L8835 Photo 10 L8836 Photo 11 L8938 Photo 12 L8939 Photo 13 L9126 Photo 14 L9127 Photo 15 L9128 *Photo 1-96 The smallest scale in the photos is 1 mm

20 242 J. ENOMOTO and Y. HIRAO AAS XV Photo 16 L9129 Photo 17 L9130 Photo 18 L9131 Photo 19 L9132 Photo 20 L9133 Photo 21 L9134 Photo 22 L9251 Photo 23 L9252 Photo 24 L9253 Photo 25 L9254 Photo 26 L9255 Photo 27 L9256 Photo 28 L9257 Photo 29 L9258 Photo 30 L9259 *Photo 1-96 The smallest scale in the photos is 1 mm

21 2006 Lead Isotope Ratios of Lead Objects 243 Photo 31 L9339 Photo 32 L9340 Photo 33 L9341 Photo 34 L9465 Photo 35 L9466 Photo 36 L9467 Photo 37 L9468 Photo 38 L9469 Photo 39 L9470 Photo 40 L9471 Photo 41 L9472 Photo 42 L9473 Photo 43 L9474 Photo 44 L9475 Photo 45 L9476 *Photo 1-96 The smallest scale in the photos is 1 mm

22 244 J. ENOMOTO and Y. HIRAO AAS XV Photo 46 L9539 Photo 47 L9540 Photo 48 L9541 Photo 49 L9542 Photo 50 L9543 Photo 51 L9544 Photo 52 L9545 Photo 53 L9546 Photo 54 L9547 Photo 55 L9548 Photo 56 L9549 Photo 57 L9601 Photo 58 L9602 Photo 59 L9603 Photo 60 L9604 *Photo 1-96 The smallest scale in the photos is 1 mm

23 2006 Lead Isotope Ratios of Lead Objects 245 Photo 61 L9605 Photo 62 L9606 Photo 63 L9607 Photo 64 L9608 Photo 65 L9609 Photo 66 L9610 Photo 67 L9611 Photo 68 L9612 Photo 69 L9901 Photo 70 L9902 Photo 71 L9903 Photo 72 L9904 Photo 73 L9905 Photo 74 L99067 Photo 75 L9907 *Photo 1-96 The smallest scale in the photos is 1 mm

24 246 J. ENOMOTO and Y. HIRAO AAS XV Photo 76 L9908 Photo 77 L9910 Photo 78 L9912 Photo 79 L9913 Photo 80 L9914 Photo 81 L9915 Photo 82 L9916 Photo 83 L9917 Photo 84 L9918 Photo 85 L9919 Photo 86 L9920 Photo 87 L9921 Photo 88 L9922 Photo 89 L9924 Photo 90 L9925 *Photo 1-96 The smallest scale in the photos is 1 mm

25 2006 Lead Isotope Ratios of Lead Objects 247 Photo 91 L9926 Photo 92 L9927 Photo 93 L9928 Photo 94 L9929 Photo 95 L9930 Photo 96 L0005 *Photo 1-96 The smallest scale in the photos is 1 mm

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