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Keywords: The present study is a multi-analytical approach for the characterization of several potsherd samples, dated from
Late-Classic Late Classical to the Hellenistic period at three different archaeological sites of Northern Greece: Pella, Thasos
Hellenistic and Samothrace. Ceramic petrography, Scanning Electron Microscopy coupled with Energy Dispersive
Ceramics Spectrometry (SEM-EDS) and X-Ray Powder Diffraction Analysis (XRPD) were applied for the determination of
Petrography
the chemical and mineralogical characteristics of the studied ceramics as well as the morphology of the clay with
X-Ray Spectroscopy
high resolution SEM images. Magnetic measurements on the sherds enriched the present study and when
Archaeomagnetism
combined with the archaeometrical approach described above, contribute to the characterization of the material
on its suitability for archaeomagnetic experiments. The overall obtained results confirm a local provenance and
techniques used for the pottery production.
⁎
Corresponding author.
E-mail address: aidona@geo.auth.gr (E. Aidona).
https://doi.org/10.1016/j.jasrep.2019.102097
Received 6 May 2019; Received in revised form 6 November 2019; Accepted 12 November 2019
2352-409X/ © 2019 Elsevier Ltd. All rights reserved.
Y. Santos, et al. Journal of Archaeological Science: Reports 29 (2020) 102097
Fig. 1. Map focus on the northern coast of Greece. Samples originate from 3 different regions in: Pella west of Thessaloniki; the island of Thasos east of Halkidiki
peninsula (Chalcidice) and the island of Samothrace further to the east.
a protocol for obtaining data from both analytical methods and basic due to river-transported sediments which have filled in the estuary, the
magnetic experiments such as thermomagnetic and hysteresis loop ex- city stood on a shallow, but navigable lagoon (Fouache et al., 2008;
periments. Vouvalidis, 2013).
A strong emphasis is also recently given by several researchers on The archaeological site of Pella has a great reputation as it is related
the investigation of the firing conditions within the kiln, during ceramic to the kingdom of Philip II and his son Alexander the Great. A recent re-
manufacturing, by both petrographic and magnetic measurements opening of the excavation lead to important restorations, and created a
(Jordanova et al., 2018; Rada et al., 2011). This approach, though fully visitable site (Akamatis and Lilimpaki-Akamati, 2015).
promising, is not directly related to the scope of the present study which In 2008 an organized pottery workshop was unearthed and studied
aims first to investigate the physical and chemical properties of three in the quarter of the public baths, at the northwest part of the town
groups of ceramics, and to establish relations between the material’s block (Fig. 2). The workshop comprised a well, two cisterns for cleaning
composition and the regional geology in the vicinity of the corre- the clay and depositories in pits. Two pottery kilns were found in the
sponding archaeological sites. At a second level, this outcome could northeast room, both pear-shaped with medium to small dimensions,
enhance their relevance for archaeomagnetic studies through the pos- that is 1.30–1.55 m width to 1.80–2.10 m length. Both kilns presented
sible correlation of the ceramics magnetic properties and the char- similar architectural characteristics and evidence for high firings
acterization of the clay fabric.
The production of all studied samples belongs to three different sites
in Northern Greece (Fig. 1): Pella, Thasos and Samothrace from west to
east. The samples date from late 5th to late 3rd century BCE. (Late
Classical to the Hellenistic Period).
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Fig. 3. Representative studied samples from Pella (A) Samothrace (B) and Thasos (C).
according to observed vitrification. Traces of fired floors were clear and 2.3. Samothrace (Site code SM)
pottery fragments were found in both kilns, abundant in kiln 1 and less
numerous in kiln 2. The size of the fired pots was rather small, as can be The island of Samothrace is situated in the northeast part of the
expected from the dimensions of the kilns, and the products were un- Aegean (Fig. S3). The island is part of the Circum-Rhodope Belt
painted. Because of the big amount of ceramics found within the kilns it (Heimann et al., 1972; Kauffmann et al., 1976), a series of Triassic-
is assumed that they were in operation during their destruction and Jurassic continental margin sedimentary and volcanic rocks that sur-
possibly their last firing (dated at 250–225BC) was not completed round the crystalline Serbo-Macedonian and Rhodope Massifs. Litho-
(Lilimbaki-Akamati and Akamatis, 2008). The material we selected logically, five units have been distinguished in Samothrace from bottom
comes from the two kilns, is labelled as PE01 (from kiln 1) and PE02 to top: I) the basement which consists of a series of Late Jurassic low-
(from kiln 2) and consists of small handles, bottoms and body fragments grade metamorphic sedimentary and volcanic rocks (Tsikouras and
of sherds. Hatzipanagiotou, 1995) II) a low-grade meta-ophiolitic complex; III) a
calc-alcaline granite; IV) tilted volcano-sedimentary formations and V)
mostly horizontal Upper Miocene-Pliocene sediments which consist
2.2. Thasos (Site code TH) mainly of conglomerates, sandstones, shales and nummulitic limestones
(Christofides, 2000; Eleftheriadis et al., 1994). The lower north-east,
Thasos is the northernmost island in Greece and is separated from west and south-west slopes of the island are covered by Tertiary vol-
the mainland by only 10 km. The interior of the island is mountainous canic rocks in the form of domes, dykes, lava flows and abundant
and belongs to the Rhodope geological zone, thus largely composed of pyroclastic formations mainly of andesitic composition (Eleftheriadis
metamorphic rocks (Fig. S2). These formations are divided into several et al., 1994) (Fig. S3).
units formed basically of muscovite schists, biotite schists and gneisses The island hosts one of the most peculiar archaeological sites in
whereas coarse-grained marbles and dolomites are overlying these Greece, which flourished in the second half of the 4th BC century and
series. Stratigraphically higher units follow the same lithological trend continuously expanded until the end of Hellenistic times. This site,
of gneisses, schists, marbles and dolomites. Alluvial deposits occur in Palaeopolis, is situated at the northern part of the island and comprises
the major bays, in the northeast, east and southwest, and especially the Sanctuary of the Great Gods, a Tholos, and several buildings used
along the northwest coast (Zachos, 1982). for the mystic ceremonies of Kaviria. An extended complex of ceramic
Remains of several production sites for transport amphorae have workshops was excavated in the late 1980s close to the North coast,
been located and reported by Picon and Garlan (1986) and Garlan around 5 km east of Palaeopolis. The workshops’ activity was placed
(1986), all concentrated around the coast of the island, except from the between the late Hellenistic and the Early Imperial period. Around
northwest to southeast. Workshops were in operation from the end of 500 m further to the East three ceramic kilns, of updraft type, were also
the fifth or beginning of the fourth centuries through to the second or brought to light (Karadima-Matsa, 1994) and for this reason the area
even the beginning of the first century BC. More than 20.000 fragments was named Keramidharia. The biggest kiln was studied archae-
of stamped handles are classified and stored in the archeological mu- omagentically in the past (Spatharas, 2005; Spatharas et al., 2011). The
seum of Thasos. The presently studied collection comes from four kiln was buried afterwards for preservation, but in the surrounding
groups of amphorae handles labelled as TH (05, 06, 07, 08) and covers slopes of the mound several fragments of common, unpainted pottery
the period from 285 to 266 BC. (jars, plates, handles) were spread, originating from the kiln’s produc-
tion. The samples of the present study were collected precisely in this
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Y. Santos, et al. Journal of Archaeological Science: Reports 29 (2020) 102097
area. The archaeomagnetic dating of the kiln in combination with OSL the same chemical composition do not have the same crystallographic
on the fragments suggests a possible date for the sherds between 340 structure (e.g. calcite and aragonite).
and 221 BCE. Additional information on the kiln’s dating can be found Mineralogical characterization of the ceramic samples as well as
in the supplementary material. their firing conditions were performed by X-ray powder diffraction
(XRPD) using a water-cooled Rigaku Ultima in conjunction with
3. Materials and analytical methods powder diffractometer with CuKa radiation, a step size of 0.05° and a
step time of 3 s, operating at 40 kV and 30 mA.
A total of 23 fragments from the three sites were examined within a The collections studied here were initially selected for an archae-
framework of archaeological information on typology (Fig. 3). None of omagnetic study. In order to cross-check the information compiled
the three groups could be considered as “fine ware” since they are through the experiments described above with a focus to magnetic
mostly unpainted (PE) amphorae handles (TH) and other commonware minerals included in our fragments, two classical magnetic experiments
(SM). From each fragment 2 to 3 specimens (apart only one exception) were performed:
were cut in order to be used for the different methods applied in this a) Magnetic susceptibility and its variation with temperature
study. In total, 48 specimens were studied. The mean size of each (thermomagnetic analysis) is a key tool for the identification of iron
fragment was 3X4 cm in surface and 1–2 cm in thickness, while spe- oxides within fired clays and for monitoring possible alterations during
cimens followed the geometry of the fragment. More details on the heating and cooling cycles. Important information can be obtained
material are included in the corresponding paragraphs for each site. through their shape, reversibility and calculation of Curie temperatures.
Microscopic examination combines several analytical techniques The Curie points for the corresponding samples have been calculated
such as ceramic petrography, scanning electron microscopy (SEM) and through the second derivative procedure (Petrovsky and Kapicka,
X-Ray powder diffraction analysis in order to better investigate the raw 2006). For this experiment we used the equipment in Paris IPG. A
material sources. Kappabridge KLY 3 was used in order to determine the Curie point of
Defining the petrographic fabric groups was initially based upon the magnetic carriers, as well as their stability during heating. The
their occurrence in the archaeological collections that were sampled, experiments were carried out in air. Susceptibility values were recorded
the extent of production centres and availability. This has allowed the continuously from room temperature up to 550 °C and back to room
regional geology of each area to be taken into consideration during the temperature. The equivalent equipment in the Geophysical Laboratory,
fabric characterization. University of Thessaloniki, MS2 Bartington susceptibility meter with
Petrography has been performed on 15 pottery specimens and re- the MS2WF attached furnace, was also used for complementary mea-
vealed a fine fabric for Pella, a coarse, a medium to fine and a fine surements from room temperature up to 700 °C.
fabric for Thasos, a coarse, a medium and a fine fabric for Samothrace b) Hysteresis loops are also a standard experiment for rock mag-
ceramics. All but one polished thin-sections used for petrographic netism studies. Their shape and calculated parameters provide im-
analysis were coated with carbon in order to achieve conductivity at the portant information on the nature and size of magnetic grains. These
Scanning Electron Microscopy Laboratory of Aristotle University of experiments were conducted in the Physics Department of Aristotle
Thessaloniki. At least one sample per petrographic fabric has been University of Thessaloniki, on a PAR 155 magnetometer with a 2T
analysed by SEM with the aim of complementing the results of the electromagnet.
petrographic analysis. Images and chemical analyses were performed
with a SEM (JEOL JSM-840A, Tokyo, Japan) equipped with an Energy 4. Results
Dispersive Spectrometer - EDS (INCA 250, Oxford) with 20 kV accel-
erating voltage and 0.4 mA probe current. Backscattered electron (BSE) 4.1. Ceramic petrography
images were taken in order to determine the different mineralogical
phases in the clay matrix. Chemical composition of the clay paste was Thin section petrography is based on compositional analysis and
measured using a beam size of 5 x 5 μm. On each sample 30 analyses of provides data for the raw material selection and the reconstruction of
clay paste were performed. All data were normalized to 100%. technology (Peterson, 2009). Petrographic analysis allowed the classi-
SEM provides valuable information regarding the degree of refine- fication of the samples into fabric classes based on a common range of
ment of the clay used, tempering and the firing conditions during the explicit properties and not only from typology and macroscopic ana-
ceramic production. Therefore it is widely used in archaeometric stu- lysis. Since petrography can reveal significant points for archaeometric
dies on ceramics (Froh, 2004; Knappet, 2011 among others). This analysis, it was the first step done in this research and provided pre-
technique permits surface details to be obtained and statistical analyses liminary information concerning the fabric and the minerals included in
to be performed to fully characterize the samples. the samples.
X-ray Powder Diffraction spectroscopy is based on the fact that In order to better investigate these issues, 15 pottery sherds were
crystals diffract X-ray with an angle characteristic of the crystal and thin-sectioned and studied under the polarizing microscope (Zeiss
consequently of the material. The angle and the intensity of the peaks Axioskop Pol.) following the systematic description proposed by
can give information about the phases present in the sample. That can Whitbread (1986; 1995). Each Fabric Class was based on the clay ma-
be used for identification of general mineralogical composition and trix, the compositional differences (the presence of different inclusions)
neo-formed minerals. and the fabric coarseness.
By identifying the mineral phases present in ceramics, one can es- It is important to bear in mind that the nomenclature for each fabric
timate the firing temperature which the ceramic products reached class is based on the set of samples from a specific area. For example we
during the vitrification process. So, the main goal of XRPD analysis is have fine fabric classes from Pella, Thasos and Samothrace, but that
the recognition of the mineral phases, especially new microcrystalline does not imply that all of these fabrics can be classified in the same
minerals formed by firing and from those the determination of the firing category. Regarding the contribution of petrographic analysis an
temperature and atmosphere condition in the kilns. However, it is im- overview on the fabrics is required (Tables 1 and 2).
portant to bear in mind that XRPD can identify minerals only above 3% Regarding Pella fine fabric samples, though the geology of Pella is
of the overall sample weight. Also XRPD analysis can confirm the data mostly based on alluvial sediments, volcanic rock fragments are not
found by petrography and SEM-EDS analyses as well as complete a full uncommon. In fact, intense volcanic activity took place northwest from
mineralogical composition of the studied samples by distinguishing Pella and fragments from these rocks, most likely trachyte due to its
polymorph compounds. X-Ray diffraction can distinguish polymorphs texture and orientation of feldspars, would reach Pella as sediments
by identifying the crystallography of each compound. Compounds with (Higgins and Higgins, 1996; Vougioukalakis, 2002; Eleftheriadis et al.,
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Table 2
Petrographic analysis of the studied samples. Groups are labeled as in Table 1. “X” checks the presence of the particular mineral or rock fragments within the sample.
Petrographic Fine Fabric Medium Fabric Coarse Fabric
Groups
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Fig. 4. (a) Pella Fabric, XP, Sample PE01-01. Volcanic rock fragment; potentially trachyte (x10) 1.4 mm wide, (b) Thasos fine fabric, XP. Sample TH 07-05. Clay
pellet with calcite linings, also known as hypo-coating (x10; 1 mm wide), (c) Samothrace coarse metamorphic fabric, XP, Sample SM-15.Metamorphic rock fragments
have been identified. Fabric feature. (x5; 2 mm wide).
by SEM micrographs, the surface morphology between rim and core 4.3. X-ray powder diffraction analysis
shows variations (Fig. 5). The outer rim shows a smooth, continuous,
non-porous texture while the inner core is characterized by fine pores As stated before, the mineralogical composition depends on the
with a diameter less than 1 μm. On the other hand, the chemical regional geology and the potters’ habits and experience.
composition of the clay matrix, as shown by EDS analysis is similar. The The estimated firing temperature for PE01 sample is T ≈ 750 to
morphological difference between the core and the rim is ascribed to 800 °C. The presence of tremolite confirms that this temperature could
the different firing conditions as will be discussed in a following not exceed 800 °C as such a mineral would not be present (Grapes,
paragraph. 2006; Xu et al., 1996). Data from petrographic analyses also confirm
Therefore, additional data from XRPD are needed to confirm the the firing temperature mentioned above since the micromass for Pella
mineralogical composition of the samples, distinguish polymorphs by fine fabric has been described as optically slightly active, when almost
identifying the crystallography of particular minerals and provide complete dehydroxylation of clay minerals happens (Rathossi et al.
characterization of the clay used. 2004; 2010) (Fig. 6).
Furthermore, sample PE02-09 belongs to the same fabric group as
all the other samples and the micro mass can be described as medium/
slightly optically active (Fig. 6) so its firing temperature was probably
Table 3
Chemical composition of the different clays. Values represent average of 30 area (5 μm × 5 μm) analyses. All data are normalized to 100%. Analyses of inner and
outer layers of representative samples are also given.
SAMPLE PE01-07 PE02-07 PE02-08 PE02-09 TH06-01 TH06-05 TH06-08 TH07-05 SM-12 SM-15 SM-18
inner outer inner outer
FORMULA wt% wt% wt% wt% wt% wt% wt% wt% wt% wt% wt% wt% wt%
Na2O 4,23 5.57 0,69 0,96 1,56 1,85 1.87 0,88 2,97 2,14
MgO 2,1 1.71 3,42 3,31 2,23 4,99 4.58 3,44 3,66 4,5 3,66 4,81
Al2O3 19,69 17.89 21,1 22,59 22,74 17,95 15.97 23,05 14,65 23,55 29,9 21,97 22,97
SiO2 64,07 69.93 57,24 58,35 61,29 55,75 58.32 65,43 53,48 53,05 53,23 61,04 60,39
K2O 2,78 2.25 2,59 2,6 2,91 3,8 3.82 2,53 26,12 3,34 0,66 0,68 1,55
CaO 0,85 0.3 1,76 1,4 2,23 9,23 8.96 1,51 2,94 5,94 1,61 2,84 1,72
FeO 4,5 2.59 8,07 9,64 6,59 5,73 5.05 4,41 4,22 7,56 8,17 7,46 6,23
TiO2 3,63 0,61 0,69 0,56 1,18 0,71 0,7
Cr2O3 0,49 0.02 0,23 0,38 0,42 0,33 0,29
MnO 0,46 0.08 0,18 0,24 0,36 0,26 0,36 0,75
BaO 0,48 0,58
SO3 5,81
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4.4.1. Pella
Among the fragments which were retrieved from the two Pella kilns
for the archaeomagnetic study, four representative samples were se-
lected according to their color and shape.
First the monitoring of the magnetic susceptibility variation with
temperature (thermomagnetic analysis) on these specimens was per-
formed up to 550 °C in order to detect the reversibility of the heating
and cooling curves. A very similar pattern was observed for all (Fig. S4).
Following this, three specimens were selected and heated up to 700 °C
in order to calculate their Curie temperatures (Fig. 7).
For two out of three the calculated Curie points provide values in
the expected range of 496 °C−506 °C, indicating the dominance of ti-
tanomagnetite. For sample PE01-08 the Tc is very low, around 210 °C.
Fig. 5. Backscattered electron micrographs of sample PE01-07 – Outer (top)
This will be discussed together with similar results from Thasos.
and inner (bottom) layer comparison.
Hysteresis loops were performed, to our best, on the same material
as for the thermomagnetic analysis, and to the one used for petrography
and SEM. Therefore we used the following samples: PE01-01, PE01-08,
PE02-07, PE02-08 (Fig. 7). From the shape of the loops and the cal-
culated parameters the following characteristics can be observed: For
PE01-01 dominance of single domain (SD) titanomagnetite. For PE01-
08 a mixture of two magnetic components most probably one super-
paramagnetic and one SD titanomagnetite. For PE02-07 the shell is
pseudo -single domain (PSD) titanomagnetite with a higher quantity
while the core is SD titanomagnetite with low quantity. Finally for
PE02-08 a mixture of two magnetic components, most probably PSD
and SD titanomagnetite is documented.
4.4.2. Thasos
Nine groups of stamped amphorae handles from Thasos were sam-
pled in the past and the magnetic properties of several fragments, be-
longing to groups 1–5 are under study by A. Genevey and D.
Kondopoulou. The groups were organized through their dating and not
through provenance areas. Therefore we tried to investigate some
fragments from groups 5, 6, 7 and 8 in order to enlarge our database.
Fig. 6. XRPD spectra of representative specimens from Pella and Thasos. We used the same approach as for Pella: the first set was heated up to
550 °C (TH05-05, TH06-05, 08, Fig. S5). Then thermomagnetic analyses
slightly higher T ≈ 800 °C to 850 °C which could also be explained by up to 700 °C were performed on specimens from group 6 for a better
the higher content of hematite formed. coverage: TH06-01, TH06-03, TH06-04 and TH06-08 (Fig. 8). In all
All samples from Thasos clearly bear white mica, which can be cases, the susceptibility values are very low, the curves show a marked
preserved up to 900 °C, however the strong reflection recorded for such alteration around 350–450 °C corresponding to possible mineralogical
a mineral and the absence of neo-formed minerals suggests that the transformations. The calculated Curie temperatures are T = 486 °C
firing could not have exceeded 750 °C (Rathossi and Pontikes 2010; only for sample TH-06-08 while for the 3 remaining very low values
Kondopoulou et al., 2014). In addition the small amounts of calcite in were calculated (114°–172 °C).
sample TH06-07 indicate also that the firing temperature was below Hysteresis loops were performed on fragments: TH06-01, TH06-05,
750 °C. Results from sample TH07-05 indicate the presence of calcite TH06-08 (Fig. 8). For sample THGR06-01 a mixture of SD/PSD and MD
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Table 4
Results by XRPD for sites PE and TH, presenting the estimated firing conditions, micro mass description and minerals abundances (%). Q: Quartz, K-fd: K-Feldspars,
Pl: Pagioclase, C: Calcite, M: Muscovite, Tr: Tremolite, He: Hematite, Py: Pyrite.
SAMPLE ESTIMATED FIRING TEMPERATURE (°C) MICROMASS DESCRIPTION (OPTICAL ACTIVITY) IDENTIFIED MINERALS (%) REFERENCE
Q K-fd Pl C M Tr He Py
PE01-07 750° – 800° C Slightly optically active; light brown 77 6 9 1 3 4 Present study
PE02-09 800° −850⁰ C Slightly optically active; light brown 79 9 12 Present study
TH06-01 650°-700⁰ C Optically Active; Brown. 72 18 8 2 Present study
TH06-05 700° −750⁰ C Slightly optically active; very light brown 80 4 4 2 7 4 Present study
TH06-08 650°-700⁰ C Slightly optically active; very light brown 73 18 2 6 Present study
TH07-05 650°-700⁰ C Medium optically active; brown 56 5 7 17 6 9 Present study
titanomagnetite is observed while for THGR06-05 considerably bigger 15 and SM-18 three of which are fully reversible (Fig. S6) and up to
amounts of MD are present. In THGR06-08 SD or PSD titanomagnetites 700 °C on SM-13 and SM-15 (Fig. 9). The Tc calculated are between 430
in small amounts are dominant. and 440 °C, indicating the possible dominance of titanomagnetites in
The comparison of the two datasets is very promising as both in- the samples.
dicate weak magnetization for samples TH06-05 and TH06-08 which Hysteresis loops were obtained for fragments SM-12 and SM-A
are the two overlapping cases. (Fig. 9) in addition to SM-19 published in Rathossi et al. (2018). Both
samples contain MD grains of magnetite/titanomagnetite. Sample SMA
contains a significantly higher quantity of magnetic grains than sample
4.4.3. Samothrace SM-12 in which a very small quantity of magnetic grains is found.
Three of the ceramics retrieved from Samothrace were previously
studied for archaeomagnetism, and relevant information in parallel
with petrography is given in Rathossi et al., (2018). Thermomagnetic
analysis up to 550 °C was done on new fragments: SM-12, SM-13, SM-
Fig. 7. (Top) Thermomagnetic analysis of three Pella samples. Susceptibility is given in 10-5SI units. (Bottom) Hysteresis loops for four Pella samples.
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Fig. 7. (continued)
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Fig. 8. (Top) Thermomagnetic analyses for four Thasos samples. Susceptibility is given in 10-5 SI units. (Bottom) Hysteresis loops for three Thasos samples.
6 wt% of calcium oxide are considered as non-calcareous clays. In all kiln, and have been fired between 650° −800 °C (Rathossi et al., 2018).
studied samples, with the exception of sample TH06-01, CaO content is The calcite deficiency that was witnessed in the majority of samples
less than 6 wt%, confirming the original petrographic observation that may indicate that either the raw clays were extracted from a non-cal-
the clays used for the production of the vessels are non-calcareous. careous deposit or were not refined with calcite temper. Quartz was
Sample TH06-01 has a high CaO content, 9.23 wt%, indicating a dif- detected in all samples. This mineral persists on firing up to 1000 °C,
ferent clay source for this sample. Thasos amphorae have been divided and thus it indicates that the ceramic derived from silica-rich raw
in two groups based on their clay composition and on a previous re- material. Quartz may be an indigenous mineral of natural clays or may
levant study on prehistoric pottery (Kondopoulou et al., 2017). The first be an intentionally added temper. Except quartz, feldspars are also
group has been produced from calcareous clay which points to a source evident in all samples, while the preservation of primitive minerals such
near marbles, dolomites and Neogene sediments while the second group as: clay minerals, white mica, hornblende and neo-formed such as: iron
has been produced from a non-calcareous clay, pointing to a source oxides, mullite helps on estimating the firing conditions of analysed
near metamorphic rocks. samples.
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Fig. 8. (continued)
safely that the materials used are the same both for the kiln and its present study we selected three different geological zones with specific
products, since these common use ceramics are not very elaborated and characteristics and we enriched the obtained data with magnetic mi-
were attributed to the local workshop (Karadima et al., 2002). There- neralogy measurements. This combination is increasingly adopted for
fore the information provided by Spatharas, (2005; 2011) in terms of the archaeometric studies on ceramics and we favored it aiming to the
magnetic mineralogy should be relevant to the one we cite here. A close improvement of the success in archaeomagnetic studies by appropriate
examination of this dataset indicates prevailing titanomagnetites, material selection.
mostly MD, and a few cases with mixtures of SD/PSD grains, both for Petrography performed on 15 pottery samples revealed a fine fabric
the kiln’s clays and the produced ceramics. for Pella, a coarse, a medium and a fine fabric for Thasos, a coarse, a
medium and a fine fabric for Samothrace ceramics. The majority of
5.2. Implications and general context. these fabrics seem to have been locally produced.
From the petrographic point of view, the observed samples share
The pottery of the Hellenistic period proves to be common and many similarities, but a few minerals are more specific of the origin
uniform and at the same time varying depending on the tradition and area for each set of samples. The presence of metamorphic rocks in a
the circumstances of different regions in the Hellenistic world. high quantity, for instance, is persistent in Thasos amphorae.
Increasingly affluent consumers during this period were eager to en- Consistency in the composition and micromorphology of Thasian am-
hance their private homes and gardens with luxury goods. These lavish phorae from various production sites suggests that similar clay sources
items were manufactured on a grand scale as never before, so it is safe were used in different parts of the island (Whitbread, 1995). Following
to conclude that pottery recipes were well diffused in the Hellenistic the geological evidence, sedimentary clays (other than recent alluvial
world and, as a result, assume that the potters shared common deposits) are only present in the south-western part of Thasos and, in
knowledge on ceramic production. most cases these deposits are situated at some distance from the pro-
Several archaeometric studies in connection with raw materials duction sites. According to Peacock (1970) the potters used two clays,
were performed on Hellenistic pottery in this part of the Mediterranean each taken from different localities on the island. The author reports
(Neyt et al., 2012; Marzec et al., 2018 and references therein) apart clear differences between the clays collected at these localities referring
from Greece where the list is long (for an overview see Drougou and to their color and grain size: yellowish brown and relatively fine, or
Touratsoglou, 2012; Ackermann, 2018 and references therein). For the reddish brown and rather coarse.
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Fig. 9. (Top) Themomagnetic analyses on Samothrace samples. Susceptibility is given in 10-5 SI units. (Bottom) Samples SMA and SM- 12 hysteresis loops.
Table 5
Compilation of samples and techniques applied in the present study. Number of specimens depends on the methods used. XRPD results from Samothrace (SM) are
from Rathossi et al. (2018).
Sample Specimens Petrography XRPD SEM-EDS Thermomagnetic Hysteresis
PE01-01 2 X X X X
PE01-07 3 X X X X
PE01-08 2 X X X X
PE02-07 2 X X X X
PE02-08 2 X X X
PE02-09 2 X X
TH05-02 2 X X X
TH05-05 2 X X X
TH05-07 2 X X
TH06-01 3 X X X X X
TH06-03 1 X
TH06-04 1 X
TH06-05 3 X X X X X
TH06-08 3 X X X X X
TH07-05 3 X X X X
TH08-01 1 X
SM – a, b 2 X X X
SM – 3 2 X X
SM − 12 2 X X X X
SM − 13 2 X X
SM − 15 2 X X X
SM − 18 2 X X X
SM − 19 2 X X X
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Y. Santos, et al. Journal of Archaeological Science: Reports 29 (2020) 102097
Ceramic groups from Samothrace were previously investigated, to- (Lilimbaki-Akamati and Akamatis, 2008).
gether with clay surveying (Karadima et al., 2002), through XRF ana- An important contribution of petrography and XRPD analysis in the
lysis. Several groups were isolated among which some of local and present research was to assist on the estimation of the firing tempera-
others of non-local origin. Two among these groups, named 2 and 3 by tures. Table 4 presents a general characterization of the studied samples
the authors, due to their high contents in chromium and nickel, have by XRPD analyses. The maximum firing temperature of each sample is
been assigned to the areas of Palaeopolis and Keramidharia, where our also indicated according to the presence or absence of particular mi-
samples were collected. These are compatible with the proximity of nerals. For instance the estimated firing temperatures of Samothrace
gabbro outcrops, which increased the concentrations of Cr and Ni samples are T ≈ 650°-800 °C. The micromass of studied samples are
within the sediments resulting from alteration. Elemental analyses of optically active (clay minerals, T ≈ 600°–650° C) to slightly active
the clay from our Samothrace samples show existence of Cr2O3 in small (almost complete dehydroxylation of clay minerals, T ≈ 750°–800 °C).
quantities in samples SM-12 and SM-15 as well as higher amounts of Moreover, the coexistence of both hematite and magnetite at tem-
FeO, while sample SM-18 lacks Cr2O3 and has smaller amounts of FeO. peratures below 1000 °C suggests firing in a mild oxidizing atmosphere.
The first two samples possibly point to areas near the alteration of the (Rathossi et al., 2018; Rathossi and Pontikes, 2010)
gabbro formations that exist at the centre of the island while the latter Apart all technological and archaeological input provided by com-
derive from a different location. This observation is in accordance with bined sets of optical methods, one application of the obtained in-
Karadima et al., (2002) as reported above. formation directly connects with the field of archaeomagnetism. As
The minerals identified by spectroscopy suggest that all samples stated in a previous section, the possible contribution of optical
correlate with each other while each set group bears some particular methods to improve the outcome of such studies, is still under ex-
minerals compared to each other group set, in relation to the area amination as it has already been underlined in recent publications
where the samples were produced. The local geology is characterized (Kondopoulou et al., 2017).
by the exclusive minerals from each sample set, e.g sillimanite in Combination of analytical and rock magnetic methods is increas-
Thasos samples. Thasos samples correlate to the maximum with both ingly explored worldwide in the last decade for estimating various
Pella and Samothrace samples, in terms of fine fabric. Fine fabric from technological aspects of ceramic production and especially provenance
Samothrace has similar aspects as Pella fine fabric samples. Therefore and firing temperatures. As an example, Rada et al. (2011) suggested
we can conclude that the potters used a preferred type of clay or/and a that IRM acquisition curves as well as thermomagnetic measurements
similar production technique to obtain fine fabrics. can be used to distinguish various pottery groups and as indicators for
SEM-EDS analyses provided also information regarding the clay reducing or oxidizing conditions respectively. In more recent studies
texture and composition. It confirmed the use of non-calcareous clay for (Jordanova et al., 2018; 2019) extensive experimental procedures on
the production of the samples under study, with the exception of Bulgarian collections establish protocols leading to such information.
sample TH06-01. Furthermore, SEM results enhance the suggestion that Nevertheless such an approach is beyond the scope of our research
potters had followed similar if not identical recipes, and the major based mostly on analytical methods and basic rock magnetic results.
difference refers to the non-plastic inclusions, that could have origi- The combination of petrographic observations, SEM and X-ray dif-
nated either from the clay source or from the added material (e.g fraction analysis was used, apart assessing the firing conditions (tem-
temper). perature, atmosphere), for estimating the proportion of Fe-bearing
The petrographic, mineralogical and geochemical analyses indicate minerals in order to cross-check this outcome with the magnetic
that all the observed samples were produced from non-calcareous clay properties of the three collections. This cross-checking proved to be
with similar composition due to the overall low percentage of calcium partly efficient as will be explained below.
oxide and the bloating porous microstructure displayed by the BSE In Table 5 we have compiled the totality of experiments performed
microphotographs. All samples differ very little both in texture and on the 23 fragments studied. In the majority of them, at least two dif-
chemical composition. The discrimination of sample TH06-01, which ferent measurements were done. We will now focus to cases where all
has the highest CaO content, 9,23 wt%, probably indicates an exception (5/5) or 4/5 experiments are available, mostly for Pella and Thasos and
From the macroscopic examination, samples from Pella and Thasos one from Samothrace. For Pella, samples PE01-07 and PE02-07 are
and one sample from Samothrace, show an outer red/dark red margin studied with 4/5 methods. Both samples contain FeO but in lower
and an inner grey core. When examined with SEM-EDS, these areas amounts for PE01-07. They also belong to the same petrographic fabric
reveal a different microstructure. Margins are non-porous and the sheet class: Pella Fine Fabric (Table 1). All Thasos samples display alteration
like habit of the clay minerals is evident while the cores exhibit fine indications at low temperatures ~300°–400 °C. Together with their
pores with a diameter of less than 1 μm. The difference in color and magnetic content of MD grains and rather low firing temperatures (less
morphology is attributed to the differing firing conditions (Maniatis and than 700 °C) these samples do not sound promising for archaeointensity
Tite, 1981). The more reddish outer margin points to oxidizing condi- studies. Finally, most of Samothrace samples do not seem to alter
tions during firing while the gray-colored inner core points to reducing during heating, but did not reach very high temperatures apart from SM
conditions. Based on this fact, firing of these samples is assumed not to – 19 which is the only one that has provided successful archae-
be completed, in accordance with archaeological information, for in- omagnetic results in a preliminary study (Rathossi et al., 2018). The
stance in Pella where the kilns appear to be destroyed during firing cross-checking of information provided both by optical and magnetic
Table 6
Comparative information provided by optical and magnetic methods.
Sites Methods Pella Thasos Samothrace
Petrography Fine fabric (volcanic and Coarse, medium and fine fabrics (indication Coarse, medium and fine fabrics (volcanic fabric with
metamorphic inclusions) for metamorphic/volcanic origin) fragments of andesite and titanite/metamorphic)
SEM High % FeO, Low % FeO, High % FeO,
Low % TiO2 No TiO2 Low % TiO2
XRPD (Firing temperatures) 700 °C–850 °C 750 °C–800 °C 650 °C-700 °C 650 °C–800 °C
Magnetic Mineralogy (Tc) 494 °C–506 °C 290/558 °C, SD/PSD 486 °C 434 °C–440 °C
Hysteresis titanomagnetites 114 °C–172 °C Mixture of SD/PSD and MD MD titanomagnetites
titanomagnetites
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Y. Santos, et al. Journal of Archaeological Science: Reports 29 (2020) 102097
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