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Material Evidence for the use of Attic White-Ground Lekythoi Ceramics in

Cremation Burials

Article  in  Journal of Archaeological Science · May 2010

DOI: 10.1016/j.jas.2009.11.026

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 Journal of Archaeological Science 37 (2010) 936–940

Contents lists available at ScienceDirect

Journal of Archaeological Science

journal homepage: http://www.elsevier.com/locate/jas

Material evidence for the use of Attic white-ground lekythoi ceramics

in cremation burials
Marc S. Walton a, *, Marie Svoboda b, Apurva Mehta c, Sam Webb c, Karen Trentelman a
a
Getty Conservation Institute, Los Angeles, CA, USA
b
J. Paul Getty Museum, Los Angeles, CA, USA
c
Stanford Synchrotron Radiation Lightsource, Menlo Park, CA, USA

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

Article history: White-ground lekythoi ceramics offer important evidence for funeral practices in Ancient Greece (5th
Received 18 August 2009 century BC). The images painted-on these oil containers provide the best visual narrative for the events
Received in revised form surrounding death, including indications that the vessels themselves were used as part of the funerary
6 November 2009
rites. However, until now, their specific function and treatment within the funeral ceremony was not well
Accepted 17 November 2009
understood. We present here material evidence that the vessels were ritually burned, together with the
body of the deceased, during cremation, as evidenced by a diffuse purplish-red discolouration found on
Keywords:
many white-ground lekythoi. Through EPMA and mXAS studies, we show that: (1) this characteristic
Egyptian blue
White-ground lekythoi purplish-red discolouration is due to the presence of metallic copper nano-particles embedded in
Purplish-red discolouration a glassy layer; (2) this metal-glass matrix formed as the result of a high temperature reaction between
Copper nanoparticles painted-on Cu-based pigments (e.g., Egyptian blue) and the white-ground ceramic slip; and (3) the
Attica reaction occurred under a reducing environment. Given the mortuary context for these vessels, we
Greece propose the reduction firing to which the vessels were exposed was that associated with the cremation
Cremation of the body. The observation of discontinuous formation of the purplish-red discolouration along
SEM adjoining fragments supports the hypothesis that the vessels were broken prior to being burned. The
EPMA
majority of lekythoi in museum collections lack information on their original archaeological context, and
XANES
our data suggest the presence of this purplish-red discolouration may serve as a visual marker for
EXAFS
cremation. As such, it is expected our findings will provide a new basis for interpreting how this
important class of ceramic, and associated iconographic imagery, relates to Athenian funerary practices
and the ancient Greek notion of death.
Ó 2009 Elsevier Ltd. All rights reserved.

1. Introduction
Evocative descriptions of death and its attendant rituals are
found throughout ancient Greek mythology and in the Homeric
poems (Kurtz and Boardman, 1971; Sourvinou-Inwood, 1995). Our
understanding of the Greeks’ attitude toward the afterlife has
further been enhanced by archaeological excavations which have
provided extensive material evidence of funerary practice (Morris,
1992). One of the most important object types excavated from graves
dating to the 5th century BC is the white-ground lekythos (see
Fig. 1A). The white-ground slips of these ceramics were painted with
depictions of the basic events of the funeraldprothesis, procession,
inhumation, and subsequent visitation of the grave by the livingdas
* Corresponding author at: Getty Conservation Institute, Collections Research
Laboratory, 1200 Getty Center Drive, Suite 700, Los Angeles, CA 90049-1684, USA.
E-mail address: mwalton@getty.edu (M.S. Walton).
well as the transfigurative journey of the deceased from the world of
the living into the afterlife (Nakayama, 1982; Garland, 1985). This
painting is often colourful and carefully executed employing
a palette of green (malachite, CuCO3$ Cu(OH)2), blue (Egyptian blue;
mineral cuprorivaite, CaCuSi4O10), red (vermilion, HgS), and orange
(iron earths, coloured by Fe2O3) colours. Many of these pigments are
fugitive at typical firing temperatures, and thus must have been
applied to the vessels after their initial firing (Scott and Taniguchi,
2002; Wehgartner, 2002).
In addition to these intentionally applied pigments, a distinctive
purplish-red discolouration appears as diffuse fields and isolated
spatters of colour on the surface of many Attic white-ground
lekythoi (see Koch-Brinkmann, 1999 for an indication of the
numbers of polychromed lekythoi with this discolouration).
Although lacking correspondence to decorative elements, this
discolouration frequently is found near areas painted with the
pigment Egyptian blue, as illustrated in Fig. 1B, where islands of
vibrant blue colour can be seen within the large diffuse purple-red

0305-4403/$ – see front matter Ó 2009 Elsevier Ltd. All rights reserved.
doi:10.1016/j.jas.2009.11.026
 M.S. Walton et al. / Journal of Archaeological Science 37 (2010) 936–940
Fig. 1. (A) Greek white-ground lekythos from the Antikensammlung Staatliche Museen zu Berlin (F 2683) showing purplish-red discolouration. (B) Detail showing purplish-red
discolouration associated with overlying Egyptian blue pigment. (For interpretation of the references to colour in this figure legend, the reader is referred to the web version of
this article).
discolouration. The differential appearance of adjoining sherds on
some vessels (see Fig. 1) in which the purplish-red discolouration
does not continue across a break implies that the vessel was broken
prior to the formation of this coloured material. The diffuse and
spattered appearance of these purplish-red areas further suggests it
was not an intentional element of design (Koch-Brinkmann, 1999;
Wehgartner, 1988, 2002).
The work presented here constitutes the first systematic
investigation into the material properties of this purplish-red dis-
colouration. The composition and morphology of the purplish-red
discolouration was investigated first by electron probe microanal-
ysis (EPMA) and scanning electron microscopy (SEM). Micro X-ray
absorption spectroscopy (mXAS) techniques including X-ray
absorption near edge structure (XANES) spectroscopy and
extended X-ray absorption fine structure (EXAFS) spectroscopy
were then employed to examine the local chemical environment
and electronic state of elements within this material. The use of
mXAS techniques has been gaining popularity for application to
archaeological problems as these techniques provide information
on the valence state of atoms and also bond lengths and local
coordination number (Pradell et al., 2005; Roque et al., 2006; Nakai
et al., 1999; Arletti et al., 2005; Pages-Camagna et al., 2006). Such
information can be very useful for understanding the high
temperature histories associated with the manufacture of ancient
materials.
We consider here samples of the purplish-red colour taken from
two lekythoi: a huge lekythos from the Antikensammlung Staat-
liche Museen zu Berlin (accession number F 2683), and a lekythos
depicting Charon on the river Styx from the Harvard Art Museums
(1960.338). The ultimate aim of this research is to understand the
processes by which the purplish-red discolouration formed and to
determine what its presence on an Attic white-ground lekythos
may suggest for how this ceramic type was incorporated into
ancient Greek burial practices.
937
2. Experimental
2.1. Sample mounting
Samples were removed by adhering acrylic rods (1 mm diam-
eter) to the ceramic using cyanoacrylate ‘‘super glue’’ adhesive
(Loctite Super Glue, Henkel Consumer Adhesive, Inc., OH). After the
glue penetrated the ceramic and dried, the rod was broken away
from the object taking with it a thin lens of the ceramic surface
(typically, 100 mm thick and 0.3 mm wide). The rod/sample
composite was then embedded in epoxy resin, which, after curing,
was ground and polished to a mirror finish using a series of dia-
mond pastes (down to 1 mm grit, Metadi Diamond Suspension,
Beuhler Ltd, IL). After sputter coating 70 nm of carbon onto the
blocks, the samples were then subjected to electron imaging and
analysis.
2.2. Scanning electron microscopy and electron probe
microanalysis
Imaging of the samples was performed using a FEI/Philips XL30
ESEM FEG field-emission environmental scanning electron micro-
scope in high vacuum mode; backscatter electron images were
acquired using 25 kV and 0.245 pA. Quantitative elemental analysis
was performed using a Cameca SX100 electron probe micro
analyzer (EPMA) fitted with four wavelength dispersive X-ray
spectrometers (WDS). Line scans and point analyses were per-
formed using 20 kV and 10 nA for all elements with a beam
diameter of 2 mm. A set of well-characterized minerals (C.M. Taylor
Company, San Jose, CA) were used as standards for calibration. The
quality of the standardization process and instrumental drift was
monitored by repeatedly analyzing a secondary glass standard
(Corning-D, Corning Museum) before and after each analysis
session.
938 M.S. Walton et al. / Journal of Archaeological Science 37 (2010) 936–940
2.3. mXANES, and mEXAFS
X-ray absorption spectroscopy (XAS) measurements were per-
formed on the hard X-ray microscope located at beam line 2–3 at the
Stanford Synchrotron Radiation Lightsource (SSRL). Beam line 2–3
utilizes Pt-coated mirrors in a Kirkpatrick–Baez configuration to
focus the incident beam to a 2  2 mm spot size. The incident beam
energy was tuned using a Si(220) monochromator. Samples were
attached to a high precision XYZ stage oriented 45 to the incident
beam. The X-ray absorption signal was detected at 90 to incident
beam using either a Vortex silicon drift detector or a 3 element Ge
detector. Cu K-edge (8979 eV) mXANES and mEXAFS were collected
by scanning through the XANES at step sizes of 0.35 eV and EXAFS
regions at step size of 0.05 1/Å . For all experiments, a Cu foil standard
was used to calibrate the beam energy to 8979 eV.
3. Results
A backscatter electron image (BEI) of a representative cross-
section taken from a purplish-red area with overlying Egyptian blue
(EB) pigment is shown in Fig. 2A. In this image, a thin layer (5–
10 mm) of glass (appearing as a solid mid-grey tone in the BEI) can
be seen separating the EB (seen to be composed of stacked lathes)
from the ceramic slip. EPMA of this glass layer found it to be rich in
silica, with a total alkali (Na þ K) content of about 3 wt%, which is at
the lower end of previous analyses of the interstitial glass which
forms during the manufacture of EB (Hatton et al., 2008). The
relatively low alkali content of this glass layer is consistent with our
findings (discussed in depth below) that these values are lower
than expected due to interaction with the underlying ceramic slip.
However, the most significant features in this image are the small,
spherical, high Z-contrast particles lying at and just below the
glass/ceramic slip interface, determined by EPMA to be copper-rich.
The diameter of these spheres ranges between 50 nm and 400 nm,
with the majority falling between 80 nm to 100 nm (see inset in
Fig. 2A). These Cu-rich nano-particles resemble, in both size and
shape, metallic structures that have been identified in Roman
period dichroic glass (Barber and Freestone, 1990) and Islamic
period ceramic luster decoration (Pradell et al., 2005; Roque et al.,
2006). Colour in these nano-particulate materials is caused by the
absorption of light at their respective surface plasmon resonances
(Pradell et al., 2008). Our discovery of copper-rich nano-particles
within the purplish-red discolouration on white-ground lekythoi
A B
Fig. 2. (A) SEM backscatter electron image of a cross-section of Egyptian blue (EB) and underlying copper particles at interface between glass phase and ceramic. Inset shows high
magnification image of copper particles. (B) Quantitative electron microprobe line scans of Cu, Al, and Ca starting from the EB (D ¼ 0 mm) and terminating in the ceramic (D ¼ 5 mm).
(For interpretation of the references to colour in this figure legend, the reader is referred to the web version of this article).
therefore suggests a similar mechanism is responsible for this
distinctive colouration.
To evaluate the chemical relationship between the aluminum-
rich illite slip layer, the glass layer and the copper-rich particles,
a series of electron probe micro-analyses were acquired (dotted line
Fig. 2A) starting in the EB layer, scanning across the glass layer and
a relatively large copper-rich particle, and terminating in the slip
layer. Fig. 2B shows the concentrations of Ca, Al and Cu, the
elements that demonstrate the most significant variations, as
a function of position. The concentrations of both Cu and Ca are
highest in the EB and gradually decrease across the glass layer. The
slight bump in Cu content near the glass-ceramic slip interface
corresponds to the location of the Cu-rich particle. By contrast, the
Al profile exhibits the opposite trend: the lowest concentration is
found in the EB, with a gradual increase across the glass layer, with
the highest concentration found in the ceramic slip. These data
indicate a bi-directional diffusion into the glass layer: Al in the
ceramic slip has undergone dissolution (Chakraborty et al., 1995)
and diffusion into the glass layer, while Cu and Ca, associated with
the EB pigment, have similarly diffused into the glass layer from the
pigment layer. Similar diffusive interaction between ceramic bodies
and glass is well known from research on glazes (Molera et al.,
2001; Walton and Tite, in press). Based on the diffusive behaviour
observed in Fig. 2B, we conclude the vessel must have been heated
to 900–1000  C (melting temperature range of the glass) and
maintained there for sufficient time to initiate slip dissolution and
achieve significant diffusion driven mass transfer. EB would have
been applied to the surface only after the illite clay white-ground
vessel had been fired in a kiln (Scott and Taniguchi, 2002; Weh-
gartner, 2002). Therefore, our observation of diffusion of Ca and Cu
from EB into the glass indicates the vessel must have been sub-
jected to a subsequent, secondary firing, not associated with its
manufacture. Furthermore, the inconsistent appearance of the
purplish-red discolouration across the vessel suggests this firing
was not carefully controlled.
In order to identify the mineral form of the Cu-rich nano-parti-
cles and better understand the chemical nature of the secondary
firing that formed them, Cu K-edge mXANES spectra, shown in
Fig. 3A, were collected from a Cu foil standard, the Cu-rich particles,
the interstitial glass layer, and the EB. The position of the absorption
edge of the XANES spectrum for the Cu-rich particles is identical to
that of the copper foil standard (8979 eV), indicating the Cu-rich
particles are present in the metallic state (Cuþ0). Furthermore, the
similarity of the modulations at higher energy suggests very similar
18
16 Egyptian blue ceramic
14
Cu
12
Al
10
wt%
Ca
8
6
4
2
0
0 2 4 6
Distance µm
 M.S. Walton et al. / Journal of Archaeological Science 37 (2010) 936–940
A
coppe r foil standard
Normalized Absorption
coppe r-rich particle s
inte rstitial glass
Egyptian Blue
8970 8990 9010 9030
Energy (eV)
Fig. 3. (A) Cu K-edge XANES spectra of the Cu foil standard, Cu-rich particles, glass layer, and EB from the cross-section shown in Fig. 2. (B) EXAFS spectrum of Cu particle (open
circles) compared to Cu foil demonstrating that copper particles have a bulk metallic structure.
local chemical environments. These findings are further strength-
ened by the mEXAFS spectrum of the Cu-rich nano-particles, shown
in Fig. 3B, which shows nearly exact correspondence to that of a Cu
metal foil, indicating that the first several coordination shells around
the Cu atom in the Cu-rich particles are indistinguishable from
coordination shells observed in metallic Cu foil.
The Cu K-edge mXANES spectrum from the interstitial glass layer
shows a large pre-edge peak similar to those typically associated
with Cuþ1 species. However, the energy at which this peak appears
(near 8986 eV) is at the high end of the range reported in the
literature of between 8983 eV and 8986 eV (Kau et al., 1987;
Gonella et al., 2005; Lamberti et al., 1998, 2003). The intensity and
position of this peak, attributed to the dipole allowed 1s / 4p
electronic transition, has been shown to correlate with the coor-
dination number (Kau et al., 1987). Peak positions above 8985 eV
are associated with 4-coordinate Cuþ1 complexes, but typically
have significantly lower amplitude than the white line, in contrast
to the peak observed in the spectrum shown in Fig. 3A. Therefore,
although the XANES spectrum of the interstitial glass layer suggests
the Cu atoms are present in a valence state of þ1, further study is
necessary to understand the significance of the observed shift in
the position of the prominent pre-edge feature.
The position of the Cu K-edge and the general shape of the
spectrum taken from the EB is similar to previously published
XANES spectra of Egyptian blue, and other Cuþ2 oxides, in terms of
absorption edge energy, shape and position of the white line at
8996 eV (Pages-Camagna et al., 2006; Shimizu et al., 2001; Kau
et al., 1987). Additionally, the XANES spectrum shows a pre-edge
feature near 8980 eV, attributed to the 1s / 3d electronic transi-
tion and one of the diagnostic features of Cuþ2 species (Kau et al.,
1987; Shimizu et al., 2001).
Similar to the mechanism by which metallic nano-particles are
formed in modern silicate glass materials (Roque et al., 2006), our
findings indicate that reduction of the Cuþ1 dissolved in the glass layer
resulted in the formation of the metallic copper nano-particles. Taken
together with the diffusion data presented above, this suggests that
the uncontrolled, secondary firing to which the white-ground leky-
thoi were subjected, also occurred in a reducing environment.
4. Discussion and archaeological implications
The structural and chemical similarity of the purplish-red dis-
colouration found on white-ground lekythoi to metallic nano-
939
20
B
15
10
5
K3 Chi(k)
0
-5
-10
-15 Cu Part ic les
Cu Foil
-20
-25
1 3 5 7 9 11
k
particles produced in controlled laboratory conditions necessitates
the consideration as to whether it might be a pigment deliberately
produced by reduction of a copper salt. This hypothesis was put forth
by Noll et al. (1975, 1974) who mentioned the purplish-red material
found on lekythoi in two surveys on painting on ancient ceramics.
Other than its presence on the described Attic white-ground leky-
thoi, a nano-particulate Cu red pigment used to decorate ceramics is
completely unknown prior to the 8th century AD (Pradell et al.,
2008), casting considerable doubt on its intentional application
here. Furthermore, the appearance of the discolouration on the
vessels is inconsistent with it having been deliberately applied.
These anecdotal arguments however are substantiated by the
diffusion and chemical state information presented here, which
provides material evidence this purplish-red discolouration
occurred as a result of the vessels having been subjected to pro-
longed secondary reducing atmosphere firing at high temperatures
around 1000  C. Taken together with the fact that white-ground
lekythoi were associated exclusively with funerary rituals, this
suggests that the secondary firing of these vessels must have been in
a smoke-filled, and thus reducing, fire at the grave site.
Archaeological excavations supplement this analytical conclu-
sion with ample evidence of cremation at the grave coming from
the Keremeikos region of Athens (Kurtz and Boardman, 1971). Fine
ceramicsdincluding white-ground lekythoidtypically found in
association with cremations were burned in offering trenches
adjacent to graves that also contained charred items typically
associated with banquet services (Hampe, 1960; Noble, 1985;
Houby-Nielsen, 1992, 1996). Interestingly, archaeologists have
noted a variability in the soot deposits found on sherds, from which
they conclude the pottery found in these trenches was ostensibly
deliberately broken and then burned (Houby-Nielsen, 1992, 1996),
consistent with our assertion that the differential appearance of the
purplish-red discolouration on adjoining sherds reflects the vessel
having been broken prior to burning. Our data provide the first
material evidence linking the appearance of the purplish-red dis-
colouration with the deliberate breaking and burning of the vessel
as part of a cremation ceremony. Therefore, the presence of this
purplish-red discolouration alone may serve as a diagnostic marker
that a particular white-ground lekythos was used in a cremation.
Unfortunately, the majority of lekythoi in museum collections were
not archaeologically excavated under controlled conditions, and
thus any direct link associating them with a funeral ritual has been
lost. However, the evidence presented here provides a new means
940 M.S. Walton et al. / Journal of Archaeological Science 37 (2010) 936–940
by which this class of ceramic may be directly linked with the
cremation process, thereby enabling archaeologists and art histo-
rians to confidently include a much a larger number of these
objects in their analysis, which in turn has the potential to
dramatically change our understanding of Athenian funerary ritual.
5. Conclusions
In summary, our findings provide the physical evidence linking
the purplish-red discolouration found on white-ground lekythoi
with ritual activities associated with cremation. These data provide
new and specific information on Athenian funerary practices, in
particular that lekythoi were not simple burial gifts but were
vessels richly embellished by potters with the sole purpose of being
broken and burned in a funerary ritual. Based on these chemical
and archaeological data, we now have a more complete under-
standing of how white-ground lekythoi were used in the ritual
setting and the unusual conditions in which the purplish-red
discolouration formed.
Acknowledgements
Portions of this research were carried out at the Stanford
Synchrotron Radiation Lightsource, a national user facility operated
by Stanford University on behalf of the U.S. Department of Energy,
Office of Basic Energy Sciences. We would like to thank Ursula
Kaestner of the Antikensammlung Staatliche Museen zu Berlin and
Susanne Ebbinghaus, Kathy Eremin, and Henry Lie of Harvard Art
Museums for providing samples for this study. We appreciate the
comments and discussions with David Saunders and Jerry Podany
of the J. Paul Getty Museum. Also we thank Giacomo Chiari, and
Catherine Schmidt of the Getty Conservation Institute for reading
and commenting on earlier versions of this work.
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