Journal of Archaeological Science xxx (2012) 1e9

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Journal of Archaeological Science

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Tracing the source of Late Neolithic Spondylus shell ornaments by stable isotope
geochemistry and cathodoluminescence microscopy
Bernadett Bajnóczi a, Gabriella Schöll-Barna a, Nándor Kalicz b, c, Zsuzsanna Siklósi c, *,
George H. Hourmouziadis d, Fotis Ifantidis d, Aikaterini Kyparissi-Apostolika e, Maria Pappa f,
Rena Veropoulidou g, Christina Ziota h
a
Hungarian Academy of Sciences, Research Centre for Astronomy and Earth Sciences, Institute for Geological and Geochemical Research, Budaörsi út 45, H-1112 Budapest, Hungary
b
Hungarian Academy of Sciences, Research Centre for the Humanities, Institute of Archaeology, Úri utca 49, H-1014 Budapest, Hungary
c
Eötvös Loránd University, Institute of Archaeological Sciences, Múzeum körút 4/B, H-1088 Budapest, Hungary
d
Aristotle University of Thessaloniki, Department of Archaeology, Greece
e
Ephorate of Palaeoanthropology & Speleology of Southern Greece, Hellenic Ministry of Culture, Greece
f
16th Ephorate of Prehistoric and Classical Antiquities, Thessaloniki, Hellenic Ministry of Culture, Greece
g
Museum of Byzantine Culture, Thessaloniki, Hellenic Ministry of Culture, Greece
h
30th Ephorate of Prehistoric and Classical Antiquities, Aiani, Kozani, Greece

a r t i c l e i n f o a b s t r a c t

Article history: Determination of the source of Spondylus objects is essential for the interpretation of Late Neolithic
Received 16 November 2011 exchange systems and the social role of shell ornaments. We performed stable isotope analysis combined
Received in revised form with cathodoluminescence microscopy study on ornaments (beads, bracelets) made of Spondylus shells
3 September 2012
excavated at the Aszód-Papi földek archaeological site in Hungary, to define their origin. For comparison
Accepted 20 September 2012
Spondylus finds from Neolithic sites of Greece, modern Spondylus shells from the Aegean and the Adriatic,
as well as fossil Spondylus and Ostrea shells from the Carpathian Basin were also examined. Oxygen
Keywords:
isotope composition of Spondylus finds from Aszód ranges between
1.9 and 2.1& and overlaps with the
Spondylus
Late Neolithic ornaments
oxygen isotope range of shell objects from other Neolithic sites. Modern Spondylus shells from the
Stable isotope Aegean and the Adriatic show overlapping d18O values with one another and with the Neolithic objects;
Cathodoluminescence while recent shells of the Black Sea clearly are separate isotopically from the Mediterranean ones and
Provenance analysis most of archaeological artefacts. Spondylus shells from the Aszód site have Mediterranean origin; their
source can be the Aegean or the Adriatic. Based on a former strontium isotope study the use of fossil
Spondylus shells is excluded as raw material used for ornaments, however, in recent years the use of fossil
shells was reintroduced. The shell ornaments from Aszód-Papi földek and the fossil oyster shells
collected from the Carpathian Basin exhibit some overlapping oxygen isotope values; however, cath-
odoluminescence microscopy indicates that the Spondylus objects retained their original aragonite
material. Diagenetic calcite, which occurs typically in the fossil shells, was not detected in the ornaments
suggesting that the studied objects were made of recent shells. Calcitic parts observed in some Spondylus
objects are not related to fossilisation.
Ó 2012 Elsevier Ltd. All rights reserved.

1. Introduction
Spondylus gaederopus, or thorny oyster, is a bivalve mollusc
preferring warm-water seas. S. gaederopus species currently live in
the Mediterranean e mainly in its eastern part, the Aegean and the
Adriatic e cementing themselves to rocks or coral in a depth of 6e
30 m. The width of a mature shell varies between 6 and 12 cm,
* Corresponding author. Tel.: þ36 1 411 6500/2116; fax: þ36 1 411 6553.
E-mail addresses: siklosi.zsuzsanna@btk.elte.hu, siklosizs@gmail.com
(Zs. Siklósi).
recent shells are usually smaller than those known from
prehistory. There are considerable differences in shape and size of
the lower and the upper valves. The lower valve is oval or round,
definitively thick, while the upper valve is round, thinner, thorny
and purple on its outer surface. These characteristics determined
the shape and size of the ornaments made from them (Tsuneki,
1987; Miller, 2003; Chapman and Gaydarska, 2007; Pappa and
Veropoulidou, 2011; Siklósi and Csengeri, 2011).
One of relevant issues regarding Neolithic Spondylus ornaments
is the origin, i.e. provenance of the shell raw material used for
preparing artefacts. Based on stable isotope geochemical analyses

0305-4403/$ e see front matter Ó 2012 Elsevier Ltd. All rights reserved.
http://dx.doi.org/10.1016/j.jas.2012.09.022

Please cite this article in press as: Bajnóczi, B., et al., Tracing the source of Late Neolithic Spondylus shell ornaments by stable isotope
geochemistry and cathodoluminescence microscopy, Journal of Archaeological Science (2012), http://dx.doi.org/10.1016/j.jas.2012.09.022
2 B. Bajnóczi et al. / Journal of Archaeological Science xxx (2012) 1e9
Shackleton and Renfrew (1970) proposed that the likely source of
the Neolithic Spondylus shells was the Mediterranean, specifically
the Aegean. Spondylus in recent years does not live in the Black Sea,
however, Todorova supposed on the basis of the great amount of
Neolithic and Copper Age Spondylus finds from the Black Sea coast
of Bulgaria that Spondylus could live not only in the Mediterranean,
but also in the Black Sea in this period. Todorova (2000, 2002)
proposed that during the “climate optimum” the Black Sea could
have been a habitat for Spondylus, therefore she did not exclude the
Black Sea as a possible provenance.
Researchers unanimously excluded the possibility of using fossil
Spondylus shells based on the results of strontium isotope analysis
performed by Shackleton and Elderfield (1990). The overwhelming
majority of Spondylus shell raw material used for preparing orna-
ments was supposedly to be contemporary to the Neolithic causing
several researchers to reconstruct a long-distance exchange system
from the Aegean through the Balkan and Central Europe to the Paris
Basin (Séfériadès, 1995a, 1995b, 2000; Müller, 1997; Kalicz and
Szénászky, 2001; Dimitrijevi c and Tripkovic, 2003; Siklósi, 2004).
In the last few years the idea of using fossil shells for making
ornaments during the Neolithic has risen again (Dimitrijevi c and
Tripkovi c, 2006; Sümegi, 2009). There are fossil Spondylus sites
for example in the territory of Eastern Bulgaria (Chapman and
Gaydarska, 2007). This fact is thought-provoking as this is the
same area where the usage of Spondylus ornaments has the longest
duration (see later) (Müller, 1997; Todorova, 2000, 2002).
Despite seemingly successful application of the isotope
methods, studies of Shackleton and Renfrew (1970) and
Shackleton and Elderfield (1990) are not “without potential
problems” (Douka, 2011). The amount of analysed samples is
relatively small, e.g. nine Spondylus artefacts from four archaeo-
logical sites were analysed for stable isotope composition, while
empirical dating by comparison of 87Sr/86Sr ratio of shells to the Sr
isotope evolution curve of seawater was performed only on three
Neolithic Spondylus artefacts and one fossil Spondylus crassicosta.
In addition, these studies did not check in detail the signs of
postdepositional processes or diagenetic alteration (recrystalli-
zation) of artefacts, which can modify the shell mineralogy as well
as the original isotope values (Douka, 2011). After the above-
mentioned two publications application of isotope geochemical
methods was not widely used in the research of Neolithic Spon-
dylus ornaments. Later only Todorova (2002) published stable
isotope data of Spondylus artefacts (17 objects) and interpreted
them as indicating two biotopes.
During stable isotope analysis ratios of oxygen and carbon
isotopes (18O/16O, 13C/12C) of carbonate, the mineral constituent of
shell, are measured. It is generally agreed that carbonate of bivalve
shells is precipitated in equilibrium with ambient seawater (Epstein
et al., 1953), this approach is also proven for S. gaederopus (Maier
and Titschack, 2010). The oxygen isotope composition of shell
carbonate depends on the oxygen isotope composition of seawater,
which covaries linearly with salinity, and the temperature of
carbonate precipitation (Hoefs, 2009). Different temperature and/
or oxygen isotope composition of seawater in different habitats
provides opportunity for distinguishing shells from different
sources based on the oxygen isotope composition. During their
early study Shackleton and Renfrew (1970) used this assumption
and expected that Black Sea is isotopically more negative than the
Mediterranean due to its water budget. Isotope analyses of recent
Nassa reticulata and Chamelia gallina species from the Black Sea
seemed to confirm their hypothesis and isotope values of recent
shells did not overlap with the values of Spondylus artefacts from
Bulgarian, Greek and Serbian archaeological sites, therefore arte-
facts were supposed to be originated from the Aegean rather than
the Black Sea.
Please cite this article in press as: Bajnóczi, B., et al., Tracing the source of Late Neolithic Spondylus shell ornaments by stable isotope
geochemistry and cathodoluminescence microscopy, Journal of Archaeological Science (2012), http://dx.doi.org/10.1016/j.jas.2012.09.022
The assumption of Shackleton and Renfrew (1970) regarding the
difference in stable isotope composition of the Black Sea and the
Mediterranean seems to be valid. Surface waters of the eastern
Mediterranean exhibit d18O values between 1.30 and 1.66& (Pierre,
1999) or may have even more positive values up to 2.2& (Gat et al.,
1996), while the surface waters of present-day Black Sea have more
negative d18O values (Swart, 1991),
2.8& in average with standard
deviation of 0.34& (Ranke et al., 1999). Therefore basic prerequisite
that the basins are different in isotope composition can be assumed
and successful provenance study of shells can be expected provided
that the calcium carbonate of the shells is deposited under isotopic
equilibrium conditions or very close to equilibrium with environ-
mental waters.
While the local, i.e. Aegean source can unequivocally be
assumed for the Spondylus ornaments in the find material of Greek
archaeological sites, the Aegean origin is not evident in case of
artefacts found in the continental European sites. The possibility of
Adriatic origin has also to be taken into account.
Our study intends to extend the number of archaeological
samples analysed by using the stable isotope method combined
with non-destructive cathodoluminescence microscopy, the latter
is used to check whether shell artefacts preserved their original
mineralogy. We performed analysis on Spondylus ornaments found
at the Late Neolithic Aszód-Papi földek site (Hungary) and exam-
ined Spondylus finds from Neolithic sites in Greece, which are
roughly contemporaneous with the Aszód settlement. The aim of
our research is to determine the provenance of the raw material of
Spondylus ornaments, i.e. whether the shells were recent ones
originating from the Mediterranean or Black Sea or were fossil
specimens. Recent Spondylus shells from the Adriatic and the
Aegean were analysed as a comparative material. There are several
geological sites in the Carpathian Basin where fossil Ostrea shells
can be collected in great amount and fossil Spondylus can be found
within cca. 50 km vicinity of Aszód (Csepreghyné Meznerics, 1954),
therefore we cannot reject the possibility of using fossil shells
without further research. Miocene Spondylus fossils and fossils of
a related species, Ostrea from the vicinity of the site and from
a distant locality in Romania were studied both for mineralogy and
geochemistry in order to identify possible fossil shells in the find
material.
2. Archaeological context
Spondylus ornaments as prestige goods played an important role
in the expression of social inequality and prestige manipulation all
through the Neolithic of the Carpathian Basin, but their usage
changed considerably during this period (Kalicz and Szénászky,
2001; Siklósi, 2004; Siklósi and Csengeri, 2011).
The first sporadic Spondylus ornaments e exclusively brace-
lets e appeared during the Early Neolithic (cca. 6000e5500 cal
BC) in the Carpathian Basin (Kalicz and Szénászky, 2001;
Siklósi, 2004).
From the beginning of the Middle Neolithic (cca. 5500e5000 cal
BC) the usage of Spondylus ornaments suddenly dispersed in the
Carpathian Basin. During this period Spondylus ornaments reached
even the area of present-day Poland, Germany and France (Willms,
1985; Müller, 1997; Séfériadès, 1995a, 1995b; 2000).
In the Middle Neolithic mainly large, heavy ornaments were
used with high raw material requirement and were prepared
individually. The characteristic Middle Neolithic types were large
pendants made of a whole shell valve, V-Klappen, massive bracelets
and large beads found mainly in graves and hoards, very rarely in
settlement features (Kalicz and Szénászky, 2001). In this period
male, female as well as children’s graves contained Spondylus
ornaments, although there are local differences (Siklósi, 2004).
 B. Bajnóczi et al. / Journal of Archaeological Science xxx (2012) 1e9 3

Spondylus ornaments had an important role in the expression and
manipulation of prestige or social inequality in this period. They
were the privilege of the few and the acquisition of Spondylus must
have been strongly limited. Ornaments placed into the grave could
be particularly valuable, especially if we take into consideration
that in the Middle Neolithic burials without grave goods were very
common. It seems that in this period only a narrow section of the
population had the right to be buried in the territory of the
settlement (Siklósi and Csengeri, 2011). There were competing,
rivalry families or lineages in the Middle Neolithic that expressed
and manipulated their prestige as well as social and economic
influence by exchanging and wearing exotic ornaments.
Contrary to this, since the transition from the Middle to the Late
Neolithic (cca. 5100e4500 cal BC), considerable changes can be
observed in Spondylus usage. First, considerable changes in
costumes or fashion can be witnessed: necklaces, belts, bracelets
and anklets consisting of composite, multi-row, tiny beads appear
instead of heavy, one-row necklaces and belts. These ornaments are
smaller and finished in a more sophisticated way. At the same time
this might mean that the “mass production” of shell ornaments
started, which is also evidenced by the size homogeneity of tiny
beads. Secondly, according to the data from Late Neolithic graves,
Spondylus prestige raw material became accessible to larger groups
of society in small amounts (Siklósi and Csengeri, 2011).
Compared to the former period the expression form of prestige
also changed. Wearing Spondylus ornaments was limited almost
only to women and children (most probably girls). In this period
new raw materials appeared in the manifestation and manipulation
of prestige, which gradually took over the role of Spondylus.
Together with access of bigger social groups the importance of
Spondylus ornaments as prestige goods decreased, but a new raw
material also appeared: copper. Copper ornaments were accessible
only to a narrow group and they were able to take over the role
which Spondylus ornaments were increasingly unable to play. More
and more frequently limestone or marble beads supplemented
Spondylus string of beads as imitations. On the one hand, this shows
the importance and value of Spondylus. On the other hand, it also
indicates that short-distance connections became more and more
intensive, and long-distance exchange gradually became scarce
(Siklósi, 2004).
Viewing the usage of Spondylus ornaments in a wider
geographical frame, one can observe that the northern and western
boundary of the distribution of Spondylus ornaments were the
Carpathian Basin during the Late Neolithic, that is its distribution
was strongly repressed (Müller, 1997). This tendency continued in
the Early Copper Age (cca. 4500e4000 cal BC), when limestone
beads decisively replaced Spondylus beads and copper became the
primary symbol of prestige. However, Spondylus ornaments were
continually used in the Lower Danube region during this period
indicating the change of exchange networks.
Based on the above considerations, it is extremely important to
determine the provenance of Spondylus objects or their raw
material in terms of the explanation of Late Neolithic relations and
social role of Spondylus ornaments, and to determine the trans-
portation distance and quantity of these objects.
In this study we are focusing on a Late Neolithic site, Aszód-Papi
földek which is situated in the Gödöllo} Hills, in Northern Hungary,
cca. 40 km east of Budapest (Fig. 1). At the site N. Kalicz conducted
excavations between 1960 and 1987, and revealed remains of a Late
Neolithic settlement and 224 Late Neolithic graves. The ceramic

Fig. 1. Locality of the Spondylus ornaments, fossil and modern Spondylus and Ostrea shells examined in this study. Neolithic archaeological sites: 1. Aszód-Papi földek, 2. Dispilio, 3.
Theopetra Cave, 4. Kleitos, 5. Makriyalos, modern Spondylus shells: 5. Makriyalos, 6. East Thermaikos Gulf, 7. Polychrono Beach, 8. Rovinj, 9. Vir, 10. Peljesac, fossil Spondylus shells:
11. Sámsonháza, 12. Lapugiu de Sus, fossil Ostrea shells: 13. Buják.

Please cite this article in press as: Bajnóczi, B., et al., Tracing the source of Late Neolithic Spondylus shell ornaments by stable isotope
geochemistry and cathodoluminescence microscopy, Journal of Archaeological Science (2012), http://dx.doi.org/10.1016/j.jas.2012.09.022
4 B. Bajnóczi et al. / Journal of Archaeological Science xxx (2012) 1e9
material of the site represents both the pottery of Early Lengyel
culture (Transdanubia) and Tisza culture (Great Hungarian Plain)
(Kalicz, 1985, 2006, 2008). This strong relationship towards the
Great Hungarian Plain can be explained by the geographic situation
of the site. Besides ceramics, stone raw materials and several
Spondylus items reflect the extensive relations of the past
community which lived at the site.
3. Materials and methods
To perform easier sampling relatively large (larger than about
1 cm) beads (19 pieces), one intact and one fragmentary bracelet
were selected from the find material of the Aszód site for stable
isotope analysis. We also analysed Spondylus finds from Neolithic
sites in Greece (Fig. 1): Kleitos (Kozani), Makriyalos (Pieria), Dis-
pilio and Theopetra Cave (15 pieces; Ziota, in press; Ziota et al., in
press; Pappa and Veropoulidou, 2011; Hourmouziadis, 2002;
Ifantidis, 2011; Kyparissi-Apostolika, 1999, 2011). For comparison
we measured modern Spondylus shells from the Aegean (from
Greece: Chalkidiki (Thermaikos Gulf, Polychrono Beach) and
Makriyalos (Pieria, Thermaikos Gulf), 3 pieces) and the Adriatic
(from Croatia: Rovinj, Vir and Peljesac Peninsula, 3 pieces) (Fig. 1).
Fossil (Miocene) Spondylus shells from two localities (Hungary:
Sámsonháza and Romania: Lapugiu de Sus) as well as fossil Ostrea
shells (from Hungary: Buják) were analysed (5 and 2 pieces,
respectively).
The shell of S. gaederopus is composed of two carbonate
minerals: the outer layer is made of calcite and the inner layer is
made of aragonite. The hinge, which joins the upper and lower
valves together, is fully aragonitic, while near the margin the
proportion of calcite increases and the edge of the shell margin is
entirely calcitic (Titschack et al., 2009; Maier and Titschack, 2010).
According to the orientation of growth lines larger beads of the
Aszód material were made from the thickest part of the shell, i.e.
umbo and hinge, therefore they are originally composed of arago-
nite. Smaller beads may have been made from the hinge as well as
the marginal part of the shell. Bracelets were made by removal of
the umbo; one of their fronts is most probably the hinge. Modern
and fossil shells studied for comparison were sampled at the hinge
(except Ostrea). During sampling the original calcite-bearing parts
of the Spondylus shells were avoided, because calcitic marginal
parts have d18O value more negative by 0.8e1.0& than aragonitic
parts (Maier and Titschack, 2010), therefore isotope results can be
more negative than expected.
Cathodoluminescence microscopy is a useful and inexpensive
analytical method to determine carbonate constituents (aragonite
and/or calcite) of shells non-destructively. The ornaments of the
Aszód site and the fossil shells were studied by this technique when
their size permitted. Cathodoluminescence (CL) is an emission of
visible light by an excited substance due to the bombardment of
a high-energy electron beam originating from a cathode. Excitation
is caused by luminescence centres like impurities and crystal lattice
defects in the substance. Due to the different luminescence colours
of aragonite and calcite, mineralogy of the shells could be identified
easily. The aragonite constituent of shells has mainly weak blue CL,
which can be related to crystal lattice defects (Marshall, 1988). Parts
of some aragonitic beads rarely show green CL due to substitution
of manganese (II) for calcium (II) in the carbonate lattice. Any
calcitic regions in the shell can be located by its characteristic
yellow-orange to orange-red CL colour caused by the presence of
manganese substitution in the calcite lattice. Cathodoluminescence
examination was performed using Reliotron “cold-cathode”
equipment mounted on Nikon Eclipse E600 microscope and oper-
ated at 6e10 keV acceleration voltage, the setup allows studying
relatively large (several cm sized) objects. Photos were made by
Please cite this article in press as: Bajnóczi, B., et al., Tracing the source of Late Neolithic Spondylus shell ornaments by stable isotope
geochemistry and cathodoluminescence microscopy, Journal of Archaeological Science (2012), http://dx.doi.org/10.1016/j.jas.2012.09.022
Nikon Coolpix 4500 digital camera using automatic exposure and
defocused electron beam.
Previous to stable isotope analysis contaminations on the
surface of the shells were removed by polishing. Bracelets, modern
and fossil shells were polished only on the sampling area; beads
were polished on the whole surface. Mechanically cleaned samples
were treated by sodium hypochlorite solution to remove any inter-
granular organic matter, and then washed with distilled water and
finally cleaned using an ultrasonic bath. Sampling was made by
drilling (ø ¼ 0.6 mm) minimally at three (rarely two) spots in each
shell or ornament in the direction of shell growth. Stable carbon
and oxygen isotope compositions of approximately 150e200 mg
carbonate samples were determined applying the carbonate-
orthophosphoric acid reaction at 72  C and using automated GAS-
BENCH II equipment attached to a mass spectrometer. 18O/16O and
13 12
C/ C ratios of the evolved CO2 gas were measured using
a Thermo Finnigan Delta Plus XP continuous flow mass spectrom-
eter. Standardization was conducted using in-house reference
materials calibrated against NBS-18 and NBS-19 international
standards. The stable isotope compositions are expressed as d13C
and d18O values in & relative to V-PDB (Vienna Pee Dee Belemnite)
international standard, where d ¼ (Rsample/Rstandard
1)  1000, R is
the 18O/16O or 13C/12C ratio. The analytical reproducibility is better
than 0.2&. Results were averaged for each shell or object and
average values with standard deviations are indicated on d18O vs.
d13C plots.
4. Results and discussion
Average d18O values of Spondylus ornaments from Aszód-Papi
földek vary between
1.9 and 2.1& and average d13C values are
between
2.0 and 1.4& (Table 1, Fig. 2). The isotope data of Spon-
dylus objects from the archaeological excavations of Tell Goljamo
Delcevo, Gradeshnitsa (Bulgaria), Sitagroi (Northern Greece) and
Vinca (Serbia) published by Shackleton and Renfrew (1970) range
from
1.2 to 0.0& for d18O and from 0.0 to 1.2& for d13C. Spondylus
artefacts from Durankulak (NW-Bulgaria) and several Austrian
archaeological sites have d18O values between
1.1 and 1.0& and
d13C values between
1.3 and 1.9& published by Todorova (2002).
The stable isotope range of the ornaments from Aszód overlaps
with the formerly published isotope data (Fig. 2). Similar over-
lapping is visible between the isotope data of Spondylus finds from
Neolithic sites in Greece measured in this study (average d18O
values from
2.3 to 0.8&, average d13C values from
0.4 to 1.9&)
and the isotope data of Spondylus ornaments from Aszód (Table 1,
Fig. 2). The Aszód objects show the largest range of d18O values
among all measured archaeological finds due to most positive d18O
values of some ornaments (1.7e2.1&).
Modern Spondylus shells from the Adriatic have average d18O
values between
1.1 and 1.3& and average d13C values between 0.4
and 1.4& (Table 1, Fig. 3). The oxygen isotope compositions of shells
show a shift to more positive values southward in the Adriatic
(from Rovinj to the Peljesac Peninsula). Stable isotope compositions
of the modern Spondylus shells from the Aegean (Chalkidiki and
Makriyalos) range from 0.3 to 0.6& for oxygen and from 0.6 to 1.9&
for carbon (Table 1, Fig. 3). High-resolution stable isotope analysis of
a recent Spondylus shell from Rhodes (Greece) performed by Maier
and Titschack (2010) exhibited d18O values between 0.3 and 2.2&
and d13C values between
0.4 and 1.7& for the aragonitic part
(Fig. 3). The isotope data of the Aegean shells overlap with the
isotope data of the Adriatic shells, except the shell from Rovinj with
more negative d18O value (Fig. 3).
The d18O distribution of the Mediterranean surface waters
shows a south-north and west-east increase mirroring the distri-
bution of surface salinity, both are controlled by evaporation
 B. Bajnóczi et al. / Journal of Archaeological Science xxx (2012) 1e9 5

Table 1
d18O and d13C values (&, V-PDB, average  standard deviation) of the Spondylus ornaments, modern and fossil Spondylus and Ostrea shells analysed in this study. n: number of
subsamples from each artefact or shell.

Sample no. n d18O (&, V-PDB) d13C (&, V-PDB)

av.  st. dev. av.  st. dev.
Aszód-Papi földek site
80.35.124 e bead no. 1 3 2.1  0.7 0.8  0.7
80.35.124 e bead no. 2 3 0.3  1.8 0.4  1.6
80.35.124 e bead no. 3 3 1.8  0.6 0.5  0.6
80.35.124 e bead no. 5 3 0.0  0.2 0.2  0.1
80.35.411 e bead no. 2 3 1.7  0.6 0.3  0.6
80.35.411 e bead no. 3 3 1.0  0.6
0.2  0.7
80.35.411 e bead no. 5 5
0.6  1.5
2.0  1.5
Grave nr. 175, 3, square 59 e bead no. 1 3 0.1  0.2 0.6  0.3
Grave nr. 175, 3, square 59 e bead no. 2 3 0.6  0.7 0.3  0.2
Grave nr. 175, 3, square 59 e bead no. 3 3
1.0  0.5 1.4  0.2
Trench D, pit a e bracelet fragment 3 0.8  0.6
0.2  0.3
80.35.209 e bead no. 1 3 0.3  0.2 0.4  0.1
80.35.209 e bead no. 2 3
0.4  0.5
0.5  0.4
80.35.209 e bead no. 3 6
0.3  1.6 0.1  0.3
80.35.209 e bead no. 4 6 0.8  1.1
0.2  0.3
80.35.209 e bead no. 5 6 0.9  0.2 0.0  0.2
80.35.423 e bead no. 1 3
1.9  0.9 0.0  0.2
80.35.423 e bead no. 2 2
1.6  1.4
1.5  0.3
Grave nr. 175. 4e5. e bead 3
0.4  0.7 0.7  0.0
80.35.154 e bracelet 2
0.3  0.2 0.2  0.0
81.72.5 e bead 5
1.2  0.9
0.1  0.8
Neolithic sites from Greece
Dispilio K1622 3 0.4  0.9 0.1  0.2
Theopetra Cave
313a 3 0.1  0.3 0.4  0.2
Theopetra Cave e 168/88 3 0.1  0.5
0.2  0.2
Kleitos, Kozani e #001 4
0.9  1.0
0.2  0.3
Kleitos, Kozani e #002 3
0.7  0.4 0.9  0.1
Kleitos, Kozani e #003 3 0.8  0.8 1.0  0.0
Kleitos, Kozani e #004 2
0.4  0.5
0.4  0.2
Makriyalos, Pieria e #005 4
2.3  0.3
0.2  0.2
Makriyalos, Pieria e #006 3 0.0  1.1 0.2  0.2
Makriyalos, Pieria e #007 3 0.2  0.8 1.9  0.1
Makriyalos, Pieria e #008 3
0.2  0.6 0.3  0.2
Makriyalos, Pieria e #009 3
0.5  0.6 1.1  0.4
Makriyalos, Pieria e #0010 3
0.5  1.0 0.9  0.7
Makriyalos, Pieria e #0011 3
0.7  0.3 0.5  0.2
Makriyalos, Pieria e #0012 3 0.5  0.4 0.2  0.1
Modern Spondylus shells
Adriatic Sea, Rovinj 8
1.1  0.5 0.6  0.4
Adriatic Sea, Vir 4 0.6  0.3 1.4  0.2
Adriatic Sea, Peljesac Peninsula 4 1.3  0.5 0.4  0.4
Chalkidiki (East Thermaikos Gulf) e #0013 3 0.6  0.9 0.6  0.2
Chalkidiki (Polychrono Beach) e #0014 5 0.3  1.1 0.7  0.3
Makriyalos, Pieria (West Thermaikos Gulf) e #0015 3 0.5  0.1 1.9  0.1
Fossil Spondylus shells
Sámsonháza, Hungary e M.62.2986 4
1.3  0.4 1.0  0.3
Sámsonháza, Hungary e M.57.2088 e #1 4
1.6  0.6 1.8  0.2
Sámsonháza, Hungary e M.57.2088 e #2 2
2.7  1.4 1.4  0.5
Sámsonháza, Hungary e M.57.2088 e #3 3
5.3  1.0
1.3  1.2
Lapugiu de Sus, Romania e M.60.8423 3 0.2  0.1 1.3  0.0
Fossil Ostrea shells
Buják, Hungary #1 12
3.2  0.8
0.2  1.3
Buják, Hungary #2 9
2.7  1.3 0.1  0.8

(Pierre, 1999), however, the variation of d18O is relatively small
(0.36&) in the eastern Mediterranean, which results in the
overlapping of isotope data of shells originating in the Aegean
and the Adriatic. Therefore precise, marine basin-specific prove-
nance determination of shell ornaments from the Mediterranean
based only on stable isotopes is difficult to perform. Most of the
isotope range of Aszód ornaments overlaps with the isotope
range of Spondylus shells from both Mediterranean marine basins
(Fig. 3). While the Aegean is the obvious source for Spondylus
finds of the Neolithic sites in Greece, for the shells of the Aszód
ornaments the source can be either the Aegean or the closer
Adriatic.
The isotope data of N. reticulata and C. gallina shells from the
Black Sea measured by Shackleton and Renfrew (1970) range
from
4.3 to
1.7& for d18O and from
3.8 to 0.3& for d13C. These
d18O values are more negative than the d18O values of Spondylus
shells from the Aegean and Adriatic as well as the majority of shell
ornaments from Aszód site, while for the carbon some overlapping
exists among species from the Black Sea and Spondylus from the
Mediterranean and the Aszód site (Fig. 3).
The difference in the d18O values of recent shells of the Black Sea
and the Mediterranean shells can be attributed to the difference in
the d18O of the seawaters with more negative values for the Black
Sea (Black Sea:
2.8  0.34& vs. Mediterranean: 1.30e1.66&;
Pierre, 1999; Ranke et al., 1999). However, the shell isotope
composition of the two Black Sea species can be influenced by (i)
their potentially different living conditions (e.g. different temper-
ature) compared to Spondylus or (ii) the species/genus-specific

Please cite this article in press as: Bajnóczi, B., et al., Tracing the source of Late Neolithic Spondylus shell ornaments by stable isotope
geochemistry and cathodoluminescence microscopy, Journal of Archaeological Science (2012), http://dx.doi.org/10.1016/j.jas.2012.09.022
6 B. Bajnóczi et al. / Journal of Archaeological Science xxx (2012) 1e9
Fig. 2. d18O vs. d13C plot for Spondylus ornaments from the Aszód site and the Neolithic
sites of Greece (Kleitos, Makriyalos, Theopetra Cave and Dispilio) analysed in this study
and isotope data of Spondylus artefacts from Tell Goljamo Delcevo, Sitagroi, Gra-
deshnitsa and Vinca published by Shackleton and Renfrew (1970) and from Duran-
kulak and several Austrian archaeological sites published by Todorova (2002).
fractionation during carbonate precipitation. Therefore isotope
data of the shells of the two species from the Black Sea should be
compared with that of the same/similar species from the
Mediterranean.
Chamelea (Chamelia) gallina, striped venus clam, lives under the
surface of clean and muddy sand at a depth of between 5 and 20 or
even 55 m, (Carter, 2008) its habitat is similar to that of Spondylus
regarding the water depth. From the Mediterranean the shells of
this species were analysed from the Gulf of Trieste and exhibited
d18O values between
3.5 and 1.5& and d13C values between
about
4 and
0.8& (Keller et al., 2002). Although the northern
Adriatic surface seawater is depleted in 18O compared to the
southern Adriatic due to the inflow of continental waters (Stenni
et al., 1995), the isotope data indicate that C. gallina does not
precipitate its shell carbonate in isotopic equilibrium with seawater
resulting in more negative isotope values (Keller et al., 2002). These
data partly overlap with the data of the same species from the Black
Sea; however, the latter was regarded to be precipitated in isotopic
equilibrium with the water of the Black Sea by Shackleton and
Renfrew (1970).
Nassa (Hinia, Hinea) reticulata, netted dog whelk, is a Gastropod
living in low water spring tide to shallow sublittoral in the sandy
substrate (Chambers, 2008). Shells of a related species, Nassa
mutabilis were collected from a depth of about 10 m along the
central Italian coast of the Adriatic and both d18O and d13C values
vary between about
1.0 and 2.6& (Cespuglio et al., 1999). The
CaCO3 of the Nassa shell is precipitated under isotope equilibrium
conditions or very close to equilibrium with the environmental
water (Cespuglio et al., 1999). Considering that the northern Adri-
atic surface seawater has more negative d18O values than the
southern one, isotope data of the Mediterranean Nassa shells are
well distinguished from data of the Black Sea Nassa shells, at least
for oxygen.
The above considerations indicate that the recent shells of the
Black Sea can be separated from the Mediterranean ones based
mainly on the oxygen isotope composition, and the present-day
Black Sea can be excluded as a possible source of Spondylus orna-
ments. According to Todorova (2002) stable isotope composition of
the Durnakulak objects indicate that their shells were precipitated
from colder water than shells of the Austrian artefacts and
Please cite this article in press as: Bajnóczi, B., et al., Tracing the source of Late Neolithic Spondylus shell ornaments by stable isotope
geochemistry and cathodoluminescence microscopy, Journal of Archaeological Science (2012), http://dx.doi.org/10.1016/j.jas.2012.09.022
Fig. 3. d18O vs. d13C plot for Spondylus ornaments from the Aszód site and for modern
Spondylus shells from the Aegean and the Adriatic (data for aragonite from Maier and
Titschack (2010) and new data measured in this study). The range of d18O and d13C
values for Spondylus from the Aegean and the Adriatic as well as for recent Nassa
reticulata and Chamelia gallina shells from the Black Sea published by Shackleton and
Renfrew (1970) are indicated outside the box.
originated from a different biotope than the Black Sea. However, the
somewhat lower d18O values of the Durankulak objects (Fig. 2)
indicate that these shells were precipitated from warmer seawater
based on the fractionation between aragonite and water
(Grossmann and Ku, 1986) and do not overlap with the isotope data
of the recent Black Sea shells.
Shackleton and Renfrew (1970) excluded the possibility that
Black Sea could have had an isotopic composition closer to that of
the Mediterranean a few thousand years ago. Later Todorova (2002)
assumed and recently Haimovici (2007) agreed that in the 6th and
5th millennia BC (during the “climate optimum”) the Black Sea was
warmer and has more salt content than today due to the inflow of
Mediterranean seawater with Mediterranean species, therefore it
could have been a habitat for Spondylus probably with a closer
isotope composition of seawater to the Mediterranean. After the
end of the “climate optimum” some of the Mediterranean species,
among others Spondylus disappeared (Haimovici, 2007) due to the
growing water mass and decreasing salt content (Todorova, 2002).
Based on the pronounced increase in d18O value (as well as in
87
Sr/86Sr and Sr/Ca ratio) of the shells of Black Sea molluscs Major
et al. (2006) demonstrated that there was an incursion of the
Mediterranean seawater at 9.4 ka BP cal; however, after this time
and until the present-day d18O values of the Black Sea shells vary
very minimally. Therefore we agree with the usually accepted idea
(e.g. Sümegi, 2009) that Spondylus species did not live during
Holocene in the Black Sea due to its different ecological (salinity,
temperature) demands.
During the malacological analysis of the Aszód find material
Sümegi (2009) found alterations in the beads which he inter-
preted as results of possible recrystallization, postburial alter-
ation, and presumably presence of fossil shells. Recrystallization
of shell, i.e. alteration of metastable aragonite to stable (low-
magnesium) calcite and accordingly the change of the stable
isotope composition (isotopic shift to more negative d18O and d13C
values compared to the intact aragonitic shell) can be caused by
fossilization (diagenesis) as well as postburial interaction of shells
with soil and groundwaters, an example for diagenetic alteration
of Spondylus shells is published by Titschack et al. (2009).
According to cathodoluminescence microscopy analysis the
Spondylus beads are made of aragonite (Fig. 4aeb). Translucent,
 B. Bajnóczi et al. / Journal of Archaeological Science xxx (2012) 1e9 7

Fig. 4. Spondylus beads from the Aszód site (stereomicroscope and cathodoluminescence microscope images). A, B: shell bead, C, D: shell bead with translucent, “crystalline” stripe,
E, F: shell beads with white aragonitic and yellow calcitic parts. (For interpretation of the references to colour in this figure legend, the reader is referred to the web version of this
article.)

“crystalline” zones along the margin of the beads or transecting
the beads can be observed by naked eye as well as by stereomi-
croscope; however, they are composed of aragonite based on the
luminescence colour (Fig. 4ced). These “crystalline” zones are
parallel with growth lines in several cases; therefore we suppose
that they are evidently the original parts of shells from which the
beads were made.
Three of the studied Aszód beads contain yellow crystalline zone
(Fig. 4eef) made of pure calcite and sharply separated from the
main aragonitic material of beads. One possible explanation is that
these beads were originally made from both the inner (aragonitic)
and the outer (calcitic) parts of the shell. However, in one of the
beads the edge of the yellow calcitic part is irregular indicating
dissolution, and the growth lines continuously run from the
aragonitic to calcitic part (Fig. 4f). The contact of the outer calcite
layer with the inner aragonitic layer in an intact Spondylus shell is
sawtooth-shaped (Titschack et al., 2009), therefore at least in the
case of this bead the postburial interaction with soil waters and
recrystallization to calcite is most likely.
Mean d18O values of fossil Spondylus and Ostrea shells vary
between
5.3 and 0.2& and their mean d13C values vary
between
1.3 and 1.8& (Table 1, Fig. 5). Isotope range of fossil shells
is separated from the isotope range of the majority of beads,
however, considering only the oxygen isotope composition, d18O
values of fossil shells partly overlap with the d18O values of orna-
ments from the Aszód site. Isotope geochemistry in itself, in spite of
the diagenetic modification of isotope composition of fossil shells,
seems to be not enough for differentiating between recent and
fossil shells, but cathodoluminescence microscopy helps in their
separation. Analysis revealed that diagenetic calcite appears in the
aragonitic shell of fossil Spondylus as tiny spots indicating that
partial recrystallization of aragonite was induced by fossilization.
This microstructure is in accordance with microstructural charac-
teristics of diagenetically modified Spondylus shells from Rhodes
described by Titschack et al. (2009). The studied Ostrea shells are
entirely composed of calcite, indicating diagenetically more
evolved microstructure. Therefore the homogeneous aragonitic
material of studied Aszód shell ornaments with the lack of diage-
netic calcite indicates that their raw material was recent Spondylus
shell.
5. Conclusions and archaeological implications
The Spondylus ornaments of the Late Neolithic Aszód-Papi föl-
dek site were made from contemporary shells originating from the
Mediterranean. The Black Sea can be excluded as a possible source
of Spondylus raw material as suggested earlier by Shackleton and
Renfrew (1970).

Please cite this article in press as: Bajnóczi, B., et al., Tracing the source of Late Neolithic Spondylus shell ornaments by stable isotope
geochemistry and cathodoluminescence microscopy, Journal of Archaeological Science (2012), http://dx.doi.org/10.1016/j.jas.2012.09.022
8 B. Bajnóczi et al. / Journal of Archaeological Science xxx (2012) 1e9
Fig. 5. d18O vs. d13C plot for Spondylus ornaments from the Aszód site and fossil
Spondylus and Ostrea shells.
Modern Spondylus shells from the Aegean and Adriatic have
greatly overlapping d18O values, therefore it is difficult to separate
shells from the two marine basins based solely on stable isotope
composition. Due to the large range of d18O values measured in the
Aszód ornaments, their Spondylus shells are Aegean or Adriatic in
origin. For the more precise determination of the Mediterranean
source of shells the next step of research should focus on finding
chemical (elemental) fingerprints characteristic for specific sea
regions. Chemical analysis of numerous modern Spondylus shells
measuring their trace element compositions and comparison with
the similar parameters of the artefacts might help tracing back the
source of shell objects. Provenance determination by chemical
means was successfully applied for Busycon and Olivella biplicata
shell artefacts in the United States (Claassen and Sigmann, 1993;
Eerkens et al., 2007).
Signs of recrystallization related to fossilization (diagenesis)
were not observed on the studied Aszód beads contrary to fossil
Spondylus and Ostrea shells; therefore use of fossil Spondylus
sources in the close and far vicinity of the Aszód site cannot be
proven. Our results support the earlier conclusion of Shackleton
and Elderfield (1990). Calcitic parts observed in some aragonitic
beads are not related to diagenesis, rather to postburial interaction
with soil solutions.
The results of stable isotope analyses harmonize well with
archaeological observations. Spondylus used as prestige raw mate-
rial arrived in the Carpathian Basin from distant regions, from the
Aegean and/or the Adriatic coasts during the Late Neolithic (Kalicz
and Szénászky, 2001; Siklósi, 2004). This raw material with difficult
accessibility was perfectly suitable to express and manipulate social
inequality.
Typological and chronological differences can be established on
the basis of semi-finished products, waste material and Spondylus
ornaments found at the Mediterranean coast that question the
existence of a uniform long-distance exchange network from the
Aegean to the Paris Basin. Instead there could have been chrono-
logically and regionally changing exchange systems and social
relations (Müller, 1997; Kalicz and Szénászky, 2001; Siklósi, 2010).
Compared to our earlier knowledge the number of limestone
imitations is surprisingly high, but its majority concentrated in one
grave at the Aszód site which was the richest grave in Spondylus
ornaments; almost half of the beads found in this grave were made
from limestone (Sümegi, 2009). This observation also modifies
Please cite this article in press as: Bajnóczi, B., et al., Tracing the source of Late Neolithic Spondylus shell ornaments by stable isotope
geochemistry and cathodoluminescence microscopy, Journal of Archaeological Science (2012), http://dx.doi.org/10.1016/j.jas.2012.09.022
considerably the formerly supposed sudden increase of Spondylus
usage during the Late Neolithic. It seems that we cannot reckon
with the sudden increase of the quantity of Spondylus ornaments
between the Middle and the Late Neolithic taking into consider-
ation the types, sizes and manufacture technique of Spondylus
ornaments, we rather experience stagnation or slight decrease.
Nevertheless, more and more limestone beads appear as imitations
among the Spondylus beads. Their sizes correspond to the original
Spondylus beads; therefore little if any difference could be seen
during wearing which indicates increased social manipulation by
prestige goods (Siklósi and Csengeri, 2011).
Acknowledgement
The research was funded by the Hungarian Scientific Research
Fund (OTKA 75677 ‘Aszód-Papi földek Late Neolithic site: connec-
tion between East and West’). Zsuzsanna Siklósi’s work is sup-
ported by the European Union and co-financed by the European
Social Fund (TÁMOP-4.2.1./B-09/1/KMR-2010-0003). We thank
Marcel Buri c (University of Zagreb, Department of Archaeology),
Alfréd Dulai and Zoltán Fehér (Hungarian Natural History Museum)
for providing us fossil and recent Spondylus shells as comparative
material. We also thank Norbert Faragó (Eötvös Loránd University,
Institute of Archaeological Sciences), András Markó (Hungarian
National Museum), and Zsuzsanna Tóth (Eötvös Loránd University,
Institute of Archaeological Sciences) for their help in the identifi-
cation of fossil Spondylus sites. Suggestions of the two anonymous
reviewers are greatly acknowledged.
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