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Journal of Archaeological Science 44 (2014) 180e193

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Journal of Archaeological Science

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

Searching for consistencies in Châtelperronian pigment use

Laure Dayet a,*, Francesco d’Errico a,b, Renata Garcia-Moreno a

aCNRS UMR 5199 PACEA, Préhistoire, Paléoenvironnement, Patrimoine, Université de Bordeaux, CS 50023, 33615 Pessac, FrancebDepartment of Archaeology, History, Cultural Studies and Religion, University of Bergen, Norway

a r t i c l e i n f o

Article history:Received 17 December 2013Received in revised form29 January 2014Accepted 31 January 2014

Keywords:PaleolithicNeanderthalIron oxidesManganese oxidesPortable XRFm-XRDSEM-EDS

* Corresponding author. University of Bordeaux, Chistoire, Paléoenvironnement, Patrimoine, AvenueFrance. Tel.: þ33 540002840.

E-mail addresses: la.bouillot@gmail.com, l.dayet-b(L. Dayet).

http://dx.doi.org/10.1016/j.jas.2014.01.0320305-4403/� 2014 Elsevier Ltd. All rights reserved.

a b s t r a c t

Evidence supporting the hypothesis that Neanderthals developed cultural adaptations comparable tothose associated with the Upper Palaeolithic is controversial, and come from a handful of sites, mainlyattributed to the Châtelperronian. Pigments play a growing role in this debate. We present a criticalreview of available information on Châtelperronian pigment use, and submit pigment lumps from threeChâtelperronian sites, Roc-de-Combe (Lot), Le Basté, and Bidart (Pyrénées Atlantiques) to a microscopic,elemental and mineralogical analysis using multifocus optical microscopy, SEM-EDS, XRF, Raman, andmXRD techniques. The thirty-nine pigment lumps from Roc-de-Combe consist of a great variety of redand black iron and manganese oxide rich rocks, probably collected at close and relatively distant sources.A third of the pieces from Roc-de-Combe and one piece from Bidart and Le Basté bear percussion marksand facets produced by grinding. Our results demonstrate that a consistent use of pigments, interpretedas reflecting site function, occurs at sites located in the South-western area of the known distribution ofthe Châtelperronian. Considering that this area is distant from the location of the earliest Proto-Aurignacian and Early Aurignacian sites from Germany and Austria, and that available radiocarbondating indicate a chronological anteriority of Roc-de-Combe Châtelperronian, we argue that the hy-pothesis that Châtelperronian pigment use results from Neanderthal ‘acculturation’ is improbable.

� 2014 Elsevier Ltd. All rights reserved.

A key question in human evolution is when in prehistory humancultures similar to ours emerged and to what extent we share‘modern’ cultural traits and cognition with anatomically archaicpopulations such as Neanderthals. Intentional burials, personalornaments, abstract and depictional representations, complextechnology, and systematic use of pigment, which is the focus of thepresent work, are generally interpreted, although with nuances, ascultural behaviors reflecting ‘modern’ cognition. In Europe, most ofthe evidence supporting the hypothesis that Neanderthals devel-oped cultural adaptations comparable to those associated withlater Upper Paleolithic and historical high latitude hunter-gathererpopulations come from a handful of sites attributed to the Châ-telperronian and Uluzzian technocomplexes. Evaluation of thesignificance of this evidence is hampered by its rarity and by con-troversies surrounding the stratigraphic integrity and dating of keysites, the cultural attribution of specific archaeological finds, and

NRS-UMR 5199 PACEA, Pré-des Facultés, 33615 Pessac,

ouillot@pacea.u-bordeaux1.fr

the taxonomic affiliation of the human groups responsible for theaccumulations of the archaeological layers.

The association in the Châtelperronian levels of Grotte du Renne(Arcy-sur-Cure, Burgundy) of Neanderthal remains, a large numberof personal ornaments, bone toolse some of which are decoratede

, and pigments, has been interpreted as evidence for the accultur-ation of late Neanderthals by invading Aurignacian Moderns(Mellars, 1989, 2005; Hublin et al., 1996, 2012), independent in-vention by Neanderthals of Upper Paleolithic cultural features(d’Errico et al., 1998; Zilhão and d'Errico, 1999; Zilhão, 2007) orreworking of archaeological layers (White, 2001; Higham et al.,2010). Spatial analysis of key finds (Caron et al., 2011; Zilhãoet al., 2011) and new 14C dating (Hublin et al., 2012) contradictsthe hypothesis that major taphonomic admixture or post-depositional disturbance affected the Grotte du Renne strati-graphic integrity, as proposed by previous dating attempts (Highamet al., 2010), instead supporting the hypothesis that the makers ofthe Châtelperronian were Neanderthals. However, no consensusexists on the interpretation of this site. Some authors are reluctantin ascribing the ‘modern-like’ cultural traits recorded at Grotte duRenne to Neanderthals, arguing instead that the Châtelperronianmay have been made by modern humans (Higham et al., 2011a;Bar-Yosef and Bordes, 2010). Others use the new evidence to

Table 1Archaeological sites with Châtelperronian levels in which pigment lumps were found according to the literature.

Site Department Excavation, layer Attribution Description Quantity Processing Reference

Grotte du RenneArcy-sur-Cure

Yonne Leroi-Gourhan,layers X to VIII

Reliable Red, black and yellow,Fe and Mn oxides

>2000 Crushed Salomon et al., 2008;Caron et al., 2011Ground

Grotte du BisonArcy-sur-Cure

Yonne David, layer D Not enoughinformation

Red and yellow e No processing? David et al., 2005

Les Fées Allier Bailleau Uncertaina ‘Fe and Mn ores’ e e Bailleau, 1869Delporte, layer B0 Uncertaina Red e e Delporte et al., 1999;

This studyLes Cottés Vienne Soressi Reliable e e e Soressi, personal com.Grande Roche Quinçay Vienne Soressi Reliable e e e Soressi, personal com.Roche-à-Pierrot

Saint-CésaireCharente maritime Lévêque Not enough

informationcRed e e This study

Bos-del-Ser Corrèze Bouyssonie, single level Uncertaina Red e e Bouyssonie, 1923La Ferrassie Dordogne Peyrony, layer E Uncertainb Red and black e ‘Scraped’ Peyrony, 1934Roc-de-Combe Lot Bordes, layer 8 Reliable Red and black 36 e de Sonneville-Bordes, 2002Bidart Pyrénées Atlantique Chauchat, single level Reliable Red 1 e Chauchat, 1968Le Basté Pyrénées Atlantique Chauchat, level 3bmoy Reliable Red 3 e Chauchat, 1968Les Tambourets Haute-Garonne Laville, single level Reliable Red and yellow,

‘hematite and limonite’2 ‘Facetted’ Scandiuzzi, 2008

Labeko Koba Spain Arrizabalaga, level IX Reliable ‘Limonite’ 15 Knapped, scrapped? Rios Garaizar, 2008Aranbaltza Spain Savage excavation,

single level?Not enoughinformation

‘Ochre’ 1 ‘Used’ Rios-Garaizar et al., 2012

a Probable admixture of Châtelperronian and Aurignacian (Zilhão and d'Errico,1999; Zilhão et al., 2006).b Probable admixture of Châtelperronian and Mousterian deposits (Texier, 2009).c Châtelperronian level contains Mousterian tools (Soressi, 2011).

Fig. 1. Location of sites where pigment lumps have been reported in Châtelperronian layers.

L. Dayet et al. / Journal of Archaeological Science 44 (2014) 180e193 181

Fig. 2. Châtelperronian black (RDC6 and 10) and red (RDC13-15, 26, 30) pigment lumps from Roc-de-Combe, and red pigment lumps from Bidart and Le Basté (BST1). (Forinterpretation of the references to colour in this figure legend, the reader is referred to the web version of this article.)

Fig. 3. Large block of Châtelperronian red pigment from Roc-de-Combe (RDC35) composed of 17 refitted fragments and bearing evidence of abrasion. (For interpretation of thereferences to colour in this figure legend, the reader is referred to the web version of this article.)

L. Dayet et al. / Journal of Archaeological Science 44 (2014) 180e193182

Table 2Contextual data and description of the black and red pigment lumps from Roc-de-Combe (Lot).

N� Context Macroscopic exam

Layer Square Hue Length (cm) Width (cm) Thick. (cm) Weight (g) Description

RDC1 C8 Und. Black, yellow 3.4 1.8 1.2 7 FragmentRDC2 C8 K 9 Black 2.8 2.5 1.5 11 Nodule fragmentRDC3 C8 K 9 Black, yellow 2.9 2.6 2.5 16 Nodule fragmentRDC4 C8 K 9 Black 2.7 1.6 0.9 6 Nodule fragmentRDC5 C8 Und. Black 2.1 2.0 1.0 2 FragmentRDC6 C8 J 9 Black, brun 1.8 1.5 0.9 3 Nodule fragmentRDC7 C8 Und. Anthracite 1.8 1.5 0.8 3 FragmentRDC8 C8 K 9 Anthracite 1.3 1.1 0.7 1 FragmentRDC9 C8 K 9 Black 3.2 2.0 1.5 13 Nodule fragmentRDC10 C8 J 9 Dark brown, yellow 3.8 2.3 1.8 18 Nodule fragmentRDC11 C8 Und. Red purple 0.9 0.6 0.4 0 FragmentRDC12 C8 I 10 Red purple 5.6 3.6 3.5 131 Large pebble fragmentRDC13 C8 K 9 Orange, Red 4.0 2.6 1.9 25 Small pebbleRDC14 C8 K 9 Yellow, Red 4.9 2.6 1.8 28 PebbleRDC15 C8 K 9 Red purple 4.4 2.9 2.3 19 FragmentRDC16 C8 J 9 Red 2.0 1.9 0.9 4 FragmentRDC17 C8 I 10 Red purple 1.9 0.9 0.9 2 FragmentRDC18 C8 H 10 Red purple 1.1 0.9 0.8 1 FragmentRDC19 C8 H 10 Red purple 2.2 1.9 0.8 3 FragmentRDC20 C8 G 10 Red purple 2.8 2.5 0.3 4 FragmentRDC21 C8 G 10 Red purple 2.6 2.2 0.2 2 FragmentRDC22 C8 H 10 Red 1.3 1.1 0.5 1 FragmentRDC23 C8 H 10 Red purple 3.1 1.9 1.0 9 FragmentRDC24 C8 I 9 Red purple 2.9 2.0 1.4 12 NoduleRDC25 C8 I 10 Red, red purple, yellow 2.7 1.5 0.9 4 Nodule fragmentRDC26 C8 J 9 Red purple 2.7 2.1 1.2 6 FragmentRDC27 C8 J 9 Red purple 1.7 1.4 0.4 1 Cortical flakeRDC28 C8 J 9 Red 1.6 1.5 0.6 2 FragmentRDC29 C8 K 9 Red, red purple 3.7 2.1 1.5 16 FragmentRDC30 C8 K 9 Red purple 3.4 2.2 1.9 15 FragmentRDC31 C8 K 9 Red purple 4.2 2.3 2.0 29 Pebble fragmentRDC32 C8 K 9 Red, red purple 3.5 2.0 0.6 6 FragmentRDC33 C8 K 9 Red purple 3.2 1.9 1.7 14 Pebble fragmentRDC34 C8 H 9 Red, red purple, yellow 4.0 3.5 1.4 18 NoduleRDC35 C8 J 9 Red, yellow surface 9.9 6.7 6.7 580 Fragmented block

L. Dayet et al. / Journal of Archaeological Science 44 (2014) 180e193 183

suggest contemporaneity between Châtelperronian Neanderthalsin France and the Early Aurignacian moderns in Central Europe,which reinforces, in their view, the acculturation scenario (Hublinet al., 2012; Talamo et al., 2012; Higham et al., 2011). Others relyon the same evidence to argue in favor of a precedence of theChâtelperronian over the Proto- and Early Aurignacian, supportingthe scenario of an independent invention of UP innovations byNeanderthals (Caron et al., 2011; Zilhão, 2013; Banks et al., 2013a).

Long considered as a pillar supporting the idea that Neander-thals were the makers of the Châtelperronian technocomplex, thepresence of a Neanderthal partial skeleton, interpreted as a sec-ondary burial, in the Châtelperronian layers of the Roche-à-Pierrot,at St.-Césaire, has been recently called into question (Bar-Yosef andBordes, 2010; Bordes and Teyssandier, 2012; Soressi, 2011). Nodetailed description of the stratigraphy at the location where thepurported burial was found is available, and the associated lithicassemblage includes a large proportion of Middle Palaeolithic toolsopening the possibility of a Mousterian burial disturbed by Châ-telperronian occupations. Although reappraisal of the stratigraphicevidence (Zilhão, 2013) and recent direct radiocarbon dating of theskeleton (Hublin et al., 2012) supports its attribution to the

Table 3Contextual data and description of the red pigment lumps from Bidart and Le Baste (Bas

N� Context Macroscopic exam

Layer Square Hue Width

BIDART Und. Red purple, yellow 3.7BST1 3bm F5 Red purple, yellow 2.3BST2 3bm G4 Red purple 1.4BST3 3bsup S3 Red, red purple, yellow 2.1

Châtelperronian rather than the Mousterian, this contention relieson a single 14C determination andmay be contradicted in the futureby ongoing research (Bordes and Teyssandier, 2012).

The above examples illustrate how difficult it is to reach definiteconclusions from few sites. Paucity of meaningful associations re-inforces ambiguities inherent to the interpretation of Paleolithicsequences and jeopardizes attempts to identify consistencies lead-ing to a commonly accepted scenario. One research strategy topartially overcome this problem is to enlarge the sample of thestudied sites and conductmore in-depth analysis in each category ofthe material culture. This may allow to either corroborate or inval-idate inferences fromexcavations conducted atmain sequences andto search for temporal and spatial patterns that would remaininvisible if research remained focused only on a handful of sites.Applicationof this strategy to the lithic analysis of threeundescribedChâtelperronian assemblages has recently led Bachellerie (2011)and Roussel (2013) to propose that the Châtelperronian lithic tech-nology represents a distinct cultural adaptation with no obviouslinks with preceding Mousterian and following Aurignacian tech-nologies. Detailed analysis of bone tools from three Uluzzian siteshas identified consistencies in the choice of the species and the type

que coast).

(mm) Thick. (mm) Weight (g) Description/type of piece

2.6 62 Pebble fragment1.2 6 Pebble fragment1.4 18 Nodule fragment1.2 9 Nodule

L. Dayet et al. / Journal of Archaeological Science 44 (2014) 180e193184

of bone used, blank production, technique of manufacture, andresharpening, as well as significant differences between sites in thesize of the bone awls’ tips (d’Errico et al., 2012).

This approach has been scarcely applied to the cultural compo-nents that many would consider more relevant for the debate on theemergence of modern culture. Although understandable for materialculture categories rarely found at Châtelperronian and Uluzzian sitessuch as personal ornaments, lack of research ismore surprising in thecase of pigments, documented at a number of sites and playing agrowing role in thedebateon theemergenceof ‘modernity’. In the lastdecade many have associated the use of pigmental material to sym-bolically mediated behaviors (McBrearty and Brooks, 2000; d’Errico,2003; Henshilwood and Marean, 2003; Hovers et al., 2003; Zilhão,2006; d’Errico and Stringer, 2011). Others have inferred behavioralcomplexity from the use of pigment as a loading agent to produceadhesives for hafting (Wadley et al., 2009). In comparisonwith whathas been done elsewhere, instances of pigment use at

Table 4Description of the raw materials and modifications observed on the pigment lumps from

N� ‘Geology’ XRF XRD

Rock texture Rock structure Porosity Main elementsa

RDC1 Sand Massive Porous Ca, Mn, Ba, P Romanecquartz (g

RDC2 Clay-Sand Massive Compact Mn, Si, Ba PyrolusitRDC3 Clay-Sand Massive Compact Mn, Fe, Si (Ba) Pyrolusit

kaoliniteRDC4 Clay-Sand Massive Compact Mn, Si, Ba (Fe) PyrolusitRDC5 Clay-Sand Massive Porous Ca, Mn, Ba, P HydroxyRDC6 Clay-Sand Massive Compact Mn, Si (Ba, Fe) Pyrolusit

quartz (RRDC7 Clay Massive Compact Mn, Ba PyrolusitRDC8 Clay Massive Compact Mn, Ba e

RDC9 Sand Granular Compact Si, Mn, Ba (Fe) PyrolusitRDC10 Sand Granular Compact Mn, Fe, Si (Ba) Pyrolusit

RDC11 Sand Granular Compact Si, Fe e

RDC12 Sand Granular Compact Si, Fe HématiteRDC13 Silt Massive Compact Fe, Si (Ca) Illite/mic

hematiteRDC14 Clay-Sand Massive Compact Si, Fe Goethite

quartz, kRDC15 Clay-Sand Massive, granular Porous Fe, Si HematiteRDC16 Clay Massive Compact Fe, Si HematiteRDC17 Sand Granular Porous Si, Fe HematiteRDC18 Sand Granular Compact Si, Fe e

RDC19 Sand Lightly laminated,Granular

Compact Si, Fe Hematite

RDC20 Clay Lightly laminated Compact Fe, Si HematiteRDC21 Clay Lightly laminated Compact Fe, Si e

RDC22 Clay Massive Some pores Fe, Si e

RDC23 Sand Lightly laminated,Granular

Some pores Si, Fe Quartz, hkaolinite

RDC24 Silt Massive Compact Si, Fe HematiteRDC25 Clay Massive Compact Fe, Si Hematite

kaoliniteRDC26 Clay Massive Compact Fe, Si GoethiteRDC27 Clay Massive Compact Fe, Si HematiteRDC28 Clay Lightly laminated Compact Fe, Si HematiteRDC29 Sand Granular Compact Si, Fe Hematite

hydroxyaRDC30 Clay-Sand Massive Compact Fe, Si GoethiteRDC31 Sand Granular Compact Si, Fe e

RDC32 Sand Granular Compact Si, Fe Goethitekaolinite

RDC33 Sand Granular Compact Si, Fe Quartz, hRDC34 Clay Massive, globular Some pores Fe (Si) HematiteRDC35 Clayesilt Massive Compact Si, Fe Hematite

Absence of evidence is symbolized by a ‘0’.a Na, Mg and Al cannot be detected with the instrument used.

Châtelperronian and Uluzzian sites have not been studied with theattention they deserve. The rich collection of mineral pigments fromthe Châtelperronian layers of Grotte duRenne is the only one that hasbeen submitted to an extensive study (Salomonet al., 2008; Salomon,2009; Caron et al., 2011), albeit conducted four decades after the endof the excavation. The large quantity of red and black pigmentrecovered at the Grotte du Renne may indicate that pigment use ismore intense anddiversified in theChâtelperronian than inprecedingMousterian facies, but this observation needs to be verified byenlarging the number of studied sites.

The aim of this work is to 1) critically examine the evidence forpigment use in the Châtelperronian, 2) analyse with an appropriateresearch strategy pigment materials from three Châtelperroniansites in order to document patterns of raw material selection,processing, and use, 3) search for behavioral consistencies, and 4)evaluate the significance of the results for scenarios attempting to

Roc-de-Combe.

Raman Technological study

Percussionmarks

Striations Nb facets

hite, calcite,oethite?)

Romanechite,calcite

Unlikely 0 0

e e Unlikely 0 0e, quartz, calcite,(goethite?)

e Present 0 0

e, goethite e Unlikely 0 0lapatite, quartz e Unlikely 0 0e, hematite,omanechite)

Romanéchite?,hematite

Unlikely Parallel 2

e e Unlikely 0 1 probablee Unlikely 0 0

e, goethite e Unlikely 0 0e (quartz) Goethite,

hematite0 0 0

e Unlikely 0 0, quartz e Present 0 0as, quartz,, kaolinie, calcite

e 0 Parallel 2 probables

, hematite,aolinite

e 0 Some, parallel 1, 1 probable

, quartz, goethite e Present Some, parallel 2, quartz, kaolinite e Present 0 2 probables, quartz (goethite) e Unlikely 0 0

e Unlikely 0 0, quartz e Unlikely 0 1 possible

, quartz, kaolinite e Unlikely 0 0e Unlikely 0 0e Present 0 0

ematite, calcite,, hydroxyapatite

e Present 0 0

, quartz e Unlikely 0 0, goethite, quartz, e Unlikely 0 0

, hematite, quartz e Present Parallel 4, quartz, kaolinite e Present 0 0, quartz, kaolinite e Unlikely 0 2 probables, quartz, kaolinite,patite

e Present 0 0

, hematite, quartz e Present 0 0e Present 0 0

, quartz, hematite, e Present 0 0

ematite, kaolinite e Present 0 0, goethite, quartz e 0 0 0, kaolinite, quartz e Unlikely Parallel 2

Fig. 4. Micro-X-ray diffraction spectra for two black (RDC1, RDC2) and two red coarse(RDC33) and fine grained (RDC34) Châtelperronian pigments lumps from Roc-de-Combe. The black lumps are composed of romanechite, pyrolusite, and smallamounts of iron oxides. The red lumps are composed of variable amounts of quartz,hematite and kaolinite in function of their texture. R: Romanechite; C: calcite; G:goethite; P: pyrolusite; H: hematite; Q: quartz; K: kaolinite.

L. Dayet et al. / Journal of Archaeological Science 44 (2014) 180e193 185

model Neanderthal cultural adaptations before and at the time ofModern Human expansion into Europe.

1. Châtelperronian pigment use: a review

Conventionally described as the earliest industry of the UpperPalaeolithic, the Châtelperronian derives its name from the site of la

Grotte des Fées, at Châtelperron, Allier, France. Châtelperronianlithic technology is characterized by the use of large flakes onwhicha crest is prepared as cores to produce medium size, triangular insection, laminar blanks (Pellegrin, 1995; Roussel, 2013). Theseblanks are retouched on one side to shape a diagnostic tool type,called Châtelperronian point or knife. Burins, end-scrapers, anddenticulate, often produced on blanks resulting from the prepara-tion of these cores, are also part of the Châtelperronian tool kits. Amicrolaminar component, recorded at the single site of Quinçay(Roussel, 2011, 2013), corresponds to the final stage of the samereduction sequence. The distribution of the ninety-two caves andopen-air sites that yielded Châtelperronian’s diagnostic toolscovers central and south western France and extends into NorthernSpain (Pelegrin and Soressi, 2007; Bachellerie, 2011; Roussel, 2011).Based on the critical revision of the few sequences that would havefeatured interstratifications of Aurignacian and Châtelperronianlayers (Bordes, 2002, 2003), a consensus exists on the fact thateverywhere across its known geographic range the Châtelperro-nian stratigraphically underlies the Proto-Aurignacian and overlieslate Mousterian facies such as the Denticulate and the Mousterianof Acheulean tradition. Reliable 14C ages for the Châtelperronian fallin between 45 ka cal BP and 42 ka cal BP (Higham et al., 2010; Zilhãoet al., 2011; Hublin et al., 2012).

Mining of published and gray literature conducted in theframework of this study reveals that at least fourteen Châ-telperronian sites, i.e. an eighth of the total number of sites re-ported for this technocomplex, have yielded possible evidence forpigment use, mostly in the form of lumps of mineral pigments(Table 1; Fig. 1). At three of these sites, excavated long ago, layerswere shown to be reworked, which makes the attribution of thepigment lumps to the Châtelperronian uncertain. At Saint-Césaire,our preliminary analysis of the collections from Lévêque excavationhas identified possible pigment lumps in the Châtelperronian layerEjop sup. However, the presence in this layer of Mousterian diag-nostic tools (Soressi, 2011), calls into question the cultural attri-bution of the pigment lumps. At the Grotte-du-Bison, recovered redlumps are interpreted as natural fall of iron oxide concretions fromthe roof (David et al., 2005).

In the reminder of the cases the anthropogenic origin of thepigments and their attribution to the Châtelperronian can beconsidered reliable. However, it should be noted that pigmentlumps are mentioned in excavation reports or studies on lithicassemblages and have not been submitted to any in-depthanalysis. The most reliable contexts include the open-air sitesof Bidart (Chauchat, 1968; Bachellerie, 2011) and Les Tambourets(Bricker and Laville, 1977) where lumps of pigments wererecovered in uniquely Châtelperronian cultural horizons with noMousterian or Upper Palaeolithic levels. The use of pigment inthe Châtelperronian is further demonstrated by its discovery atthe recently excavated site of Labeko Koba, Spain (Rios Garaizar,2008). The discovery of pigment lumps in the Châtelperronianlayers of the Roc-de-Combe sequence, one of the few sites thatpresumably featured an Aurignacian-Châtelperronian interstrat-ification, is mentioned in the original Bordes and Labrot (1967)publication. Reassessment of the site formation process basedon vertical distribution of diagnostic artefacts and refitting hasled Bordes (2003) to convincingly refute the hypothesis that suchan interstratification existed outside the cave entrance. Thisstudy has, however, also shown that the stratigraphic sequenceinside the cave, and in particular Châtelperronian layer 8 in band9 from where most of the pigment analysed in the present studycomes from, has suffered no detectable post-depositionaldisturbance. This level has been recently dated to between39,540 � 970 14C BP (Gif-101264) and 45,100 � 2100 14C BP (Gif-101265) (Zilhão et al., 2006).

Fig. 5. Flake removals on three pigment lumps from Roc-de-Combe. Impact points are identified by black arrows. RDC12 presents contiguous removals produced by using a naturalflat surface as a striking platform.

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Comparable taphonomic analysis conducted at the site of LeBasté (Bachellerie, 2011), which has also yielded lumps of pigment,has identified an undisturbed Châtelperronian level (3bmoy).Pigment lumps were recovered during recent excavations in theChâtelperronian layers at Quinçay and Les Cottés (Soressi, personalcommunication) but no information is yet available on thismaterial.

The only collection of Châtelperronian pigments submitted to avariety of analyses is that recovered by Leroi-Gourhan at the Grottedu Renne in the Yonne region of France (Couraud, 1991; Salomon,2009; Caron et al., 2011). Pigment processing tools and about 18 kgof red, black and yellow pigment lumps come from the three layers(VIII, IX, X) attributed to this technocomplex. This material hasrecently played a role in the debate on the stratigraphic integrity ofthe site. Caron et al. (2011) have argued against the hypothesis of areworking of the layers and incorporation of pigment, personal or-naments and bone tools by percolation from the Proto-Aurignacianlayer VII by noticing that the Châtelperronian layers have yielded 36times more pigment than the Proto-Aurignacian. In addition, theyhave pointed out that, contrary to what one could expect under thepercolation scenario, pigmentmass andnumber gradually increasesfrom the top to the bottomof the Châtelperronian layers and 14.6 kgof pigment were found in the lowermost Châtelperronian level X.Analysis of the lumps of mineral pigments shows that black pig-ments contain diverse manganese oxides, the most frequent beingpyrolusite and, to a lesser degree, manganite, romanechite, andhollandite. Redpigments consist of three categoriesof hematite-richrocks associated to different proportions of calcite, quartz, kaolinite,and goethite (Salomon et al., 2008). Petrographic and PIXE analysisreveal that black pigments are remarkably homogeneous in theircomposition and could come from a single, still unidentified, source(Salomon, 2009; Beck et al., 2012). The composition of the red pig-ments is more variable and suggests collection from at least threedifferent geological iron-enriched formations, each outcroppingwithin 10 km from the site. Technological analysis suggests that thelumps were pounded and in some cases ground on lower grind-stones, which led to the formation of characteristic facets (Salomonet al., 2008; Salomon, 2009).

These results are valuable, but considering their uniqueness,they cannot be used to draw general conclusions on pigment use in

the Châtelperronian. In order to fill this gap, in this study weanalyze lumps of pigments recovered at three sites from the South-West of France featuring undisturbed Châtelperronian layers: Roc-de-Combe, Le Basté and Bidart.

2. Material and methods

The material from Roc-de-Combe is currently curated at theMusée National de la Préhistoire, Les Eyzies-de-Tayac, France.Pieces identified as pigmental material during Bordes and Labrotexcavation consist of 34 individual lumps of red and black pigmentand 68 additional fragments originally forming a single block(Figs. 2 and 3; Table 2). All pigment lumps were recovered in thearea inside the cave (squares I to K) or close to the drip line (squareH) where the Châtelperronian layer 8 presents, according to therecent taphonomic analysis of the sequence (Bordes, 2003), no orminimal indication of stratigraphic disturbance. Table 2 providesinformation on the stratigraphic and spatial provenance of theobjects. Le Basté and Bidart collections are curated at the Centre deConservation et d’Etude, Hasparren, Basque Region. At Le Bastéthree pigment lumps were discovered in Châtelperronian layer3bmoy (Table 3). A single piece was found at Bidart in the soleChâtelperronian level identified at this site (Table 3; Fig. 2).

The objects were examined with a Leica S8 APO stereomicro-scope to visually characterize the raw material and identify tracesof anthropogenic modification. The latter were photographed witha motorized Leica Z6 APOA, equipped with a DFC420 digital cameralinked to a LASMontage and LeicaMap DCM3D computer software.Morphology, hue, size, weight, texture (clay to silt: fine grained;sand: coarse grained), structure (granular, massive, laminated),degree of porosity, presence of cortex or patina, identifiablemineralparticles and fossils were systematically recorded. The identifica-tion of human modifications was based on criteria established bySalomon (2009), Hodgskiss (2010), Rifkin (2012), and Dayet et al.(2013). We recorded evidence of knapping and crushing (pointsof impact, flake scars, negative and positive bulbs) as well as surfacefeatures indicating grinding (number, location, and section of thefacets, orientation and type of striations).

Non-invasive chemical analyses were conducted on the surfaceof the pieces. They required no preparation or sampling. The

Fig. 6. Abrasion facets covered by parallel and sub-parallel striations on a black (RDC6) and three red lumps from Roc-de-Combe, and Bidart. The orientation of the striations isindicated by white arrows. (For interpretation of the references to colour in this figure legend, the reader is referred to the web version of this article.)

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analyses were systematically performed on the cleaner and flatterareas of each piece. Each of the 39 pieces from the three sites wasanalysed with a portable X-ray Fluorescence (pXRF) spectrometer,in order to estimate their elemental composition. Twenty-ninelumps were submitted to mineralogical analysis using a micro-beam X-ray Diffraction (mXRD). Complementary analyses byRaman Spectrometry and X-ray analyses coupled with observationunder a scanning electron microscope (SEM-EDS) were performedon four black pigments.

The XRF measurements were carried out using a portableSPECTRO xSORT X-ray fluorescence spectrometer from Ametek,equipped with a silicon drift detector (SDD) and a low power W X-ray tube with an excitation source of 40 kV. Measurements wereacquired in the air with a constant working distance by using a leadreceptacle to which the spectrometer is fixed. Light elements suchas Na, Mg, and Al are not detected with this technique. An area of8 mm in diameter was analysed. Spectra acquisition times were setto 60 s. The spectrometer is internally calibrated by an automated

Fig. 7. Close-up view of lump RDC26 showing percussion marks and abrasion facets shaping a point. A: close-up view indicating precedence of knapping over grinding. B: adjacentfacets covered by parallel striations blunting the tip.

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measure of the contents of a standard metal shutter. A DR-Nstandard was used to control the reproducibility of the measures.Because of the heterogeneous distribution of elements in Mn-richsamples and the presence of heavy elements such as Ba, reliablequantitative analysis of black pigments could be performed.Elemental analyses were also conducted with SEM-EDS in order toevaluate heterogeneity in elemental composition.

For red and red-yellow pigments, a second calibration wasoperated with the software X-labpro in order to improve accuracy.We develop a new and flexible calibration adapted to the highvariability in mineral composition of ferruginous rocks composingthe archaeological collections. Themass attenuation coefficient andcalibration slopes were adjusted for seven major and trace ele-ments by using height certified standards with variable content ofiron oxides (from 0.26 to 95% in Fe2O3), quartz, calcium carbonatesand clay minerals, as well as four references created in our pre-mises, in which iron is found only in the form of hematite, the mostabundant iron oxide found in archaeological pieces (SOM Table S1e3 and Fig. S0). The dedicated references were analysed by ICP-OES

Fig. 8. Left: proportion of ground lumps from Roc-de-Combe in function of iron content (afunction of iron content (above) and grain size (below).

for major elements, and ICP-MS for trace elements at the Serviced’Analyse des Roches et Minéraux (Nancy, France). The slopes of thefinal calibration curves fall at 1.0 and the R2 is systematically higherthan 0.95 for the seven elements studied. For the three mostabundant elements, Fe, Si and Ca, the relative differences betweenmeasured and theoretical values are lower than 10% when: Feconcentration is higher than 2%, Si concentration is higher than15%, and Ca concentration higher than 10%.

Results of semi-quantitative XRF analyses were used to exploretrends in geochemical composition that could help in identifyingprovenance, and to evaluate differences between modified andunmodified lumps. Principal component analysis of XRF values forfive major and trace elements (Si, Fe, Ca, Ti, V) was conducted withthe software STATISTICA by using the logarithm of the valuesweighted by the mean of all elements, i.e. the centred log ratio (clr)(Aitchison, 1986).

The SEM used is a FEI Quanta 20 from the BIC laboratory, Uni-versity of Bordeaux 2. Backscattered electron images (BSE) andelemental analyses were conducted under a high vacuum mode by

bove) and grain size (below); right: proportion of lumps showing percussion marks in

Fig. 9. Results of a PCA of the Centered logarithm ratio (clr) of the more frequentlydetected elements (SiO2, Fe2O3, CaO, TiO2, V2O3). Measurements on the same groundpiece are identified by complex hulls. A: weight of each element along Component 1and 3; B: Component 3 in function of component 1; C: Biplot of the Fe2O3 clr infunction of TiO2 clr.

L. Dayet et al. / Journal of Archaeological Science 44 (2014) 180e193 189

using accelerating voltage of 15 kV and 18 kV. BSE images werecollected with a SiLi detector and EDX analyses were made possibleby an SDD-EDAX detector.

Micro-XRD analyses were performed at the C2RMF, Palais duLouvre, Paris, on a dedicated laboratory-made device using aRigaku monochromatic source (l ¼ 1.54186 Ǻ) and a 200 mmcollimator. Themaximumvoltage and current were set at 45 kV anda 660 mA respectively. A 2D Rigaku imaging plate detector (R-AXISIVþþ) and a motorized X, Y, Z, 4 positioning system with an in-dependent q axis were used. Acquisition time was fixed to 3 min.The circular diffractograms were calibrated in 2q, and transformedinto linear ones through the software Fit2D v.12.077 developed byAndy Hammersley (ESRF, Grenoble, France). Data treatment wasdone with EVA� software (Bruker), and mineral phases wereidentified by using the ICDD� database (PDF2).

We used, in parallel, a Raman spectrometer coupled with amicroscope (SENTERRA Dispersive Raman Microscope, Bruker),with an internal calibration. The analyses were done with a532 nm laser and a maximum power of 15 mW to avoid trans-formation of the mineral phases. Acquisitions of 20e60 s andmultiple co-additions have been used. The working area wasobserved through the integrated color camera, and data werecollected with the software OPUS. The pigment lumps weredirectly set on the motorized microscope plate without any sam-pling or preparation.

3. Results

3.1. Roc-de-Combe

3.1.1. Black pigmentsThe 10 black lumps from Roc-de-Combe are all small concre-

tions or fragments of concretions with a maximum length of 4 cm.There is one refit between two fragments (RDC2 and 4). The blackpigments feature either a clay texture with fine particles, a sandtexture with coarse quartz grains, or a mixture of the two(Table 4). They are mainly composed of manganese oxides, themost abundant being pyrolusite (Fig. 4 and Fig. S1 to S10). Thepresence of barium indicates that mixed oxides, such as roma-nechite or oxides of the hollandite group, are present in variableproportion along with pyrolusite. Romanechite was identified insome lumps but not in all of those containing barium. It is wellknown that mixed oxides are difficult to identify by conventionalX-ray diffraction and Raman spectrometry (Ospitali et al., 2006;Lahlil et al., 2012). Iron is often detected in black lumps, and he-matite and goethite are present in at least five black lumps, theirpresence being correlated with the presence of red or yellowpatches on the objects. Two lumps show a different mineralcomposition, with significantly lower manganese content: one ismainly composed of calcite (RDC1), the other is rich in hydroxy-apatite (RDC5). They are black but they do not contain a sufficientamount of manganese oxides to be effectively used as pigments.The analysis of the geological map (1/50,000) of the area whereRoc-de-Combe is located (Municipality of Payrignac) does notreport outcrops or concretions of manganese oxides or manganese(Astruc, 1990).

A single black lump shows a point of impact and a flake scar thatmay indicate a reduction of the initial volume by percussion. Asmall piece displays two slightly convex facets covered by parallelsmoothed striations, indicating it was ground on a lower grind-stone (Fig. 6).

3.1.2. Red pigmentsA total of almost 1 kg (978 g) of red lumpswas recovered in layer

8 during the Bordes and Labrot excavation. A set of 68 fragments

Table 5Description of the raw materials and modifications observed on the pigment lumps from Bidart and Le Basté.

N� ‘Geology’ XRF XRD Raman Technological study

Rock texture Rock structure Porosity Main elementsa Percussion marks Striations Nb facets

BIDART ClayeSand Massive Compact Fe (Si) Hematite, goethite, quartz e Present Parallel 1BST1 Clay Massive Compact Si, Fe Quartz, hematite, goethite e Present 0 0BST2 Clay Lightly laminated Compact Si, Fe Hematite e Unlikely 0 1 probableBST3 Clay Lightly laminated Compact Fe (Si) Quartz, boehmite, kaolinite, hematite e 0 0 0

Absence of evidence is symbolized by a ‘0’.a Na, Mg and Al cannot be detected with the instrument used.

L. Dayet et al. / Journal of Archaeological Science 44 (2014) 180e193190

(RDC35) originating from a single block and including a refit ofseventeen pieces (580 g), accounts for the two thirds of the totalweight (626 g). Surfaces and edges of fragments from the interior ofthe block are less weathered than those from the outer surface,suggesting post-depositional fragmentation. Two other lumps(RDC20 and 21) found in the same square refit and bear similarfresh breaks.

3.1.2.1. Raw materials. Red lumps consist of granular sandy rocks ormassive clayish rocks (description in Table 4). The former aremainly composed of silicon and contain less than 50% of iron, whilethe latter show higher iron content. Calcium appears, with a fewexceptions, as a minor component (less than 5% in CaO). A singlepiece shows significant higher Ca content (RDC13), probablybecause of the presence of a thin calcitic deposit. Similar mineralphases are detected in coarse and fine grained materials, the dif-ference between them being mainly due to variations in minerals’proportions (Fig. 4 and Fig. S11 to 35). Hematite is systematicallypresent along with goethite in red-yellowish samples. They areassociated with quartz and, in some instances, with kaolinite.

Coarse grained materials are mostly composed of quartz grains,and they are identified as ferruginous sandstones (N ¼ 10). Fine-grained materials are mainly composed of iron oxide and containvariable amounts of clay minerals. Most of red lumps recovered atRoc-de-Combe showing a fine grained texture are massive, afeature suggesting that they could originate from iron crusts or finegrained ferruginised sedimentary rocks such as claystone. Theircrystallinity is too low to consider an hydrothermal origin.

Substantial sources of iron oxide are found 7 km from the site(Astruc, 1990). They consist of iron crusts of decametric size over-laying Oligocen sands. They are also described as ‘sandstones’because of the presence of quartz grains embedded in the ferru-ginous matrix. Our data on coarse grained lumps and lumps with amixture of coarse and fine grains match the mineralogical dataavailable for this formation, and are consistent with the fact thatiron crusts are generally heterogeneous in structure and texture(Ambrosi and Nahon, 1986; Milnes et al., 1987). Fine grained ironrich lumps could have come from this formation or any otherdismantled iron crust from the region.

3.1.2.2. Anthropogenic modifications. The red and red-yellowishlumps bear more traces of modification than the black lumps.One or several percussion impacts due to knapping or crushing arepresent on 12 out of 25 red pieces (Table 4; Fig. 5). The technique

Table 6Expected presence of pigment lumps and pigment processing tools at residentialand logistic Châtelperronian sites.

Residential sites Logistic sites

PigmentsQuantity High Low/no pigmentsColor Red and black Red?Variability High Low

Processing tools Presence Absence

used is difficult to identify due to the lack of features diagnostic of aparticular process such as, for instance, the opposite impact pointson a flake removal for crushing on an anvil, or clear positive andnegative single bulbs of percussion for knapping.

Evidence for grinding, in the form of flat or slightly convex facetscovered by fine parallel striations, are observed on four red and onered-yellowish lump (RDC13; 14; 15; 26; 35) (Fig. 6). The smoothedaspect of the lumps’ surfaces and ridges suggests, however, that thisnumber may represent an underestimation of the use of thistechnique. Most of the facetted pieces show 1 or 2 facets. They wereprobably ground on a lower grindstone to produce fine mineralpowder. After refitting, the larger piece (RDC35) shows two striatedfacets. This object represents, to the best of our knowledge, thelargest and heaviest lump of ground red pigment ever described inthe literature. One piece (RDC26) differs from the others in that itpresents flake scars and four small adjacent facets shaping a point(RDC26). Analysis of the ridge between the scar removal and theground facets indicate that the piece was first knapped and sub-sequently ground to create a pointed morphology (Fig. 7A). Tinyadjacent facets blunting the tip (Fig. 7B) likely result from the use ofthis object as a ‘crayon’ to mark a hard material with thin lines.

3.1.2.3. Raw material selection vs anthropogenic modifications.Interesting patterns appear when results on raw material prefer-ence and type of modification are contrasted (Fig. 8). Percussionmarks are mostly recognized on pieces with a ratio of iron oxide tosilica (Fe2O3/SiO2) lower than 0.5 or higher than 2, which corre-sponds respectively to normalized Fe2O3 weight concentrationslower than 30% (poor in iron oxide, rich in quartz) or higher than50% (richer in iron oxide than in quartz). Lumps with low ironcontent mostly consist of sandstone and along with lumps withhigh iron content they likely come from compact iron crusts. Theseare hard materials, suggesting that percussion may have beenpreferentially applied to harder rawmaterials. In contrast, abrasiontraces are only recorded on pieces containingmore than 30% of ironoxide and a ratio of iron oxide to silica higher than 0.5, indicatingthat grinding was preferentially applied to non-siliceous finegrained material. In addition, Principal Component Analysis of thecentred logarithm ratio of the five major, minor and trace elementsmore frequently detected in red lumps shows that ground piecespresent intermediate amounts of these elements in comparison tonon ground pieces. This is particularly clear when combiningComponent 1 and 3 (Total variance: 63%) (Fig. 9B). Titanium on theone hand, and iron and vanadium on the other, mostly contribute tothe variance of the axes (Fig. 9A and C). This pattern, which parallelsthe above mentioned siliceous versus ferruginous material pattern,may also reflect an intentional choice.

3.2. Le Basté and Bidart

The three red pigment lumps from Le Basté show a fine grainedtexture, compact or slightly stratified structures and variable ironoxide contents (Table 5). Sporadic outcrops of Senonian red marnsand Tryassic clayrocks present in the local area are possible sources

L. Dayet et al. / Journal of Archaeological Science 44 (2014) 180e193 191

for two lumps (Lamare, 1962; Burger et al., 1971). The presence ofaluminum oxy-hydroxide (bohemite, gAlOOH) in the last onestrongly suggests that it originates from bauxitic formations. Theclosest geological formations reported as ‘bauxitic’ are located25 km south to the site. The piece from Bidart is a fragment of anodule made of pure iron oxide with concentrations of quartzgrains. No comparable iron-rich pebbles, iron concretions ordismantled iron crusts are reported on the geological map coveringthe area.

Scant anthropogenic modifications were identified on Le Bastéand Bidart lumps: percussion impacts on a lump from Le Basté andthe lump from Bidart, and a ground facet on the latter (Fig. 6).

4. Discussion and conclusion

Our review of available evidence for Châtelperronian pigmentuse and results obtained in the framework of the present studyindicate that pigmental materials were regularly used at Châ-telperronian sites, and are not restricted to the Grotte du Renne.Pigments are not present at all Châtelperronian sites but, whenpresent, they show consistencies that need to be explored in orderto reach a better understanding of the role played by this rawmaterial in late Neanderthal cultural adaptations. Commonalities incolor preferences and processing techniques appear whencomparing the Grotte du Renne record with that of Roc-de-Combe,Bidart, and Le Basté. Within samples of relatively large size, weobserved that red pigments appear more commonly used thanblack ones, and that both crushing and grinding were applied inorder to produce pigment powder. A preference for local sources ofred pigments, well documented at Grotte du Renne (Salomon,2009), is suggested at the three sites that we have analysed byavailable information on the location of geological formationscontaining iron rich minerals, the texture of recovered pigmentlumps, and their elemental composition. Results obtained on thelatter, however, need to be refined in the future and complementedby the analysis of samples from local formations. Although theorigin of black pigment lumps is still unknown at Grotte du Renneand Roc-du-Combe, the relative scarcity of manganese sourcessuggests that they were collected, at both sites, at more distantoutcrops than red pigment.

Another striking feature highlighted by our analysis is thebroad variety of raw materials used at Roc-de-Combe to producepigmental material, including coarse and fine rocks characterizedby different hardness, hue, mineral phase composition, andextremely variable iron and manganese contents, for respec-tively, red and black pigments. Such diversity can be hardlyattributed to behavioral fickleness considering the fact thatcompositionally distinct fine grained materials were preferen-tially selected for producing fine pigment powder by grinding,while hard and coarse raw materials were preferentially pro-cessed by crushing. The identified pattern better fits the hy-pothesis that pigments of different color and composition wereinvolved in activities of different nature and purpose, possiblyincluding both functional and symbolic tasks (Table 6). Powderproduced by crushing coarse grained pigmental materials, char-acterized by a wide granulometric range, is an effective loadingagent (Wadley et al., 2009). Directly grinding fine grained pig-mental materials on a lower grindstone produces sorted finepowder (Salomon, 2009), more suitable for a use as pigment or ascovering agent. Identification of pigment residues on Châ-telperronian artefacts may help to test the hypothesis thatpigment was used in a variety of activities at Châtelperroniansites. At the Grotte-du-Renne, red residues have been reportedon at least two polished bone awls (d’Errico et al., 2003). Theresidues and associated wear pattern are interpreted as resulting

from contact between bone tools and tinted skins, which impliesthe use of a fine mineral powder as pigment or as a protectiveagent in hide treatment. No data on the presence of pigmentresidues on Châtelperronian stone tools are available.

The hypothesis that differences in composition and treatment ofpigment reflect different activities entails that they may also reflectdifferences in site function. Since at residential sites pigments arelikely to be involved in a more varied array of activities, we canexpect to find larger amount of pigments, both black and red, and ahigher variability in composition, color and texture. Pigment pro-cessing tools will be preferentially or exclusively found at thosesites. The Grotte-du-Renne and Roc-de-Combe records closelymatch this expectation. In contrast, logistic sites at which no orfewer domestic and symbolic activities were taking place, will becharacterized by the absence of, or very sporadic pigment use,eventual disposal of unsuitable rawmaterials, and accidental loss ofsmall quantities of good quality manuported pigment lumps. Bidartand the many e particularly open air e Châtelperronian sites atwhich no pigment was found, fall in this category. One of the mainfunctions of the former, the production of lithic blanks and Châ-telperronian points, may have been conducted in parallel to activ-ities requiring a reduced quantity of red iron-rich powder and nomanganese oxides. Lithics recovered at Le Basté indicate that,although several activities were carried out, human occupationswere not as intense as one may expect at a residential site(Bachellerie, 2011). The presence of only few pigments reflects thissituation.

Although the scenario highlighted above fits well the fourChâtelperronian sites for which data on pigment use are nowavailable, it needs to be tested in the future by enlarging the sampleof pigment collections studied, and applying to them the sameresearch strategy that we have adopted here. The interest of thisapproach lays in the fact that by combining information on rawmaterial provenance, texture, size, composition and treatment, andby contrasting results from different sites, one has better chances toelaborate realistic scenarios on the role played by pigment within atechnocomplex such as the Châtelperronian, and can better explorethe significance and implications of identified consistencies.

The first implication of the consistencies highlighted by ourresults is, as already mentioned above, that the 18 kg of black andred pigment lumps found in Châtelperronian levels VIII-X of Grottedu Renne cannot be considered anymore as an isolated occurrenceand interpreted as the result of the percolation of these objectsfrom the overlying Proto-Aurignacian level VII, as implied byHigham et al. (2010) and Mellars (2010). The inevitable corollary ofthis observation is that pigment use is an inherent feature of Châ-telperronian cultural adaptation.

A number of reasons contradict the idea that such a use shouldbe attributed to an ‘acculturation’ of indigenous Neanderthals bypurportedly contemporaneous Modern Human populations colo-nizing Europe from East to West as proposed by some authors(Hublin et al., 1996, 2012; Mellars, 1999).

’Acculturation’ is a term used in the anthropological literature toeither designate cultural interactions based on an ‘asymmetrical’relationship, where one can observe an “absorption by the accul-turated of cultural behaviors of the acculturators” (d’Errico et al.,1998: page S3) or a synonym of ‘cultural contact’ (see Cusick,1998; Stein, 2002 for a discussion). Interpreting the Châtelperro-nian as an instance of ‘acculturation’ implies, according to the firstdefinition, that the Châtelperronian entirely or partially resultsfrom contact with Proto- or Early-Aurignacian populations and thatno obvious impact of this process would be visible on the latter. Thesecond definition anticipates that, if cultural contact occurred, itaffected both populations with more or less visible effects on theirmaterial culture.

L. Dayet et al. / Journal of Archaeological Science 44 (2014) 180e193192

The obvious precondition for debating this issue is that a degreeof chronological overlap existed between the Châtelperronian, onthe one hand, and the Proto- or Early Aurignacian on the other.There is disagreement over the existence of such overlap. Châ-telperronian levels are systematically found below Proto-Aurignacian and Early Aurignacian levels (Zilhão and d’Errico,1999), and at sites where this occurs, as at those where it doesnot, 14C dating confirms the chronological precedence of the Châ-telperronian over the Aurignacian (Hublin et al., 2012). Bayesianmodeling of reliable 14C ages for the Pro-Aurignacian and the EarlyAurignacian confirms this pattern (Banks et al., 2013a,b). Someauthors contend that single instances of Early Aurignacian sitesolder than the Proto-Aurignacian and reflecting a precocious AMHcolonization of Europe prior or penecontemporaneous to the Châ-telperronian exist in Germany (Higham et al., 2012, 2013) andAustria (Nigst and Haesaerts, 2012). Others discard this evidence byobserving that the sites in question feature complex taphonomichistories (Banks et al., 2013b).

A precocious emergence of the Aurignacian in Central Europewould leave open the possibility, though, that significant culturalinteractions between late Neanderthals and early Aurignacianpopulations occurred and that, as a consequence, either theemergence of the Châtelperronian as a whole or particular as-pects of its material culture could result from Neanderthal directcontact with newly arrived AMH. A number of reasons contradictthe idea that Châtelperronian pigment use should be attributedto cultural exchange with early Aurignacian populations. First,there is consistent evidence that Neanderthal Mousterians usedpigment in Western Europe well before the emergence of theChâtelperronian and the arrival of AMH (Beyries and Walter,1996; Demars, 1992; Cârciumaru and Tutuianu-Cârciumaru,2009; Soressi and d’Errico, 2007; Zilhão et al., 2010; Roebroekset al., 2012). Recent discoveries not only confirm that Neander-thals used black, red and yellow pigment, but also show that thisuse could have been rather intense (Bodu et al., 2013). Second,the hypothesis that this cultural trait were borrowed from theneighboring Aurignacian by an already existing Châtelperronianwould imply that such traits spread from the East to the Westand that we should preferentially find them close to the pre-sumed area of contact. Such expectation is not matched byavailable data and our results on pigment use. The 14C ages ob-tained for the Châtelperronian levels of Roc-de-Combe that hasyielded the pigment lumps analysed in the present study, ob-tained at a site located at more than 700 km from the purportedarea of contact, are much older than the oldest 14C age obtainedfor Geïssenklosterle, the site considered by some authors as theearliest known instance of AMH presence in Europe (Highamet al., 2012).

Finally, the hypothesis of an asymmetrical cultural transfer re-quires the transmitted cultural trait to be an inherent feature of theacculturating culture. The archaeological record is in contradictionwith this expectation: evidence for pigment use is scant at Proto-Aurignacian sites from Eastern Europe, and the only evidence foundin the lower levels of Geissenklösterle consists of red spots referred toas ‘ochre’, observed in the sediment of level IIIA (Hahn, 1988).

All of this clearly goes against the hypothesis that Châtelperro-nian Neanderthals were submitted to an ‘asymmetrical accultura-tion by proximity’ and rather favors the hypothesis that pigmentuse represents, as with other elements of Châtelperronian materialculture, an original and independent aspect of this late Neanderthalcultural adaptation. Future research in this topic needs to increasethe number of Châtelperronian pigment collections analysed, andcontrast the results obtained with data, still scant, on pigment usein the Pro-Aurignacian, Early Aurignacian, and Mousterian faciespreceding the Châtelperronian.

Acknowledgment

The authors thank François Bachellerie for kindly sharing dataon Le Basté and Bidart, Marie Soressi for communicating informa-tion on the discovery of pigments at Les Cottés, William Banks andBrad Gravina for helpful discussions, and Ana BogdanMajkic for hercritical reading of the manuscript. We are grateful to FrançoisMirambet and the Centre de Recherche et de Restauration desMusées de France (Palais du Louvre, Paris) for XRD facilities. Thisresearch has been supported by a grant from the EuropeanResearch Council (FP7/2007/2013, TRACSYMBOLS 249587).

Appendix A. Supplementary data

Supplementary data related to this article can be found at http://dx.doi.org/10.1016/j.jas.2014.01.032.

References

Aitchison, J., 1986. The Statistical Analysis of Compositional Data. Monographs onStatistics and Applied Probability. Chapman & Hall Ltd, London (UK), p. 416.

Ambrosi, J.P., Nahon, D., 1986. Petrological and Geochemical differentiation ofla-teritic iron crust profiles. Chem. Geol. 57, 371e393.

Astruc, J.G., 1990. Notice explicative de la feuille géologique de Gourdon au 1/50000. BRGM, Orléans.

Bachellerie, F., 2011 (Thèse de doctorat). Quelle unité pour le Châtelperronien?Apport de l’analyse taphonomique et techno-économique des industries lith-iques de trois gisements aquitains de plein air : le Basté, Bidart (Pyrénées-Atlantiques) et Canaule II (Dordogne), vol. 1. Université Bordeaux, p. 439.

Bailleau, J.-G., 1869. Grotte des Fées de Chatelperron. Desrosiers, Moulins.Banks, W.E., d’Errico, F., Zilhão, J., 2013a. Human-climate interaction during the

Early Upper Paleolithic: testing the hypothesis of an adaptive shift between theProto-Aurignacian and the Early Aurignacian. J. Hum. Evol. 64, 39e55.

Banks, W.E., d’Errico, F., Zilhão, J., 2013b. Revisiting the chronology of the Proto-Aurignacian and the Early Aurignacian in Europe: a reply to Higham et al.’scomments on Banks, et al. (2013). J. of Human Evol. 65 (6), 810e817.

Bar-Yosef, O., Bordes, J.G., 2010. Who were the makers of the Châtelperronian cul-ture? J. Hum. Evol. 59, 586e593.

Beck, L., Salomon, H., Lahlil, S., Lebon, M., Odin, G.P., Coquinot, Y., Pichon, L., 2012.Non-destructive provenance differentiation of prehistoric pigments by externalPIXE. Nucl. Instrum. Methods Phys. Res. Sect. B Beam Interact. Mater. Atoms273, 173e177.

Beyries, S., Walter, P., 1996. Racloirs et colorants à Combe-Grenal. Le problème de laretouche Quina. In: Bietti, A., Grimaldi, S. (Eds.), Reduction Processess («Chaînes Opéra-toires ») for the European Mousterian, Rome, May 26e28 1995.QuaternariaNova 6, 167e185.

Bodu, P., Salomon, H., Leroyer, M., Naton, H.-G., Lacarriere, J., Dessoles, M., 2013. Anopen-air site from the recent Middle Palaeolithic in the Paris Basin (France): lesBossats at Ormesson (Seine-et-Marne). Quat. Int. Available online 28 October2013, 1e21.

Bordes, F., Labrot, J., 1967. La stratigraphie du gisement de Roc de Combe et sesimplications, vol. 64. Bulletin de la Société Préhistorique Française, Paris,pp. 15e28. Etudes et Travaux 1.

Bordes, J.-G., 2002. Les interstratifications Châtelperronien/Aurignacien du Roc-de-Combe et du Piage (Lot, France). Analyse taphonomique des industries lith-iques; implications archéologiques. Université Bordeaux I, p. 365.

Bordes, J.-G., 2003. Lithic taphonomy of the Chatelperronian/Aurignacian in-terstratifications in Roc de Combe and Le Piage (Lot, France). In: Zilhão, J.,d’Errico, F. (Eds.), The Chronology of the Aurignacian and of the TransitionalTechnocomplexes: Dating, Stratigraphies, Cultural Implications. Instituto Por-tuguês de Arqueologia, Lisbon, pp. 223e244.

Bordes, J.G., Teyssandier, N., 2012. The upper paleolithic nature of the Châ-telperronian in south-western France: archeostratigraphic and lithic evidence.Quat. Int. 246, 382e388.

Bouyssonie, J., 1923. Station préhistorique aurignacienne de Bos- del-Ser (Corrèze).In: Association Française pour l’Avancement des Sciences, pp. 617e622, 47esession.

Bricker, M., Laville, H., 1977. Le gisement Châtelperronien de plein air des Tam-bourets (commune de Couladère, Haute-Garonne). Bull. la Soc. Préhist. Fr. 74,505e517.

Burger, J.J., Bocherens, R., Endrey, G., Verdier, P., Richert, J.P., Arrents, C., Gros, H.,Lorsignol, S., Kieken, M., Thibault, C., 1971. Carte géoléologique de France (1/50000), feuille. Hasparren (1002). Notice explicative par Kieken M., Thibault.BRGM, Orléans.

Cârciumaru, M., Tutuianu-Cârciumaru, M., 2009. L’ocre et les récipients pour ocrede la grotte Cioarei. Ann. d’Univ. Valahia Targoviste e Sect. d’Archéologied’Histoire 11 (1), 7e19.

Caron, F., d’Errico, F., Del Moral, P., Santos, F., Zilhão, J., 2011. The reality of Neandertalsymbolic behavior at the Grotte du Renne, Arcy-sur-Cure. PLoS ONE 6, e21545.

L. Dayet et al. / Journal of Archaeological Science 44 (2014) 180e193 193

Chauchat, C., 1968 (Thèse de doctorat). Les industries préhistoriques de la région deBayonne, du Périgordien ancien à l’Asturien, vol. 2. Université de Bordeaux I.

Cusick, J., 1998. Historiography of acculturation: an evaluationof concepts and theirapplication in archaeology. In: Cusick, J. (Ed.), Studies in Culture Contact:Interaction, Culture Change, and Archaeology. Southern IllinoisUniversity, Car-bondale. Occasional Paper 25.

Couraud, C., 1991. Les pigments des grottes d’Arcy-sur-Cure (Yonne). Gall. Pré-histoire 33, 17e52.

d’Errico, F., 2003. The invisible frontier. A multiple species model for the origin ofbehavioral modernity. Evol. Anthropol. 12, 188e202.

d’Errico, F., Borgia, V., Ronchitelli, A., 2012. Uluzzian bone technology and its im-plications for the origin of behavioural modernity. Quat. Int. 259, 59e71.

d’Errico, F., Julien, M., Liolios, M., Vanhaeren, M., Baffier, D., 2003. Many awls in ourargument. Bone tool manufacture and use from the Chatelperronian andAurignacian layers of the Grotte du Renne at Arcy-sur-Cure. In: Zilhão, J.,d’Errico, F. (Eds.), The Chronology of the Aurignacian and of the TransitionalTechnocomplexes. Dating, Stratigraphies, Cultural Implications. Instituto Por-tugues de Arqueologia, Lisbon, pp. 247e270.

d’Errico, F., Zilhão, J., Baffier, D., Julien, M., Pelegrin, J., 1998. Neanderthal accultur-ation in western europe? A critical review of the evidence and its interpreta-tion. Curr. Anthropol. 39, S1eS44.

d’Errico, F., Stringer, C.B., 2011. Evolution, revolution or saltation scenario for the emer-gence of modern cultures? Philos. Trans. R. Soc. B: Biol. Sci. 366 (1567), 1060e1069.

David, F., Connet, N., Girard, M., Miskovsky, J.-Cl, Mourer-Chauvire, C., Roblin-Jouve, A., 2005. Les niveaux du Paléolithique supérieur de la grotte du Bison(Arcy-sur-Cure, Yonne) : couches A à D. Rev. Archéologique l’Est 54, 5e50.

Dayet, L., Texier, P.-J., Daniel, F., Porraz, G., 2013. The ochre resource in the middlestone age of Diepkloof rock Shelter (Western Cape, South Africa): procurement,processing and hypotheses of use. J. Archaeol. Sci. 40, 3492e3505.

Delporte, H., Surmely, F., Urgal, A., 1999. Châtelperron: Un grand gisement pré-historique de l’Allier. Conseil Gene de l’Allier, Moulins.

Demars, P.-Y., 1992. Les colorants dans le Moustérien du Périgord. L’apport desfouilles de F. Bordes. Bull. la Soc. préhistorique l’Ariège 47, 185e194.

de Sonneville-Bordes, D., 2002. Les industries du Roc-de-Combe (Lot) : Périgordienet Aurignacien. Préhistoire du sud-ouest 9 (2), 121e161.

Hahn, J., 1988. Die Geissenklösterle-Höhle im Achtal bei Blaubeuren I. Fundhorizontbildung und Besiedelung im Mittelpaläoli- thikum und im Aurignacien.

Henshilwood, C., Marean, C., 2003. The origin of modern human behavior:critique of the models and their test implications. Curr. Anthropol. 44 (5),627e651.

Higham, T., Basell, L., Jacobi, R.M., Wood, R., Bronk Ramsey, C., Conard, N.J., 2012.Testing models for the beginnings of the Aurignacian and the advent of figu-rative art and music: the radiocarbon chronology of Geißenklösterle. J. Hum.Evol. 62, 664e676.

Higham, T., Brock, F., Bronk Ramsey, C., Davies, W., Wood, R., Basell, L., 2011.Chronology of the site of Grotte du Renne, Arcy-sur-Cure, France: implicationsfor Neanderthal symbolic behaviour. Before Farming 2011/2.

Higham, T., Jacobi, R.M., Julien, M., David, F., Basell, L., Wood, R., Davies, W., BronkRamsey, C., 2010. Chronology of the Grotte du Renne (France) and implicationsfor the context of ornaments and human remains within the Châtelperronian.Proc. Natl. Acad. Sci. U. S. A. 107, 20234e20239.

Higham, T., Wood, R., Moreau, L., Conard, N., Ramsey, C.B., 2013. Comments on’Human-climate interaction during the early Upper Paleolithic: testing thehypothesis of an adaptive shift between the Proto-Aurignacian and the EarlyAurignacian’ by Banks et al. J. Hum. Evol. 65 (6), 806e809.

Hodgskiss, T., 2010. Identifying grinding, scoring and rubbing use-wear on exper-imental ochre pieces. J. Archaeol. Sci. 37 (12), 3344e3358.

Hovers, E., Shimon, I., Bar-Yosef, O., Vandermeersch, B., 2003. An early case of colorsymbolism: ochre use by modern humans in Qafzeh cave. Curr. Anthropol. 44(4), 491e522.

Hublin, J.-J., Spoor, F., Braun, M., Zonneveld, F., Condemi, S., 1996. A late Neanderthalassociated with Upper Palaeolithic artefacts. Nature 381, 224e226.

Hublin, J.-J., Talamo, S., Julien, M., David, F., Connet, N., Bodu, P., Vandermeersch, B.,Richards, M.P., 2012. Radiocarbon dates from the Grotte du Renne and Saint-Césaire support a Neandertal origin for the Châtelperronian. Proc. Natl. Acad.Sci. U. S. A. 109, 18743e18748.

Lahlil, S., Lebon, M., Beck, L., Rousselière, H., Vignaud, C., Reiche, I., Menu, M.,Paillet, P., Plassard, F., 2012. The first in situ micro-Raman spectroscopic analysisof prehistoric cave art of Rouffignac St-Cernin, France. J. Raman Spectrosc. 43,1637e1643.

Lamare, P., 1962. La feuille de Bayonne au 1/50 000. Son cadre morphologique et sescaractères géologiques. Bull. Serv. la Carte géol. 8, 411e459.

McBrearty, S., Brooks, A.S., 2000. The revolution that wasn’t: a new interpretation ofthe origin of modern human behavior. J. Hum. Evol. 39 (5), 453e563.

Mellars, P., 1989. Major issues in the emergence of modern humans. Curr.Anthropol. 30 (3), 349e385.

Mellars, P., 1999. The Neanderthal problem continued. Curr. Anthropol. 40 (3), 341e350.

Mellars, P., 2005. The impossible coincidence. A single-species model for the originsof modern human behavior in Europe. Evol. Anthropol. 14 (1), 12e27.

Mellars, P., 2010. Neanderthal symbolism and ornament manufacture: the burstingof a bubble? Proc. Natl. Acad. Sci. U. S. A. 107, 20147e20148.

Milnes, A.R., Bourman, R.P., Fitzpatrick, R.W., 1987. Petrology and mineralogy of’laterites’ in southern and eastern Australia and southern Africa. Chem. Geol. 60,237e250.

Nigst, R., Haesaerts, P., 2012. L’Aurignacien en Basse Autriche : résultats prélimin-aires de l’analyse technologique de la couche culturelle 3 de Willendorf II et sesimplications pour la chronologie du Paléolithique supérieur ancien en Europecentrale. L’anthropologie 116, 575e608.

Ospitali, F., Smith, D.C., Lorblanchet, M., 2006. Preliminary investigations by Ramanmicroscopy ofprehistoric pigments in the wall-painted cave at Roucadour,Quercy, France. J. Raman Spectrosc. 37, 1063e1071.

Pellegrin, J., 1995. Technologie lithique : le Châtelperronien de Roc-de-Combe (Lot)et de La Côte (Dordogne). Editions du CNRS, Paris.

Pelegrin, J., Soressi, M., 2007. Le Châtelperronien et ses rapports avec le Moustérien.In: Vandermeersch, B., Maureille, B. (Eds.), Les Néandertaliens, biologie et cul-tures. C.T.H.S, Paris, pp. 283e296. Documents préhistoriques 23.

Peyrony, D., 1934. La Ferrassie: Moustérien-Périgordien-Aurignacien. Préhistoire I,1e92.

Rifkin, R.F., 2012. Processing ochre in the Middle Stone Age: testing the inference ofprehistoric behaviours from actualistically derived experimental data.J. Anthropol. Archaeol. 31 (2), 174e195.

Rios Garaizar, J., 2008. Nivel IX (Chatelperroniense) de Labeko Koba : gestión de laindustria lítica y función del sitio. Munibe 59, 25e46.

Rios-Garaizar, J., Libano Silvente, I., Garate Maidagan, D., 2012. El yacimiento cha-telperroniense al aire libre de Aranbaltza (Barrika, Euskadi). Munibe 63, 81e92.

Roebroeks, W., Sier, M.J., Nielsen, T.K., De Loecker, D., Parés, J.M., Arps, C.E.S.,Mücher, H.J., 2012. Use of red ochre by early Neandertals. Proc. Natl. Acad. Sci. U.S. A. 109 (6), 1889e1894.

Roussel, M., 2011. Normes et variations de la production lithique durant le Châ-telperronien : la séquence de la Grande-Roche-de-la Plématrie à Quinçay(Vienne). Prehistory, University of Paris Ouest Nanterre e La Défense, p. 564(Doctoral thesis).

Roussel, M., 2013. Méthodes et rythmes du débitage laminaire au Châtelperronien:comparaison avec le Protoaurignacien (Blade production methods and patternsin the Châtelperronian: a comparison with the Protoaurignacian). ComptesRendus Palevol 12 (4), 233e241.

Salomon, H., 2009. Les matières colorantes au début du Paléolithique supérieur :sources, transformations et fonctions. Université de Bordeaux 1, Bordeaux(Thèse de Doctorat).

Salomon, H., Vignaud, C., Coquinot, Y., Pagès-Camagna, S., Pomiès, M.-P., Geneste, J.-M., Menu, M., Julien, M., David, F., 2008. Les matières colorantes au début duPaléolithique supérieur. In: Caractérisation chimique et structurale, trans-formation et valeur symbolique, pp. 17e23. Technè Hors-série.

Scandiuzzi, R., 2008. Les Tambourets: un gisement châtelperronien de plein air auseuil des Petites Pyrénées. Université Toulouse II, Toulouse (Mémoire demaster).

Soressi, M., 2011. Révision taphonomique et techno-typologique des deux ensem-bles attribués au Châtelperronien de la Roche-à-Pierrot à Saint-Césaire. L’an-thropologie 115, 569e584.

Soressi, M., d’Errico, F., 2007. Pigments, gravures, parures : les comportementssymboliques controversés des Néandertaliens. In: Vandermeersch, B.,Maureille, B. (Eds.), Les Néandertaliens, biologie et cultures. C.T.H.S., Paris,pp. 297e309. Documents préhistoriques.

Stein, G.J., 2002. From passive periphery to active agents: emerging perspectives inthe archaeology of inter-regional interaction. Am. Anthropol. 104, 903e916.

Talamo, S., Soressi, M., Roussel, M., Richards, M., Hublin, J.-J., 2012. A radiocarbonchronology for the complete Middle to Upper Palaeolithic transitional sequenceof Les Cottés (France). J. Archaeol. Sci. 39, 175e183.

Texier, J.-P., 2009. Histoire géologique de sites préhistoriques classiques du Périgord: une vision actualisée. In: La Micoque, la grotte Vaufrey, le Pech de l’Azé I et II,La Ferrassie, l’abri Castanet, le Flageolet, Laugerie Haute. Éditions du Comité destravaux historiques et scientifiques, Paris, p. 190.

Wadley, L., Hodgskiss, T., Grant, M., 2009. Implications for complex cognition fromthe hafting of tools with compound adhesives in the Middle Stone Age, SouthAfrica. Proc. Natl. Acad. Sci. U. S. A. 106 (24), 9590e9594.

White, R., 2001. Personal Ornaments from the Grotte du Renne at Arcy-sur-Cure.Athena Rev. 2, 41e46.

Zilhão, J., 2006. Neandertals and moderns mixed, and it matters. Evol. Anthropol.15, 183e195.

Zilhão, J., 2007. The emergence of ornaments and art: an archaeological perspectiveon the origins of behavioural “modernity”. J. Archaeol. Res. 15, 1e54.

Zilhão, J., 2013. Neandertal-modern human contact in Western Eurasia: issues ofdating, taxonomy, and cultural associations. In: Akazawa, T., Nishiaki, Y., Aoki, K.(Eds.), Dynamics of Learning in Eanderthals and Modern Humans: CulturalPerspectives. Springer Verlag, Japan, pp. 21e57.

Zilhão, J., Angelucci, D., Badal-García, E., d’Errico, F., Daniel, F., Dayet, L., Douka, K.,Higham, T., Martínez-Sánchez, M.J., Montes-Bernárdez, R., Murcia-Mascarós, S.,Pérez-Sirvent, C., Roldán-García, C., Vanhaeren, M., Villaverde, V., Wood, R.,Zapata, J., 2010. Symbolic Use of Marine Shells and Mineral pigments by IberianNeandertals. Proc. Natl. Acad. Sci. U. S. A. 107, 1023e1028.

Zilhão, J., d’Errico, F., 1999. The chronology and taphonomy of the earliest Auri-gnacian and its implications for the understanding of Neanderthal extinction.J. World Prehistory 13, 1e68.

Zilhão, J., d’Errico, F., Bordes, J.G., Lenoble, A., Texier, J.P., Rigaud, J.P., 2006. Analysisof Aurignacian interstratification at the Châtelperronian-type site and impli-cations for the behavioral modernity of Neandertals. Proc. Natl. Acad. Sci. U. S. A.103, 12643e12648.

Zilhão, J., d’Errico, F., Julien, M., David, F., 2011. Chronology of the site of Grotte duRenne, Arcy-sur-Cure, France: implications for radiocarbon dating. BeforeFarming 2011/3.