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Coins, artefacts and isotopes-archaeometallurgy and Archaeometry

Authors:
  • Curt Engelhorn Zentrum Archäometrie and University of Heidelberg

Abstract

Archaeometallurgy is one of the earliest manifestations of archaeometric research, using science-based approaches to address cultural–historical questions. This review first outlines the extent of the field, defining in some detail the main branches of archaeometallurgy, and their specific methodological approaches. It then looks at some of the early publications pioneering archaeometallurgical research, to set the scene for the publication pattern of archaeometallurgy in general, and the role that Archaeometry played in publishing archaeometallurgical research. The analysis of archaeometallurgy-themed publications in Archaeometry, their change over time and their relationship to the total range of work done in the field indicates that there is a rather narrowly defined and specific type of archaeometallurgy that gets published in Archaeometry, initially with a strong focus on coin and object analysis, often combined with method developments. The more recent developments in isotope-based studies in archaeometallurgy find only a limited representation in the journal, despite the leading role that the Isotrace Laboratory played in this discipline, for some considerable length of time. More recently, this Archaeometry-specific ‘flavour’ of archaeometallurgy seems to weaken, with an increase of papers on iron and on primary production in general, subjects still much under-represented.
Archaeometry
50
, 2 (2008) 232–248 doi: 10.1111/j.1475-4754.2008.00389.x
*Received 22 November 2007; accepted 4 December 2007
†Corresponding author: email th.rehren@ucl.ac.uk
© University of Oxford, 2008
Blackwell Publishing Ltd
Oxford, UKARCHArchaeometry0003-813X0003-813X© University of Oxford, 2008XXXOriginal Articles
Coins, artefacts and isotopes—archaeometallurgy and ArchaeometryTh. Rehren and E. Pernicka
COINS, ARTEFACTS AND ISOTOPES—
ARCHAEOMETALLURGY AND
ARCHAEOMETRY
*
TH. REHREN†
UCL Institute of Archaeology, 31–34 Gordon Square, London WC1H 0PY, UK
and E. PERNICKA
Institut für Ur- und Frühgeschichte und Archäologie des Mittelalters, Universität Tübingen, 72070 Tübingen,
Gemany and Curt-Engelhorn-Zentrum Archäometrie, C5, Zeughaus, 68159 Mannheim, Germany
Archaeometallurgy is one of the earliest manifestations of archaeometric research, using
science-based approaches to address cultural–historical questions. This review first outlines
the extent of the field, defining in some detail the main branches of archaeometallurgy, and
their specific methodological approaches. It then looks at some of the early publications
pioneering archaeometallurgical research, to set the scene for the publication pattern of
archaeometallurgy in general, and the role that
Archaeometry
played in publishing
archaeometallurgical research. The analysis of archaeometallurgy-themed publications in
Archaeometry
, their change over time and their relationship to the total range of work done
in the field indicates that there is a rather narrowly defined and specific type of
archaeometallurgy that gets published in
Archaeometry
, initially with a strong focus on coin
and object analysis, often combined with method developments. The more recent develop-
ments in isotope-based studies in archaeometallurgy find only a limited representation in the
journal, despite the leading role that the Isotrace Laboratory played in this discipline, for
some considerable length of time. More recently, this
Archaeometry
-specific ‘flavour’ of
archaeometallurgy seems to weaken, with an increase of papers on iron and on primary
production in general, subjects still much under-represented.
KEYWORDS:
ARCHAEOMETALLURGY, COINS, ISOTOPES, PUBLICATION PATTERN
8 University of Oxford, 2008
INTRODUCTION
Archaeometry as an academic field can trace its roots back to several diverse academic ‘families’.
Created through the marriage of physical and historical sciences 50 years ago, archaeometry
combines specialized applications of science-based approaches to archaeological and historical
questions with subdisciplines such as geophysical prospection and remote sensing, absolute
dating, ceramic studies, geoarchaeology, archaeobotany and archaeozoology, and archaeo-
metallurgy. The establishment of the journal
Archaeometry
in 1958 served as a milestone
in the formalization of archaeometry as a mature scientific discipline; but how successful has
it been in catering for the needs of the various subdisciplines?
As is the case with many other subdisciplines of archaeometry, archaeometallurgy has
evolved into a subfield in its own right. A number of journals now specialize in archaeometallurgy,
and numerous conferences exclusively devoted to metals in antiquity have been organized
Coins, artefacts and isotopes—archaeometallurgy and
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since the 1980s. However,
Archaeometry
was the first journal at the interface of natural and
historical sciences, and has long remained its backbone; but by and large, archaeometallurgy
only played a minor role among the topics covered. This, clearly, has something to do with the
mother institute behind the journal, the Research Laboratory for Archaeology and the History
of Art (RLAHA), and its offspring, the Isotrace Laboratory. We leave it to others to present
and discuss the formal and historical aspects of the relationship between these three. Here,
we focus on a view from the outside, on the impact that the journal has had over the past half-
century on the study of ancient metallurgy. To do so, we need to sketch out the size, shape
and content of the ‘field’ of archaeometallurgy, before assessing its major research outlets and
the role that
Archaeometry
played in this.
What is archaeometallurgy?
Metal objects play a significant role in most post-Neolithic societies, as reflected in the
denominations for major archaeological periods (Copper Age, Bronze Age and Iron Age). The
sequentiality of these units reflects the perceived stepped introduction of major metals and
alloys, spanning from the earliest use of a few native metals (mainly copper), probably some
10 000 years ago, and continuing to this day with the development of ever more sophisticated
alloys based on the more than 70 different metals in the periodic table of elements. Broadly
speaking, archaeometallurgy deals with all aspects of metal production, distribution and usage
in the history of mankind (Fig. 1). Archaeometallurgists often concentrate on periods before
c
.
ad
1500, when only seven metals were known, together with a number of their alloys; that
is, gold, copper, lead, silver, tin, iron and mercury, and the alloys of copper (copper–arsenic,
copper–tin, copper–tin–lead and copper–zinc), silver (silver–copper and silver–gold), pewter
Figure 1 The archaeometallurgy cycle (after Ottaway 1994).
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(tin–lead) and iron (iron–carbon and iron–phosphorus), although there are good reasons to extend
archaeometallurgy to much more recent periods (e.g., Goodway and Odell 1988; Gilmour and
Northover 2003; Rehren 2006; Bourgarit and Plateau 2007). Thus, it is not primarily the age
of the material studied that defines archaeometallurgy, but the application of scientific methods
to address cultural–historical questions. Reliance on scientific methods is often dictated by the
‘ahistorical’ nature of the crafts well into the recent past, resulting in at best patchy contemporary
textual documentation being available.
The first use of metals some 10 000 years ago was from natural occurrences as native metals,
which did not require elaborate mining and smelting. This early metallurgy is limited to specific
geological areas and is typical of the earliest use of gold, silver, copper, iron and mercury. The
use of these native metals initially followed earlier, rather mechanical, approaches to lithic
materials. However, supply of metals increased dramatically with the inception and spread of
mining and extractive metallurgy, the origin of which is not yet clear, but seems to have risen
in the late sixth millennium
bc
; at the same time, genuinely metallurgical production and
manufacturing techniques were developed, considerably expanding the use and versatility of
metals. The emergence of alloys, both natural and intentional, further widened the range and
appeal of metals available. In spite of these innovations and the subsequent, almost global,
spread of metallurgy, the geological limitation of metal production to areas rich in specific
ores remained. This necessitated or stimulated developments in other fields such as economics,
politics, warfare or trade, to match the spread in knowledge with a similar spread of the material.
Many civilizations flourished in areas devoid of metal ores, such as the large river valley cultures
of Egypt, Mesopotamia and the Indian subcontinent; other areas were rich in one metal but not
another. Thus, mechanisms of trade and exchange, and methods for the recycling of or substituting
for metals, were of considerable importance from an early period onwards, and their study is
firmly within the realm of archaeometallurgy.
A major division separates the primary production of metal from the manufacturing of
artefacts; namely, the nature of the skills required for each. Primary production—that is, mining,
beneficiation and smelting—requires a keen eye for specific minerals, their relevant properties,
such as colour, hardness, smell, mechanical behaviour under stress, chemical behaviour at
high temperatures and so on, and knowledge of the necessary associated materials, such as
fuel, technical ceramics and fluxes. The archaeological evidence for this type of activity is
mostly waste material such as slag, furnace and crucible fragments. Manufacturing, on the
other hand, requires a fine understanding of the behaviour of metals and alloys, over a range
of temperatures from cold to fully liquid, combined with the artistic skill required to make
both the functional and beautiful objects desired by patrons. Similarly, archaeometallurgy
separates into a number of parallel main strands, based on the nature of the materials available
for study (waste versus artefact), the skills involved (smelting versus manufacturing) and the
archaeological context (workshop sites versus consumer sites). Of course, the division into
primary production of metals and manufacture of artefacts is not absolute, and considerable
overlap exists between the two strands; indeed, this division took some time to develop, and much
of the earliest evidence suggests that the first metallurgists were covering the entire metallurgical
chaîne opératoire
, from ore prospection to artefact production. This division does hold true,
however, for the bulk of archaeometallurgy, and is mirrored in different analytical approaches,
reflecting the different nature of the materials involved and questions asked. We will also use
this division to structure the following review.
It may be added that primary production in particular has a strong overlap with a third
strand; namely, mining archaeology, the investigation of ancient mines with archaeological
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methods of documentation, excavation and typology. However, since papers on this subject are
not represented in
Archaeometry
, we will not deal with it further. Similarly, we will not
attempt to cover the other end of the archaeometallurgy cycle (Fig. 1), the corrosion and
conservation of artefacts during and after burial, aspects that are also not typically covered by
publications in
Archaeometry
.
PRIMARY PRODUCTION OF METALS
The geological link between the often remote ore deposit and the main production sites, with
their evidence for smelting operations to extract the metal from the ore, offers a unique window
into the activities carried out, away from the typically urban consumption areas. Almost universally,
the waste materials remained in the immediate vicinity of the site of production, providing
reliable evidence of the activities and technologies employed here. Metallurgical activity
leaves three main types of evidence: metal as raw lumps and spills, semi-finished products and
objects for repair or recycling; associated products such as discarded ore, slag, matte and
speiss; and remains of tools and installations, such as crucibles, hammers, tongs, furnaces or
hearths. Of these, slags are typically the best preserved, most abundant and most informative.
However, they are also least accessible by traditional archaeological methods such as typology
or stylistic analysis, but require scientific analysis and expert interpretation to reveal the
information that they contain. Even the most fundamental of identifications are not always
possible using field methods and visual inspection. Metallurgical slag can be confused with
geological material, or artificial materials from processes other than metallurgy. The differenti-
ation between primary production or smelting on the one hand, and secondary production or
re-working on the other hand, is often indicated by the wider archaeological context, but this
cannot be taken for granted. It can be difficult in the field to distinguish between ferrous and
non-ferrous metallurgy, or between iron smelting and smithing. However, studying the waste
material can yield very specific information about metallurgical processes and ore types,
production technologies and scale of production. Identifying and understanding these aspects
of production is at the core of the archaeometallurgical analysis of slag.
The production and working of metal is controlled by two main factors: technical constraints
and cultural traditions. While there are certain fixed physico-chemical conditions to be met for
specific metallurgical operations such as smelting, alloying, refining, casting and recycling,
there are many different configurations that may meet these conditions. The composition and
quantity of the resulting materials, primarily metal and slag, reflect both factors. It is by
identifying the fixed physico-chemical constraints that the culturally determined configurational
factors can be revealed, producing archaeologically relevant information (Rehren
et al
. 2007,
and literature therein).
The first issue addressed by slag analysis is the identification of the type of metallurgical
process that created it, and the metal and ore type smelted or worked at a given site. Ore
deposits comprise two complementary materials: the rich mineral and the gangue or host rock.
Ore beneficiation mechanically separates the rich mineral from the gangue. By smelting, the
metal is then extracted from the rich mineral through a series of chemical reactions, while
transforming remaining gangue into slag. Depending on circumstances, other waste or inter-
mediate products form, such as matte (metal sulphides) and speiss (transition metals combined
with elements of the fifth main group of the periodic table of the elements, mainly arsenic and
antimony). The type of ore, such as oxidic, sulphidic or complex, is at best broadly reflected in
the composition of the smelted metal. The slag, however, contains all the gangue components
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as well as components of the rich mineral, modulated by the smelting conditions. In effect, the
waste gives a much more complete representation of both the ore body and the smelting
conditions. This picture is complicated through the addition, conscious or not, of further
material to the slag, such as fluxes, eroded furnace wall material and fuel ash (Serneels and
Crew 1997; Kronz 1998; Crew 2000; Veldhuijzen and Rehren 2007).
This leads to the identification of the nature of the operation. Metallurgical processes
require elevated temperatures, typically in the range of 800–1400
°
C, and a wide spectrum of
redox conditions, spanning from highly oxidizing to strongly reducing. Each metallurgical
process has its own characteristic combination of temperature and redox condition. Neither
can be determined directly, but both find their direct expression in the mineralogical make-up
of the slag. Identifying these parameters is crucial for the basic identification of the technological
process, as well as for identifying its particular configurational aspects, and relies heavily on
mineralogical analysis (e.g., Bachmann 1982).
Finally, production remains are often well preserved and the best available indicator for the
scale of operation of a given workshop or smelting site. Careful determination of total slag
quantity and composition, in combination with an assumed or directly determined ore quality,
can provide good estimates of metal production quantities by using mass balance calculations.
Similar estimates can be made for workshop remains such as crucibles (Rehren and Papakhristu
2000) or smithing debris (Crew 1991; Serneels and Perret 2003); quantities can be determined
either for a site overall, or on an average annual basis if the lifespan of the site or workshop is
known. Such quantification is crucial for discussions of subsistence or surplus production,
craft specialization and trade relationships.
METAL WORKING AND DISTRIBUTION
The use of metal objects can be seen as falling into one of three broad categories: decorative
(jewellery, inlays and other accessories), military (arms and armour) and utilitarian (coinage,
tools and general implements). These exploit the different metal properties perceptible in
antiquity, such as colour, sonority, density, malleability, hardness and so on. One reason to
analyse metal objects is to understand whether, for a given object, these properties have been
either selectively exploited, or even modified to suit the purpose. This information acquaints
the archaeometallurgist with the state of metallurgical knowledge, or relative priorities of these
parameters, of the person or society producing the object. Another reason for analysis is to
discuss the functionality of objects; for example, whether funerary or dedicatory objects were
made for display only or for real use. Reconstructing the techniques used to work metals by
studying the waste left behind is a more process-oriented field, which focuses on the workshops
and their activities.
Chemical, and in particular isotopic, analysis is the main avenue towards identifying the
geological origin of a given object, and directly addresses issues of trade and movement of
objects. This begins with the desire to classify objects by material types and to identify
similarities and differences in composition in order to form groups, using parameters that are
independent of, and often complementary to, traditional archaeological typologies and art
historical criteria. Finally, there is the necessity to identify the most suitable conservation
methods to restore or preserve metal objects, and conservation science has its own important
role to play within archaeometallurgy. Thus, four main research fields prevail in the analysis
of metal objects: identifying their original composition and current condition, classifying by
compositional groups, reconstructing metallurgical practice from shaping (casting, mechanical
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deformation etc.) and joining (welding, brazing etc.) to finishing (decoration techniques), and
locating the geological origin of the metal.
ANALYSING ARCHAEOMETALLURGY
The metallurgical analysis in archaeology has to be broadly separated into two main strands,
one aiming to study metal artefacts and the other concerned with the production waste. Both
can use the entire range of analytical methods available; however, several approaches have
been particularly successful and are therefore more widely adopted than others.
Primary production
Analysis of slag and ore in archaeology draws almost exclusively from Earth science methods,
primarily geochemistry, ore petrology and igneous petrology. Ideally, this involves a multi-
element method such as X-ray fluorescence (XRF) or inductively coupled plasma excitation
with optical emission spectrometry (ICP–OES), in combination with optical and electron
microscopy for the study of the texture of the sample and an assessment of mineralogical
parameters. Ideally, the research question and aim should govern the choice of analytical
method(s). In reality, costs of analysis and ease of access to or availability of instruments and
expertise often play a decisive role in selecting methods of analysis. For all quantitative
methods, it is imperative to monitor and report data quality (accuracy and precision) through
publishing results for analysis of certified reference materials along with the unknown samples, in
order to be able to compare data from different laboratories.
Metallurgical smelting slag often occurs in huge quantities, accumulated over long periods
and measuring tons, or even thousands of tons. Sampling methods developed for Earth sciences
are often appropriate for stratified profiles and reducing large sample volumes through
homogenization and quartering into aliquots. Curatorial constraints are often more important
in the analysis of other waste materials, such as crucible fragments, which have a stronger
developed object character and typically do not occur in such large quantities. Here, cross-sections
prepared for reflected light microscopy (RLM) and scanning electron microscopy (SEM) with
attached energy-dispersive spectrometry (EDS) are more suitable than bulk chemical analysis.
SEM–EDS has relatively high detection limits in the order of 0.1 wt% for most elements, and
therefore provides only basic chemical information; however, it offers a high spatial resolution
of what is analysed, ideal for complex and multi-phase materials such as crucibles with internal
slag coatings and external vitrification layers. A balance between the curatorial desire to minimize
the sampling impact and the analytical need for a representative sample is sometimes difficult
to achieve, and may require the use of non-invasive and non-destructive methods such as surface-
XRF or micro-XRF (Tite
et al
. 2002).
Artefact analysis
For artefact analysis, it is often important to use methods that do not alter the physical integrity
of the metal objects, such as neutron activation analysis (NAA), X-ray fluorescence analysis
(XRF), proton-induced X-ray emission or gamma emission (PIXE or PIGE), or X-ray fluorescence
analysis with synchrotron radiation (SR–XRF). NAA is not strictly non-destructive, as the
object can only be returned after the decay of the artificially induced radioactivity, and only
relatively small objects can be irradiated in a reactor. Since some nuclides have rather long
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half-lives, it is necessary to initially determine the composition of the object by other means
before the high sensitivity of neutron activation analysis can be sensibly employed. A typical
case is unalloyed copper. From the matrix element only short-lived radionuclides are formed and
after a decay period of a few days up to 20 elements can be determined at trace levels (Hancock
et al
. 1991; Kuleff and Pernicka 1995; Rapp
et al
. 2000). After a few weeks, the radioactivity
has usually fallen below detectable levels. It is often important to analyse a sample non-
destructively so that other methods can be used to determine other parameters on the same
sample. A typical example is the combined trace element and lead isotope analysis of copper
and copper-based alloys. An integral part of good laboratory practice is the documentation of
the analytical procedure, and the storage of part of the analysed material for future reference.
This may sometimes lower the sample mass available and consequently increase the detection
limits for certain elements for methods that require a sample to be removed and dissolved,
such as atomic absorption analysis (AAS) and excitation with an inductively coupled plasma
either for optical emission spectrometry (ICP–OES) or mass spectrometry (ICP–MS). Often, the
optimum choices are methods that remove a minute amount of material through evaporation or
ablation, such as laser ablation ICP–MS or secondary ion mass spectrometry (SIMS). However,
these instruments have rather small sample chambers, so that only small objects can be analysed.
Larger objects require sampling that is often easy to carry out, unless it is for gold objects.
In these cases, relatively elaborate techniques such as PIXE or synchrotron XRF are required
for analysis.
Isotope analysis
In the 1960s, a fundamentally new method was arising from advances in geochemistry;
namely, the analysis of lead isotope ratios for the investigation of the provenance of metals
(Brill and Wampler 1965; Grögler
et al
. 1966). The first tentative studies began to flourish in
the 1970s, fuelled by a collaboration of W. Gentner and G. A. Wagner at the Max-Planck-Institut
für Kernphysik in Heidelberg and N. H. Gale at the University of Oxford. This group systematically
studied the provenance of ancient Greek silver coins, using both trace element and lead
isotope analysis, combined with extensive fieldwork on lead–silver deposits in the Aegean. The
approach encompassed not only analyses of metals but also geological and mining archaeological
field work, as well as mineralogical studies of ores and metallurgical remains (Gale
et al
. 1980;
Wagner and Weisgerber 1985, 1988). A similar holistic approach, albeit without lead isotope
analysis, was followed in the studies on chalcolithic copper metallurgy by E. N. Chernykh
(1978). The breakthrough of provenancing by isotope ratios came with the extension of the
lead isotope analysis to copper and copper-based alloys (Gale and Stos-Gale 1982). By the
combination of lead isotope ratios and trace element patterns it became possible, for the first
time, to relate with high probability metal artefacts to specific ore deposits, something that had
been aimed at for more than 100 years. The work culminated with major syntheses for the
metal from Cyprus by Stos-Gale
et al
. (1997), and for the south-east European Chalcolithic by
Pernicka
et al
. (1997). The merit of lead isotope studies has not been uncontested; a controversial
paper by Budd
et al
. (1993) sparked off a discussion both in the
Journal of Mediterranean
Archaeology
and in
Archaeometry
, with a number of comments in volume 35 (1993). However, it
is now widely accepted and applied to a range of other materials such as glass and pigments
(Lilyquist and Brill 1993; Shortland 2006).
Recent developments have tried to exploit the isotope ratios of other metals of archaeological
interest for provenancing, such as tin (Begemann
et al
. 1999), copper (Klein
et al
. 2004) or
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osmium (Junk and Pernicka 2003); so far, success has been limited. More promising seems to
be a combination of metallographic, chemical and isotope analysis of iron (Schwab
et al
.
2006; Degryse
et al
. 2007).
A major problem is still the dating of metal by physical methods. There is often enough
carbon in ancient iron to be measured by accelerator mass spectrometry, and this has indeed
been used for dating purposes (Enami 2004; Scharf
et al
. 2004). However, Craddock
et al
. (2002)
pointed out that carbon in ancient iron can derive from various sources, including geological
ones such as limestone, which decomposes to carbon dioxide in the furnace, resulting in erroneously
high ages. For base metals the radioactivity of
210
Pb has been employed for authentication
work (Pernicka
et al
. 2008). This method was originally introduced to archaeometry by Keisch
(1967), for the authentication of lead white pigment in paintings. The only authentication
method for gold based on the U,Th–
4
He dating method is just being developed (Eugster
et al
.
2008).
It is interesting to see how, for more than two decades, much of this development was
driven also by N. Gale and S. Stos-Gale at the Isotrace Laboratory in Oxford, part of the same
RLAHA that was and is the home of
Archaeometry
; and yet how modest the impact of isotope
studies in archaeometallurgy has been on the publication profile of
Archaeometry
. There has
been a relative surge of isotope-related papers from the 1990s onwards (see below), but the
bulk of the discussion and method development appears to have been published elsewhere.
There is one remarkable exception to this, though, when a paper that was reviewed with con-
trasting results was openly discussed in the journal. Partly in reaction to the criticism aired by
Budd
et al
. (1993), the Isotrace Laboratory published a series of papers on lead isotope ratios
of ores from various regions where they had worked.
Metallography and manufacturing
A major and uniquely metallurgical method for the study of artefacts is metallography, using
optical and scanning electron microscopes/microprobes. The main emphasis of this approach
is on the identification of particular structures preserving some of the manufacturing history
of an object. Pioneering work has been done by Gowland (1912) and Bergsoe (1937),
followed by the work of C. S. Smith (collected in Smith 1981). Numerous papers by Tylecote,
Lechtman, Kolchin, Bielenin, Pleiner and Maddin and co-workers during the second half of the
20th century developed metallography to a routinely applied approach in archaeometallurgy—
to mention just a few particularly prolific scholars, who are representative of a much larger
group. Analysing iron and steel requires accurate determination of the carbon content at levels
between 0.01 wt% and 1 wt%. Few of the analytical instruments used in non-ferrous metal
analysis are capable of doing this, and methods established in industry normally require much
larger and better-preserved samples than are typically available in archaeology. Here, optical
metallography is the most appropriate method not only to determine the carbon content, but
also to reconstruct the working history of the object under study. Significantly, metallography
enables the reconstruction of a sequence of events, as opposed to a mere description of the
status quo. Not only is the working history preserved in the microstructure of the metal, but also
subsequent changes in composition or condition by use, corrosion or conservation treatment.
While much of this, such as grain size and shape, phase identification and detailed composition,
can be quantified, it is still the overall and often qualitative assessment of the spatial relationship
between different phases and individual metal grains that renders metallography as much an
experience-based as a quantitative method. It would go beyond the scope of this review to list
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the wide range of studies of archaeological metal artefacts that are based on this method, covering
all the known metals of antiquity—and a number of less well known ones, too, such as platinum
(Bergsoe 1937), zinc (Rehren 1996), antimony (Shortland 2002) and aluminium (Bourgarit
and Plateau 2007).
Alloying, refining, casting and recycling all produce their own compositionally distinct
types of waste material, typically in much lower quantities than smelting and often in close
relationship to technical ceramics such as crucibles and hearths. These workshop wastes are
different from the primary production residue. Significantly, they are often more removed
from equilibrium conditions than most other archaeometallurgical materials. This results in the
preservation of intermediate stages of the various operations that were carried out at the workshop,
alongside raw materials, intermediate products and finished products in varying proportions.
As in metallography, it is the assessment of the spatial and chronological relationship between
the different phases present that enables the microscopist to interpret these residues in a way
that is not possible for a more quantitative and instrument-based analysis.
In summary, archaeometallurgy is a rather broad and diverse field, and draws from an
equally wide range of scholarly and analytical methods of study. Metals play a fundamental role
in the social, economic and technological fabric of almost all post-Neolithic societies. The study
of ancient metal production and manufacturing, and of the trade in raw metal and finished
metal objects, includes such diverse approaches as optical microscopy, physical, chemical and
isotopic analysis, and experimental reconstruction. How is this wealth and diversity of
archaeometric approaches reflected in the literature?
PUBLISHING ARCHAEOMETALLURGY
Studies of archaeological metal objects, their production and their manufacturing methods
were already pioneered in the early 19th century by eminent chemists. M. H. Klaproth (1815)
published the first ever quantitative analysis of an alloy, on a Roman coin (Caley 1949). Others
include J. F. Gmelin (1783), G. Pearson (1796), J. J. Berzelius (1836) and M. Berthelot
(1906). Particularly relevant were the works by F. Wibel (1863, 1864), who addressed many
archaeometallurgical topics and problems, such as the composition and identification of native
copper, more than a century ago. Comparatively systematic studies of the composition of
ancient metal objects were performed by von Fellenberg on bronzes (1866) and von Bibra on
bronzes, iron and silver (1869, 1873). There was little further progress until the late 1920s,
when the Sumerian Metals Committee was appointed by the Royal Anthropological Institute,
triggered by the exceptional finds at the Royal Cemetery at Ur in Mesopotamia (Woolley
1931). It reported on the origin of Sumerian copper, assuming that its nickel content could be
indicative of the ore source (Desch 1928–38). From these interim reports it is obvious that the
original objective was not really achieved, but they resulted in the creation of a further unit,
the Ancient Metal Objects Committee, in 1939.
In the 1930s, a new analytical method—optical emission spectrometry, nowadays called
atomic emission spectrometry—was introduced. This technique allowed the determination of
many elements at trace levels using minute sample masses and was the basis for the development
of a new interdisciplinary field, geochemistry. Like their predecessors, geochemists also
became interested in ancient metallurgy, and the first programmatic paper on provenance
determination appeared in 1934 (Noddack and Noddack 1934). During this time, large analytical
programmes on ancient metals and ores were started by Witter (1935, 1938) and Pittioni
(1932) as well as Preuschen and Pittioni (1937), which led to the publication of major summary
Coins, artefacts and isotopes—archaeometallurgy and
Archaeometry 241
© University of Oxford, 2008,
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works (Otto and Witter 1952; Pittioni 1957) with a compilation of some 6000 analyses of
prehistoric metal objects, mainly from Europe. This was called the first phase of analytical
archaeometallurgy by Härke (1978), who provides a comprehensive summary of the history of
archaeometallurgy. In this period, the Ancient Mining and Metallurgy Committee was founded
in London by H. H. Coghlan, and it initiated analyses of ancient metal artefacts along the lines
of the pioneering works of Otto and Witter. The second phase began with another large-scale
programme, initiated by S. Junghans in Stuttgart—the Studien zu den Anfängen der Metallurgie—
which eventually produced and published more than 22 000 analyses of metal objects (Junghans
et al.
1960, 1968, 1974). Many laboratories in Europe (Vienna, Moscow, Baku, Milan, Rennes
and London) joined this endeavour, with the aim of identifying the composition of metal
objects in different periods and identifying the sources from which the raw material came. One
of these laboratories was the Research Laboratory for Archaeology and the History of Art in
Oxford (Blin-Stoyle 1959; Britton 1961; Britton and Richards 1963). Following the observation
that many of the OES analyses were not comparable between laboratories, it was believed that
metal analyses by OES were ‘a waste of time’ (Hall 1970). The programme was stopped and
metal analyses were then performed by neutron activation analysis (Gordus 1967) or by
atomic absorption analysis (AAS—e.g., Cowell 1987). This marked the beginning of the third
phase, according to Härke (1978), characterized by the employment of other and more accurate
analytical techniques for metal analysis, rather than OES.
The work focusing on metal artefacts was complemented by studies of the primary production.
While chemists pioneered the analysis of metal objects, it was mostly metallurgists and
geologists who drove the development of the metallurgical aspects of archaeometallurgy.
General works on the history of metals and metal production appeared from the second half of
the 19th century onwards (Zippe 1857; Rossignol 1863; Andree 1884; Rössing 1901; Neumann
1904; Gowland 1912; Bergsoe 1937; Marechal 1962). These were accompanied and followed
by papers by, for example, Morton and Wingrove in the late 1960s and early 1970s (see Morton
and Wingrove 1969, 1972), C. S. Smith from the 1950s to the late 1970s, R. Tylecote from the
1960s to the 1980s, H. G. Bachmann from the 1960s and R. Maddin from the mid-1970s
onwards, often in collaboration with mining archaeologists such as B. Rothenberg, G. Weisgerber,
B. Jovanovic and C. Domergue. The literature here is vast and dispersed over a wide range of
journals in the engineering and natural sciences, archaeological journals and excavation
monographs. Good bibliographies are contained in books such as Tylecote (1987), Rostoker
and Bronson (1990), Craddock (1995) and Pleiner (2000).
Significantly, this rich history of serious and often large-scale studies has been published
predominantly in form of monographs, or as articles in established journals in the ‘mother
disciplines’ of the authors. Until 1958, there was no specific publication outlet dedicated to the
interdisciplinary work crucial for the new progress being made.
Specialist journals
These pioneers in archaeometallurgy literally had to invent the field, and had little pre-existing
academic structure to work with. This lack of structure included the absence of dedicated journals,
and as a result they founded their own journals: in 1966, Ronald Tylecote established the
Journal of the Historical Metallurgy Society
(now known as
Historical Metallurgy
). It appears
that the term ‘archaeometallurgy’ itself was coined only in 1973 by B. Rothenberg (Goodway
1992), when he established the Institute for Archaeo-Metallurgical Studies, publishing much of
its work in the
iams
newsletter, now the
iams
journal. Significant results in archaeometallurgy
242
Th. Rehren and E. Pernicka
© University of Oxford, 2008,
Archaeometry
50
, 2 (2008) 232–248
grew out of the work of the scientific laboratories of major museums, such as the British
Museum, the Deutsches Bergbau-Museum (DBM) and the collective Berlin museums. Both
the BM and the DBM organized series of international conferences in archaeometallurgy,
providing important venues for the exchange of ideas and development of projects; many of these
conferences were published, either as British Museum Occasional Papers, or as supplements
(‘Beihefte’) to the DBM’s house journal,
Der Anschnitt
. A series of conferences under the title
‘Beginnings of the Use of Metals and Alloys’ (‘BUMA’) was established by R. Maddin and
Tsun Ko in 1981, and recently had its sixth incarnation in Beijing. The
Bulletin of the Metal
Museum
was set up in 1976, the year after the foundation of the Metals Museum by the Japan
Institute of Metals. It was a special case in that it did not so much publish primarily research by
the staff or members of the backing institution, but relied heavily on invited papers and sub-
missions from outside the museum. This journal ceased to exist in 2003, due to the closure of
the Metals Museum.
Archeomaterials
, starting in 1986, was explicitly more wide-ranging,
rather than focusing on ancient metals, although many of its papers were concerned with
archaeometallurgy; in contrast to the other examples mentioned above, it had no institutional
or organizational structure behind it, but was backed by one individual, William Rostoker.
Following his death in 1991,
Archeomaterials
ceased to appear in 1993, after only seven volumes.
Three journals set up in the tradition of
Archaeometry
need to be mentioned. The Journal of
Archaeological Science first appeared in 1974, followed by Revue d’Archéometrie, in 1977;
both cover the entire range of archaeometry, including papers on archaeometallurgy, without
any particular link to a laboratory. The annual Berliner Beiträge zur Archäometrie was first
published in 1975 by the Rathgen Research Laboratory, founded in 1888 as the Chemical
Laboratory of the Royal Museums in Berlin. Like Archaeometry, it is closely linked to a
particular laboratory; it has carried a range of papers on archaeometallurgy, most notably
reports on the composition of metal artefacts, conducted in the tradition of the earlier large
series of object analyses.
Archaeometallurgy in Archaeometry
Thus, and while there was—and still is—a range of specifically archaeometallurgical journals
and series, Archaeometry, established in 1958, was ahead of the game by a decade or two. Its
position and starting vision were typical of the time; as stated by Edward Hall, its founding
editor, it was meant to report (primarily but not exclusively) on work done by staff of the
Research Laboratory for Archaeology and the History of Art at Oxford University. It aimed to
rapidly circulate results of completed research as well as to report on only partially successful
work ‘not worthy of normal publication’, and of interim results of work in progress (Hall
1958).
This policy of also publishing interim and unsuccessful work did not prevail for long. Soon,
Archaeometry became an outlet for full-blown research papers, with the same standards of
peer review and subsequent delay in publication as other major journals. However, the emphasis
on work done within the laboratory and its various co-operative ventures was less easy to
overcome, and remained visible for decades to come. This is not the place for a detailed break-
down of papers by subdiscipline within the journal, and how this has changed over time; suffice
it to say that in the first decade, papers on dating methods and geophysical prospection both
featured equally strongly, with the latter very abruptly disappearing after 1971 and the former
gaining significantly from 1970 onwards. There are volumes in the 1970s where papers on
dating make up between one third and one half of all the published papers. From the 1980s
Coins, artefacts and isotopes—archaeometallurgy and Archaeometry 243
© University of Oxford, 2008, Archaeometry 50, 2 (2008) 232–248
onwards things become more balanced, with relatively stable ratios between papers on dating,
ceramics, organic materials, metals and other topics.
Looking more closely at the number and topics of papers in Archaeometry, archaeometallurgy
started strong, with two out of five in the first year. But while the number of papers published
quickly increased to a typical 15–20 per year throughout the 1960s, contributions on metals
remained at around 1–3 papers per year (ppy) until 1971. By this time, the average number of
papers per year in the journal had risen to more than 20, and remained at 20–25 ppy for the
next 25 years. Throughout this period, archaeometallurgy contributed regularly between 2 and
5 ppy; a figure that has not significantly improved since then, hovering at 5–6 ppy for the past
10 years or so. At the same time, the overall number of papers in the journal has increased sig-
nificantly. From 1995 onwards there were around 30 ppy overall, a number which has further
increased to 40–50 ppy in the past five years. Thus, we see a strong and sustained overall
increase in papers in Archaeometry, particularly for the past decade or so, but less so in papers
dealing with archaeometallurgical topics. Based on pure numbers, archaeometallurgy papers were
most prominent in the mid-1970s, when they constituted around 20% of all papers published;
since then, the share of archaeometallurgy papers within Archaeometry has fallen to nearer
15%, and even as low as 10%.
Despite the broadening of the scope and range of topics published in Archaeometry beyond
the immediate interests of the staff and associates of the RLAHA, a rather specific profile of
archaeometallurgy was still visible; some topics were strongly represented in Archaeometry,
while others were nearly absent. Most notably, there was a very strong focus on chemical analysis
of gold and silver coins and bronze artefacts; the entire second volume is on bronze analysis.
Coin and artefact analysis were almost the only archaeometallurgical topics for the first five
years of publication, and up to the mid-1980s there were also regularly one or two papers on
the development of methods of chemical analysis of metals, often using coins as test cases
(e.g., Meyers 1969). Thus, coins featured both as objects of study in their own right and as
convenient (and relevant) test materials. From the early 1970s onwards, they were increasingly
accompanied by papers reporting the composition of other types of metal artefacts, most often
bronze objects, and discussions of analytical method developments (e.g., Hughes et al. 1976).
These three subgroups (coins, bronze artefacts and method development) make up, in almost equal
parts, the bulk of all archaeometallurgy papers for more than a decade, from 1972 to 1985.
However, the frequency of ‘coin papers’ dropped dramatically in the mid-1980s: before
1986, coins were typically represented with one or two ppy, but from 1986 onwards this
dropped to an average of 0.5 ppy. This decline was initially not compensated for by the
publication of other archaeometallurgy papers, and there was a noticeable lull in such
papers in Archaeometry from 1986 to 1991. Not only had the supply of coin papers dried up,
but also the publication of papers on other metal artefacts had all but ceased. Thus, over the
five years there were only 2–3 ppy on archaeometallurgy.
A major change took place in 1992: for the next 12 years the trend was reversed by a sudden
and sustained emergence of isotope-related papers. However, this was rather late, with the first
paper on lead isotopes in 1985 by Mabuchi et al., 20 years after Brill and Wampler (1965)
introduced the method to archaeology. The next one appeared in 1988, and it was not until
1992 that a constant delivery of two or three such papers per year set in. This has already been
briefly commented on above, in the context of lead isotope studies in archaeometallurgy. Due
to the importance of LI analyses for the reconstruction of ancient trade patterns, they are of
major interest and direct significance for archaeology, probably more so than trace element
patterns of objects, which are more difficult to interpret.
244 Th. Rehren and E. Pernicka
© University of Oxford, 2008, Archaeometry 50, 2 (2008) 232–248
Most remarkable is the very low frequency of papers to do with iron metallurgy. This is a
massive and significant deviation from the archaeological reality on the ground and the quantity
of excellent work done in the field. Iron is of overwhelming importance in nearly all cultures
of the past two millennia or so, from the Roman period onwards in Europe, from the Han
dynasty onwards in China, and throughout the metal-using history of sub-Saharan Africa. Not
only are studies of iron artefacts or metallography in general exceedingly rare in Archaeometry
(Knox 1963 and Charles 1973 are rare exceptions), but so are studies in iron smelting.
Some of this may be the mirror effect of the prevalence of iron-related papers in Historical
Metallurgy, with its strong tradition of iron- and steel-specific papers. Only in the past few
years do we see more iron-themed papers published in Archaeometry, probably indicating a
broadening of the author base of the journal.
A similar lacuna is the near-total absence of papers presenting or discussing primary
production or more technological process-oriented studies. The recent papers on early copper
production in the Alps (Höppner et al. 2005; Tumiati et al. 2005) and on reconstructed EBA
copper smelting (Pryce et al. 2007) are probably the first papers concerned with copper smelting
ever to be published in Archaeometry, and Heimann et al. (2001) and Paynter (2006) the first
ever for iron smelting.
Thus, in conclusion, it is fair to state that Archaeometry has been a consistent, but never
a major, outlet for archaeometallurgy. Over the half-century of its existence, about 185
archaeometallurgy papers have appeared in its pages, many of them innovative and stimulating
further research. What is remarkable is the rather clear profile of most of these papers, which
gives archaeometallurgy in the pages of Archaeometry its very own flavour.
CONCLUSION
This year, Archaeometry is turning 50. During this time, it has grown out of its origins as an
outlet for some ongoing work from a particular laboratory into a leading journal covering the
entire range of archaeometric research with authors from around the globe.
As one of the constituent parts of science-based archaeology, archaeometallurgy has a firm
place within the journal, but with a particular profile. The range of archaeometallurgical
papers typically printed in Archaeometry differs significantly from the overall range of activity
in the field. This partly reflects the much earlier origins of archaeometallurgy, particularly in
central Europe, which had established their own traditions with regard to publishing in other
journals. However, it also reflects the emergence of a number of smaller, specifically archaeo-
metallurgical, journals soon after Archaeometry first appeared, which have their own focus and
emphasis, and cater for a considerable amount of the work done in archaeometallurgy. Thus,
more process-specific work, and work concerned with iron making and iron or steel objects, is
often published in either Historical Metallurgy or in Archeomaterials (while it still existed);
papers with particular reference to Asian metallurgy often appeared in the Bulletin of the Metals
Museum, printed in Japan. In contrast, Archaeometry traditionally has an emphasis on physical
and chemical approaches to archaeometry, manifest in the majority of papers dealing with
chemical analysis of coins and other metal artefacts, often combined with method development,
whereas papers based on metallography or the analysis of waste materials, such as slags and
technical ceramics, are much under-represented. Of particular interest is the situation concerning
the application of lead isotope studies in archaeometallurgy. The Isotrace Laboratory, as part
of the RLAHA, has been for many years one of the two leading laboratories in this area, but
relatively little evidence of this shows in Archaeometry itself. More recently, this division is
Coins, artefacts and isotopes—archaeometallurgy and Archaeometry 245
© University of Oxford, 2008, Archaeometry 50, 2 (2008) 232–248
beginning to blur, and the past five years have seen slightly increasing numbers of papers on
both iron and metal smelting in general, topics which were virtually absent during the first
40 years of publication activity.
It would take an altogether different (but certainly interesting) paper to investigate the
conscious and subconscious decisions that are taken, by authors and editors alike, and that drive
these patterns in publication behaviour. Suffice it here to say that these patterns have their
roots in the past, shape the present, and will certainly continue to exist in one form or another
in the future. We are confident that Archaeometry will further develop its special contribution
to archaeometallurgy, and we wish it every success in this endeavour, for decades to come!
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