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Journal of Archaeological Science 54 (2015) 99e109

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Journal of Archaeological Science


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

The colour of ceramics from Bell Beaker contexts in NW Spain:


relation to elemental composition and mineralogy

Oscar rez a, *, Beatriz Prieto b, M. Pilar Prieto-Martnez c, Cruz Ferro-Va
Lantes-Sua zquez d,
Antonio Martnez-Cortizas b
a
Unidade de Arqueometra (RIAIDT), Universidad de Santiago de Compostela (USC), Edicio Cactus s/n, Campus Vida, Santiago de Compostela, Spain
b
Dpto. Edafoloxa e Qumica Agrcola, Facultade de Bioloxa USC, Campus Vida, Santiago de Compostela, Spain
c
Dpto. Historia I, Facultade de Xeografa e Historia, Praza da Universidade, n 1. USC, Santiago de Compostela, Spain
d
Instituto de Ciencias del Patrimonio, Consejo Superior de Investigaciones Cientcas, Edicio Monte da Condesa, bajo, Campus Vida, Santiago de
Compostela, Spain

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

Article history: In this paper we characterise the mineralogical and elemental composition and the colour (CIELab space)
Received 14 November 2013 of Bronze Age pottery sherds from NW Spain, using X-Ray diffraction, X-Ray uorescence and reectance
Received in revised form spectroscopy, respectively. For half of the samples we also determined the content in secondary iron oxi-
20 November 2014
hydroxides (sFe, iron extracted with dithioniteecitrate), using atomic absorption. The aim of the
Accepted 27 November 2014
investigation was to study the relationship between the colour and the elemental and mineralogical
Available online 5 December 2014
composition, and to explore the intentionality of the resulting colour. Samples had a low luminosity and
were located in the quadrant of the CIELab space ranging from red to yellow (hab: 0e90 ), showing low
Keywords:
Early Bronze Age
hue variability but a wider range of variation in chromaticity. In terms of composition they showed a
Bell beaker large mineralogical (12 different minerals were identied) and chemical (from acidic/felsic to basic-
Pottery ultrabasic/mac compositions) variation.
Geochemistry A principal components analysis using elemental composition and colour parameters demonstrated
Mineralogy that luminosity (L*) depends on organic matter (OM) content and to a lesser extent on sFe content.
Colourimetry Chromaticity (C*ab) depends on sFe content, but also on the felsic/mac relative composition and OM
CIELab system content, while hue (hab) is only related to iron mineral phases. We also veried that these general trends
differ to a certain extent depending on whether the pottery contains amphibole or not: the effect of sFe
on L* and of OM on b* (yellowing) and C*ab was only detected for pottery sherds without amphibole,
while an increase in felsic in relation to mac minerals has a more decisive effect on the chromaticity
(C*ab) of the amphibolic clays. Thus, colour seems to result from the interplay between i) the original
colour of the raw material/clays, ii) compositional factors (overall composition -felsic vs mac-, and sFe
and OM content), and iii) interactions between composition and processing (sFe and ring conditions
controlling yellowing). We interpret that there was an intentional selection of raw materials (felsic or
mac) and their processing (addition of iron oxides and organic matter) and a control over the ring
conditions in order to give the vessels a specic colour.
2014 Elsevier Ltd. All rights reserved.

1. Introduction in the 2nd millennium BC and are usually associated to the Bell
Beaker phenomenon (see Vander Linden, 2006 for a recent syn-
From the end of the 3rd millennium BC a series of progressive thesis). These changes are detected in the archaeological record and
economic and social changes occurred in Europe, which culminated mainly consist, on one hand, in the intensication of already known
technologies and, on the other, by the introduction of new elements
in the material culture pointing to a new knowehow. Changes in
all aspects of the social life, settlement patterns, intensive use of the
* Corresponding author.
E-mail addresses: oscar.lantes@usc.es (O. Lantes-Suarez), beatriz.prieto@usc.es soil, beginning and development of metallurgy, control on the
(B. Prieto), pilar.prieto@usc.es (M.P. Prieto-Martnez), cruz.ferro@usc.es (C. Ferro- exploitation and transformation of raw materials (salt, int, copper,
V
azquez), antonio.martinez.cortizas@usc.es (A. Martnez-Cortizas).

http://dx.doi.org/10.1016/j.jas.2014.11.032
0305-4403/ 2014 Elsevier Ltd. All rights reserved.
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O. rez et al. / Journal of Archaeological Science 54 (2015) 99e109

gold), generalization of individual burials with standardized goods upside-down bell shape, well-nished glossy red clays, and a
showing the existence of different social statuses, occur at a pan- decoration using geometric designs, normally made with combs or
European level. shells, around straight horizontal lines; although there are also
Although at the beginning most of the research focused on the regional groups with their own unique elements (Harrison, 1980).
origin and diffusion of the Bell Beaker, since the 70s of the last On the contrary, the undecorated pottery from this period was
century, sparked by Glockenbecher Symposion Oberried of 1974 made with very rough clays and in different shapes, although
(Lanting and van der Waals, 1976), regional studies started to certain vessels with a better appearance were deposited in tombs
develop leading to a signicant progress in research. Thanks to the (Prieto-Martnez, 1999). The undecorated pottery is the more var-
international conferences promoted by the Association d'Arche- ied group and has been the object of a recent monograph (Besse,
ologie et Gobelets as vehicle of continuous updating on this subject 2003). The decorated non-Bell Beaker pottery is an intermediate
(see for example Nicolis, 2001; Czebreszuk and Szmyt, 2003; Baioni type, usually similar to Bell Beaker pottery in terms of shape and
et al., 2008; Prieto and Salanova, 2013), it can now be stated that technology, but with quite different decoration, using impressions
bell beaker was a long-term phenomenon, distributed along a large made with nails or punches (Prieto-Martnez, 2011). No clear
area which covers most of Europe (Fig. 1) and with an increasing regional groups can be seen in these two categories.
number of sites. Diachronic studies are also needed to evaluate the NW Spain is one of the relevant Bell Beaker regions of Western
intensity and importance of the changes in particular areas (for Europe. The pottery from the region was studied from a stylistic and
example in the evolution of the domestic space in northern Europe; formal perspective (Castillo, 1928; Criado and Va zquez, 1982;
Artursson, 2009). Harrison, 1977; Prieto-Martnez, 1999), and dened as a unique
Due to the large differences in the introduction, development regional category in recent studies (Prieto-Martnez, 2011). Its
and end of the process of change, interpretations of the bell beaker composition, mineralogy and the origin of the raw materials were
phenomenon are diverse among regions, being assumed as the end studied in more recent years (Martnez Cortizas et al., 2008, 2010,
of the Neolithic, in areas with a less intense and more progressive 2011; Prieto Martnez et al., 2008, 2009a, 2009b).
change, as in France (Salanova, 2000) or The Netherlands (Lanting A number of anthropological (Miller, 1985) and archaeological
and van der Waals, 1976); or the beginning of the Bronze Age, studies (Prieto-Martnez, 1999; for Galician Bell Beaker contexts)
where changes were more abrupt with regard to previous cultural have shown that colour, and especially the colour of pottery, had an
phases, as in NW Spain (Prieto Martnez, 1999) or Norway (Prescott, important symbolic signicance depending on the social context in
1996). which the pottery was used (Rock, 1985). However, the wide range
Pottery is one of the crafts that changes in a more obvious way in of colours found on occasions in the same pottery, due to the ring
this period. Both in Europe and in Galicia three types of pottery can conditions and post-depositional processes, makes it difcult to
be found: decorated Bell-Beaker, undecorated and decorated non- arrive at a standard description for the vessels (Olaetxea, 2000). For
Bell Beaker (Prieto-Martnez, 1999). Bell Beaker pottery is a well- these reasons, very few studies have covered the subject of colour,
standardised type of decorated pottery found throughout much especially in ancient pottery, and particularly in the case of pottery
of Europe between approximately 2600 BC and 1500 BC, the exact from Bell Beaker contexts. The majority of them adopt a qualitative
age depending on the region (Mller and Willigen, 2001). It is the approach, either subjective or using Munsell colour keys, from
rst pan-European ceramic style, whose basic features are an amongst which we would highlight several that focus on the

Fig. 1. Map showing the location of the archaeological sites.


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O. rez et al. / Journal of Archaeological Science 54 (2015) 99e109 101

Table 1 explored the relationship between the colour and the elemental
Number of Early Bronze Age ceramic samples from NW Spain analysed for each and mineralogical composition of pottery in a study of sherds from
archaeological site and style.
different prehistoric periods in a specic area of the northewest
Site Bell Beaker Non-Bell Undecorated Context Total Iberian Peninsula.
decorate (dBB) Beaker (ND) In this study we present a quantitative characterisation of the
decorated
(dNBB)
colour, mineralogical and elemental composition of pottery from
Bell Beaker contexts of the north-west Iberian Peninsula, with the
Devesa do Rei 13 2 18 Ceremonial 33
aims of i) evaluating its relationship with geochemical composition,
Fraga do Zorro 2 14 19 Funerary 35
Zarra de Xoacn 6 e e Domestic 6 and ii) to obtain clues on the intentionality behind the choice of the
A Romea 3 e 1 Funerary 4 raw materials in order to achieve a nal colour.
A Forxa e e 2 Funerary 2
Forno dos 1 e e Funerary 1
Mouros 2. Material and methods
All 25 16 40 81
2.1. Samples

elemental composition as the cause of the colour (Constantinescu A total of 81 pottery samples were analysed (Table 1, Fig. 2). They
et al., 2005; Manning, 1975; Stewart et al., 2002; Weerd et al., were recovered from six Early Bronze Age archaeological sites
2004). representing three different contexts: Devesa do Rei, a ceremonial
Few studies have explored the causes of the colour of the pottery context; Forno dos Mouros, A Forxa, Fraga do Zorro and A Romea,
by measuring it quantitatively. Studies of this kind have basically funerary context; and Zarra de Xoacn, a domestic context (Fig. 2).
been carried out since the 1990s, within two main lines of research: The samples were selected according to chromatic, mineralogical
one focussing on the elemental composition of the ceramic bodies and geochemical variability and low degree of alteration, from a
as the cause of the colour and another focussing on its dependence group of 181 pottery samples previously characterized (Prieto et al.,
on the ring process (Cultrone et al., 2011; Molera et al., 1998) and 2011), and as being representative of the variability of Bell Beaker
vitreous bodies (Molera et al., 1997; Yang et al., 2005). Other studies pottery from NW Spain.
have explored the oxidation states of iron as the reason behind the
reddening of pottery clays, using techniques such as Mo ssbauer
2.2. Site location
spectrometry (Maritan et al., 2006; Nodari et al., 2004), or extrac-
tion using potassium permanganate (Nodari et al., 2004, and ref-
The location of the archaeological sites is shown in Fig. 1. They
erences therein). The relationship between the composition and
belong to three areas of Galicia (the northewest Iberian Peninsula):
colour has also been explored in other materials, such as soils
Devesa do Rei, A Romea, and Zarra de Xoacn are located in the Ulla-
(Gunal et al., 2008; Sanchez-Maran ~o
n et al., 2004; Torrent et al.,
Deza area; Forno dos Mouros in Sierra de O Bocelo; and Fraga do Zorro
1980, 1983; Viscarra Rosel et al., 2009), waste rocks (Azzali et al.,
and A Forxa in the south-east of Galicia.
2011), talc (Soriano et al., 2002) or kaolin (Gamiz et al., 2005).
The Ulla-Deza area has a varied lithology, predominated by a
Recently, Prieto Lamas et al. (2011) analysed the relationship
substrate of acidic metamorphic rocks (slates, schists, paragneisses,
between the quantitative colour and formal, stylistic and contex-
carbonaceous schists), including small areas and narrow bands of
tual variables in pottery from Bell Beaker contexts, verifying that
amphibolite. Other rocks present are quartz dikes, alkaline granites
pottery from domestic and ceremonial contexts had a higher red
(granites, orthogneisses, intrusive rocks), calcalkaline granites
component, pottery from the settlements was the darkest, while
(granodiorites), basic schists, basic and ultrabasic rocks and detritic
the pottery from the funerary context had a more yellowish tone
materials (especially colluvial and uvial sediments) (Divar
than the rest. It was also found that the decoration was associated
Rodrguez et al., 1982; Gonza lez Lodeiro et al., 1974; Klein et al.,
with colour, whereby the Bell Beaker pottery is redder and darker
1982a, 1982b).
than the non-Bell Beaker or undecorated pottery. These authors
Sierra de O Bocelo mainly consists of large bands of granitic
suggested that a quantitative determination of the colour makes it
rocks, specically coarse grained orthogneisses. There are
possible to establish differences between sherds that are not visible
numerous outcrops of amphibolite, basic and ultrabasic rocks
to the naked eye. Martnez Cortizas et al. (2008) also partially
(including peridotites); and in a 10 km radius from the settlement

Fig. 2. Ceramic categories for pottery from Bell Beaker contexts: (1) Undecorated pottery. (2) Decorated Bell Beaker pottery. (3) Decorated non-Bell Beaker pottery (from Prieto,
2011).
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O. rez et al. / Journal of Archaeological Science 54 (2015) 99e109

acidic and carbonaceous schists, and basic paragneisses can also be In order to quantify the concentrations, calibrations were carried
found (Pablo Macia  et al., 1981). out beforehand using certied reference materials (NIST). The
The south-east of Galicia is much more uniform, with dominant biophilic elements, C and N, were determined using a Leco TruSpec
acidic schists (with quartz-muscovite mineralogy) and granitic CHNS elemental macrosample (500 mg) analyser.
rocks, although Tertiary sediments, formed by clays with variable
amounts of quartz pebbles, are also abundant (Nun ~ o Ortea et al., 2.5. Mineralogy
1981). No basic and ultrabasic rocks are found within a radius of
25 km from the settlements. The mineralogy was characterised in the nely milled samples
The main secondary minerals found upon weathering in the using the X-Ray diffraction technique. A Philips PW1710 diffrac-
soils formed over these materials are mostly kaolin-type clays, tometer was used with BraggeBrentano q/2q geometry with a Cu
gibbsite (in the absence of organic matter), mica degradation anode. DIFFRACplus EVA software from Bruker AXS was used to
products (interstratied illite-vermiculite), quartz and traces of K- quantify the relative abundance of the minerals. It is important to
feldspars (when present in the rock) (Silva and Guiti an, 1984). note that the mineralogical data refer to the crystalline fraction (as
this is the fraction that is detected by XRD).
2.3. Determination of the colour
2.6. Secondary iron extraction
The colour was determined in nely ground and homogenised
samples placed in 8 mm-high cylinders with a diameter of 15 mm.
The secondary iron oxides and hydroxides were determined
We are aware that the colour of the powdered sample may differ
after extraction with sodium dithionite citrate according to
from that of the surface of the original vessel (or pottery fragment),
Holmgren (1967). This extractant combines the action of a com-
but this procedure enables us to obtain comparable and repeatable
plexing and a reducing agent, providing a good estimate of the
colour, chemical and mineralogical data from the same sample.
amount of secondary iron (which includes the solubilisation of the
Thus, it enables an appropriate statistical treatment of the data and
crystalline iron oxides and hydroxides, low crystalline forms of iron
to draw consistent interpretations on the relationship between
and iron in complexes with organic matter). Iron content was
colour and composition. Our assumption is that the factors inu-
determined using ame atomic absorption spectrometry (FAAS)
encing the colour of the powdered sample are the same as those
(Perkin Elmer 1100B).
inuencing the colour of the whole surface of a vessel -their weight
may vary depending on the actual colour of different sections. Thus,
although we do not investigate the actual colour of the surface, we 2.7. Statistical analysis
can obtain information on the factors affecting its variability -even
if the distribution of colour in the vessels is not known. The relationship between the chemical composition, miner-
The measurements were made using a Colour-Eye XTH reec- alogy and colour parameters was evaluated using correlation,
tion spectrophotometer, with a measurement aperture diameter of ANOVA and principal components analysis (PCA). As the data for
5 mm, taking three readings at three randomly-selected points on the mineralogical and elemental composition are typical examples
the surface, expressing the results as the mean of the three read- of compositional data (Aitchinson et al., 2002; Baxter et al., 2008),
ings. The measurement conditions were: D65 illuminant and we applied a centred log ratio transformation prior to statistical
observer 2 . The colour measurements were expressed using the analysis, as recommended by various researchers (Aitchison, 2003;
CIELab colour system, which is widely used by the scientic com- Baxter and Freestone, 2006). The statistical analyses were per-
munity and in industry, as it is the most uniform colour space from formed using the SPSS Statistics 20 software.
a perceptual point of view (Berns, 2000; Vo lz, 2001). The CIELab In the description and discussion of the PCA results below we
system is organised around three axes, L*, a* and b*, forming a mention the communalities, which account for the percentage of
sphere: the L* axis is associated with the luminosity of the colour the variance of each element explained by the signicant principal
and varies from 100 (white) to 0 (black), while the a* and b* axes, components. The communality for any variable is computed as the
which are orthogonal to the L* axis, indicate colour directions: a* sum of the squares of its loadings in the extracted principal com-
the red direction, a* the green direction, b* the yellow direction ponents. The square of a loading of a variable in an individual
and b* the blue direction. Another way of expressing this system component is thus taken as a measure of the proportion of variance
is by polar coordinates (C*ab, hab), which are highly intuitive in of the element related to the underlying factor reected by that
relation to the way the colour is perceived. The chroma, component. In this way, apart from the total variance explained, we
C*ab (a*2 b*2)1/2, varies from the centre of the sphere (achro- can get an estimation of the fractionation of the communalities, i.e.
matic) towards the exterior (increasing chromaticity), and the hue, an idea of the relative weight of each underlying factor in the dis-
hab arctan (b*/a*), is expressed in degrees, where red 0 , tribution of the analysed elements.
yellow 90 , green 180 and blue 270 .
3. Results and discussion
2.4. Elemental composition
3.1. Colour parameters
The elemental composition was analysed using X-Ray uores-
cence (XRF) in nely milled and slightly compacted samples. Two Luminosity (L*) varied between 21 and 55 units (mean and d.t.:
energy-dispersive X-Ray uorescence spectrometers with an Si(Li) 37 8), a* between 1 and 22 (8 5), b* between 5 and 34 (19 8),
detector were used (Martnez Cortizas et al., 2008). The chemical chromaticity (C*ab) between 5 and 40 (21 9) and hue (hab) be-
elements that were detected in concentrations above the quanti- tween 54 and 78 (68 6 ) (Table 2). These values indicate that
cation limits were grouped as major and minor elements (Si, Al, the samples have a low luminosity and are located in the quadrant
Fe, Ti, Mg, Ca and K); lithogenic trace elements (Ga, Rb, Sr, Y, Zr and of the CIELab space ranging from red to yellow (hab: 0e90 ). Fig. 3
Nb); and metallic trace elements (Cr, Mn, Ni, Cu, Zn, Pb). Other el- shows the position of the samples projected on the a*eb* plane.
ements such as Mg, Cl, Se and Th were only detected in some The samples show low hue variability but a wider range of variation
samples, and in many of them were close to the quantication limit. in chromaticity.
 Lantes-Sua
O. rez et al. / Journal of Archaeological Science 54 (2015) 99e109 103

Table 2 and calcite e were only found in a few samples, with a frequency
Descriptive statistics (average, standard deviation, maximum and minimum values) 10%. The other three e halloysite, amphibole and chlorite e are
for the CIELab colour parameters of the Early Bronze Age pottery from NW Spain.
(dBB: decorated Bell Beaker; dNBB: decorated non-Bell Beaker; ND: non-decorated).
relatively frequent (68%, 49% and 15% respectively). The mean
concentration of the minerals in the samples that contain them is
L* a* b* C*ab hab high for quartz, plagioclase and chlorite (37 15, 25 15 and
dBB Avg 38 11 23 26 66 22 22%, Table 4) and very low for talc, kaolinite and calcite
Std 7 6 7 9 7 (5%). Chlorite is almost exclusively present in samples that also
Max 51 22 32 37 78
contain amphibole. The rest of the minerals have concentrations
Min 21 1 5 5 54
dNBB Avg 41 7 18 19 68 between 16 and 7% (potassium feldspar 16 12%; halloysite
Std 10 4 7 8 4 13 6%; mica 8 7%; amphibole 9 12%; hematite 16 10%; and
Max 53 15 28 32 76 anatase 7 4%). It is important to note the number of minerals
Min 22 1 5 5 62
detected, but also the large diversity in the compositions of the
ND Avg 36 7 16 18 69
Std 8 5 7 8 5
pottery. For example, talc is characteristic of ultrabasic materials,
Max 55 21 34 40 76 while potassium feldspar is characteristic of acidic materials.
Min 21 2 6 7 55 XRD analysis enables the detection of crystalline phases of
All Avg 37 8 19 21 68 mineral material. Since we analysed bulk samples, the mineralogy
Std 8 5 8 9 6
corresponds to both the signal of clays and inclusions. Nevertheless,
Max 55 22 34 40 78
Min 21 1 5 5 54 the large difference between the mineralogy of the pottery and that
of the rock weathering products of the study area, which are the
more likely source for the clays, suggests that the inclusions may
have a higher weight in the detected mineralogy. This idea is
3.2. Elemental analysis
supported, for example, by the relative abundance of plagioclase
(present in >85% of the samples) and amphibole (49% of the sam-
Table 3 shows a summary of the concentrations of the elements
ples), two highly weatherable minerals that are almost absent in
that were analysed, grouped according to decorative style of the
the rock weathering products. Other minerals, as kaolinite, the
pottery (decorated Bell Beaker, decorated non-Bell Beaker and
main phyllosilicate in the clay fraction of the raw materials, be-
undecorated pottery), and for the whole set of samples. The range
comes invisible to XRD, as it loses its crystalline structure when
of concentrations is quite varied and covers from typical felsic (i.e.
the ring temperature exceeds 500e700  C (Capel et al., 1985;
granitic) to typical mac (i.e. basic and ultrabasic) compositions.
McKenzie, 1970: 526; Velde, 1992: 174). Thus, its low frequency
The former are characterized by larger concentrations of elements
and content in the samples is not surprising. In fact, the correlation
like Si, K, Rb, Zr, Nb and Pb, while the later show larger concen-
structure between the mineralogical and elemental composition
trations of Ca, Mg and metallic elements such as Cr and Ni. Further
was moderate; we only found signicant positive correlations for
details on the composition are provided by the PCA analysis.
three of the minerals (Table 5): chlorite with Ca, Mg, Mn, Cr and Ni;
amphibole with Fe, Ca and Ti; and quartz with Si, Zr and Nb.
3.3. Mineralogy

Twelve minerals were detected in the crystalline fraction of the 3.4. Relationship between colour and ceramic composition
pottery sherds (Table 4). Four of them e quartz, plagioclase, mica
and potassium feldspar e are very frequent, found in more than In order to determine the compositional factors that inuence
85% of the samples. Another ve e kaolinite, talc, anatase, hematite the colour of the selected pottery samples, we performed a prin-
cipal components analysis using the total concentration of chemical
elements and the CIELab colour parameters (scalar: L*, a*, b*, and
polar: C*ab and hab). Five principal components explained 82% of
the total variance (Table 6). Almost all variables showed a high
(>70%) communality (total length of the bar in Fig. 4), with the
exception of Mn (48%) and Sr (67%). Given that the aim of this
research was to determine the compositional factors inuencing
the colour of ceramics, we began by interpreting the principal
components from a geochemical point of view, thereby attempting
to identify the factors underlying the variations in elemental
composition, and then evaluating the effect of these factors on the
colour.
The rst principal component (Cp1, 40.5% of total variance)
shows high positive loadings (>0.7, i.e. more than 49% of the vari-
ance of the element) for Si, Al, K, Ga, Rb, Y, Nb, and Pb, and a
moderate loading for Zn (0.58), while Fe, Ti, Ca, Cr, Mn and Ni show
moderate to high negative loadings (0.65 to 0.87) (Table 6). El-
ements with positive loadings are characteristic of felsic mineral
(K-feldspar, mica, quartz) compositions, while those with negative
loadings are characteristic of mac (amphibole, plagioclase, chlo-
rite) compositions. This is supported by the correlations found
between minerals and elemental composition of the ceramics,
mentioned above (Table 5). Thus, we interpret this component as
reecting the relative dominance of felsic/mac (F/M) composi-
Fig. 3. Position of the samples projected in the a*eb* plane. tions (since we analysed bulk samples, the terms felsic and
104  Lantes-Sua
O. rez et al. / Journal of Archaeological Science 54 (2015) 99e109

Table 3
Descriptive statistics (average, standard deviation, maximum and minimum values) for the concentrations of the elements determined in the Early Bronze Age pottery from
NW Spain. Major and minor elements in mg g1, trace elements in mg g1 (dBB: decorated Bell Beaker; dNBB: decorated non-Bell Beaker; ND: non-decorated) *The descriptives
provided here for Mg are only for samples with concentrations above the detection limit.

C N Si Al Fe Ti Ca Mg* K Ga Rb Sr Y Zr Nb Cr Mn Ni Cu Zn Pb

dBB Avg 16.0 1.3 184.8 103.3 95.9 15.1 8.2 15.8 22.0 30 124 75 29 218 12 692 596 163 39 71 25
Std 5.8 0.4 31.6 17.8 47.0 7.5 7.6 11.1 7.7 7 62 46 10 80 4 1935 440 508 25 23 9
Max 26.0 2.1 243.4 132.0 203.4 33.7 31.6 62.0 43.7 47 245 248 64 468 27 9937 2065 2597 98 133 46
Min 3.4 0.5 131.9 57.0 29.0 4.5 0.6 5.0 10.6 15 48 29 12 71 4 49 81 1 2 33 10
dNBB Avg 10.3 0.6 228.7 116.9 53.8 9.0 4.4 7.7 29.6 33 252 102 33 179 14 192 302 45 38 113 27
Std 8.0 0.2 36.2 17.0 22.3 4.4 4.3 2.7 7.1 6 68 50 9 37 3 214 294 45 17 45 9
Max 26.3 1.0 284.3 144.4 87.9 17.4 16.5 12.1 39.8 43 369 190 51 228 19 669 1118 133 60 184 43
Min 2.8 0.3 176.6 83.1 17.3 2.2 0.8 2.9 21.6 19 138 34 21 94 8 5 30 1 6 38 17
ND Avg 16.0 1.1 208.8 108.0 64.7 11.5 6.6 11.5 24.5 30 191 100 30 188 12 451 694 117 33 82 28
Std 9.4 0.4 32.7 16.5 42.0 7.6 5.8 5.1 7.7 6 109 54 8 71 2 280 728 89 19 34 12
Max 39.8 2.0 262.4 141.6 174.2 33.1 22.9 54.9 38.7 42 423 285 53 398 17 7657 4178 2116 93 180 59
Min 2.6 0.4 120.6 63.8 12.6 2.0 0.8 1.0 10.6 17 45 23 17 84 6 5 23 1 1 43 10
All Avg 14.9 1.1 205.0 108.2 72.5 12.1 6.7 12.1 24.7 30 182 92 30 196 12 478 588 118 36 84 27
Std 8.3 0.5 36.3 18.1 44.4 7.3 6.5 9.2 8.0 6 100 52 9 71 3 1383 641 371 20 36 11
Max 39.8 2.1 284.3 144.4 203.4 33.7 31.6 62.0 43.7 47 423 285 64 468 27 9937 4178 2597 98 184 59
Min 2.6 0.3 120.6 57.0 12.6 2.0 0.6 1.0 10.6 15 45 23 12 71 4 5 23 1 1 33 10

Table 4
Descriptive statistics (average, standard deviation, maximum and minimum values) of the relative abundance (percentage) of the minerals identied in Early Bronze Age
pottery from NW Spain. Values are given for samples in which the mineral is present (n). (dBB: decorated Bell Beaker; dNBB: decorated non-Bell Beaker; ND: non-decorated.
Qtz: quartz, Pg: plagioclase, Mic: mica, K-F: K-feldspars, Hal: halloysite, Amp: amphibole, Chl: chlorite, Kao: kaolinite, Tal: talc, Ant: anatase, Cal: calcite, Hem: hematite).

Qtz Pg Mic K-F Hal Amp Chl Kao Tal Ant Cal Hem

dBB Avg 34 24 8 17 14 14 26 e 2 e e 21
Std 15 18 6 16 7 13 34 e 1 e e 6
Max 62 61 26 73 28 56 75 e 3 e e 25
Min 1 1 1 2 4 1 3 e 1 e e 17
dNBB Avg 40 27 7 15 11 4 e 2 e e e e
Std 14 10 8 6 4 4 e 1 e e e e
Max 65 50 34 26 18 10 e 3 e e e e
Min 16 16 2 6 3 1 e 2 e e e e
ND Avg 37 25 9 15 13 7 21 5 3 5 e e
Std 15 16 7 10 7 11 17 5 1 2 e e
Max 70 63 31 44 29 49 57 14 4 6 e e
Min 14 1 1 1 5 1 2 1 1 3
n 79 78 72 68 53 40 13 8 6 4 3 3
All Avg 37 25 8 16 13 9 22 4 3 7 1 16
Std 15 15 7 12 6 12 22 4 1 4 0 10
Max 70 63 34 73 29 56 75 14 4 13 1 25
Min 1 1 1 1 3 1 2 1 1 3 1 6

mac are used here to indicate the overall composition of the by the principal components (86% and 84% respectively), the largest
pottery, including both the clays and the inclusions). part (48% and 56%) is related to Cp1, in particular to mac com-
The second component (Cp2, 18.0% of total variance) is associ- positions (given the negative loadings), while the rest (38% and
ated to part of the variance of Sr and Rb (loadings 0.67 and 0.39) on 19%) is associated to Cp2 (Fig. 4) and, consequently, should reect
one side, and of Fe and Ti (loadings 0.62 and 0.44) on the other the variation in Fe and Ti mineral phases other than the mac
(Table 6). Of the total variance of Fe and Ti concentrations explained minerals. Rubidium and Sr are characteristic elements of K-feldspar
and plagioclase respectively, as well as calcite in the case of Sr
(although this mineral was only found in three samples), in which
Table 5 they isomorphically substitute for K and Ca (Enghag, 2004: 79, 89,
Pearson coefcients for the correlation between mineral abundance and element 90, 310), respectively. As these minerals do not contain Fe, their
concentrations of the Early Bronze Age ceramics from NW Spain. (n: number of increase in a sample may contribute to a relative dilution of the Fe
samples; ns: not signicant, p > 0.05).
concentration. Thus, Cp2 most probably reects the variation in the
n Chlorite Amphibole Quartz content of secondary Fe (sFe) phases, like Fe oxides and hydroxides
12 40 81 (Ti tends to co-precipitate with Fe during the formation of sec-
ondary mineral phases; Taboada et al., 2006) in the ne fractions of
Si ns ns 0.50
Fe ns 0.70 ns the clays.
Ti ns 0.67 ns The third component (Cp3, 12.4% of total variance) is almost
Ca 0.74 0.75 ns exclusively related to C and N (0.92 and 0.85) (Table 6), and can
Mg 0.70 ns ns
be safely interpreted as reecting the organic matter (OM) content
Zr ns ns 0.56
Nb ns ns 0.51 of the ceramics.
Mn 0.63 ns ns The fourth component (Cp4, 6.4% of total variance) only shows a
Cr 0.64 ns ns high positive loading for Cu (0.81), and low values, although sig-
Ni 0.69 ns ns nicant (i.e. representing at least a 10% of the variance of the
 Lantes-Sua
O. rez et al. / Journal of Archaeological Science 54 (2015) 99e109 105

Table 6
Loadings of the variables, eigenvalues (Eigv) and variance explained (var) by the
extracted principal components in the PCA using all samples. The largest (positive
and negative) loadings in each principal component are in bold.

Cp1 Cp2 Cp3 Cp4 Cp5

Al 0.91 0.21 0.02 0.04 0.01


Nb 0.88 0.13 0.01 0.01 0.27
K 0.87 0.21 0.05 0.03 0.06
Ga 0.87 0.24 0.02 0.23 0.07
Rb 0.85 0.39 0.16 0.09 0.14
Si 0.82 0.30 0.03 0.09 0.08
Y 0.77 0.18 0.06 0.00 0.26
Pb 0.75 0.13 0.10 0.40 0.31
Zn 0.58 0.09 0.41 0.45 0.16
Mn 0.66 0.14 0.14 0.05 0.04
Fe 0.69 0.62 0.08 0.06 0.09
Ti 0.75 0.44 0.06 0.03 0.32
Ca 0.79 0.13 0.07 0.37 0.12
Ni 0.80 0.11 0.30 0.11 0.14
Cr 0.87 0.12 0.18 0.16 0.06
Sr 0.28 0.67 0.14 0.18 0.31
C 0.19 0.01 0.92 0.07 0.04
N 0.06 0.14 0.85 0.28 0.03
Cu 0.02 0.13 0.28 0.81 0.16
Zr 0.42 0.04 0.01 0.36 0.74
L* 0.02 0.27 0.90 0.01 0.01
a* 0.28 0.89 0.15 0.07 0.13
b* 0.35 0.80 0.37 0.02 0.11
C*ab 0.34 0.84 0.31 0.01 0.12
h ab 0.15 0.84 0.01 0.27 0.12
Eigv 10.1 4.5 3.1 1.6 1.2
Var 40.5 18.0 12.4 6.4 4.7

element) for Zn (0.45), Ca (0.37), Pb (0.40) and Zr (0.36)


(Table 6). We do not have an explanation for this component.
The fth component (Cp5, 4.7% of total variance) shows a high
loading (0.74) for Zr and a small one (0.32) for Ti (Table 6). Zirco-
nium is almost exclusively hosted by zircons, while Ti can be a
structural element in biotite and in Ti bearing-minerals like Fig. 4. Communalities of the elements and colour parameters used in the PCA analysis
ilmenite, rutile, anatase or titanite (Klocmann and Ramdohr, 1961: of the Early Bronze Age ceramic samples from NW Spain (Cp1, red; Cp2, orange; Cp3,
425, 442, 449, 569, 619; Taboada et al., 2006). This factor can be gold; Cp4, beige; Cp5, light yellow).

interpreted as the variation in the content of trace, small size,


resistant, minerals. (decrease in C*ab). Gunal et al. (2008), analysing the relationship
Regarding the colour parameters, their variance is only signi- between soil properties and colour, also found L* to be a good
cantly allocated into the rst three principal components (Cp1, F/M predictor of the content of organic matter in epipedons. Secondary
composition; Cp2, sFe phases; and Cp3, OM content) (Table 6). Fe is responsible for reddening (increase in a* and decrease in hab),
Luminosity, L*, is primary dependent (i.e. covaries) on organic yellowing (increase in b*), enhanced chromaticity (increase in C*ab)
matter content (81% of L* variance) and shows a small (7%) sec- and lightening (increase in L*) of colour. While the relative F/M
ondary dependence on sFe (Fig. 4; see also SI_Fig. 1 for a detrending composition seems to have a slight effect on reddening and chro-
of the effects of the signicant principal components in each case). maticity, all increasing as the mac component increases.
Increasing organic matter content in the ceramics produces a A close inspection of the data revealed that half of the samples
darkening (decrease in L*) of colour, while luminosity increases analysed contain amphibole and the other half does not and, as
with the content of sFe. Parameter a* is mostly dependent (79% of mentioned in Section 3.3, all samples containing chlorite (13) also
the variance) on sFe and marginally (8%) on the content of F/M contain amphibole. An ANOVA test indicated that the group formed
minerals (Fig. 4, SI_Fig. 1), both producing a reddening of the colour by the samples containing amphibole (i.e. mac compositions) has
as their contents increase. Parameter b* seems to depend on the signicantly (p < 0.01) higher contents of the elements showing
content of sFe (64% of the variance), organic matter (14%) and F/M negative loadings in Cp1 (Fe, Ti, Ca, Cr, Mn, and Ni), while the group
composition (12%) (Fig. 4, SI_Fig. 1). Iron in primary (mac) and of samples without amphibole (i.e. with felsic compositions) has
secondary minerals produces an increase in b* (yellowing) while signicantly higher contents of the elements with positive loadings
OM content decreases b* values. on Cp1 (Si, Al, K, Ga, Rb, Y, Nb, Zn and Pb). As for the colour pa-
As for the polar parameters, C*ab (chroma) shows the same rameters, the rst group has signicantly higher values for a*, b*
behaviour as b*: dependence on sFe (70% of the variance), F/M and C*ab, while the second group has signicantly higher values for
composition (12%) and OM (10%) (Fig. 4, SI_Fig. 1). Thus, chroma- hab. There was no signicant difference (p 0.60) in luminosity
ticity is increased by the presence of sFe and mac minerals and between the two groups.
decreased by OM content. While parameter hab, hue, is only Consequently, we decided to perform separate PCA analyses for
signicantly controlled (71% of the variance) by sFe phases. Hue samples with and without amphibole (in Fig. 5, a selection of ce-
decreases (i.e. increase in reddening) with increasing sFe content. ramics of these groups). The number of components extracted for
These results suggest that OM content is responsible for dark- each group, the basic geochemical associations sharing variance
ening (decrease in L*), decrease in b* and loss of chromaticity with the colour parameters, and the direction of the changes were
106  Lantes-Sua
O. rez et al. / Journal of Archaeological Science 54 (2015) 99e109

Fig. 5. Selection of pottery with amphibolic compositions (with chlorite [1] and without chlorite [2]) and non-amphibolic compositions (without chlorite [3]).

the same as in the PCA with all samples: one component ac- the same way, the effect of the OM content on b* and C*ab (13% and
counting for the sFe, another related to the OM, and another one 10% of their variance) is only detected for this group, while the
accounting for the relative abundance of F/M minerals (in Table 7 effect of the relative abundance of F/M minerals is mainly expressed
we report the loadings for the colour parameters). There was a in the group with amphibole, affecting b* (21% of the variance) and
small increase in the total explained variance (2% and 3% for sam- C*ab (17%). Since these two groups may represent two main
ples with and without amphibole respectively) and in the com- different sources of raw material, the results suggest that the
munality of a* (9%) and hab (11% and 18%). But most interesting are original colour of the clays also plays a role in the end colour of the
the changes in the relative weight of the factors. The effect of sFe on pottery. Luminosity and chromaticity of light coloured (non-
luminosity is now only found for the group without amphibole, amphibolic, i.e. felsic) pastes are more affected by OM and sFe
accounting for a much larger percentage (20%) of the L* variance. In content than dark coloured (amphibolic, i.e. mac) pastes. On the
other hand, the relative increase in mac minerals seems to have a
Table 7
more determinant effect on the chromaticity of already mac
Loadings of the colour parameters in the PCA analyses carried out separately in the pastes.
amphibolic and non-amphibolic samples. (sFe: secondary Fe, OM: organic matter; In studies on the colour of Neolithic pottery from Romania and
FeM: relative abundance of felsic/mac minerals). Loadings of the primary factors Bulgaria, Constantinescu et al. (2005) found that certain chemical
are in bold and those of the secondary factor are in italics.
elements such as Mn (in the form of jacobsite or pyrolusite) were
Amphibolic sFe OM FeM

L* 0.07 0.89 0.19


a* 0.95 0.02 0.25 Table 8
b* 0.82 0.11 0.46 Correlation between extractable Fe (FeDC) and CIELab colour parameters, and mul-
C*ab 0.87 0.07 0.41 tiple regression functions. (R: correlation coefcient of the multiple regression;
h ab 0.94 0.05 0.04 Error: error of the estimate).
Non-amphibolic
FeDC Regression function R Error
L* 0.45 0.84 0.02
a* 0.95 0.13 0.24 a* 0.60 1.27 FeDC e 0.69 F/M e 0.54 OM 0.87 0.7
b* 0.87 0.37 0.25 b* 0.61 1.22 FeDC e 0.54 F/M e 0.62 OM 0.82 0.6
C*ab 0.90 0.32 0.25 C*ab 0.62 1.26 FeDC e 0.59 F/M e 0.61 OM 0.83 0.6
h ab 0.90 0.13 0.08 h ab 0.41 1.01 FeDC 0.66 F/M 0.41 OM 0.65 0.8
 Lantes-Sua
O. rez et al. / Journal of Archaeological Science 54 (2015) 99e109 107

used in the composition of the colourings applied. In studies of contents have an important inuence on colour. However, there is a
carbonated soils, Viscarra Rossel et al. (2009) found that the lu- signicant difference between these two components: while
minosity of the samples was strongly correlated with calcite con- organic matter is burnt out during ring and it is the amount and
tent. In the pottery analysed in our study, we ruled out that these type of organic compounds (Kaal et al., 2014) which remain that
minerals played any important role in the colour. Our results are inuence the parameters of colour, the iron oxi-hydroxides content
more in line with the classical work by Shepard (1954), who sug- is not affected but the oxidizing/reducing conditions may have an
gested that iron and organic matter were, together with ring effect on reddening (Canti and Linford, 2000; Linares et al., 1983;
conditions, responsible for the colour. Maritan et al., 2006; Nodari et al., 2004). In fact, in some of the
To check the hypothesis that sFe phases play a signicant role on pottery we analysed, similar iron oxi-hydroxides contents corre-
the colour of the ceramics, a selection of half of the samples (42) spond to different a* (redness) values, which could be due to the re-
was extracted with Na-dithionite/citrate. The extracted Fe showed crystallisation of the hematite depending on oxidising conditions,
only a moderate correlation with colour parameters (a*, b*, Cab* and ring temperature, etc. Lantes-Sua rez et al. (2010) also proposed
hab) (Table 8), suggesting that although it is related to colour other that the ring process was controlled for certain types of decorated
properties/components may also have a signicant control. Using pottery, verifying that it had been red twice, once for the ceramic
stepwise multivariate regression analysis we found that the body and again to x a kaolin-based decoration.
reddening (a*) and chromaticity (Cab*) of the samples can be pre- Both, use and post-depositional processes (occurred after
dicted with high accuracy using sFe, F/M composition (Cp1 scores) burial) are also likely to inuence the colour of the ceramic creating
and OM content (Cp3 scores) (Table 8). If OM (Cp3) is eliminated some uncertainties into intentionality (as they would modify the
from the predicting variables, as expected, C is loaded into the orginal colour of a vessel). A few of the samples analysed showed
regression equation (data not shown). These results indicate that darkened areas most likely due to daily use of the vessel for cooking
the expression of colour in the ceramics increases with increasing purposes. But this did not affect the whole surface of the vessels.
extractable Fe and mac minerals (negative F/M scores) contents Regarding post-depositional changes, it is worth mentioning that
and is decreased by increasing OM contents. For almost all samples all samples recovered were buried in acidic, weakly to moderately
(35 out of 42) extractable Fe, F/M composition and OM explain developed soils, ruling out the precipitation of secondary carbon-
almost all the variation in a* and Cab* (R 0.94); but a few of them (7) ates (which may have produced lighter colours), although incor-
separate from the main trend although showing a similar slope and poration of soil organic matter and a certain degree of leaching of
also a highly signicant correlation (R 0.98), which may indicate the the more mobile elements (Ca, K, Mg) cannot be discarded. Kaal
inuence of another process (oxidation conditions, ring temper- et al. (2014) studied the molecular composition of the organic
ature, cooking time, etc) not represented by the analysed prop- matter of some of the samples analysed in our study, and found no
erties. No formal or stylistic feature seems to be related to these two evidence of a signicant incorporation of soil organic matter. And as
groups. for changes in the content of mobile elements, we were not able to
Our results are consistent with studies on soil colour. Azzali et al. detect a clear effect -but this issue may require a more detailed
(2011) found that yellowing (b*) was correlated with goethite and evaluation with a larger dataset and more information on the
reddening (a*) with hematite contents, while Gunal et al. (2008) geochemical soil environment for each pottery sherd.
found a good correlation between yellowing (b*) and the amount Our results indicate that composition has a dominant effect on
of Fe extracted with sodium dithoiniteecitrate. the colour of the samples, other factors (ring conditions, use and
post-depositional change) playing a minor role. The effect of sec-
3.5. Intentionality of the colour ondary iron phases on yellowing (positive) and reddening (nega-
tive) can be both a compositional and processing (i.e. ring
Our ndings suggest that there are differences in the colour of conditions) effect. In line with the results obtained by Azzali et al.
the pottery that would seem to depend on the initial colour of the (2011) for soils, increased yellowing may have been due to condi-
clays used to produce them. In pottery with felsic compositions, tions prone to goethite formation and not hematite. In any case, the
both the luminosity and chromaticity are more directly associated minor role apparently played by other factors than composition
with iron oxi-hydroxides and organic matter content, while the may also be due to the fact that we analysed bulk, powdered
chromaticity of the mac pottery mainly depends on the relative samples. This may have resulted in a minimization of, for example,
proportion of mac minerals. This would suggest that the raw the changes induced by processes that mostly affect the surface of
material could have been selected intentionally in order to obtain a the vessels (as use and post-depositional conditions).
specic vessel with a specic colour. Selection of raw materials is One nal question that still needs to be answered is which
also supported by the comparison of pottery composition to that of criteria predominated in the selection, control over the composi-
the available geological materials: for example, there is a notable tion of the clays and the ring process in order to improve the
absence of pottery with chlorite but without amphibole, when functionality of the pottery or the nal colour that was required.
there are numerous sources of these minerals in the study area Perhaps both aspects e its functionality and choice of colour e were
(Pablo Macia  et al., 1981). As proposed by Prieto Lamas et al. (2011), connected.
for the set of pottery samples we studied, the use of raw materials
varied depending on the context, style and shape. Prieto-Martnez 4. Conclusions
(1999, 2011) also proposed the intentional use of colour in pottery
recovered from megalithic tombs in north-western Spain, in which The aim of this study was to attempt to identify the composi-
red was preferred in comparison to the wide range of colours found tional factors that inuence the colour of prehistoric Bell Beaker
in pottery from domestic sites. For the Bell Beaker pottery with the pottery from north-western Spain, and to explore the underlying
most complex decoration a preferential use of felsic compositions intentionality in obtaining it. The majority of the pottery samples
was found, while the simple Bell Beakers and undecorated pottery had a low luminosity and was in the a*eb* quadrant ranging from
with the nest clays had mac compositions. red to yellow. The elemental and mineralogical composition was
The ring process was also a stage at which the prehistoric highly varied. Correlation between the elemental and mineralogical
potters could intentionally control the colour of the vessels. In this composition was modest, which may be due to the fact that the
study we found that iron oxi-hydroxides and organic matter mineralogy essentially reects the crystalline fraction, while the
108  Lantes-Sua
O. rez et al. / Journal of Archaeological Science 54 (2015) 99e109

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This article was funded through the project Ceramic Styles in exploratory case study from NW Spain. Archaeometry 56 (Suppl. 1), 187e207.
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