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Cypriot Byzantine glazed pottery: a study of the Paphos workshops
Article in Archaeometry · October 2009
DOI: 10.1111/j.1475-4754.2009.00502.x
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Archaeometry 52, 4 (2010) 628–643
doi: 10.1111/j.1475-4754.2009.00502.x
CYPRIOT BYZANTINE GLAZED POTTERY: A STUDY OF
THE PAPHOS WORKSHOPS*
A. C. CHARALAMBOUS,1,2 A. J. SAKALIS,2 N. A. KANTIRANIS,3
L. C. PAPADOPOULOU,3 N. C. TSIRLIGANIS,2 and J. A. STRATIS1†
1
Laboratory of Analytical Chemistry, Department of Chemistry, Aristotle University, GR-54124, Thessaloniki, Greece
Laboratory of Archaeometry, Cultural and Educational Technology Institute, ‘Athena’ Research Centre, Tsimiski 58,
GR-67100, Xanthi, Greece
3
Department of Mineralogy-Petrology-Economic Geology, Aristotle University, GR-54124, Thessaloniki, Greece
2
Twenty-five samples of Byzantine glazed pottery from two archaeological sites between Limassol and Paphos region (Cyprus), dated between the 12th and 15th century AD were studied
using micro X-ray fluorescence spectroscopy, scanning electron microscopy and X-ray diffraction analysis. It was found that all the glazes contain lead, following the main manufacturing process of medieval pottery in the Mediterranean territory, while some of them contain
tin, possibly for better opacity. Furthermore, it is shown that copper, iron and cobalt with
nickel are responsible for the decoration colours. Finally, the application of principal component analysis revealed significant differentiation for some of the samples.
KEYWORDS: CYPRUS, MICRO X-RAY FLUORESCENCE SPECTROSCOPY,
X-RAY DIFFRACTION ANALYSIS, SCANNING ELECTRON MICROSCOPY,
PRINCIPAL COMPONENT ANALYSIS
INTRODUCTION
Cyprus presents a long tradition in glazed pottery, mainly dated from the 12th to the 15th century
ad. Archaeological findings confirm the presence of several glazed pottery workshops in many
areas of Cyprus. The most important workshops were in the area of Paphos, on the southwestern
side of the island, and in the area of Lapithos, on the northern side of the island, near the city of
Kyrenia. The specific workshops of Paphos and Lapithos were active from the 12th century and
some of them, especially in the area of Lapithos, until the 19th century. Because of the location
of the island, between three continents and near the Middle East, occupation by the Franks
(1192–1489) and the Venetians (1489–1572), and due to trade, the manufacture and the decoration technology of the local glazed pottery exhibits significant influences from these areas
(Papanikola-Bakirtzis 1996).
Pottery receives more attention perhaps than any other type of artefact since large amounts
are continuously excavated at archaeological sites. Its typological and analytical study enables
the investigation of many interesting aspects of ancient culture, trade and technology (Rice
1987). Lead-glazed pottery was widely spread around the regions of the Mediterranean Sea.
The main characteristic of the 12th century Byzantine glazed pottery, developed mainly within
the Byzantine Empire, was the application of the sgraffito technique. Sgraffito is the term used
to describe redware pottery in which, with the aid of a sharp tool, decorations have been
*Received 7 November 2008; accepted 27 June 2009
†Corresponding author
© University of Oxford, 2009
Cypriot Byzantine glazed pottery
629
scratched into a thin layer of clay slip. Byzantine potters used to apply a coating of white slip
and a colourless lead (Pb) glaze over the ceramic body, and further decorated the surfaces with
a colourful variety of incised and painted designs (Papanikola-Bakirtzis 1999). The Byzantine
Pb glazes are easily formed, obtain lustrousness and opacity at low temperatures and are also
easily coloured with oxides of other metals, such as copper (Cu) and iron (Fe). The main
characteristics of the Paphos workshops are the reddish clay ceramics with white slip coating
and mainly sgraffito decoration with a glaze of green, yellow, brown and orange colour.
Cypriot glazed pottery should be considered and studied as a branch of Byzantine glazed
pottery displaying the same technology and decorative techniques as pottery in Byzantium
(Papanikola-Bakirtzis 1996).
An important category of glazed pottery is the tin-opacified glazes, originally produced in Iraq
during the eighth century ad (Mason and Tite 1997). Initially, tin-opacified glazes were alkali
glazes containing only 1–2% PbO. However, in Spain and for the early production of Italian
majolica, the lead oxide contents tended to be higher (up to about 55% PbO) with lower alkali
contents (down to about 3% Na2O plus K2O) (Tite et al. 1998).
Glazed pottery from Cyprus has not attracted much interest in terms of analytical studies. To
date, only a few studies on the provenance of the Cypriot ceramics have been performed.
Specifically, instrumental neutron activation analysis (INAA) was used to study pottery samples
from southwestern Cyprus (including the Paphos area) obtained from 38 archaeological sites,
dated from the Neolithic through to the Roman period. The results indicated that the large
majority of the ceramics are likely to be local products (King et al. 1986; King 1987).
Furthermore, Megaw and Jones studied glazed ceramic material dated from the fifth to the 15th
century from three regions in Cyprus (Lapithos, Lemba and Dhiorios) with optical emission
spectroscopy, revealing discrimination of the three regions (Megaw and Jones 1983; Jones
1986).
Micro X-ray fluorescence spectroscopy (m-XRF) is a non-destructive, fast, multi-elemental
technique, which analyses the surface layer and determines major, minor and trace elements in
thin and thick samples of all sizes and forms (Padilla et al. 2005; Papadopoulou et al. 2006).
Together with the micro-XRF technique, X-ray diffraction (XRD) and scanning electron microscopy (SEM-EDS) techniques are widely used to complete an archaeometric characterization of
pottery (Rice 1987).
In the present work, a portable m-XRF spectrometer is used for the non-destructive analysis of
25 medieval glazed ceramics from two different archaeological sites in Cyprus. Additionally,
XRD and SEM-EDS are used to study certain samples in order to confirm the experimental
results from m-XRF analysis.The basic aims of this study were:
(1) To determine the mineralogical and chemical composition of the ceramic bodies in order to
investigate their manufacture technology and the provenance of the specific samples.
(2) To determine the chemical composition of the glazes in order to characterize the colours of
the decorations.
(3) To suggest possible origins of the studied material and to contribute to the explanation of
observed technological differences based on existing archaeological knowledge which claims
that the material originates from Paphos workshops.
Furthermore, the statistical treatment of the quantitative data using multivariate exploratory
techniques (principal component analysis, PCA) in combination with the archaeological information provides certain indications concerning the provenance of the studied material and offers
possible justifications for any observed discrimination of the material. This study is expected to
provide useful knowledge on the local glazed pottery technology.
© University of Oxford, 2009, Archaeometry 52, 4 (2010) 628–643
630
A. C. Charalambous et al.
EXPERIMENTAL PROCEDURE
Description of samples
The investigated glazed ceramic sherds were excavated at the Kepir Mosque in the city of
Limassol and at the church of Panagia Galactotrofousa in the Fasouri area, 15 km west of
Limassol, both located in the south of Cyprus. Kepir Mosque was built during the 16th century
near a Byzantine church, while Panagia Galactotrofousa was built during the 11th century. The
excavation of the Kepir Mosque was performed in 1993 and the church of Panagia Galactotrofousa in 2002 under the supervision of the Cyprus Department of Antiquities (Prokopiou 1997).
The samples are dated between the 12th and the 15th century ad. The archaeologists believe
that the origin of the samples is from the Paphos area workshops, due to the similarities in
the manufacture technology (plain, painted and especially scraffito decoration with glaze layer
mainly on the inner side of the ceramic object) and the colour of the glazes (green, yellow, brown
and orange). Quantitative analysis was performed for all the samples by non-destructive means,
using m-XRF spectroscopy, while further analysis applying SEM-EDS and XRD techniques
was performed on specific samples of interest in order to minimize the destruction of samples.
Samples K1–K18 were excavated in the Kepir Mosque, while the remaining samples, K27 –K33,
were excavated in Panagia Galactotrofousa (Table 1). The samples were decorated using green,
yellow, orange, brown, black and blue glazes, as shown in Table 1. Furthermore, samples K18,
K32 and K33 show optical differences in both the clay microstructure and the glaze decoration
style compared with all the other samples. Specifically, these samples have painted decoration of
blue and light blue, which is typical of Italian majolica pottery. Therefore they could be trade
products due to the occupation of Cyprus by Venice during the 15th century.
Micro X-ray fluorescence spectroscopy
Quantitative analysis of the ceramic bodies was performed using portable m-XRF spectroscopy.
The portable m-XRF spectrometer (SPECTRO, COPRA model, Austria) used in this work
incorporates a side window X-ray tube with Mo anode (Oxford Instruments, Series 5011 XTF),
a straight monocapillary lens and a solid-state Si Peltier-cooled detector (8 mm Be window,
3.5 mm2 active area, 300 mm nominal thickness). The maximum tube voltage is 50 kV and its
maximum current is 1 mA. The nominal beam diameter is <150 mm at the position of the sample.
The angle of incidence of the primary X-ray beam on the sample surface is 48° (relative to the
surface), while the angle between the sample and the detector is 42°. All measurements are
performed under atmospheric pressure and no filters were used.
The m-XRF measurements were performed in a point scan mode on several points, which were
selected to cover the entire surface of the glaze. In particular, three to five measurements were
performed on the surface of the glaze-over-paste in all colour areas. Furthermore, three measurements were performed on the ceramic body for each sample, after removal of a small part of
the surface ceramic body layer with a drill and a tungsten carbide cutter to eliminate possible
surface contamination effects. All samples were cleaned with ultra-pure water and dried in the
oven at 110°C. Reported concentrations are mean values of the three or five measurements per
sample. The applied voltage was 40 kV, the current 0.7 mA and the measurement time 300 s,
based on a preliminary investigation of the optimum experimental parameters. The standard
reference material SARM 69 (MINTEK, Republic of South Africa) was used as a calibration
standard, while the standard reference material Geostandard VS-N (SARM-CNRS, France) was
© University of Oxford, 2009, Archaeometry 52, 4 (2010) 628–643
K.M.
K.M.
K.M.
K.M.
K.M.
K.M.
K.M.
K.M.
K.M.
K.M.
K.M.
K.M.
K.M.
K.M.
K.M.
K.M.
K.M.
K.M.
P.G.
P.G.
P.G.
P.G.
P.G.
P.G.
P.G.
K1
K2
K3
K4
K5
K6
K7
K8
K9
K10
K11
K12
K13
K14
K15
K16
K17
K18
K27
K28
K29
K30
K31
K32
K33
K.M. = Kepir Mosque; P.G. = Panagia Galactotrofousa.
Excavation area
Sample index
Reddish-2.5YR 4/8
Reddish-2.5YR 5/6
Reddish-2.5YR 4/6
Whitish-10YR 7/2
Reddish-10R 5/2
Whitish-7.5YR 7/4
Reddish-10R 5/2
Reddish-2.5YR 4/6
Reddish-2.5YR 6/8
Reddish-2.5YR 5/6
Whitish-10YR 8/4
Reddish-2.5YR 4/6
Whitish-10YR 7/4
Reddish-2.5YR 6/6
Reddish-7.5YR 8/4
Reddish-2.5 YR 4/4
Reddish-2.5YR 5/6
Whitish-5Y 9/2
Reddish-2.5YR 6/6
Reddish-5YR 7/8
Reddish-2.5YR 6/6
Reddish-5YR 7/6
Reddish-2.5YR 5/6
Whitish-2.5Y 9/4
Whitish-2.5Y 9/4
Clay colour
(Munsell range)
Fine grained
Coarse grained
Fine grained
Fine grained
Coarse grained
Fine grained
Coarse grained
Coarse grained
Fine grained
Coarse grained
Fine grained
Fine grained
Coarse grained
Fine grained
Fine grained
Coarse grained
Fine grained
Fine grained
Coarse grained
Fine grained
Coarse grained
Fine grained
Fine-grained
Fine grained
Fine grained
Macroscopic
characterization
Table 1 Description of the studied samples
Green glaze
Brown and red glaze
Brown glaze
Orange glaze
Yellow, green and brown glaze
Yellow glaze
Yellow, brown and green glaze with black lines
Brown glaze
Green and brown glaze
Yellow and brown glaze
Yellow glaze
Yellow and brown glaze with black lines
Blue decoration
Orange glaze
Brown glaze
Green and brown glaze with black lines
Yellow and brown glaze
Blue glaze
Green glaze with black lines
Yellow and green glaze
Brown glaze
Yellow and green glaze
Yellow glaze
Light blue glaze
Blue green glaze
Glaze decoration
Cypriot Byzantine glazed pottery
631
© University of Oxford, 2009, Archaeometry 52, 4 (2010) 628–643
632
A. C. Charalambous et al.
used for the quantification of Pb and the standard reference material GBW07706 (China National
Analysis Center for Iron and Steel, Beijing) was used for the quantification of tin (Sn). All
standard reference materials were prepared in pressed pellets by thoroughly mixing the powder
with a cellulose binder in a 4:1 (reference material/binder) ratio, while pressing was performed
using an 11-ton hydraulic press (Specac, UK). X-ray spectra were deconvoluted and fitted using
a suitable software package (WinAxil v 4.0.1).
X-ray diffraction
The quantitative mineralogical composition of the samples was determined by powder XRD.
Powder XRD analysis was performed using a diffractometer with an Ni-filtered Cu Ka radiation
(Philips PW1710, The Netherlands) source on randomly oriented samples. Subsamples were cut
off the glazed ceramic samples and powdered in an agate mortar. The samples were scanned over
the interval 3–63° 2q at a scanning speed of 1.2°/min. Quantitative estimates of the abundance of
the mineral phases were derived from the powdered XRD data, using the intensity of specific
reflections, the density and the mass absorption coefficient for Cu Ka radiation for the minerals
present. Corrections were made using external standard mixtures of the detected mineral phases
(Guinier 1963; Kantiranis et al. 2004). Amorphous phase content was calculated according to the
methodology proposed by Kantiranis et al. (2004). The detection limit for crystalline and amorphous phases was 12% w/w.
Scanning electron microscopy
The morphology and chemical microanalysis of the studied glazed pottery sherds was performed
on the outer surface and on polished sections by SEM-EDS (Jeol JSM-840, Japan), a scanning
electron microscope, equipped with an Oxford ISIS300 Energy Dispersion Analyser. To minimize volatilization of alkalis in the studied samples, the electron beam spot size was enlarged and
the counting time decreased. The measuring conditions were: voltage 15 kV, electron beam
current ~3 nA and spot size 1 mm2, while counting time was 60 s. Different minerals (micas,
carbonates, feldspars) and pure metals were used as probe standards.
RESULTS AND DISCUSSION
Micro X-ray fluorescence spectroscopy
Most of the ceramic bodies have a reddish colour while samples K4, K6, K11, K13, K18, K32
and K33 are characterized by a yellow-white colour (see Table 1).
The m-XRF spectra of Figure 1 present the differences between the ceramic body and the glaze
composition of sample K18. The main differences were the high amounts of Ca, Ti, Fe and Sr in
the ceramic body and the high amounts of S and Pb in the glaze. These significant differences
exist in the composition of the ceramic body and the glaze in all samples. All ceramic bodies
contain a small amount of Pb as a result of the leaching of Pb from the transparent glaze during
firing (Fabbri et al. 2000). The main characteristic of the glazes is the high amount of Pb that
follows the main manufacturing trend in Cyprus during the studied Byzantine period (12th–15th
centuries ad). The two primary methods of producing lead glazes were either to apply Pb, PbO
to the surface of the pottery body, or to apply a mixture of PbO and silica (Tite et al. 1998). The
presence of significant amounts of Sn in the ceramic body (0.08–0.18% w/w) of samples K18,
© University of Oxford, 2009, Archaeometry 52, 4 (2010) 628–643
Cypriot Byzantine glazed pottery
633
Figure 1 m-XRF spectra of the clay and the blue glaze of the sample K18.
K32 and K33 is probably due to the leaching of Sn from the transparent glaze during firing
(Fig. 1). Sn was used in glazed pottery for the creation of opacified glass (Allan 1973; Al-Saad
2002).
The chemical compositions of both the ceramic bodies and the glazes are presented in Tables 2
and 3, respectively.
PCA of the ceramic bodies, based on m-XRF elemental analysis data, illustrates the differences
of the samples, as shown in Figure 2. A weak difference of the studied material is observed based
on the first principal component. Samples on the left side of the PCA (K1, K2, K10, K13) show
increased concentration of K and Si together with low concentrations of Cr and Ca. However,
samples on the right of the PCA (K4, K6, K29) present high concentrations of Cr, Ca and Ni. The
chemical composition of the ceramic bodies is compared with already analysed material from the
Paphos (Lemba, Kouklia) (Megaw and Jones 1983; Jones 1986) and Limassol areas (Amathus)
(Jones 1986), taking into consideration the different techniques used for analysis (Fig. 3).
According to this comparison, glazed ceramic samples with increased Cr and Ca concentrations
seem to originate from Limassol while samples with low concentration of Cr and Ca could
possibly originate from Paphos (Fig. 2). Samples K3 and K8 are different from the other samples
due to their higher content of Ti while sample K33 has a very high amount of Ca and significant
amounts of Mn and Cu. Samples K3, K8 and K33 reveal stronger differences and could possibly
have been manufactured in different workshops from other areas of Cyprus or were trade
products from other territories.
The green colour of the lead glazes is usually related to the presence of Cu2+ or Fe2+ in the
glaze, whereas the yellow to brown colours are related to Fe3+ oxides and complexes (Molera
et al. 1999). Elemental analysis of the glazes confirms these observations, showing that green
glazes are rich in Cu, as seen in Figure 4. The blue glaze (sample K18) contains Co, Sn and
significant amounts of Ni. It seems that Co-based pigments were well known for their beautiful
blue colour due to the CoO4 complex. Finally, Fe3+ is responsible for the brown, yellow, black and
red in the glazes; however, black glazes also contain Mn and yellow glazes also contain Cr.
© University of Oxford, 2009, Archaeometry 52, 4 (2010) 628–643
K1
K2
K3
K4
K5
K6
K7
K8
K9
K10
K11
K12
K13
K14
K15
K16
K17
K18
K27
K28
K29
K30
K31
K32
K33
K2O
wt% 1 stdev
2.44 1 0.07
3.08 1 0.26
1.37 1 0.11
1.50 1 0.26
3.08 1 0.03
2.00 1 0.05
3.31 1 0.17
0.84 1 0.05
3.47 1 0.03
3.13 1 0.62
2.01 1 0.14
3.13 1 0.45
0.75 1 0.06
3.14 1 0.22
2.96 1 0.28
3.00 1 0.46
3.42 1 0.33
1.63 1 0.21
2.77 1 0.59
3.47 1 0.20
1.37 1 0.21
3.05 1 0.04
2.50 1 0.05
0.48 1 0.02
1.20 1 0.02
SiO2
wt% 1 stdev
61.00 1 2.00
58.00 1 2.00
54.00 1 2.00
58.33 1 3.51
59.55 1 2.08
56.33 1 2.00
55.67 1 2.00
54.00 1 3.00
51.00 1 2.00
53.50 1 2.31
56.33 1 2.52
52.33 1 3.79
52.67 1 5.13
53.67 1 2.52
51.33 1 3.51
54.33 1 6.35
55.67 1 3.03
44.67 1 2.53
56.00 1 4.16
58.00 1 3.00
54.67 1 3.13
55.33 1 1.53
53.67 1 1.53
45.00 1 3.46
47.67 1 2.87
3.63 1 0.20
5.87 1 0.59
4.43 1 0.32
15.80 1 0.66
5.73 1 0.96
22.33 1 1.15
3.27 1 0.31
3.01 1 0.53
8.57 1 0.90
6.20 1 0.85
24.33 1 0.58
8.00 1 1.00
7.03 1 1.17
6.10 1 0.20
19.70 1 3.16
19.33 1 1.23
6.43 1 0.32
19.33 1 3.79
21.33 1 4.04
13.17 1 0.32
13.00 1 3.46
11.93 1 0.55
8.67 1 0.49
16.13 1 0.51
23.33 1 2.65
CaO
wt% 1 stdev
0.89 1 0.10
0.82 1 0.16
2.23 1 0.25
0.81 1 0.10
0.86 1 0.12
0.66 1 0.11
0.76 1 0.04
1.40 1 0.17
0.92 1 0.08
0.71 1 0.16
0.64 1 0.03
0.83 1 0.12
0.12 1 0.02
0.79 1 0.06
0.72 1 0.13
1.07 1 0.25
0.93 1 0.15
0.73 1 0.12
0.9 1 0.11
0.92 1 0.07
0.87 1 0.21
0.87 1 0.05
0.81 1 0.13
0.71 1 0.01
0.87 1 0.06
TiO2
wt% 1 stdev
7.60 1 0.50
6.77 1 0.55
12.83 1 0.21
8.80 1 1.01
7.37 1 0.31
6.87 1 0.32
6.83 1 0.35
10.07 1 0.90
7.60 1 0.36
7.07 1 1.47
7.30 1 0.46
8.13 1 1.01
0.83 1 0.15
7.30 1 0.30
5.60 1 0.78
9.27 1 0.60
8.20 1 0.56
6.23 1 1.33
9.33 1 0.58
10.53 1 0.49
11.67 1 2.52
8.47 1 0.15
6.73 1 0.21
7.23 1 0.15
8.00 1 0.52
Fe2O3
wt% 1 stdev
0.11 1 0.02
0.07 1 0.01
0.22 1 0.02
0.21 1 0.02
0.09 1 0.01
0.15 1 0.01
0.09 1 0.01
0.22 1 0.03
0.09 1 0.01
0.07 1 0.02
0.16 1 0.01
0.10 1 0.02
0.07 1 0.03
0.15 1 0.01
0.09 1 0.01
0.15 1 0.04
0.14 1 0.02
0.11 1 0.02
0.13 1 0.01
0.16 1 0.01
0.02 1 0.001
0.13 1 0.01
0.16 1 0.03
0.16 1 0.02
0.27 1 0.08
MnO
wt% 1 stdev
250 1 60
150 1 80
130 1 70
470 1 200
330 1 60
700 1 300
500 1 200
230 1 100
500 1 300
120 1 50
230 1 100
465 1 100
160 1 70
500 1 200
120 1 70
400 1 100
190 1 100
170 1 40
500 1 100
200 1 100
450 1 130
230 1 100
160 1 80
260 1 100
240 1 35
Cr
ppm 1 stdev
Table 2 m-XRF elemental analysis of the clays of the samples
125 1 50
70 1 20
50 1 10
230 1 100
100 1 30
300 1 130
120 1 50
100 1 50
140 1 60
80 1 20
190 1 100
160 1 60
100 1 50
160 1 90
82 1 20
120 1 20
120 1 50
110 1 20
190 1 70
190 1 35
250 1 80
125 1 70
120 1 70
100 1 60
100 1 20
Ni
ppm 1 stdev
200 1 40
65 1 10
85 1 20
70 1 20
125 1 25
90 1 20
50 1 10
300 1 60
73 1 20
73 1 20
90 1 20
70 1 20
90 1 20
50 1 10
80 1 20
160 1 50
80 1 20
150 1 40
140 1 30
100 1 20
90 1 20
70 1 20
80 1 20
90 1 20
430 1 60
Cu
ppm 1 stdev
125 1 25
85 1 20
120 1 20
90 1 20
70 1 20
90 1 20
80 1 20
80 1 20
90 1 20
87 1 20
110 1 20
50 1 10
80 1 20
80 1 20
100 1 20
70 1 15
110 1 20
90 1 20
85 1 15
120 1 20
60 1 10
110 1 20
80 1 20
130 1 30
70 1 10
Zn
ppm 1 stdev
634
A. C. Charalambous et al.
© University of Oxford, 2009, Archaeometry 52, 4 (2010) 628–643
K2O
wt% 1 stdev
0.55 1 0.06
0.55 1 0.02
0.72 1 0.02
0.3 1 0.04
0.94 1 0.07
0.35 1 0.02
0.4 1 0.04
0.3 1 0.01
0.35 1 0.02
0.36 1 0.01
0.24 1 0.02
0.73 1 0.08
0.48 1 0.04
0.54 1 0.03
0.84 1 0.05
0.87 1 0.03
0.46 1 0.02
0.29 1 0.02
0.71 1 0.05
0.69 1 0.03
0.55 1 0.11
0.59 1 0.05
0.57 1 0.02
1.2 1 0.15
SiO2
wt% 1 stdev
54.19 1 1.58
52.29 1 2.39
59.9 1 1
54.22 1 1.15
54.22 1 0.58
55.45 1 1.69
52.05 1 1.15
52.04 1 1.58
50.64 1 3.51
46.36 1 2.08
57.07 1 0.58
57.79 1 2.24
47.81 1 1.73
58.19 1 1.15
58.51 1 1.63
53.48 1 2.34
53.49 1 1.53
54.92 1 1.72
51.36 1 1.35
53.59 1 2.1
51.34 1 2.13
53.48 1 3.25
49.2 1 1
54.62 1 2.73
Sample
K1-Green
K2-Brown
K2-Yellow
K3-Orange
K4-Orange
K5-Green
K5-GreenYellow
K5-Orange
K5-Yellow
K5B-Black
K5B-Yellow
K6-Orange
K6-Yellow
K7-Brown
K7-Green
K7-Yellow
K7B-Brown
K8-Brown
K9-Green
K9-GreenOrange
K10-Brown
K10-Green
K10-Orange
K10-Yellow
0.55 1 0.01
2.62 1 0.25
2.67 1 0.35
1.34 1 0.36
0.91 1 0.11
0.38 1 0.03
0.6 1 0.02
0.81 1 0.02
0.59 1 0.07
0.92 1 0.03
0.78 1 0.17
5.2 1 0.67
11.89 1 2.13
2.13 1 0.76
13.47 1 1.67
6.11 1 1.13
3.08 1 0.1
0.64 1 0.04
2.7 1 0.1
2.66 1 0.12
3.82 1 0.2
3.96 1 0.78
4.48 1 0.82
1.01 1 0.19
CaO
wt% 1 stdev
0.4 1 0.01
0.25 1 0.01
0.27 1 0.02
0.33 1 0.02
0.33 1 0.02
0.25 1 0.02
0.3 1 0.01
0.35 1 0.04
0.28 1 0.02
0.23 1 0.01
0.25 1 0.01
0.25 1 0.03
0.28 1 0.03
0.22 1 0.01
0.3 1 0.02
0.32 1 0.02
0.23 1 0.01
0.62 1 0.04
0.24 1 0.02
0.18 1 0.02
0.33 1 0.02
0.18 1 0.02
0.25 1 0.02
0.33 1 0.02
0.5 1 0.08
4.62 1 0.12
3.4 1 0.24
1.34 1 0.1
3.22 1 0.09
0.36 1 0.07
0.34 1 0.02
3 1 0.16
0.37 1 0.04
3.06 1 0.12
2.53 1 0.21
1.49 1 0.14
0.86 1 0.14
2.8 1 0.34
0.79 1 0.14
0.41 1 0.04
5.82 1 0.65
3.75 1 0.49
1.36 1 0.04
1.22 1 0.03
3.2 1 0.25
3.5 1 0.35
3.1 1 0.11
0.34 1 0.01
170 1 50
230 1 40
170 1 30
280 1 50
210 1 40
150 1 30
100 1 30
160 1 40
100 1 40
150 1 40
140 1 50
140 1 40
190 1 40
140 1 40
230 1 50
180 1 40
250 1 40
370 1 50
200 1 40
250 1 30
180 1 40
190 1 40
200 1 40
110 1 70
300 1 100
90 1 50
100 1 50
120 1 50
210 1 60
210 1 70
100 1 50
110 1 60
110 1 60
110 1 40
100 1 50
130 1 50
180 1 60
150 1 50
300 1 100
150 1 60
150 1 70
110 1 60
110 1 60
310 1 100
110 1 60
90 1 50
80 1 30
100 1 60
280 1 70
100 1 50
120 1 70
100 1 50
130 1 60
220 1 90
120 1 60
110 1 60
140 1 80
90 1 40
100 1 50
100 1 50
120 1 50
110 1 60
200 1 80
150 1 80
100 1 40
100 1 30
130 1 70
160 1 90
100 1 60
110 1 60
90 1 50
110 1 60
3600 1 300
350 1 70
300 1 60
90 1 20
190 1 40
4000 1 400
230 1 50
240 1 50
210 1 40
180 1 40
170 1 30
200 1 50
250 1 50
350 1 60
4700 1 800
420 1 80
190 1 40
80 1 20
2700 1 400
2300 1 400
210 1 40
160 1 30
140 1 30
210 1 40
60 1 20
50 1 10
40 1 10
40 1 10
50 1 20
110 1 20
40 1 10
50 1 20
40 1 10
40 1 10
40 1 10
40 1 10
50 1 10
50 1 20
130 1 30
80 1 20
80 1 20
50 1 20
70 1 20
70 1 20
50 1 10
50 1 20
50 1 10
40 1 10
TiO2
Fe2O3
MnO
Cr
Ni
Cu
Zn
wt% 1 stdev wt% 1 stdev ppm 1 stdev ppm 1 stdev ppm 1 stdev ppm 1 stdev ppm 1 stdev
Table 3 m-XRF elemental analysis of the glazes of the samples
22.77 1 0.59
27.18 1 0.95
27.75 1 0.98
24.24 1 0.55
22.63 1 0.71
21.31 1 0.50
21.69 1 0.21
26.52 1 0.38
24.86 1 1.04
22.74 1 0.72
22.7 1 1.21
20.55 1 3.29
25.02 1 1.12
24.24 1 1.97
25.11 1 2.52
26.94 1 1.26
24.64 1 2.79
26.08 1 1.91
24.2 1 0.51
23.55 1 1.85
20.83 1 1.33
25.64 1 0.78
26.69 1 1.03
28.09 1 1.23
PbO
wt% 1 stdev
0.17 1 0.05
n.d
n.d
n.d
n.d
0.2 1 0.03
n.d
n.d
n.d
n.d
n.d
n.d
n.d
n.d
0.28 1 0.05
0.14 1 0.02
n.d
n.d
0.24 1 0.02
0.24 1 0.05
n.d
n.d
n.d
n.d
n.d
n.d
n.d
n.d
n.d
n.d
n.d
n.d
n.d
n.d
n.d
n.d
n.d
n.d
n.d
n.d
n.d
n.d
n.d
n.d
n.d
n.d
n.d
n.d
SnO2
CoO
wt% 1 stdev wt% 1 stdev
Cypriot Byzantine glazed pottery
635
© University of Oxford, 2009, Archaeometry 52, 4 (2010) 628–643
© University of Oxford, 2009, Archaeometry 52, 4 (2010) 628–643
1.4 1 0.34
0.96 1 0.26
0.46 1 0.08
0.39 1 0.08
0.46 1 0.03
0.59 1 0.02
0.57 1 0.07
0.69 1 0.03
1.18 1 0.11
0.44 1 0.03
0.25 1 0.04
0.76 1 0.06
0.42 1 0.05
0.51 1 0.16
0.54 1 0.11
0.92 1 0.11
4.73 1 0.12
5.26 1 0.12
0.48 1 0.06
0.24 1 0.02
1.48 1 0.35
1.24 1 0.12
0.12 1 0.03
0.86 1 0.02
0.76 1 0.03
1.05 1 0.27
0.25 1 0.03
2.54 1 0.04
3.65 1 0.06
51.34 1 1.83
52.9 1 2.68
56.35 1 2.15
60.04 1 2.52
52.09 1 2.08
57.07 1 1.58
49.91 1 0.58
68.46 1 2.89
52.36 1 1.97
54.91 1 1.53
51.34 1 1.77
59.9 1 2
57.76 1 3.43
51.33 1 1.73
51.35 1 3.21
50.63 1 1.53
53.1 1 3.43
52.8 1 2.97
57.77 1 1.53
50.64 1 1.72
56.32 1 2.08
57.05 1 1.58
55.63 1 1.74
62.32 1 3.41
59.64 1 2.65
52.62 1 2.31
54.92 1 1.73
60.16 1 3.12
58.13 1 2.67
K11-Orange
K11-Yellow
K12-Red
K12-Yellow
K12B-Black
K14-Orange*
K14-Orange
K14B-Orange
K15-Yellow
K16-Black
K16-Brown
K16-Green
K16-LightGreen
K16B-Red
K17-Orange*
K17-Yellow
K18-Blue
K18-LightBlue
K27-Green
K27-GreenLine
K28-Green
K28-Yellow
K29-Black
K30-Green
K30-Yellow
K30-Yellow*
K31-Yellow
K32-LightBlue
K33-BlueGreen
*Decorative pattern.
K2O
wt% 1 stdev
SiO2
wt% 1 stdev
Sample
4.38 1 0.76
5.31 1 1.12
2.09 1 0.3
1.12 1 0.1
13.99 1 1.15
9.75 1 1.18
2.49 1 0.56
4.57 1 1.29
8.99 1 2.15
2.79 1 0.26
1.92 1 0.12
2.61 1 0.12
1.44 1 0.06
6.48 1 1.18
1.34 1 0.44
1.23 1 0.35
1.92 1 0.06
3.92 1 0.17
1.64 1 0.15
3.93 1 0.42
1.36 1 0.06
0.71 1 0.08
0.94 1 0.06
1.78 1 0.27
1.76 1 0.5
4.11 1 0.67
1.25 1 0.24
3.32 1 0.54
2.79 1 0.4
CaO
wt% 1 stdev
0.23 1 0.03
0.35 1 0.03
0.23 1 0.04
0.22 1 0.03
0.22 1 0.02
0.39 1 0.02
0.19 1 0.01
0.45 1 0.05
0.32 1 0.02
0.35 1 0.02
0.3 1 0.01
0.43 1 0.01
0.45 1 0.06
0.28 1 0.03
0.22 1 0.04
0.17 1 0.01
0.18 1 0.02
0.25 1 0.03
0.35 1 0.01
0.15 1 0.02
0.08 1 0.02
0.05 1 0.02
0.63 1 0.03
0.13 1 0.02
0.09 1 0.02
0.13 1 0.04
0.15 1 0.04
0.23 1 0.02
0.22 1 0.02
1.86 1 0.06
0.63 1 0.12
2.72 1 0.3
2.28 1 0.3
1.62 1 0.15
2.49 1 0.37
1.74 1 0.09
2.96 1 0.17
1.79 1 0.04
1.24 1 0.15
3.53 1 0.29
0.67 1 0.03
0.57 1 0.03
9 1 1.73
1.21 1 0.19
0.54 1 0.03
2.39 1 0.12
1.71 1 0.2
0.67 1 0.02
0.89 1 0.11
1.62 1 0.12
1.14 1 0.05
4.62 1 0.55
0.47 1 0.03
0.3 1 0.01
0.73 1 0.19
0.41 1 0.03
0.97 1 0.16
0.61 1 0.03
160 1 70
90 1 40
160 1 40
130 1 40
180 1 60
360 1 60
280 1 40
380 1 50
260 1 40
240 1 60
270 1 70
130 1 40
150 1 50
280 1 70
260 1 40
160 1 40
300 1 80
270 1 70
120 1 40
80 1 30
380 1 90
400 1 100
600 1 100
100 1 40
120 1 30
170 1 40
200 1 40
290 1 40
270 1 70
70 1 20
170 1 80
110 1 40
140 1 40
130 1 30
130 1 60
500 1 200
180 1 80
180 1 70
140 1 40
250 1 100
130 1 40
170 1 50
120 1 40
270 1 80
140 1 50
80 1 30
100 1 40
140 1 40
100 1 30
100 1 30
230 1 50
130 1 40
130 1 40
110 1 40
280 1 70
110 1 40
110 1 50
220 1 60
120 1 60
120 1 70
100 1 40
120 1 40
120 1 40
120 1 60
200 1 70
120 1 50
110 1 40
270 1 80
220 1 60
280 1 70
270 1 80
150 1 30
170 1 60
160 1 50
1800 1 300
600 1 100
150 1 50
110 1 30
130 1 50
150 1 50
140 1 40
140 1 60
100 1 40
150 1 50
140 1 40
160 1 50
220 1 60
TiO2
Fe2O3
MnO
Cr
Ni
wt% 1 stdev wt% 1 stdev ppm 1 stdev ppm 1 stdev ppm 1 stdev
Table 3 (Continued)
130 1 30
210 1 40
350 1 100
300 1 100
120 1 40
70 1 20
80 1 20
90 1 20
110 1 20
7700 1 2000
3500 1 800
7700 1 2000
5100 1 1000
1000 1 100
60 1 10
80 1 20
150 1 50
80 1 30
5500 1 600
3100 1 300
6400 1 1000
460 1 70
460 1 100
2400 1 100
120 1 20
190 1 70
200 1 40
80 1 20
5100 1 400
Cu
ppm 1 stdev
45 1 10
44 1 10
20 1 10
20 1 10
30 1 10
40 1 10
40 1 20
40 1 10
110 1 20
90 1 20
50 1 10
80 1 20
60 1 20
30 1 10
40 1 10
40 1 20
20 1 10
20 1 10
50 1 20
30 1 10
50 1 20
20 1 10
30 1 10
90 1 20
30 1 10
30 1 10
50 1 20
40 1 10
60 1 20
Zn
ppm 1 stdev
26.15 1 3.36
23.39 1 2.99
26.45 1 1.40
24.78 1 1.51
26.54 1 2.48
24.51 1 0.91
25.81 1 1.72
22.8 1 2.12
23.05 1 2.51
25.4 1 1.72
27.51 1 1.06
21.88 1 1.50
20.94 1 0.81
22.23 1 2.06
20.8 1 2.95
21.23 1 1.83
35.8 1 1.57
34.74 1 1.67
27.77 1 1.16
25.07 1 2.67
23.42 1 2.55
24.07 1 1.45
26.45 1 2.69
21.8 1 1.38
24.07 1 2.38
26.52 1 2.64
27.43 1 1.74
30.86 1 1.63
32.28 1 1.26
PbO
wt% 1 stdev
n.d
n.d
n.d
n.d
n.d
n.d
n.d
n.d
n.d
0.21 1 0.03
0.12 1 0.02
0.17 1 0.03
0.11 1 0.02
0.1 1 0.02
n.d
n.d
2.24 1 0.12
2.37 1 0.12
n.d
n.d
n.d
n.d
n.d
n.d
n.d
0.1 1 0.02
n.d
1.57 1 0.2
1.52 1 0.1
n.d
n.d
n.d
n.d
n.d
n.d
n.d
n.d
n.d
n.d
n.d
n.d
n.d
n.d
n.d
n.d
0.42 1 0.05
0.11 1 0.01
n.d
n.d
n.d
n.d
n.d
n.d
n.d
n.d
n.d
n.d
n.d
SnO2
CoO
wt% 1 stdev wt% 1 stdev
636
A. C. Charalambous et al.
Cypriot Byzantine glazed pottery
637
Figure 2 PCA of ceramic bodies, using m-XRF elemental analysis.
X-ray diffraction
Mineralogical analysis was performed for samples K1, K12, K16, K18, K27, K28, K29, K32 and
K33. The results are presented in Table 4. All samples contain quartz and plagioclase. Calcite is
present in all samples except K29 and K32, while hematite is present in all samples expect K18,
K28, K32 and K33. Gehlenite is present only in sample K18, while analcime is present in
samples K32 and K33 (Fig. 5). Additionally, samples K18, K32 and K33 contain high amounts
of pyroxene (diopside), while they contain the lowest amount of quartz among all analysed
samples. An amorphous phase is also present in significant amounts in all samples. Diopside,
plagioclase and gehlenite are the major minerals newly formed during the firing process of the
ceramics (Heimman and Maggetti 1979; Maggetti 1981; Buxeda i Garrigós 1999), while analcime is formed after firing, mainly during burial diagenesis, by crystallization from penetrating
solutions or by alteration and transformation of certain firing minerals (Maggetti 1981) or from
the alteration of the glassy amorphous phase (Buxeda i Garrigós and Kilikoglou 2001; Schwedt
et al. 2006). According to Heimman and Maggetti (1979), calcareous sherds of raw and fine
ceramics develop diospide and gehlenite during firing. The latter mineral is obviously metastable
with respect to the composition of typical potter’s clay, and therefore has the tendency to react
with silica to yield anorthite at higher temperatures (>1050°C). This formation of hightemperature minerals depends on the original clay minerals and calcite contents of a sample, their
grain size distribution and the duration of firing. For example, K1 is moderately calcareous
(3.63% CaO) but contains detectable amounts of CaCO3 but no diopside and therefore it seems
to have been fired at a lower temperature than sample K29, which is highly calcareous (13.00%
CaO) without any calcite, which means that all the calcite has been decomposed. Furthermore,
K29 contains the highest amount of anorthite, which signifies a high firing temperature. Also,
sample K32 is highly calcareous without any calcite and all the CaCO3 has been involved in the
© University of Oxford, 2009, Archaeometry 52, 4 (2010) 628–643
638
A. C. Charalambous et al.
Figure 3 Map of southern Cyprus with the excavation areas of the studied samples and the sites of the other analysed
material. Mean values of Cr and Ca concentrations of analysed samples: Lemba (Megaw and Jones 1983), Kouklia
(Jones 1986), Amathus 1 and 2 (Jones 1986), analysed samples with low Cr, Ca concentrations, analysed samples with
high Cr, Ca concentrations.
formation of high-temperature phases, which means that sample K32 must also have been fired
at a higher temperature than the other samples. Mineralogical analysis therefore shows differences in some of the samples such as K29 and K32, which suggests the existence of different
manufacturing technology probably involving a different firing process.
Scanning electron microscopy
The results of the glaze microanalysis of samples K1, K18 and K33 are presented in Figure 6. As
can be seen, sample K1 contains a significantly higher amount of alumina and iron oxides (Fe2O3)
but a lower amount of PbO compared with the glazes of the other two samples, which is in
agreement with Tite et al. (1998). The alkali and the silica content of the glazes are quite similar
for all three samples K1, K18 and K33.
The optical differences of the quality of the ceramic body and glaze of samples K1 and K18
are shown in Figures 7 (a) and 7 (b). The ceramic body of sample K1 shows detrital quartz in an
© University of Oxford, 2009, Archaeometry 52, 4 (2010) 628–643
Cypriot Byzantine glazed pottery
639
Figure 4 PCA of glazes using m-XRFelemental analysis.
amorphous matrix. The clay quality of sample K18 is much better. The white bubbles in the glaze
of sample K18 (Fig. 7 (d)) are particles of Sn. Therefore SEM-EDS analysis confirms the m-XRF
and XRD results on the differences between K18 and K33 compared with K1 (Figs 7 (a) and
7 (c)), which is considered to be a local product, possibly from the workshops of Paphos. Samples
K18 (Figs 7 (b) and 7 (d)) and K33 show typical Italian majolica pottery decoration and could
possibly be regarded as trade products.
CONCLUSIONS
The study of 25 Byzantine glazed ceramics from two archaeological sites in the Limassol area
provides significant information on the elemental and mineralogical characterization, the provenance and the manufacturing techniques used for their production. In particular, the present
study has shown that all samples follow the main technological characteristics of lead-glazed
Byzantine pottery. Some of them (K18, K32, K33) are Sn-opacified glazed pottery and, based on
XRD and SEM-EDS analysis, they could be either trade products or local products of workshops
that followed specific technologies. The chemical composition of the ceramic bodies was compared with already analysed material from the Paphos (Lemba, Kouklia) and Limassol areas
(Amathus). According to this comparison, the samples with increased Cr and Ca concentrations
seem to originate from the Limassol area while samples with low concentrations of Cr and Ca
could originate from the Paphos area. Finally, samples K3 and K8 show significant differences
due to the high content of TiO2, and together with samples K18, K32 and K33, which show strong
archaeological differences, could be regarded as possible trade products or local products of
different decoration technology.
Concerning the glazes, the blue colour is due to the presence of Co and Ni oxides, the green
colour is due to Cu oxides and the yellow, orange, red and black colours are due mainly to Fe
oxides, in combination with Mn and Cr oxides.
© University of Oxford, 2009, Archaeometry 52, 4 (2010) 628–643
© University of Oxford, 2009, Archaeometry 52, 4 (2010) 628–643
69
66
58
21
60
45
52
8
31
Quartz
Mainly anorthite, 2diopside.
1
K1
K12
K16
K18
K27
K28
K29
K32
K33
Sample
5
6
5
–
–
14
–
–
–
Potassium
3
4
6
2
2
11
26
13
8
Plagioclase1
Feldspars
–
–
–
29
–
7
–
27
25
Pyroxene2
4
5
5
20
5
12
–
–
5
Calcite
–
–
–
–
2
–
–
–
–
Mica
5
9
6
–
3
–
12
–
–
Hematite
–
–
–
14
–
–
–
–
–
Gehlenite
Table 4 Mineralogical composition (wt%) of selected clay samples, carried out by XRD
–
–
–
–
–
–
–
36
10
Analcime
14
10
20
14
28
11
10
16
21
Amorphous
640
A. C. Charalambous et al.
Cypriot Byzantine glazed pottery
641
Figure 5 XRD spectrum of the clay of the sample K33.
Figure 6 SEM-EDS analysis of samples K1, K18 and K33.
Further studies on more samples of glazed pottery excavated in Cyprus are in progress to
enhance our knowledge of Cypriot glazed pottery.
ACKNOWLEDGEMENTS
The present work was funded partially by the Greek General Secretariat of Research and
Technology and the EC under the programme ‘Excellence in Research Institutes GSRT (2nd
round)’, sub-programme ‘Support for Research Activities in C. E. T. I.’ The authors thank the
© University of Oxford, 2009, Archaeometry 52, 4 (2010) 628–643
642
A. C. Charalambous et al.
Figure 7 Optical microscopy and SEM photomicrographs of the body–glaze interface of the samples K1 (a, c) and K18
(b, d).
archaeologist E. Charalambous for cooperation and help during the sampling and the archaeologist E. Prokopiou for the samples and the information about the archaeological sites.
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