Published by

INSTAP Academic Press

Philadelphia, Pennsylvania

2011

Metallurgy:
Understanding
How,
Learning

whY

Studies in Honor of James D. Muhly

PREHISTORY MONOGRAPHS 29

edited by

Philip P. Betancourt and Susan C. Ferrence

MU_Front_new_Layout 1 5/11/2011 10:13 AM Page iii

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Binding

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Printed in the United States of America

Library of Congress Cataloging-in-Publication Data

Metallurgy, understanding how, learning why : studies in honor of James D. Muhly / edited by Philip P. Betancourt and

Susan C. Ferrence.

p. cm. -- (Prehistory monographs ; v. 29)

Includes bibliographical references.

ISBN 978-1-931534-57-4 (hardcover : alk. paper)

1. Metal-work, Prehistoric. 2. Bronze age--Cyprus. 3. Bronze age--Aegean Sea. 4. Bronze implements--Cyprus. 5.

Bronze implements--Aegean Sea. 6. Cyrpus--Antiquities. 7. Aegean Sea--Antiquities. 8. Muhly, James David. I.

Betancourt, Philip P., 1936- II. Ferrence, Susan C., 1974-

GN799.M4M48 2011

939'.37--dc23

2011017917

FPO
FSC

MU_Front_new_Layout 1 5/11/2011 10:13 AM Page iv

AKR

excavation number, Akrotiri, Thera

cm

centimeter

dia.

diameter

EBA

Early Bronze Age

EC

Early Cycladic

EChal

Early Chalcolithic

ED-XRF

emission dispersive X-ray fluorescence

EH

Early Helladic

EM

Early Minoan

gr

gram

h.

height

HM

Herakleion Archaeological Museum

HNM

Hagios Nikolaos Archaeological
Museum

L.

length

LBA

Late Bronze Age

LC

Late Cycladic or Late Cypriot

LChal

Late Chalcolithic

LH

Late Helladic

LM

Late Minoan

m

meter

MBA

Middle Bronze Age

MC

Midlle Cycladic

MChal

Middle Chalcolithic

MH

Middle Helladic

MM

Middle Minoan

NCSR

National Center for Scientific
Research “Demokritos”

NM

National Archaeological Museum
of Greece

NMD

Neolithic Museum, Diros, Mani

pers. comm. personal communication
pers. obs.

personal observation

pres.

preserved

Abbreviations for periodicals in the bibliographies of the individual articles follow the conventions of

the American Journal of Archaeology 111.1 (2007), pp. 14–34.

List of Abbreviations

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METALLURGY: UNDERSTANDING HOW, LEARNING WHY

SEM/EDX

scanning electron microscopy and
energy dispersive microanalyses

SM

Siteia Archaeological Museum

th.

thickness

w.

width

wt.

weight

XRD

X-ray diffractometry

th.

thickness

XRF

X-ray fluorescence spectrometry

xxxii

MU_Front_new_Layout 1 5/11/2011 10:13 AM Page xxxii

The distinguished and multifarious contributions

of James Muhly to ancient history, archaeology, and
archaeometallurgy have embraced both traditional
and very new approaches to research. Muhly long
ago perspicaciously advocated that the study of the
Late Bronze Age Mediterranean metals trade had to
begin with learning all that we could about the cop-
per oxhide ingots, especially “how they were made,
why they were made and where they were made”
(Muhly 1977, 81). Muhly thereby inspired, and made
major contributions to, over 30 years of research in
this field. He was also quick to appreciate and
engage with (Muhly 1983) the new field of applying
lead isotope analysis (LIA) to the study of the prove-
nance of lead (Stos-Gale and Gale 1982), silver
(Gale, Gentner, and Wagner 1980), and especially
copper (Gale and Stos-Gale 1982). Indeed, Muhly
(2005, 508) was kind enough to describe the appli-
cation of LIA to provenancing the copper in oxhide
ingots as the second major development in the field
of copper oxhide ingot studies during the past 20

years, the first being a major increase in the corpus
of known exemplars (especially from the Bronze
Age Uluburun and Gelidonya shipwrecks and from
Sardinia [Lo Schiavo 2005]).

Another major advance has been the recent inten-

sive study of the metallography and chemical com-
position of copper oxhide ingots from the Uluburun
shipwreck (Hauptmann, Maddin, and Prange 2002).
From these studies they argued against the hypothe-
sis of the casting of oxhide ingots directly from
molten smelted copper metal from the furnace,
because they discovered angular fragments of slag
within the body of Uluburun ingots, while the direct
use of smelted copper from the furnace should carry
with it globular slag fragments, not angular. They
found that there was but weak evidence that oxhide
ingots were made by melting down bun ingots.
Moreover, Hauptmann, Maddin, and Prange (2002,
5) observed microscopic features (internal cooling
rims) in some Uluburun ingots, which they write
“could be caused by pouring several batches of

21

Copper Oxhide Ingots
and Lead Isotope Provenancing

Noël H. Gale

C H A P T E R

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NOËL H. GALE

214

the metal into a mold to complete an ingot.” This
supports earlier macroscopic observations by Pulak
(1998, 196; 2000, 142) of layered textures, which

indicate that at least some of the oxhide ingots were
finished by multiple pourings.

Implications for Lead Isotope Provenancing

Problems might ensue for lead isotope prove-

nancing if oxhide ingots were made by several
pourings of molten copper into the same mold. In
particular, if different batches of copper metal
smelted from different ore sources were brought to
a central site where the batches were melted down
and poured sequentially into the oxhide ingot
mold, where they formed a sort of layer cake struc-
ture, the lead isotope compositions of single sam-
ples that were sawed off the exterior would be
representative only of the layer of which they were
a part. This situation might be misleading if batch-
es of copper metal from different ore sources with
significantly different lead isotopic compositions
were utilized.

The existing lead isotope data suggests, however,

that such isotopically different batches of copper
metal were not used to make oxhide ingots. If they
had been, then the existing data for samples sawed
off hundreds of analyzed copper ingots would ran-
domly pick up the different batches, and quite differ-
ent isotopic compositions would be seen. In reality,
for the post–1400

B

.

C

. ingots, the limited range of

isotopic compositions found matches the range
found for Cypriot copper ores only from the Apliki
mine region (e.g., Gale 1999, 2006; Gale and Stos-
Gale 2005), and it does not reflect the isotopic com-
position of ores from, say, Sha or Kalavassos, or
Limassol Forest, or Mathiati, or any of the other ore
deposits around the Troodos (Stos-Gale et al. 1997).

Lead Isotope Analyses of Internal Core Samples

Nevertheless, it seemed important to measure di -

rectly the homogeneity or otherwise of lead isotope
compositions through the body of some copper
ingots. For this Hauptmann and Pulak provided sam-
ples taken at various points from cores drilled though
ingots from the Uluburun shipwreck. Lead isotope
analyses were made on these samples in the
Department of Earth Sciences, Oxford, using a Nu
Instrument Multicollector Inductively Coupled
Plasma mass spectrometer (MC-ICPMS; Belshaw et
al. 1998).

Analytical procedures and the numerical data

were reported by Gale (2005). In sum, the MC-
ICPMS lead isotope data for cores taken through
the three Uluburun copper oxhide and one bun

ingots support that at least some ingots were made
by the successive pouring of different batches of
molten copper into the mold. All the MC-ICPMS
data further prove that the different batches of
copper in a given Uluburun ingot come from the
same ore deposit, which has an isotopic composi-
tion identical with the earlier thermal ionization
mass spectrometry (TIMS) measurements of the
lead isotopic composition of surface samples from
some 300 Uluburun copper oxhide and bun ingots.
Consequently, the evidence derived from these
MC-ICPMS determinations of the lead isotope
compositions validates the lead isotope provenanc-
ing method for determining the ore sources of
copper used in making these ingots.

Lead Isotope Provenancing of Post–1400

B

.

C

. Copper Oxhide Ingots

Provenancing of the copper used to make copper

oxhide ingots was hampered before 1995 by the

relatively small number of lead isotope analyses
of ores from Cypriot mines. Before 1995 there

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COPPER OXHIDE INGOTS AND LEAD ISOTOPE PROVENANCING

existed 33 lead isotope analyses of Cypriot ores
made in Oxford together with a further 10 analyses
made by Hamelin et al. (1988). The Isotrace
Laboratory in Oxford had, before 1997, construct-
ed an overall “Cypriot field” by drawing an ellipse
to encompass these 43 analyses, though even then
arguments given by Hamelin et al. (1988) and
Stos-Gale et al. (1997, 85–86) suggested that this
“field” had structure, possibly folding together a
number of smaller fields characteristic of individ-
ual ore deposits in Cyprus. Moreover, we (Stos-
Gale and Gale 1994, 105–108, fig. 3.38; Gale and
Stos-Gale 1995, fig. 2) had also pointed out the
tendency for oxhide ingots found on Cyprus to plot
toward and slightly below the bottom edge of the
overall “Cypriot field” in one lead isotope dia-
gram. We had also reported that this position on
the edge of the “Cypriot field” was matched by the
lead isotope composition of the only two then
available ores from the Cypriot Apliki mine given
to us by R.F. Tylecote.

We conducted field trips to Cyprus in 1995 and

1996 to increase both the range of Cypriot ore
deposits sampled and the number of ore samples
from each deposit. Nearly 200 new lead isotope
analyses of sulphidic and oxidized ores from 26
copper mines on Cyprus were subsequently
published (Stos-Gale et al. 1997; Gale et al. 1997).
Lead isotope analyses (LIA) for ores from Cyprus
and Lavrion are shown in Figure 21.1, plotted in
the usual two diagrams, which represent orthogo-
nal plane sections through the three-dimensional
space occupied by LIA data (for details and data
for the ores analyzed from Cyprus, see Stos-Gale
et al. 1997 and Gale et al. 1997). The LIA for ores
from Lavrion are clearly separated from those for
any ores from Cyprus. Figure 21.1 shows that the
data for ores from the Cypriot Apliki mine fall
into a group that is not overlapped by the LIA for
other Cypriot ores; nor is the Apliki data over-
lapped by the LIA data for any other mines in
the Mediterranean region or Anatolia or the Near
East, generally.

These analyses showed that the mines from dif-

ferent geological regions group in five distinctive
isotopic groups, each with a substructure, related
to the geological history of the ore formation. It
was clear and was explicitly stated (Stos-Gale et al.
1997, 118), that the previous idea of an overall
“Cypriot field” had to be given up in favor of point

by point comparison of LIA data for artifacts
with the individual data for particular Cypriot ore
deposits. Stos-Gale et al. (1997) examined the par-
ticular case of the provenance of copper for 78
Late Bronze Age copper oxhide ingots found in
Cyprus, Crete, Greece, Sardinia, Turkey, and
Bulgaria. The data shows that all oxhide ingots
then analyzed, dating to 1400

B

.

C

. and later, were

made of copper consistent isotopically with only
the Apliki mining region in the geographical north
of Cyprus.

Figure 21.2 presents the lead isotope analyses of

30 copper oxhide ingots excavated from, or found
in, sites in Cyprus, plotted in relation to LIA for
Cypriot copper ores in an expanded diagram show-
ing the ores plotting with or near the ingots. The
oxhide ingots came from Enkomi (7), Kalavasos-
Ayios Dhimitrios (4), Maa (1), Maroni (5), Pyla (2),
Mathiati (4), and Skouriotissa (7); all date from the
Late Cypriot II period. All of these copper oxhide
ingots have lead isotope compositions consistent
with their production from copper coming from the
Apliki deposits alone. Their lead isotope composi-
tions clearly match no other ore deposits in Cyprus.
Not shown, for lack of space, is LIA data for LBA
copper oxhide ingots from Sardinia, mainland
Greece, Crete, Bulgaria, the Cape Gelidonya ship-
wreck, Anatolia, Syria, Israel, and Egypt—all of
which also match the LIA data for ores solely from
the Apliki deposits (Gale 1999, 2006).

The new data that we have accumulated both

for Cypriot ores and for oxhide ingots (Gale 1999,
2006) shows not an offset from, but a perfect
match between the lead isotope compositions of
the ingots and particular Cypriot ore bodies.
Those who, basing themselves largely on the view
that there is no such match, have written about a
postulated crisis in lead isotope and metal prove-
nancing studies (Budd et al. 1995, 1996) but no
longer have any evidence on which to base their
conjectures; there was and is no crisis.

We now refer to the majority of oxhide ingots

with lead isotope analyses that overlap those for
Apliki ores as post–1400

B

.

C

. Our previous refer-

ence to these oxhide ingots as being post–1250

B

.

C

. came from the fact that the great majority of

such ingots (from Cyprus, Greece, Turkey,
Bulgaria, Sardinia, and Cape Gelidonya), which
we analyzed in the earlier stages of our analytical
program, did date after approximately 1250

B

.

C

.

215

MU_CH21_Gale_new_Layout 1 5/5/2011 2:11 PM Page 215

NOËL H. GALE

216

Figure 21.1. Plot of lead isotope analyses for ores from Cyprus and Lavrion (Attica). Axis numbers denote ratios of the
number of atoms of lead (Pb) with atomic masses of 204, 206, 207, and 208.

0.820

0.825

0.830

0.835

0.840

0.845

0.850

0.820

0.825

0.830

0.835

0.840

0.845

0.850

0.820

0.825

0.830

0.835

0.840

0.845

0.850

0.820

0.825

0.830

0.835

0.840

0.845

0.850

2.09

2.08

2.07

2.06

2.05

2.04

2.09

2.08

2.07

2.06

2.05

2.04

18.7

18.6

18.5

18.4

18.9

19.0

18.8

18.7

18.6

18.5

18.4

18.9

19.0

18.8

Limni axis ores

Limassol Forest ores

Larnaca axis ores

Skouriotissa ores

Phoenix ores

Mavrovouni ores

Apliki mine ores

Ambelikou mine ores

Kalavassos

axis ores

Lavrion

ores

Sha

ores

Phorades

±0.1%

±0.1%

Lavrion

ores

Phorades Cu

slags

207Pb/206Pb

207Pb/206Pb

206

Pb/

204

Pb

208

Pb/

206

Pb

MU_CH21_Gale_new_Layout 1 5/5/2011 2:11 PM Page 216

COPPER OXHIDE INGOTS AND LEAD ISOTOPE PROVENANCING

217

Figure 21.2. Plot of lead isotope analyses of 30 copper oxhide ingots found on Cyprus in relation to lead isotope analyses
of ores from Cypriot ore deposits. Axis numbers denote ratios of the number of atoms of lead (Pb) with atomic masses
of 204, 206, 207, and 208.

0.835

0.840

0.845

0.850

0.835

0.840

0.845

0.850

0.835

0.840

0.845

0.850

0.835

0.840

0.845

0.850

Limni axis ores

Limassol Forest ores

Larnaca axis ores

Skouriotissa ores

Phoenix ores

Mavrovouni ores

Apliki mine ores

Ambelikou mine ores

“Cypriot” oxhide ingots

Phorades

±0.1%

207Pb/206Pb

208

Pb/

206

Pb

Phorades Cu slags

±0.1%

207Pb/206Pb

206

Pb/

204

Pb

18.6

18.5

18.4

18.6

18.5

18.4

2.08

2.07

2.06

2.08

2.07

2.06

MU_CH21_Gale_new_Layout 1 5/5/2011 2:11 PM Page 217

The discovery from lead isotope studies (Stos-

Gale et al. 1997; Gale 1999, 2006) that the copper
from which were made the majority of copper
oxhide ingots came from copper ore deposits in or
around the Apliki mine in Cyprus, though widely
accepted, prompted some reservations from Knapp
(1999, 2000), Kassianidou (2001, 2006), and Muhly
(2005, 508–509), which we have examined else-
where (Gale and Stos-Gale, in prep.). We reiterate
that our finding—the majority of copper oxhide
ingots were made of copper from the Apliki
deposit—was an empirical conclusion, not remotely
anticipated, which flowed inexorably from our
comparison of the lead isotope analyses of a large
number of oxhide ingots with those for the copper
deposits in Cyprus (e.g., Stos-Gale et al. 1997; Gale
1999, 2006). Among the analyzed oxhide ingots
were those excavated in Sardinia, for which two
independent laboratories (Gale 1999, 2006;
Begemann et al. 2001) have shown that their lead
isotope compositions match only the ores from
Apliki. The same laboratories (Begemann et al.
2001; Gale and Stos-Gale 1992; Gale 2006) both
showed that the Nuragic copper-based artifacts
in Sardinia had lead isotope compositions that
did not match any Cypriot ores, but rather matched
ores from Sardinia. The hypothesis advanced by
Kassianidou (2001, 2006) to explain this situation
was shown by Gale (2006) to be incorrect because it
was inconsistent with the combined lead isotope and
chemical analytical data. An explanation apparently

consistent with the lead isotope and chemical com-
positional data for Sardinian artifacts and oxhide
ingots was proffered in a recent paper read by R.G.
Valera (Marras, Valera, and Valera 2007) at the
Second International Conference on Archaeo

-

metallurgy held in Aquileia.

Those archaeologists who incline to reject the

Apliki hypothesis all affirm their belief that the
great majority of copper oxhide ingots were made
of copper smelted from Cypriot ores, largely on the
basis of lead isotope analyses. They thereby
involve themselves in a logical inconsistency. In
fact, throughout the long history of the serious
study of oxhide ingots (beginning with Buchholz
1959), there was no firm direct evidence for this
belief prior to the application of comparative
analyses of lead isotope compositions of oxhide
ingots and ores from Cyprus (Gale and Stos-Gale
1986; Gale 1991, 1999, 2006; Stos-Gale et al.
1997). But the lead isotope compositions for the
post–1400

B

.

C

. copper oxhide ingots do not in fact

match the lead isotope compositions of most
Cypriot ores (Stos-Gale et al. 1997; Gale 1999,
2006; Gale and Stos-Gale 2005). Most Cypriot
ores are in fact excluded as the source of copper for
oxhide ingots; the match is solely with the ores
from the Cypriot ore deposit of Apliki (see Figs.
21.1, 21.2). It follows that acceptance regarding
comparative lead isotope analyses showing the
great majority of copper oxhide ingots were made
of copper smelted from Cypriot ores necessarily

NOËL H. GALE

218

and had lead isotope compositions overlapping
those of ores from Apliki, with the exception
chiefly of the 19 Late Minoan (LM) IB examples
from the villa of Hagia Triada in Crete (Pugliese
Caratelli 1945; Gale and Stos-Gale 1986; Cucuzza
and Gale 2004). Later work has now shown that
LM IB copper oxhide ingots from both Gournia
and Mochlos were, however, made of copper from
the Apliki ore deposit, so it seems that this deposit
was in fact used as a source of copper for oxhide
ingots before 1250

B

.

C

., perhaps as early as

1550–1400

B

.

C

. (Absolute dates for LM IB remain

controversial [Betancourt 1998; Bietak 2003;
Manning et al. 2006].) The mine of Ambelikou,

which is the only Cypriot mine with direct evi-
dence of having been worked in the Bronze Age
(Merrillees 1984), was exploited in the Early to
Middle Cypriot periods, too early to have been a
source of copper for oxhide ingots, as is also con-
firmed by lead isotope analyses of its ores, which
do not match those of oxhide ingots (see Figs.
21.1, 21.2). The Cypriot Bronze Age copper
smelting site of Politiko-Phorades, dating to about
1600

B

.

C

. (Knapp 2003), is also too early to have

produced copper for oxhide ingots, and this, too,
is confirmed by lead isotope analyses of copper
slags from Politiko-Phorades shown in Figures
21.1 and 21.2.

Apliki Mine Deposit

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COPPER OXHIDE INGOTS AND LEAD ISOTOPE PROVENANCING

carries with it the corollary that they were made of
copper smelted from ores from the Apliki ore
deposit. The lead isotope analyses do not allow
acceptance of a Cypriot origin for the copper used
to make oxhide ingots without accepting that the
source in Cyprus is the Apliki ore deposit. It seems
possible that this northeastern Troodos mining area
had a monopoly on providing copper metal for

making the large copper oxhide ingots, though LIA
shows that many copper-based artifacts from
Bronze Age Cypriot sites were made from copper
that came from other copper ore deposits around
the Troodos. This is a new factor that needs to be
incorporated into socioeconomic discussions of
the organization of copper production on Bronze
Age Cyprus.

219

Acknowledgments

I am grateful to the Science and Engineering

Research Council (SERC), the Institute for Aegean
Prehistory (INSTAP), the British Academy, and the
University of Oxford for funding laboratory and
fieldwork, and to Dr. G. Maliotis for his invaluable

and extensive help. The MC-ICPMS analyses of
samples from Uluburun ingots were made in the
Department of Earth Sciences, Oxford, with the
help of Dr. N. Belshaw and the kind permission of
Prof. Sir R.K. O’Nions and Dr. D. Porcelli.

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