18
(This is a sample cover image for this issue. The actual cover is not yet available at this time.) This article appeared in a journal published by Elsevier. The attached copy is furnished to the author for internal non-commercial research and education use, including for instruction at the authors institution and sharing with colleagues. Other uses, including reproduction and distribution, or selling or licensing copies, or posting to personal, institutional or third party websites are prohibited. In most cases authors are permitted to post their version of the article (e.g. in Word or Tex form) to their personal website or institutional repository. Authors requiring further information regarding Elsevier’s archiving and manuscript policies are encouraged to visit: http://www.elsevier.com/copyright

Petro-mineralogy and geochemistry as tools of provenance analysis on archaeological pottery: study of Inka Period ceramics from Paria, Bolivia

  • Upload
    mta

  • View
    1

  • Download
    0

Embed Size (px)

Citation preview

(This is a sample cover image for this issue. The actual cover is not yet available at this time.)

This article appeared in a journal published by Elsevier. The attachedcopy is furnished to the author for internal non-commercial researchand education use, including for instruction at the authors institution

and sharing with colleagues.

Other uses, including reproduction and distribution, or selling orlicensing copies, or posting to personal, institutional or third party

websites are prohibited.

In most cases authors are permitted to post their version of thearticle (e.g. in Word or Tex form) to their personal website orinstitutional repository. Authors requiring further information

regarding Elsevier’s archiving and manuscript policies areencouraged to visit:

http://www.elsevier.com/copyright

Author's personal copy

Petro-mineralogy and geochemistry as tools of provenance analysis onarchaeological pottery: Study of Inka Period ceramics from Paria, Bolivia

V. Szilágyi a,f,*, J. Gyarmati b, M. Tóth c, H. Taubald d, M. Balla e, Zs. Kasztovszky a, Gy. Szakmány f

aDept. of Nuclear Research, Institute of Isotopes, Hungarian Academy of Sciences, 29-33 Konkoly-Thege Str., Budapest H-1121, HungarybMuseum of Ethnography, 12 Kossuth Sq., Budapest H-1055, Hungaryc Institute of Geochemical Research, Hungarian Academy of Sciences, 45 Budaörsi Str., Budapest H-1112, Hungaryd Isotope Geochemistry, University of Tübingen, 56 Wilhelmstr., Tübingen D-72074, Germanye Inst. of Nuclear Techniques, Budapest University of Technology and Economics, 9 M}uegyetem Rakpart, Budapest H-1111, HungaryfDept. of Petrology and Geochemistry, Institute of Geography and Earth Sciences, Eötvös Loránd University, 1/c Pázmány stny., Budapest H-1118, Hungary

a r t i c l e i n f o

Article history:Received 18 February 2011Accepted 15 November 2011

Keywords:PetrographyGeochemistryArchaeological applicationInka period potteryBolivia

a b s t r a c t

This paper summarized the results of comprehensive petro-mineralogical and geochemical (archeo-metrical) investigation of Inka Period ceramics excavated from Inka (A.D. 1438e1535) and Late Inter-mediate Period (A.D. 1000/1200e1438) sites of the Paria Basin (Dept. Oruro, Bolivia). Applying geologicalanalytical techniques we observed a complex and important archaeological subject of the region and theera, the cultural-economic influence of the conquering Inkas in the provincial region of Paria appearingin the ceramic material.

According to our results, continuity and changes of raw material utilization and pottery manufacturingtechniques from the Late Intermediate to the Inka Period are characterized by analytical methods. Thegeological field survey provided efficient basis for the identification of utilized raw material sources. Onthe one hand, ceramic supply of both eras proved to be based almost entirely on local and near rawmaterial sources. So, imperial handicraft applied local materials but with sophisticated imperial tech-niques in Paria. On the other hand, Inka Imperial and local-style vessels also show clear differences intheir material which suggests that sources and techniques functioned already in the Late IntermediatePeriod subsisted even after the Inka conquest of the Paria Basin. Based on our geological investigations,pottery supply system of the Paria region proved to be rather complex during the Inka Period.

� 2011 Elsevier Ltd. All rights reserved.

1. Introduction

Aspects of geology and archaeology are similar because bothinvestigate the limited and sporadic remnants of the past.Archaeological finds can be entirely natural materials (e.g. stonetools, building stones, bone artefacts) or artificial objects madewitha technique which can be modelled with natural geologicalprocesses (e.g. ceramics, metal objects, glass finds, textile).

On the one hand, pottery can be considered as a metasedi-mentary rock which is a result of an artificial technique: natural ornon-natural mixture of sediments which is metamorphosed by

a low pressure e high temperature (firing) process. Hence, classicalgeological investigations are powerful methods to characterize thematerials applied for ceramic making, to determine whether thesematerials could be natural or not, to establish the efficient fieldsurvey for potential rawmaterial sources and to model the possiblemixtures of the constituents. One the other hand, pottery is themost abundant find in the archaeological excavations and itsappearance (vessel shape, style) is highly influenced by thecultural-social changes. Thus, getting detailed information aboutthe raw materials and manufacturing techniques of such archaeo-logical artefacts can help to better understand the social processestaking place in a certain region and era. The application ofgeological methodology for answering archaeological questions isthe topic of the archaeometrical research.

In Inka Period (A.D. 1438e1535) archaeological excavationsfrom Ecuador to Chile there can be found an easily identifiableceramic style, the Inka Imperial which is manufactured with thequality of Cuzco Inka ware (Rowe, 1944). This type of pottery ischaracterized with the same quality and standard (concerning

* Corresponding author. Dept. of Nuclear Research, Institute of Isotopes,Hungarian Academy of Sciences, 29-33 Konkoly-Thege Str., Budapest H-1121,Hungary. Tel.: þ36 1 392 2222x3214, fax: þ36 1 392 2584.

E-mail addresses: [email protected] (V. Szilágyi), [email protected](J. Gyarmati), [email protected] (M. Tóth), [email protected](H. Taubald), [email protected] (M. Balla), [email protected](Gy. Szakmány).

Contents lists available at SciVerse ScienceDirect

Journal of South American Earth Sciences

journal homepage: www.elsevier .com/locate/ jsames

0895-9811/$ e see front matter � 2011 Elsevier Ltd. All rights reserved.doi:10.1016/j.jsames.2011.11.001

Journal of South American Earth Sciences 36 (2012) 1e17

Author's personal copy

shape and decoration) in every Inka site through the Empire. Thistype of archaeological finds is one of the examples of the Inkastandardizing intentions which can be traced in the whole Inkamaterial culture (e.g. architecture, metalworking or textiles). It isa principal question of the Inka archaeology how this standardi-zation took place in the colonized territories of the huge empire.Were these Inka Imperial style ceramics manufactured in somespecially controlled workshops (Morris, 1978; D’Altroy, 1992) or allover the empire by local potters who were taught to follow theimperial standards (Hayashida, 1998)? To answer these questionsa heterogeneous set of archaeological (ceramic, building materials)and comparative geological samples was investigated. Our aimwasto clarify three interconnected questions corresponding to theprincipal objective of the analysis: (1) whether the raw material ofthe ceramics belonging to the Inka style is similar to or differentfrom the raw material of Late Intermediate Period pottery, i.e. therawmaterial used for pottery making changed in the Inka Period orwere the same sources used as in the former period; (2) whetherthe Inka style ceramics of the Paria Basinwere made from local rawmaterial; (3) whether the material of the vessels representing InkaImperial and Inka local style is different.

The studies of ceramic collections from individual Inka periodsites similar to the research detailed in this paper are mainlyfocused on the coastal Peru region (Ixer and Lunt, 1991; Hayashida,1999; Hayashida et al., 2002, 2003a, b; Velde and Druc, 1999a;Costin, 2001) or northwest Argentina (Bertolino and Fabra, 2003;Ratto et al., 2002, 2004, 2005; Plá and Ratto, 2003). A compre-hensive study on special types of ritual ceramics from all aroundthe Empire was also published (Bray et al., 2005). Some isolatedresearches on Inka pottery are known from Ecuador (Jamieson andHancock, 2004) and Chile (Alden et al., 2006). However, the ceramicmanufacture of the Inka provincial region of the present Bolivia hasyet been investigated preliminary from archaeometrical point ofview (Williams et al., 2006).

This paper deals with the reconstruction of pottery manufactureof the Late Prehispanic Paria Basin of the Bolivian Altiplano inves-tigated by the Paria Archaeological Project (PAP) in 2004e2006.The archaeometrical investigation of pottery from Paria started in2004. Our preliminary results on petrographic observations andmineralogical analysis (Szilágyi et al., 2005, 2007; Szilágyi andSzakmány, 2009) provided a basis for the comprehensive study.The main goals of the here presented examinations are the petro-mineralogical and geochemical description of the ceramic arte-facts (to provide fundamental raw data on Inka period pottery fromBolivia), and the identification of their possible provenance andtechnological characteristics by taking comparative geologicalsamples into the investigation.

2. Background

2.1. Archaeological context

The Paria Basin is located approximately 200 km to the south-east of La Paz, Bolivia at an altitude of 3700e3800 metres abovem.s.l. The basin is situated at a strategically important geographicallocation on themargin of the Sierra de Azanaques. This range of themountainous Andes forms a natural separation between theimmense Altiplano and the more temperate valleys of Cochabambaand the eastern tropical foothills of the Andes. At this point, theParia Basin forms an ecological doorway between the differentzones and ecological levels. In this way, the territory played a vitalrole in the life of Andean ethnic groups and in the political economyof the Inka Empire, as was suggested in John Victor Murra’sinvestigations (1972, 1983).

The special role of the Paria Basin appears clearly in theethnohistoric sources (Vaca de Castro, 1908: 435) as the imperialInka road e which started from Cuzco and passed along thewestern side of Lake Titicacae bifurcated at the ancient site of Pariawith the main road heading towards Chile/Argentina and anotherbranch towards the Valley of Cochabamba (Gutiérrez Osinaga,2005) and further to Incallacta (Hyslop, 1984; Guaman Poma deAyala, 1980). At this intersection, the Inka state established anadministrative centre, one of the capitals of the provinces to thesouth from Cuzco (Fig. 1). According to Cieza de León (1973, 1985),there were great buildings (depositories and lodgings for the Inkaand the Temple of the Sun) to be constructed in the settlement.Other ethnohistorical accounts indicate that maize grown in theimperial state farms in the Valley of Cochabamba was transportedthrough ancient Paria (Repartimiento, 1977).

In this regard, the Paria Basin had a double function in the InkaPeriod. It formed the border between the different ecological levelsand e at the same time e acted as an intermediate zone in theredistribution network of the Inka Empire. The PAP studied theinterregional ecological relationships between the Andean Alti-plano and the temperate valleys, as well as the political andeconomic interactions that existed between the Inka imperialcentre and the peripheral zones. Until now, there are only unpub-lished project reports that discuss the archaeological records and

Fig. 1. Location of Paria site in the Inka Empire (map is modified after Gyarmati andVarga, 1999), the satellite picture (source: Google Earth, 2008), sketch of the Ce 1site and the view of structure BH (photo by J. Gyarmati).

V. Szilágyi et al. / Journal of South American Earth Sciences 36 (2012) 1e172

Author's personal copy

conclusions. Archaeological systematic surface survey extended toa 95.5 km2 part of the Paria Basin, and located 113 sites rangingfrom the Formative Period (B.C. 1000eA.D. 600) until the ColonialPeriod (A.D. 1535e1825). The most important and extendedarchaeological site of the basin is Paria, an Inka administrativecentre (its code is No.1 on the map). According to 14C dating ofcharcoal samples from one of the objects, the Inka conquest couldhappen at about 1400e1420. This date indicates an earlier occu-pation of the southern territory by Inkas than the classicalarchaeological interpretation. The ceramic sherds analyzed in thispaper originated from the surface collection of the identified sitesand the interior of a structure excavated at Paria in 2005.

2.2. Geological setting

The known geological history of the Paria Basin and itssurrounding started in the Palaeozoic. There are Palaeo-Mesozoicsiliciclastic sedimentary rocks (Ordovician-Devonian shales-siltstones-sandstones, Jurassic-Cretaceous sandstones) in the areaas products of flysch formation. Subsequently, PaleogeneeNeogeneclastic sedimentary and volcanic rocks (volcanites-pyroclastics andores connecting to subduction related Miocene effusive volcanicactivity) and finally Quaternary sediments (fluvial and lacustrineclay-silt-sand-gravel) were formed (GEOBOL, 1992, 1994).

From the point of view of our investigation, the most importantformations for possible rawmaterials of the pottery are the Silurianshales-siltstones-sandstones, the Miocene pyroclastics and vol-canites and those Quaternary clayey sediments which contain thefragments of the above mentioned rock types in large quantity orhave the apparently adequate physical properties (clay content-plasticity, grain size distribution) for pottery making.

In a proper sense, sediments of the Paria Basin have their directsource only from the Silurian siliciclastic sedimentary sequencesince this is the only material which can be eroded within 5 kmfrom the main archaeological site on the edges of the alluvial basin.The relatively monotonous sequence of the Silurian grey shales-siltstones-sandstones was subjected to a low grade meta-morphism (GEOBOL, 1992, 1994). In the field, the Silurian rocksform eroded ridges built of stratified (weakly folded) structures(Fig. 2). The thick, cyclical sequence (alternating finer and coarsergrained layers) forms a relatively homogeneous source for thealteration products.

The Miocene pyroclastics and volcanites connect with twomainstructures and activities.

The Morococala Volcanic Field is situated w15 km to the south-east from Paria and is in connection with the basin area throughrivers (it is at the upper course, near the beginning of the mainbranch of Jacha Uma river). The complex was formed during theMiocene (25e5 Ma ago) (Morgan et al., 1998) and resulted inwelded and non-welded rhyodacitic tuffs (ignimbrite) and lavaswhich form an extremely eroded plateau (Fig. 2).

The Soledad caldera is on the plain of the Altiplano, w30 km tothe west from Paria, the archaeological site. Its structure is a low-volume, nonresurgent “ash-flow”-type caldera (Redwood, 1987)which was formed during the Miocene (15e5 Ma ago). Theinterbedded, air-fall and non-welded ash-flow, dacitic tuffs anddacitic lavas build up the present remnants (rims) of the collapsedcaldera structure which rises above the plain of the Altiplano(Fig. 2). There is no permanent fluvial contact to the Paria Basinpresently. However, the Quaternary lacustrine environment couldpossibly connect the two areas when different sediments could bemixed.

The investigated Quaternary sediments are from the Paria Basin(with an erosional area of the Silurian sedimentary rocks and theMorococala Volcanic Field) and the surrounding of the Soledad

caldera. Their appearance is very heterogenous concerning theirgrain size, consolidation/cementation, porosity and fabric/struc-ture. However, their collective feature is that they are potentiallysuitable for pottery making either as paste (finer grained, clayeysediments) or as temper (coarser grained, silty-sandy sediments)raw materials (to favourably modify the physical properties of theplastic paste during shaping, drying and firing ceramics). All ofthem are related to former lacustrine, fluvial or recent eolianprocesses (GEOBOL, 1992, 1994). In the field, these formationsappear in variously incised valleys (Fig. 2) or seasonally water-flooded plain areas.

3. Methods

In order to describe and compare the archaeological andgeological samples, microscopic petrographic investigation (Dept.of Petrology and Geochemistry, Eötvös Loránd University of Buda-pest), X-ray powder diffraction analysis (Inst. of GeochemicalResearch, HAS, Budapest), instrumental neutron activation analysis(Inst. of Nuclear Techniques, Budapest University of Technology andEconomics), X-ray fluorescence geochemical analysis (Dept. ofGeochemistry, University of Tübingen) and prompt gamma acti-vation analysis (Dept. of Nuclear Research, Inst. of Isotopes, HAS,Budapest) were used.

Themicroscopic petrographic investigations were carried out ona Nikon ALPHAPHOT-2 polarizing microscope.

The mineral phase analyses were done on a Philips PW 1730diffractometer with a Bragg-Brentano alignment and graphitemonochromator (other parameters: CuKa radiation, 45 kV tension,35 mA intensity, 0.05e0.01� 2Q step size, 1 s time constant).

The chemical measurements provided concentrations for 11major and 29 trace elements. Since the element data detected withvarious methods have overlapped in the case of the differentsamples the most sensitive method was used for certain elementsin each case. The XRF and PGAA provided the major elementconcentrations (SiO2, TiO2, Al2O3, Fe2O3, MnO, MgO, CaO, Na2O,K2O, P2O5, H2O/LOI). Concerning the trace elements XRF resultswere applied for Rb, Sr, Ba, Zr, Nb, Y, V and Zn. For most of the othertrace elements the INAAmeasurements were used (Th, U, Hf, Ta, La,Ce, Nd, Sm, Eu, Yb, Lu, Sc, Cr, Co, As, Sb, Cs), while PGAA provided B,Cl and Gd concentrations. If one of the methods could not beapplied on a sample, the data were gained by the second mostsensitive measurement.

The INAA measurements were realized in the pool-type reactorof the Budapest University of Technology and Economics, Hungary.The samples were irradiated with a thermal neutron flux of2.4 � 1012 n cm�2s�1 for 8 h. Gamma-spectrometric measurementswere performed by an HPGe Well-type detector (resolution1.95 keV, relative efficiency 20.5%). For the evaluation of spectra,Sampo 90 software was used. Standardization was made by thesingle-comparator method (De Corte, 1987), using gold ascomparator. The thermal/epithermal flux-ratio was monitored byzirconium foils. The accuracy of the measurements was monitoredby analysing samples of the NBS SRM 1633a Coal Fly Ash StandardReference Material.

The XRF analyses were done with a wavelength dispersive X-rayfluorescence analyser (Bruker AXS S4 Pioneer X-ray spectrometer,Rh tube at 4 kW, Hahn-Weinheimer et al., 1984) on homogenizedfused beads with 1.5 g of dried (at 1050 �C over night) samplepowder mixed with 7.5 g of Li2B4O7. Loss on ignition was deter-mined at 1050 �C externally and is displayed as LOI. Analytical errorand detection limits vary and depend on element and samplecomposition. The samples were measured using an internal rockcalibration curve with 35 international standards, compiled inGovindarau (1989).

V. Szilágyi et al. / Journal of South American Earth Sciences 36 (2012) 1e17 3

Author's personal copy

The PGAA facility of the Budapest Neutron Centre is operated onan external cold neutron beam at the 10 MW Budapest ResearchReactor, Hungary (5�107 cm�2s�1

flux, for detailed description seeRévay and Belgya, 2004; Lindstrom and Révay, 2004; Révay et al.,2008). Gamma-ray spectra were measured using a calibratedHPGe detector (Belgya and Révay, 2004; Fazekas et al.,1999;Molnáret al., 2002). For the spectrum evaluation, the Hypermet PC soft-ware was used (Phillips and Marlow, 1976; Fazekas et al., 1997;Révay et al., 2001a, 2005). The quantitative analysis is based on

the k0 principle (Molnár et al., 1998). The element identificationwasperformed using the spectroscopic data libraries developed at theInstitute of Isotopes, HAS (Révay and Molnár, 2003; Révay et al.,2000, 2001b; Choi et al., 2007; Révay et al., 2004). The composi-tion was determined following the method described in Révay(2009), the uncertainties of the concentration values were deter-mined according to GUM (1993) and Révay (2006). Since thismethod is able to measure hydrogen, H2O content (which is notequal with LOI) of the samples could be calculated.

Fig. 2. Geological sketch of the Paria Basin and the eastern rim of the Altiplano with the caldera of Soledad. Stars mark the archaeological sites, while circles show the geologicalsampling points. Photos show the view of the main geographic units of the territory.

V. Szilágyi et al. / Journal of South American Earth Sciences 36 (2012) 1e174

Author's personal copy

4. Analyzed materials

In the framework of our research 206 ceramic fragments (144pieces from the excavation, 62 pieces collected from the surface), 8buildingmaterial remnants (4 adobes and 4 building stones) and 50comparative geological samples were investigated (Table 1).

4.1. Archaeological samples

The investigated archaeological finds derived from differentstages of the archaeological sampling work (field survey andexcavations). The sample set consists of 62 sherds collected at sitesfrom the Formative to the Inka period (Fig. 2), while the majority ofthe analyzed potsherds (144 pieces) were excavated from a struc-ture of Paria (site No.1).

The selected ceramic material belonged to the Inka Imperial,pre-Inka local and transitional styles (Fig. 3) (transitions amongstylistic groups are poorly observed, e.g. Bray, 2004). Inka Imperialceramics (Fig. 3a) are manufactured with the quality of Cuzco Inkaware (Rowe, 1944), which is of the same quality and standard(concerning shape and decoration) in the whole Empire. Inkapacaje ceramics (Fig. 3d), which are thought to be regional variantsof the Inka Imperial style, basically are bowls with special llamadecoration. Pre-Inka local style (Fig. 3c) means a vessel type of theLate Intermediate period (LIP, A.D. 1000/1200e1438) utilized alsoin the Inka period. Transitional styles (Inka local (Fig. 3b) andmixed(Fig. 3e) style) follow a fashion mixing the imperial and localcharacteristics concerning the form and decoration but theirquality never reach that of the Inka Imperial style. The assemblagealso contained some fragments of a special white ware whichshows regional rather than imperial characteristics. Classifying theexcavated ceramics according to the vessel forms, the major typesare the jars, bowls, plates, cooking pots and big dishes of coarsematerial, while there are only some fragments of pukus (straight-side bowls) and queros (ceremonial cups).

For the excavated Inka period structures, stone, dried andunfired brick (adobe) and clayey paste as plaster/daubwere utilizedas building materials. To sample the surely local materials used inthe Inka period, aside from ceramic fragments, four adobe samples(No. 4/3-6) were taken from an adobe structure and four fragmentsof building stones (No. 4/1-2, 4/7-8) from another structure.

4.2. Geological samples

Simultaneously with archaeological finds, 50 comparativesediments and hard rocks were also collected. Based on the abovepresented knowledge on the geological setting, the main targets ofthe sampling were the potential sources of the clay paste and silt-sand sized tempering component raw materials for the potterymaking process. These were the fine-grained alluvial sediments ofthe Paria Basin (22 samples: No. SED/01-04, No. 1/1-3, 2/1, 5/1-8, 7/1-2, 7/4-7) and the eastern rim of the Altiplano (4 samples frompresent brick clay mines: CLAY/01-04), the Silurian shale-siltstone-sandstone ridges of the Eastern Cordillera (6 samples: No. 3/1-2a-2b, 6/8, 7/3, 7/8) and the pyroclastics-volcanites of the southeastern Morococala Volcanic Field (2 samples: No. 6/4-5) and thewestern Soledad caldera (16 samples: No. 8/1-6 with subsamples).See Fig. 2 for the location of the sampling points.

5. Results

5.1. Petrographic investigations

Petrographic examinations were carried out on almost thecomplete sample collection (249 thin sections). The basic

descriptive parameters were grain size distribution, shape, round-ness, sphericity of grains, fabric and orientation, quantity andcomposition of aplastic inclusions, porosity and optical behaviourof the paste. The properties of geological samples comparable tothat of the ceramics were completed with the description of themineral and lithic fragments and the partly vitrified matrix in thecase of volcaniclastics and volcanites. Based on the petrographicclassification of pottery, it was possible tomake a comparison to thepotential raw materials e especially the tempering clasts.

The main discriminative phenomenon for ceramics was theaplastic inclusion composition, but for detailed subgrouping, thefabric and grain size distribution was also taken into consideration.The investigated 206 ceramic fragments can be classified into threemain petrographic groups: (I) pyroclastic and volcanic originated,(II) sedimentary rock originated and (III) metamorphic rockoriginated.

Group I has predominance in the collection with 106 samples. Ithas 20e30% aplastic inclusion content which is mainly volcani-clastic/volcanic rock originated and its fine-grained paste is wellsorted, weakly anisotropic or isotropic and sometimes the opticalactivity changes in bends. Further division of group I (foursubgroups) is based on the difference in the quality of the volca-niclastic (I/A with pumice, I/B with glass shard fragments), volcanicrock (I/C) and mineral (I/D without rock) grains (Fig. 4aed)(seedetailed qualitative and quantitative description in Szilágyi andSzakmány, 2009).

Subgroup I/A contains fine (50 mm) to coarse grained (300 mm),hiatal fabric ceramics dominantly with low sphericity, angular tosubangular, unweathered pumiceous tuff rock and mineral frag-ments. The ceramic paste is a micaceous, fine grained silt withvariable optical behaviour (from homogeneous anisotropic and redthrough sandwich structure to homogeneous isotropic and greypaste). The pumiceous clasts are fresh, angular grains. Subgroup I/A/a can be characterized as a fine grained ceramic group with50e100 mm dominant pumice size and it contains quartz, plagio-clase, similar quantities of coarse grained (w120 mm) biotite andfine grained (w30 mm) hornblende (rarely orthopyroxene) crystalsand occasionally volcanite or siltstone fragments. Subgroup I/A/b isa coarser grained ceramic typewith 100e275 mmdominant pumicesize and with plagioclase, quartz, biotite (w700 mm), very rarehornblende or orthopyroxene, and in some cases volcanite, meta-morphic quartzite or siltstone fragments. Accessories appear inlimited amount in both subgroups (opaque minerals), in additionsecondary phases (limonite) are present.

Subgroup I/B collects fine (50e75 mm) to coarse grained(150e175 mm), hiatal fabric ceramics dominantly with pyroclastic,very angular, low sphericity, unweathered glass shard and pumi-ceous tuff rock (15e30 w%) and mineral fragments. The micaceous,fine silty paste is anisotropic and red or isotropic. Subgroup I/B/a contains fine grained ceramics with almost only bone-shapedglass shards (with 50e75 mm dominant glass shard size) and fel-sic components (plagioclase and quartz). Subgroup I/B/b isa coarser grained (with 125e175 mm dominant glass shard size)pottery type mainly with bone-shaped glass shards and pumice(with biotite, hornblende and plagioclase phenocrysts) and subor-dinately siltstone fragments. Subgroup I/B/c is similarly a coarsergrained (with 125e175 mmdominant glass shard size) ceramic typebut with the predominance of bone-shaped glass shards and silt-stone clasts andminor content of pumice (with biotite). Subgroup I/B/d has glass shards as major constituents but with a less typicalshape (not bone- but irregular shaped), the additional pumiceclasts have only biotite content. Accessory minerals (opaque pha-ses, rare titanite) are rare in all of the subgroups.

Subgroup I/C gathers medium grained (100e125 mm) potterywith volcanic rock fragments as temper. This subordinate subgroup

V. Szilágyi et al. / Journal of South American Earth Sciences 36 (2012) 1e17 5

Author's personal copy

Table 1Chemical composition of the investigated samples. Results are gained by the combination of different methods: XRF data are with normal, PGAA with italics, INAA withunderlined letters.

Sample Type SiO2 TiO2 Al2O3 Fe2O3 MnO MgO CaO Na2O K2O P2O5 LOI(H2O) Sum(%)ppm

Rb Sr Ba Th U Zr Hf

CeramicsP/12.20. I/A/a 64.00 0.85 18.80 6.70 0.08 1.90 1.00 1.29 4.00 n.d. 0.81 99.43 165 n.d. 890 16.4 4.5 n.d. 5.2I.19.8. I/A/a 59.48 0.75 19.45 6.78 0.10 2.54 1.88 1.72 4.55 0.33 2.14 99.96 194 466 918 n.d. n.d. 155 n.d.I.20.18. I/A/a 61.00 0.82 18.89 6.31 0.10 2.01 4.01 1.86 4.05 0.35 0.79 100.39 136 377 818 n.d. n.d. 173 n.d.I.29.1. I/A/a 60.29 0.83 18.67 6.27 0.09 1.98 4.03 1.82 4.02 0.25 0.79 99.26 132 363 824 n.d. n.d. 171 n.d.

Average of I/A/a 61.19 0.81 18.95 6.52 0.09 2.11 2.73 1.67 4.16 0.31 1.13 157 402 863 16.4 4.5 166 5.2PA/4 I/A/b 62.00 0.64 19.40 4.80 0.06 2.20 1.90 2.13 4.80 n.d. 2.15 100.08 216 n.d. 1220 20.1 6.1 n.d. 6.0PA/6 I/A/b 62.21 0.73 17.98 4.95 0.05 1.49 2.08 1.93 4.87 0.39 n.d. 96.91 251 400 1132 19.7 5.5 206 5.7P/12.17. I/A/b 63.00 0.62 18.70 5.10 0.08 2.00 1.40 2.51 5.20 n.d. 1.40 100.01 228 n.d. 810 19.8 4.5 n.d. 3.6P/34.88. I/A/b 61.04 0.77 18.55 5.13 0.08 1.68 1.74 1.45 4.70 0.29 n.d. 95.75 208 384 1829 19.9 4.2 208 5.5P/92.4. I/A/b 55.45 0.86 22.08 6.40 0.06 2.14 2.72 1.87 3.64 0.19 n.d. 95.73 146 485 1743 23.3 2.4 294 8.2I.10.24. I/A/b 62.65 0.80 20.22 5.39 0.06 1.85 1.86 1.86 4.04 0.20 1.03 100.16 220 327 763 n.d. n.d. 173 n.d.I.16.24. I/A/b 60.95 0.88 22.38 5.92 0.06 1.85 1.62 1.66 3.83 0.22 0.77 100.36 210 309 850 n.d. n.d. 178 n.d.

Average of I/A/b 61.04 0.76 19.90 5.38 0.07 1.89 1.90 1.92 4.44 0.18 1.34 148 381 1192 20.6 4.5 212 5.8I.15.7. I/B/a 67.78 0.59 17.11 4.79 0.08 1.61 1.60 1.93 3.75 0.24 0.76 100.42 169 233 718 n.d. n.d. 162 n.d.I.20.6. I/B/a 59.64 0.57 17.04 5.19 0.09 1.90 4.15 1.52 5.04 0.26 3.90 99.48 201 200 839 n.d. n.d. 189 n.d.P/34.1. I/B/b 63.36 0.68 17.57 5.29 0.04 1.72 1.26 1.10 4.09 0.15 n.d. 95.46 197 251 868 21.1 6.7 254 6.8P/34.2. I/B/b 62.41 0.68 19.01 5.85 0.04 2.00 0.97 1.08 4.57 0.15 n.d. 96.97 223 236 818 21.6 6.7 205 6.1P/34.143. I/B/b 61.65 0.67 17.92 5.27 0.04 1.82 1.31 1.00 4.30 0.17 n.d. 94.34 209 238 838 19.9 6.0 221 6.5I.14.6. I/B/b 64.57 0.68 18.77 5.36 0.04 1.97 1.20 1.21 4.84 0.23 1.19 100.25 220 207 595 n.d. n.d. 217 n.d.I.15.1. I/B/b 64.11 0.71 19.21 5.54 0.04 2.20 1.29 1.21 4.54 0.18 0.89 100.11 217 242 626 n.d. n.d. 216 n.d.

Average of I/B/a 63.36 0.65 18.09 5.33 0.05 1.89 1.68 1.29 4.45 0.20 1.69 205 230 757 20.9 6.5 209 6.5BA/1 I/C/a 58.00 0.97 21.00 7.10 0.19 2.50 2.60 1.86 4.50 n.d. 1.07 99.79 187 n.d. 1600 15.5 3.2 n.d. 4.4P/1.166. I/C/a 57.99 0.76 18.41 6.27 0.11 3.21 3.26 1.93 4.36 0.25 n.d. 96.82 137 580 1257 15.5 3.4 190 5.5P/33.5. I/C/a 59.42 0.97 17.75 6.35 0.10 3.15 2.99 1.85 3.67 0.39 n.d. 96.92 119 628 1152 15.7 3.8 219 5.9P/48.101. I/C/a 58.75 0.73 19.25 6.31 0.07 2.38 2.08 1.70 4.25 0.20 n.d. 95.93 185 371 834 15.9 4.0 183 4.7I.30.5. I/C/a 59.71 0.78 18.66 6.22 0.14 3.80 3.47 2.20 4.18 0.34 1.07 100.84 138 623 1304 n.d. n.d. 187 n.d.

Average of I/C/a 58.77 0.84 19.01 6.45 0.12 3.01 2.88 1.91 4.19 0.23 1.07 153 551 1229 15.7 3.6 195 5.1P/1.186. I/C/b 60.36 0.79 18.64 5.97 0.06 1.73 1.86 1.31 4.09 0.34 n.d. 95.37 224 439 1069 16.9 4.5 157 5.0I.16.1. I/C/b 61.35 0.87 20.89 4.29 0.06 1.91 2.60 3.19 3.57 0.44 1.05 100.60 91 1084 1630 n.d. n.d. 250 n.d.

Average of I/C/b 60.85 0.83 19.76 5.13 0.06 1.82 2.23 2.25 3.83 0.39 1.05 158 762 1350 16.9 4.5 204 5.0P/12.13. I/D 63.27 0.73 18.32 5.36 0.10 2.27 3.02 1.13 3.81 0.17 n.d. 98.41 191 483 811 15.2 3.2 212 5.6P/42.9. I/D 61.23 0.76 17.62 5.82 0.09 1.88 3.31 1.02 3.72 0.15 n.d. 95.81 178 377 829 14.9 3.3 220 5.8

Average of I/D 62.25 0.74 17.97 5.59 0.10 2.07 3.16 1.07 3.76 0.16 185 430 820 15.1 3.2 216 5.7P/53.79. II/A 61.09 0.79 20.82 7.04 0.10 2.07 1.16 0.88 4.68 n.d. 1.27 99.90 183 n.d. 730 14.6 2.9 n.d. 5.9I.10.68. II/A 60.06 0.82 21.53 7.45 0.07 2.26 1.70 0.69 4.13 0.25 1.21 100.35 206 142 658 n.d. n.d. 196 n.d.I.20.14. II/A 57.73 0.75 21.95 8.66 0.06 1.79 1.71 0.75 4.35 0.97 1.28 100.22 197 270 760 n.d. n.d. 194 n.d.I.20.20. II/A 57.31 0.74 21.73 8.77 0.07 1.79 1.71 0.74 4.23 0.97 2.14 100.50 198 272 752 n.d. n.d. 190 n.d.

Average of II/A 59.05 0.78 21.51 7.98 0.08 1.98 1.57 0.77 4.35 0.73 1.48 196 228 725 14.6 2.9 193 5.9PA/1 II/B or C 64.00 0.94 19.00 6.70 0.11 2.00 0.38 1.01 4.70 n.d. 1.28 100.12 202 n.d. 1100 18.5 4.4 n.d. 7.2P/1.21. II/C 58.08 0.78 22.03 8.00 0.10 2.46 1.39 0.99 4.64 0.26 n.d. 98.94 215 237 827 n.d. n.d. 177 n.d.P/53.108. II/B 58.80 0.80 20.65 7.28 0.08 1.97 0.56 0.75 4.17 0.18 n.d. 95.42 199 136 804 n.d. n.d. 191 n.d.P/63.7. II/B 58.84 0.75 22.57 7.20 0.10 1.91 0.52 0.77 4.60 0.16 n.d. 97.63 232 142 872 16.1 3.1 209 5.941.125. II/B 61.48 0.82 21.39 5.93 0.05 1.64 1.62 0.61 4.24 0.25 2.21 100.47 207 187 1255 n.d. n.d. 221 n.d.I.7.18. II/C 61.16 0.79 22.04 8.02 0.10 1.39 0.78 0.68 3.92 0.14 1.09 100.36 216 138 1237 n.d. n.d. 224 n.d.I.13.9. II/B 60.57 0.69 19.70 7.07 0.06 2.14 1.52 0.98 3.99 0.51 2.96 100.38 175 196 625 n.d. n.d. 207 n.d.

Average of II/B-C 60.42 0.80 21.05 7.17 0.09 1.93 0.97 0.83 4.32 0.25 1.89 207 173 960 17.3 3.7 205 6.6PA/5 III 56.00 1.18 28.70 2.43 0.03 4.80 0.33 0.91 4.00 n.d. 1.43 99.81 189 n.d. 850 24.7 6.6 n.d. 5.4

Adobes4/3 Adobe 62.07 0.83 16.13 4.92 0.09 1.61 2.55 1.31 3.55 0.19 6.26 99.51 172 205 612 n.d. n.d. 203 n.d.4/4 Adobe 46.27 0.46 21.82 7.09 0.07 2.24 4.56 0.72 4.18 0.22 11.91 99.56 220 282 2297 n.d. n.d. 140 n.d.4/5 Adobe 59.78 0.69 18.65 6.16 0.12 1.63 0.89 1.21 3.82 0.20 6.41 99.55 181 211 757 n.d. n.d. 194 n.d.4/6 Adobe 58.20 0.80 19.47 6.12 0.09 1.85 1.53 1.04 4.01 0.22 5.28 98.62 193 179 712 n.d. n.d. 183 n.d.

Average of adobe 56.58 0.69 19.02 6.07 0.09 1.83 2.38 1.07 3.89 0.21 7.47 191 219 1094 180

SedimentsCLAY-01 Brickclay 71.91 0.94 13.24 5.17 0.07 1.02 0.35 1.14 2.78 0.20 3.17 100.14 129 130 358 n.d. n.d. 379 n.d.CLAY-02 Brickclay 54.17 0.92 23.41 8.05 0.12 1.75 0.45 0.50 4.82 0.18 5.94 100.50 239 263 561 n.d. n.d. 154 n.d.CLAY-03 Brickclay 75.14 0.62 11.90 4.53 0.04 1.06 0.90 1.33 2.12 0.11 2.87 100.79 103 197 376 n.d. n.d. 372 n.d.CLAY-04 Brickclay 56.83 0.83 21.05 7.27 0.12 2.11 1.90 0.85 3.66 0.16 5.84 100.77 194 94 566 n.d. n.d. 154 n.d.SED-01 River sediment,

sand77.00 0.53 10.20 4.20 0.07 0.80 0.91 1.49 2.41 n.d. 2.42 100.03 77 n.d. 500 7.2 2.2 n.d. 3.6

SED-02 River sediment,sand

75.00 0.60 10.60 4.20 0.07 1.40 0.95 1.33 2.52 n.d. 2.97 99.64 95 n.d. 550 9.0 2.8 n.d. 5.3

SED-03 River sediment,sand

88.00 0.34 4.70 2.78 0.32 0.31 0.30 0.44 1.13 n.d. 1.72 100.04 84 n.d. 370 6.7 2.1 n.d. 3.9

SED-04 River sediment,sand

70.56 0.35 7.45 3.61 0.05 0.52 0.54 1.11 1.83 0.12 n.d. 86.14 92 146 422 5.1 1.5 163 7.0

2/1 River sediment,sand

74.03 0.53 11.99 4.57 0.05 1.04 0.92 1.42 2.62 0.17 2.53 99.87 118 238 575 n.d. n.d. 200 n.d.

5/2 River sediment, silt 50.62 0.44 21.39 7.13 0.07 2.30 2.82 0.66 4.03 0.20 10.21 99.87 215 276 2175 n.d. n.d. 167 n.d.

V. Szilágyi et al. / Journal of South American Earth Sciences 36 (2012) 1e176

Author's personal copy

Nb Ta Y La Ce Nd Sm Eu Tb Yb Lu Sc V Cr Co Ni Zn As Sb Cs B Cl Gd

n.d. 1.6 n.d. 47 103 38 8.1 1.5 n.d. 3.4 0.36 16.1 n.d. 102 16.4 n.d. 104 13 22.2 60 117 600 6.814.0 n.d. 30 57 108 51 8.7 1.6 n.d. 2.8 n.d. n.d. 120 56 16.0 44.0 143 n.d. n.d. n.d. n.d. n.d. n.d.n.d. n.d. 28 39 78 36 4.8 1.2 n.d. 2.5 n.d. n.d. 134 34 16.0 37.0 121 n.d. n.d. n.d. n.d. n.d. n.d.n.d. n.d. 28 39 75 52 5.3 1.2 n.d. 2.5 n.d. n.d. 129 35 15.0 39.0 120 n.d. n.d. n.d. n.d. n.d. n.d.14.0 1.6 29 46 91 44 6.7 1.4 2.8 0.36 16.1 128 57 15.9 40.0 122 13 22.2 60 117 600 6.8n.d. 1.6 n.d. 61 121 50 8.8 1.7 n.d. 2.2 0.32 12.6 n.d. 51 11.2 n.d. 98 13 3.2 42 109 350 6.016.2 1.4 18 60 122 52 9.3 1.5 n.d. 1.6 0.21 9.8 82 62 9.2 n.d. 109 72 2.9 30 118 400 6.0n.d. 1.7 n.d. 45 82 33 5.8 1.1 n.d. 1.7 0.26 12.5 n.d. 65 10.2 n.d. 138 30 30.1 29 143 430 5.017.2 1.5 30 61 126 74 9.6 1.8 1.2 2.5 0.36 13.8 82 70 12.5 n.d. 83 13 2.5 22 n.d. n.d. n.d.18.4 1.3 25 69 137 62 9.2 1.9 0.8 1.6 0.22 13.3 97 68 13.5 15.8 95 21 1.7 12 104 582 6.419.0 n.d. 23 61 109 41 7.5 1.1 n.d. 2.4 n.d. n.d. 116 64 12.0 42.0 83 n.d. n.d. n.d. n.d. n.d. n.d.19.0 n.d. 29 57 116 50 8.2 1.2 n.d. 2.7 n.d. n.d. 140 85 15.0 70.0 95 n.d. n.d. n.d. n.d. n.d. n.d.18.0 1.5 25 59 116 52 8.3 1.5 1.0 2.1 0.27 12.4 103 66 11.9 42.6 100 30 8.1 27 95 441 5.918.0 n.d. 28 46 94 30 7.2 1.0 n.d. 2.6 n.d. n.d. 85 38 11.0 53.0 77 n.d. n.d. n.d. n.d. n.d. n.d.18.0 n.d. 28 42 98 57 9.2 1.1 n.d. 2.6 n.d. n.d. 83 43 10.0 35.0 170 n.d. n.d. n.d. n.d. n.d. n.d.15.4 1.3 29 43 92 35 7.3 1.3 0.9 2.8 0.36 13.5 104 72 11.5 8.8 92 133 9.5 37 n.d. n.d. n.d.14.4 1.4 26 48 101 35 7.8 1.3 1.1 2.8 0.37 15.5 116 88 13.8 20.0 103 154 7.2 40 n.d. n.d. n.d.15.4 1.5 25 44 93 39 7.0 1.2 0.8 2.3 0.35 14.2 105 74 10.4 n.d. 86 205 18.8 41 205 295 5.115.0 n.d. 29 49 104 47 6.5 0.8 n.d. 2.6 n.d. n.d. 111 47 12.0 63.0 87 n.d. n.d. n.d. n.d. n.d. n.d.17.0 n.d. 25 50 111 40 8.7 1.1 n.d. 2.4 n.d. n.d. 124 51 13.0 49.0 89 n.d. n.d. n.d. n.d. n.d. n.d.16.2 1.4 27 46 99 40 7.7 1.1 0.9 2.6 0.36 14 104 59 11.7 38.1 100 164 11.9 39 205 295 5.1n.d. 1.1 n.d. 43 84 43 7.6 1.5 n.d. 2.7 0.42 22.6 n.d. 118 19.0 n.d. 118 23 8.3 15 94 154 6.4n.d. 0.9 27 49 98 52 7.9 1.8 n.d. 2.4 0.32 15.8 111 60 14.8 8.4 124 14 1.4 12 n.d. n.d. n.d.n.d. n.d. 29 51 112 47 8.7 2.1 n.d. 2.6 0.31 16.6 134 118 19.6 1.3 170 10 1.6 18 n.d. n.d. n.d.14.0 1.4 28 49 103 49 8.1 1.8 1.2 2.5 0.35 15.9 110 120 16.5 n.d. 111 16 3.6 32 n.d. n.d. n.d.n.d. n.d. 26 61 119 44 6.9 1.8 n.d. 2.2 n.d. n.d. 126 32 16.0 46.0 123 n.d. n.d. n.d. n.d. n.d. n.d.14.0 1.1 27 51 103 47 7.8 1.8 1.2 2.5 0.35 17.7 120 90 17.2 18.6 129 16 3.7 19 94 154 6.416.6 1.7 19 50 98 45 7.4 1.4 n.d. 1.8 0.24 13.0 103 52 6.9 n.d. 123 53 3.4 61 n.d. n.d. n.d.n.d. n.d. 25 108 182 77 9.2 2.9 n.d. 1.9 n.d. n.d. 92 71 9.0 39.0 80 n.d. n.d. n.d. n.d. n.d. n.d.16.6 1.7 22 79 140 61 8.3 2.1 1.9 0.24 13 97 62 8.0 39.0 101 53 3.4 6114.2 1.2 33 44 92 38 7.3 1.5 0.9 2.7 0.38 14.0 108 70 13.2 28.9 87 6 2.0 260 149 78 6.014.6 1.5 31 43 93 41 7.3 1.4 1.0 2.7 0.39 14.2 106 79 13.7 13.6 85 9 9.2 163 n.d. n.d. n.d.14.4 1.4 32 44 93 40 7.3 1.4 0.9 2.7 0.39 14.1 107 75 13.5 21.3 86 7 5.6 212 149 78 6.0n.d. 1.5 n.d. 44 89 38 7.6 1.4 1.0 3.1 0.46 16.6 163 93 16.1 n.d. 110 23 6.3 43 136 86 6.421.0 n.d. 40 45 105 51 6.2 0.7 n.d. 3.7 n.d. n.d. 141 82 20.0 89.0 101 n.d. n.d. n.d. n.d. n.d. n.d.15.0 n.d. 38 51 103 42 6.7 1.0 n.d. 3.5 n.d. n.d. 144 75 17.0 14.0 407 n.d. n.d. n.d. n.d. n.d. n.d.16.0 n.d. 37 51 95 36 8.4 1.2 n.d. 3.4 n.d. n.d. 148 73 18.0 22.0 409 n.d. n.d. n.d. n.d. n.d. n.d.17.3 1.5 38 48 98 42 7.2 1.1 1.0 3.4 0.46 16.6 149 81 17.8 41.7 257 23 6.3 43 136 86 6.4n.d. 1.6 n.d. 58 130 48 9.7 1.8 1.2 4.1 0.57 17.8 n.d. 92 17.5 n.d. 120 7 1.5 12 91 60 9.015.6 n.d. 37 52 112 45 7.2 1.0 n.d. 3.4 n.d. n.d. 137 74 20.0 49.8 133 n.d. n.d. n.d. n.d. n.d. n.d.16.8 n.d. 38 44 92 48 7.1 0.8 n.d. 3.6 n.d. n.d. 129 80 16.8 15.3 92 n.d. n.d. n.d. n.d. n.d. n.d.18.0 1.5 36 46 95 42 7.8 1.5 1.0 3.0 0.42 17.8 128 87 15.3 54.5 117 26 3.8 46 130 94 6.219.0 n.d. 39 37 113 41 6.1 0.8 n.d. 3.5 n.d. n.d. 149 70 14.0 82.0 57 n.d. n.d. n.d. n.d. n.d. n.d.21.0 n.d. 51 45 129 47 9.1 1.0 n.d. 4.6 n.d. n.d. 158 75 21.0 105.0 89 n.d. n.d. n.d. n.d. n.d. n.d.16.0 n.d. 38 48 97 45 6.8 0.9 n.d. 3.4 n.d. n.d. 130 64 18.0 82.0 106 n.d. n.d. n.d. n.d. n.d. n.d.17.7 1.6 40 47 110 45 7.7 1.1 1.1 3.7 0.50 17.8 138 77 17.5 64.8 102 17 2.7 29 110 77 7.6n.d. 2.4 n.d. 72 159 80 8.9 2.5 1.5 5.1 0.62 25.4 n.d. 138 8.5 n.d. n.d. 10 1.6 19 125 n.d. 10.6

19.2 n.d. 37 41 86 33 6.5 0.9 n.d. 3.4 n.d. n.d. 112 46 12.6 51.9 67 n.d. n.d. n.d. n.d. n.d. n.d.n.d. n.d. 26 34 93 30 4.6 0.9 n.d. 2.4 n.d. n.d. 134 51 13.8 67.8 97 n.d. n.d. n.d. n.d. n.d. n.d.13.3 n.d. 33 48 106 39 5.7 0.9 n.d. 3.0 n.d. n.d. 118 49 16.4 58.6 89 n.d. n.d. n.d. n.d. n.d. n.d.16.5 n.d. 34 47 106 38 7.3 0.9 n.d. 3.1 n.d. n.d. 134 62 17.3 49.4 85 n.d. n.d. n.d. n.d. n.d. n.d.16.3 32 43 98 35 6.0 0.9 3.0 125 52 15.0 56.9 84

28.0 n.d. 57 35 91 48 6.7 0.8 n.d. 5.0 n.d. n.d. 93 51 39.0 83.0 54 n.d. n.d. n.d. n.d. n.d. n.d.22.0 n.d. 35 62 124 53 9.2 1.2 n.d. 3.3 n.d. n.d. 157 86 37.0 83.0 80 n.d. n.d. n.d. n.d. n.d. n.d.19.0 n.d. 37 29 76 28 3.7 0.7 n.d. 3.1 n.d. n.d. 82 40 11.0 88.0 56 n.d. n.d. n.d. n.d. n.d. n.d.18.0 n.d. 38 36 90 39 7.6 0.8 n.d. 3.5 n.d. n.d. 148 76 19.0 87.0 88 n.d. n.d. n.d. n.d. n.d. n.d.n.d. 0.9 n.d. 23 49 17 3.5 0.9 0.4 1.3 0.19 6.2 n.d. 30 7.8 n.d. 48 12 18.2 23 61 69 4.2

n.d. 1.0 n.d. 28 59 21 4.4 1.0 0.6 1.7 0.25 7.3 n.d. 40 9.0 n.d. 55 16 14.9 24 93 400 4.9

n.d. 0.9 n.d. 19 40 14 3.7 0.8 0.6 1.7 0.23 5.4 n.d. 24 7.2 n.d. 61 22 4.6 17 74 95 2.8

n.d. 0.6 14 15 31 13 2.5 0.6 0.4 1.5 0.23 4.1 38 21 5.2 n.d. 42 34 9.5 13 n.d. n.d. n.d.

n.d. n.d. 24 32 76 21 6.6 1.0 n.d. 2.2 n.d. n.d. 74 38 11.2 60.2 49 n.d. n.d. n.d. n.d. n.d. n.d.

n.d. n.d. 25 28 89 33 5.0 0.9 n.d. 2.3 n.d. n.d. 131 54 13.4 77.3 102 n.d. n.d. n.d. n.d. n.d. n.d.

(continued on next page)

V. Szilágyi et al. / Journal of South American Earth Sciences 36 (2012) 1e17 7

Author's personal copy

contains very varied samples with anisotropic and yellowish-reddish, silty paste and different originated volcanic clasts.Subgroup I/C/a has low sphericity, angular to subangular,unweathered, hialopilitic volcanites as aplastics with differentcomposition (from dacitic through andesitic to basaltic andesitic ebased on mineralogical and fabric observations). Subgroup I/C/b has an aplastic content of medium sphericity, subrounded,weathered, vitrophyric volcanic rock fragments.

Subgroup I/D has an almost serial fabric and contains no rockfragments (dominant grain size 50e100 mm). The major constitu-ents of these ceramics are quartz, plagioclase, biotite, hornblendeand rare orthopyroxene. All of these mineral clasts are mediumsphericity, subangular-subrounded and unweathered. Limitedopaque phases are present.

Group II (with sedimentary origin) is the other dominant petro-graphic group of the pottery assemblage with 93 representatives. Ithasmedium-coarse grained (175e200 mmand 300e1300 mm) hiatalfabric, 30e35% aplastic inclusion content. This group can be char-acterized on the base of the presence of subrounded-well rounded,low-medium sphericity, clastic sedimentary rock fragments which

are natural components of the anisotropic and brown, coarse siltypaste. Division of the group into three subgroups (II/A-B-C) is basedon the dominant grain size of the aplastic sedimentary rock clasts(Fig. 4eeg). Subgroup II/A contains pottery fragments with finegrained (claystone/shale-siltstone) sedimentary (sometimes lowgrade metamorphic) rock and mineral fragments. The aplasticinclusions themselves contain quartz, muscovite-sericite (some-times biotite) and plagioclase in a weakly-well oriented fabric.Subgroup II/B has similar composition to the previous one as regardthe aplastic inclusions but their dominant grain size is coarser(claystone-siltstone togetherwith sandstone) and their fabric do notshows any metamorphic feature. It contains both rock and mineralclasts. Subgroup II/C can be characterized with the coarsest domi-nant grain size of the aplastics since this group of pottery has mainlysandstone rock and mineral fragments as clastic constituents.Regarding the mineralogical composition, this subgroup is alsosimilar to the previous ones.

Group III (with metamorphic origin) is the smallest group in theinvestigated assemblage with 7 samples (Fig. 4h). This groupincorporates coarse grained (200e300 mm), hiatal fabric ceramics

Table 1 (continued)

Sample Type SiO2 TiO2 Al2O3 Fe2O3 MnO MgO CaO Na2O K2O P2O5 LOI(H2O) Sum(%)ppm

Rb Sr Ba Th U Zr Hf

5/3 River sediment,silty clay

66.08 0.55 15.09 6.53 0.08 1.25 0.60 0.90 2.57 0.14 5.74 99.53 141 146 484 n.d. n.d. 263 n.d.

5/4 River sediment,gravely sand

70.41 0.57 10.83 9.56 0.10 0.92 0.24 0.57 1.99 0.18 3.87 99.24 100 61 503 n.d. n.d. 210 n.d.

5/5 River sediment,sand

72.85 0.57 12.06 5.22 0.07 1.21 1.03 1.06 2.25 0.12 3.49 99.93 108 185 522 n.d. n.d. 375 n.d.

5/7 River sediment, silt 61.32 0.73 16.58 8.14 0.14 1.29 1.45 0.87 3.18 0.68 4.74 99.11 157 141 520 n.d. n.d. 230 n.d.5/8 River sediment,

silty sand76.15 0.60 10.43 5.22 0.06 0.78 0.63 1.04 1.95 0.12 2.69 99.67 89 145 572 n.d. n.d. 356 n.d.

7/1 River sediment,sand

78.24 0.51 9.84 3.68 0.05 0.90 0.97 1.35 2.15 0.16 2.09 99.94 93 233 512 n.d. n.d. 296 n.d.

7/2 River sediment,sand

80.68 0.45 7.16 5.82 0.06 0.45 0.68 1.31 1.59 0.14 1.64 99.97 66 204 529 n.d. n.d. 303 n.d.

7/5 River sediment, silt 66.12 0.65 16.57 4.63 0.06 1.42 1.30 1.91 3.21 0.16 3.63 99.65 171 289 635 n.d. n.d. 245 n.d.7/6 River sediment,

clay60.56 0.90 19.77 6.03 0.06 1.72 0.68 1.02 4.01 0.12 4.46 99.31 229 140 667 n.d. n.d. 191 n.d.

Average ofsediments

69.77 0.61 13.38 5.60 0.09 1.17 0.93 1.07 2.68 0.16 3.89 132 152 600 7.0 2.2 254 5.0

Sedimentary rocks3/2a Claystone/shale 39.43 0.82 16.85 23.31 0.11 2.52 1.44 0.54 2.81 0.10 11.03 98.96 147 64 362 n.d. n.d. 141 n.d.3/2b Sandstone 65.48 0.54 11.95 8.33 0.17 2.38 2.57 1.14 1.27 0.17 5.93 99.93 65 53 213 n.d. n.d. 167 n.d.6/8 Siltstone 57.67 0.87 21.25 7.39 0.05 2.61 0.27 0.86 4.52 0.14 4.21 99.83 227 47 609 n.d. n.d. 154 n.d.7/3 Siltstone/shale 67.84 0.77 14.33 5.23 0.06 2.07 0.48 1.95 2.85 0.16 2.68 98.40 140 68 388 n.d. n.d. 256 n.d.

Average of sed.rocks

57.61 0.75 16.10 11.06 0.10 2.39 1.19 1.12 2.86 0.14 5.96 144 58 393 179

Volcanoclastic-volcanic rocks6/4 Morococala

rhyodacitic tuff67.74 0.46 16.00 2.61 0.04 0.90 2.04 3.44 4.75 0.26 1.16 99.40 258 517 894 n.d. n.d. 196 n.d.

6/5 Morococalarhyodacitic tuff

66.96 0.46 16.45 2.52 0.03 1.26 2.10 3.24 4.64 0.26 1.52 99.45 231 526 941 n.d. n.d. 194 n.d.

Average ofMorococala tuff

67.35 0.46 16.23 2.56 0.04 1.08 2.07 3.34 4.69 0.26 1.34 244 521 918 195

8/1 Soledad prim.weath. sand

68.24 0.92 15.54 2.60 0.04 0.94 4.13 3.32 2.50 0.16 0.97 99.37 57 658 1023 n.d. n.d. 328 n.d.

8/2b Soledad dacitic tuff 62.82 0.82 15.77 4.05 0.06 2.08 3.20 2.57 4.16 0.32 4.11 99.94 152 547 1287 n.d. n.d. 256 n.d.8/2d Soledad dacitic tuff 63.14 0.82 15.50 4.22 0.06 1.85 3.19 2.72 4.33 0.32 3.53 99.66 156 553 1305 n.d. n.d. 248 n.d.8/3 Soledad dacitic tuff 68.46 0.50 15.08 2.26 0.03 0.96 2.39 3.35 3.43 0.18 2.52 99.15 122 490 1246 n.d. n.d. 154 n.d.8/5b Soledad dacitic tuff 49.38 0.61 11.69 14.44 0.07 1.17 2.15 2.72 3.77 0.37 12.18 98.56 123 539 1286 n.d. n.d. 181 n.d.8/6a Soledad dacite 68.61 0.69 15.38 3.09 0.04 1.32 2.47 3.51 4.84 0.10 0.43 100.70 151 525 862 n.d. n.d. 234 n.d.8/6b Soledad dacite 66.31 0.69 15.51 3.33 0.05 1.39 2.82 3.27 4.06 0.27 1.88 99.84 165 545 1264 n.d. n.d. 226 n.d.8/6c Soledad dacitic tuff 66.67 0.63 15.14 3.13 0.05 1.47 2.92 2.97 4.58 0.26 1.88 99.69 166 515 1337 n.d. n.d. 212 n.d.8/6d Soledad dacitic tuff 67.13 0.69 16.09 3.56 0.04 0.83 3.00 3.48 4.43 0.31 0.48 100.02 164 568 1284 n.d. n.d. 227 n.d.8/6g Soledad dacitic tuff 65.16 0.68 16.39 4.29 0.05 1.64 2.62 2.29 3.97 0.26 1.77 99.12 154 522 1576 n.d. n.d. 223 n.d.8/6h Soledad dacite 66.52 0.69 15.42 3.38 0.04 1.39 2.73 2.94 4.79 0.27 1.92 100.35 164 535 1370 n.d. n.d. 230 n.d.

Average ofSoledad rocks

64.77 0.70 15.23 4.39 0.05 1.37 2.87 3.01 4.08 0.26 2.88 143 545 1258 229

V. Szilágyi et al. / Journal of South American Earth Sciences 36 (2012) 1e178

Author's personal copy

with well rounded, medium sphericity and e in contrast to group Iand II e metamorphic mica schist rock and mineral fragments(muscovite, quartz, opaque phases) in a white, isotropic clay paste.

The eight building material remnants are divided into two types(adobes and rocks) from the point of view of the petrographicdescription. The adobe samples represented four types of adobesaccording to their colour and internal structure: (1) loose fabric, greyadobe with a high quantity of plant remnants (No. 4/3), (2) loosefabric, dark red adobe with a high quantity of plant remnants (No. 4/4), (3) loose fabric, light red adobe with a high quantity of plantremnants (No. 4/5), (4) loose fabric, yellowish brown plaster witha high quantity of plant remnants (No. 4/6). The most abundantbuilding stones are sandstones and siltstones, which clearly charac-terize the local geology. The selected building stone sampleswere: (1)fine-grained, dark grey, schistose siltstone (No. 4/1), (2) medium-grained, fine bedded reddish brown sandstone (No. 4/2), (3)medium-grained, green, micaceous sandstone with undulatebedding planes (No. 4/7), (4) greenish grey shale (No. 4/8).

The adobes are basically fine grained (from 10e30 mm to 50 mmaverage grain size), almost serial and quite dense fabric, limonitic,

partly micaceous, secondarily carbonized silty clays. Theirsecondary carbonatic and limonitic content is present in the form of75e175 mm sized nodules and dispersed mottles. The averagemineralogical composition is quartz, plagioclase, carbonate (mostprobably calcite), limonite, mica (rather biotite than muscovite),opaque phases and rare tourmaline. Occasionally argillaceous rockfragments are found too. The remnants of the plant tempering canbe observed as characteristic shaped pores or sometimesphytolithes.

The building stone samples are relatively monotonous,finely layered, clastic sedimentary rock fragments with similarmineralogical composition (normal or slightly undulatory extinc-tion quartz, fine grained muscovite or sericite (rare limonitizedmica) and weathered plagioclase, tourmaline, opaque phases,zircon and secondary limonite) but with variable dominant grainsize (from 10e50 mm to 100e150 mm).

The investigated geological samples (35 thin sections) wereseparated according to the sampling considerations and thegeological setting. The alluvial sediments of the Paria Basin and theeastern rim of the Altiplano (18 samples: No. SED/01-04, No. 1/2-3,

Table 1 (extended)

Nb Ta Y La Ce Nd Sm Eu Tb Yb Lu Sc V Cr Co Ni Zn As Sb Cs B Cl Gd

14.6 n.d. 32 38 90 34 4.6 0.7 n.d. 2.8 n.d. n.d. 101 55 14.4 72.2 75 n.d. n.d. n.d. n.d. n.d. n.d.

15.2 n.d. 33 24 69 27 4.6 0.7 n.d. 2.9 n.d. n.d. 91 57 18.5 79.3 90 n.d. n.d. n.d. n.d. n.d. n.d.

17.9 n.d. 36 35 82 36 5.2 0.8 n.d. 2.9 n.d. n.d. 87 42 12.1 83.9 58 n.d. n.d. n.d. n.d. n.d. n.d.

16.8 n.d. 57 67 96 53 8.6 1.0 n.d. 5.2 n.d. n.d. 120 63 17.5 70.3 74 n.d. n.d. n.d. n.d. n.d. n.d.18.1 n.d. 34 31 71 27 5.3 0.8 n.d. 2.8 n.d. n.d. 79 38 11.5 77.0 52 n.d. n.d. n.d. n.d. n.d. n.d.

n.d. n.d. 27 28 71 25 5.8 0.9 n.d. 2.3 n.d. n.d. 62 34 7.3 65.8 34 n.d. n.d. n.d. n.d. n.d. n.d.

n.d. n.d. 24 30 71 23 3.9 0.8 n.d. 1.8 n.d. n.d. 65 38 7.2 76.1 39 n.d. n.d. n.d. n.d. n.d. n.d.

19.4 n.d. 30 43 86 40 8.0 1.1 n.d. 2.6 n.d. n.d. 75 27 9.2 48.5 73 n.d. n.d. n.d. n.d. n.d. n.d.20.0 n.d. 38 44 107 43 7.6 0.8 n.d. 3.6 n.d. n.d. 144 64 40.1 50.5 100 n.d. n.d. n.d. n.d. n.d. n.d.

19.0 0.8 34 34 77 31 5.6 0.9 0.5 2.8 0.23 5.8 97 46 15.7 73.5 65 21 11.8 19 76 188 4.0

17.4 n.d. 39 52 91 38 12.4 1.5 n.d. 3.3 n.d. n.d. 144 116 43.6 206.0 136 n.d. n.d. n.d. n.d. n.d. n.d.11.5 n.d. 32 16 46 16 3.8 0.7 n.d. 2.9 n.d. n.d. 85 45 22.9 81.5 68 n.d. n.d. n.d. n.d. n.d. n.d.16.3 n.d. 36 39 94 37 5.8 0.5 n.d. 3.4 n.d. n.d. 169 86 13.4 79.1 78 n.d. n.d. n.d. n.d. n.d. n.d.16.6 n.d. 37 34 86 42 5.5 0.6 n.d. 3.4 n.d. n.d. 94 48 12.6 40.6 116 n.d. n.d. n.d. n.d. n.d. n.d.15.5 36 35 79 33 6.9 0.8 3.3 123 74 23.1 101.8 99

n.d. n.d. 14 65 115 42 7.5 1.4 n.d. 1.2 n.d. n.d. 47 n.d. n.d. 19.9 53 n.d. n.d. n.d. n.d. n.d. n.d.

n.d. n.d. 14 69 118 45 6.3 1.4 n.d. 1.2 n.d. n.d. 47 n.d. n.d. 20.4 51 n.d. n.d. n.d. n.d. n.d. n.d.

14 67 117 43 6.9 1.4 1.2 47 20.2 52

n.d. n.d. 46 691 1123 381 67.4 6.4 n.d. 3.8 n.d. n.d. 66 n.d. 1.4 27.6 52 n.d. n.d. n.d. n.d. n.d. n.d.

n.d. n.d. 19 51 114 39 6.2 1.5 n.d. 1.4 n.d. n.d. 91 23 6.5 34.7 82 n.d. n.d. n.d. n.d. n.d. n.d.n.d. n.d. 21 59 120 51 7.8 1.7 n.d. 1.7 n.d. n.d. 91 27 4.4 28.3 88 n.d. n.d. n.d. n.d. n.d. n.d.n.d. n.d. 18 59 109 39 6.5 1.4 n.d. 1.7 n.d. n.d. 55 19 1.5 4.2 71 n.d. n.d. n.d. n.d. n.d. n.d.n.d. n.d. 15 49 91 34 7.4 1.7 n.d. 1.0 n.d. n.d. 81 42 8.7 53.0 107 n.d. n.d. n.d. n.d. n.d. n.d.n.d. n.d. 12 62 105 36 7.4 1.6 n.d. 0.8 n.d. n.d. 65 20 5.0 48.0 56 n.d. n.d. n.d. n.d. n.d. n.d.n.d. n.d. 15 64 121 52 7.4 1.6 n.d. 1.2 n.d. n.d. 68 5 3.0 26.0 75 n.d. n.d. n.d. n.d. n.d. n.d.n.d. n.d. 19 55 112 35 6.2 1.4 n.d. 1.5 n.d. n.d. 73 18 2.1 25.2 62 n.d. n.d. n.d. n.d. n.d. n.d.n.d. n.d. 17 43 97 33 4.1 1.4 n.d. 1.3 n.d. n.d. 59 27 2.9 40.6 67 n.d. n.d. n.d. n.d. n.d. n.d.n.d. n.d. 26 57 124 54 8.9 1.7 n.d. 2.3 n.d. n.d. 77 13 9.8 5.1 213 n.d. n.d. n.d. n.d. n.d. n.d.n.d. n.d. 17 53 115 49 6.2 1.5 n.d. 1.3 n.d. n.d. 66 6 3.0 35.0 73 n.d. n.d. n.d. n.d. n.d. n.d.

20 113 203 73 12.3 2.0 1.6 72 20 4.4 29.8 86

V. Szilágyi et al. / Journal of South American Earth Sciences 36 (2012) 1e17 9

Author's personal copy

5/1-3, 5/5-8, 7/1-2, 7/4-5, 7/7) were ranging from silty clay to finegravely sand and all of those could have originated from the fluvialweathering of the Palaeozoic clastic sedimentary unit of the EasternCordillera. These weakly-medium layered, medium sphericity,rounded-well rounded, medium-well sorted sediments mainlyconsist of rock and mineral fragments of the above mentionedPalaeozoic sedimentary rocks (shales/claystones-siltstones-sand-stones) and subordinately varying quantities of weatheredvolcanic-volcaniclastic rock clasts (their content depends on thelocality and its distance from the nearest volcanic sources). Themajor mineral phases of sedimentary origin are quartz, feldspars,mica (muscovite-biotite) and clay minerals. The volcanic relatedconstituents are mainly devitrified, weathered volcanic glass withcrystallites and phenocrystals of feldspar, biotite (rarely horn-blende) and quartz.

Samples from the Silurian sedimentary ridges of the EasternCordillera (2 samples: No. 3/1-2a-2b) are weakly-well layered,medium-well sorted shales-siltstones-sandstones mainly consist-ing of quartz, feldspars, muscovite-biotite and probably clayminerals invisible under the microscope.

The pyroclastics of the south easternMorococala Volcanic Field (2samples: No. 6/4-5) are weakly welded dacitic tuffs (ignimbrites)withhighly vitric, pumiceousmatrix and feldspar (mainly plagioclaseand less K-feldspar), quartz and biotite phenocrysts. Low quantity ofaccessories is represented: opaque minerals, apatite and zircon.

The tuffs and volcanites of the western Soledad caldera (13samples: No. 8/1-3 and 8/5-6 with subsamples) have acidic-intermediate composition too. Welded dacitic-rhyodacitic tuffshave feldspar (mainly plagioclase), biotite, hornblende and minorquartz content in the vitric, pumiceousmatrix. Volcanites are dacites-rhyodacites with vitroporphyric fabric and similar phenocrysts as inthe volcaniclastics. The most abundant accessory is titanite.

5.2. Chemical analyses

Three different methods for chemical analyses of solid materials(XRFþ/-INAAþ/-PGAA) were carried out on 39 representativeceramic fragments e chosen on the basis of microscopic studies e ,

four adobe remnants and 36 geological comparative samples(Table 1). Two separate ways of processing the raw data wereapplied: 1) plotting of element concentrations in normalized,multi-elemental abundance (so called spider-) diagrams and 2)displaying the concentrations in bivariate correlation diagrams,using element ratios instead of absolute concentrations. This way, itwas possible to better outline the similarities and differencesamong the individual samples. The normalization of the multi-elemental abundance patterns was done relative to an averagevalue for Post Archaean Australian Shale (PAAS) which isa preferred standard material in geochemical sedimentary rockinvestigations for fine grained siliciclastic sediments (Nance andTaylor, 1976; Taylor and McLennan, 1985; McLennan, 1989, 2001).

The interpretation of the spider diagrams using groups definedby petrographic characteristics made it possible to check and provethe coherence of the groups by an independent method. For thisreason see Fig. 5 for each group and subgroup. Group I can begenerally characterized with basically average (similar to PAAS)major and trace element concentrations (Fig. 5aed). This pattern isaccompanied with a slight enrichment of specific cations in thesilicate phases (MgO, CaO, Na2O), P2O5, mobile trace elements (Rb,Sr, Ba), Zn and light rare earth elements, while TiO2, Fe2O3, Yb, V, Crand Co show lower concentrations compared to the referencematerial. In the cases of I/A, I/B and I/D subgroups geochemicalcomposition supports the petrographic classification, the membersof the groups are similar to each other from the point of view of thedistribution of the immobile major and trace elements. In contrastwith other subgroups of petrographic group I, subgroup I/C isincoherent from both a petrographic and a geochemical point ofview. This feature expresses the heterogeneity of the applied rawmaterials of this subgroup concerning the mineralogy of both theclay paste and the aplastics. Although some immobile elements (Zr,Nb, Y) show similar relative content in subgroup I/C, most of thesilicate cation position filling major elements vary. This character-istic makes it very probable that the individual members of thissubgroup originated from different sources.

Both major and trace element distribution of ceramics of groupII are more similar to the average composition of PAAS (Fig. 5eef).

Fig. 3. Archaeological styles of ceramic appearing at Paria Basin exemplified by plates (aeb) and bowls (cee).

V. Szilágyi et al. / Journal of South American Earth Sciences 36 (2012) 1e1710

Author's personal copy

The most variable elements are Ca, P and Eu, Zn. The completegroup II is quite coherent especially in the case of immobile traceelements. Concerning this petrographic group, on the base ofgeochemistry the subgroups cannot be distinguished as unequiv-ocally as by petrography. However, some tendencies can be out-lined in connection with the average grain size and clay content of

aplastics: i.e. finer grained subgroup II/A (with claystone/shalefragments) shows partly higher CaO and lower Eu concentrationsthan the coarser grained samples.

The major and trace element distribution of petrographic groupIII is basically different from that of the previous types (Fig. 5geh).The high TiO2, Al2O3 and average rare earth element content, and

Fig. 4. Thin section photomicrographs of the main petrographic types of pottery.

V. Szilágyi et al. / Journal of South American Earth Sciences 36 (2012) 1e17 11

Author's personal copy

Fig. 5. Major and trace element distribution of the main petrographic types of pottery.

V. Szilágyi et al. / Journal of South American Earth Sciences 36 (2012) 1e1712

Author's personal copy

the low Fe2O3, MgO, CaO and Co content of the sample underlinesa peculiar chemical character. This supports the idea of a differentgeological origin of the third group, although this suggestion isbased on one measurement only.

To present the geochemical characteristics of ceramic andcomparative sediment/rock groups, absolute concentrations as wellas ratios of elements of geochemical significance in provenanceanalysis were applied. This led us to the conclusion that immobileand partly incompatible major and trace elements should bepreferred. Fig. 6 shows bivariate correlation diagrams of major(Fig. 6a) and trace (Fig. 6b) element ratios. The main clusters ofceramics in Fig. 6a group to the lower left part of the diagramwhichcan be explained by the predominance of the finer grained andmore clay containing (with higher Al2O3 concentrations) rawmaterials (grouping in field B below the red broken line). Those canbe separated into petrographic group I with lower and group II andIII with higher K2O/Na2O ratios. The single representative of groupIII has the lowest SiO2/Al2O3 value. Considering the potential rawmaterial samples, it can be stated that major element ratios cannotdistinguish the two volcaniclastic sources: both groups of tuffs andvolcanites have relatively low major element ratios (marked withfield A).

In contrast, chemical composition of the Silurian sedimentaryrocks and sediments of the Paria Basin and of the adobe samplesdisperse in a wide range. This complex data set can be separatedinto two main clusters: a low SiO2/Al2O3 e high K2O/Na2O one anda high SiO2/Al2O3 e low K2O/Na2O one. The former is identical withthe Al2O3-rich, clayey (fine grained) sediments/rocks (marked withfield B below the red broken line), while the latter resembles thecoarser grained siliciclastic materials (above the red broken line).The trace element values and ratios in Fig. 6b outline a quitecompact grouping of ceramic samples with medium TiO2/Al2O3(0.03e0.05) and medium Yb (20e40 ppm) values. Samples ofpetrographic group II shows a bit higher Y and lower TiO2/Al2O3

values than that of group I on the average. In this bivariate diagram,the tuff related samples of the two volcaniclastic sources (low-medium TiO2/Al2O3 and low Y values) can be better distinguishedfrom each other (though they still do not have discriminativeimportance) since Morococala’s samples have lower TiO2/Al2O3ratios than Soledad’s ones. When we use this combination ofelement ratios, sediments and Silurian sedimentary rocks of theParia Basin and the adobe samples can be separated much betterand form much clearer distinctive groups than in the major

element diagram. However, the coarser grained sediments/rockscluster closer to the higher TiO2/Al2O3 and lower Y values.

Using the bulk chemistry for the characterization of theceramics, the separation of the specimens into certain subgroups isnot that clear, easy and evident as with petrography. However, thepetrographic groups I and II can be quite clearly distinguished andtheir relation to the potential raw material sources can beassumed, additionally, almost all of the immobile major and traceelements suggest the same relationships. This outlines theimportant role of aplastic inclusions in the bulk composition ofceramics. The sample set of petrographic group I (marked withfield C) is between the clusters of the pyroclastics (both Moroco-cala and Soledad, marked with field A) and of the finer grainedsediments of the Paria Basin (marked with field B). On the otherhand, the cluster of the petrographic group II overlaps well withthe set of the finer grained sediments of the Paria Basin, andespecially to the archaeological adobes from Paria and partly thebrick clays of the eastern rim of the Altiplano. It was not possible tomake a distinction between the two pyroclastic sources based onthe bulk chemistry. Utilizing the major element ratios, the finer(clayish-silty) and the coarser (sandy-gravely) sediments of thealluvial plain of the Paria basin could be separated. It was animportant feature that all of the investigated ceramics clusteredrather closer to the finer than to the coarser grained sediments.

5.3. Phase analyses

Instrumental mineralogical examination was used to determinethe crystalline and weakly crystalline phases of the fine grainedpaste of the ceramics. Interpreting these data, the estimation of themaximum firing temperature and the basic characterization of thefiring atmosphere could be done. In addition, further examinationof the firing conditions is planned. The XRD analyses were per-formed on the complete ceramic assemblage (206 pieces).

Fig. 7 shows typical representatives of each petrographicceramic group. The basic mineral phases of group I subtypes (thelower curves in Fig. 7) are quartz, different feldspar types (plagio-clase and K-feldspar) with variable crystallization stages and 10Å-type phyllosilicate phase (illite-sericite, sometimes muscovite-biotite with (002) basal reflection at 9.98 Å, weak (110) reflectionat 4.48 Å, weak triplet between 2.70 and 3.00 Å). Weak elevation ofthe baseline between 3 and 4 Å indicates the presence of amor-phous phase, especially in the case of subgroups I/A and I/B. In

Fig. 6. Discrimination of the main petrographic types (I, II, III) of pottery by geochemically significant element ratios. (a) K2O/Na2O vs. SiO2/Al2O3 and (b) TiO2/Al2O3 vs. Y diagrams.Legend: 1 e fine-grained alluvial sediments (clay-silt), 2 e coarse-grained alluvial sediments (sand-gravely sand), 3 e adobes, 4 e Palaeozoic sedimentary rocks, 5 e alluvial clayfrom recent brick mine, 6 e Soledad tuffs, 7 e Morococala tuffs, 8 e petrographic type I of ceramics, 9 e petrographic type II of ceramics, 10 e petrographic type III of ceramics;A e cluster of potential tempering materials of volcaniclastic origin, B e cluster of potential clayey paste materials of sedimentary origin, C e cluster of 1st group ceramics whichcould be modelized.

V. Szilágyi et al. / Journal of South American Earth Sciences 36 (2012) 1e17 13

Author's personal copy

addition, amphibole is present in subgroups I/A and I/D, andgoethite and hematite are in quantities of accessories. Based on themineral assemblage, no significant phase changes could be detec-ted, so the estimated maximum firing temperature could notexceed the 650e700 �C.

Group II ceramic (second curve from the top in Fig. 7) has highquartz content too, but its 10Å-type phyllosilicate is rather illite(with expressed (110) reflection at 4.49 Å, moderated (002) basalreflection at 9.98 Å and (004) reflection at 4.95 Å) and its feldsparphase is more monotypical (plagioclase). Some dolomite and traceof hematite are also present. Similarly to the samples of group I ofpottery, no high-temperature phase formation during the firingwas observed. The maximum firing temperature is estimated to bebetween 650 and 700 �C (since the carbonate content is secondary,it is irrelevant in the calculation).

Group III of pottery (uppermost curve in Fig. 7) has an absolutelydifferent XRD pattern. Together with the predominant quartz, phyl-losilicate phase with basal reflection at 9.32 Å, mullite phase (withpeaks at 5.39 Å, 4.66 Å, 3.43e3.46 Å) and an unidentifiable phaseat 3.11 Å are detectable. In addition, a small amount of K-feldsparand hematite could be identified. Due to the neoformed Al-silicate(mullite) phase, the mineral assemblage indicates high-temperature

recrystallization of the matrix at about 850e950 �C maximum firingtemperature.

Variable but permanent presence of hematite in the ceramicmaterial signifies the basically oxidative character of the firingatmosphere, even in the case of the entirely white walled vessels(e.g. petrographic group III).

6. Discussion

6.1. Provenance

Petrographic observation of ceramic fragments resulted in theclassification of the assemblage into threemain aplastic constituentmaterial groups: (I) pyroclastic and volcanic originated, (II) sedi-mentary rock originated and (III) metamorphic rock originated.Based on the aplastics’ petrology-mineralogy and the fabricfeatures, subgroups could be separated inside those groups. Con-fronting this result with the geochemical data of the local rocktypes and the knowledge on the geological setting, the applied rawmaterial (temper) sources of the first ceramic group have to be thepyroclastic areas of both the Morococala Volcanic Field and theSoledad Caldera (10e30 km far from the site, so these are near

Fig. 7. Mineralogical compositions of the main petrographic types of pottery by XRD.

V. Szilágyi et al. / Journal of South American Earth Sciences 36 (2012) 1e1714

Author's personal copy

sources). On the one hand, this conclusion contradicts Arnold’s idea(Arnold, 2005) that pottery rawmaterial comes from notmore thana 7 km distance (if we presume that the place of manufacture wasin the archaeological site of Paria and not outside of the settle-ment). On the other hand, it is in agreement with recent publica-tions which identify the source area of ceramicmaterials at a longerdistance (Valera Guarda, 2002; Alden et al., 2006). The provenancestatement for the second ceramic group is that the utilized rawmaterial (untempered silty clay paste) came from the alluvial plainof the Paria basin (max. 5 km distance from the site, so it is a localsource). There is no potential source of the third ceramic group,neither in the vicinity nor in the wider surroundings (w50 km) ofthe site. This information and the fact that the third ceramic groupis presentedwith a very low ratio in the pottery assemblage suggesta foreign (imported) origin of the petrographic group III.

There was a purposive selection of the sedimentary rockderived, fluvial sediments as raw materials both for pottery andadobe production. The adobe samples clearly agree with thegeochemical composition of the fine grained sediments of the PariaBasin. Since these adobes show expressed similarity to the materialof the second ceramic group, this provides further evidence of thelocal origin of the ceramic group II. It is not clear that the collectedlocal fine grained sediments could provide the raw material (claypaste) for petrographic group I.

Based on the fact that tuff and partly volcanic lithofragments ingroup I of ceramics are mostly quite unweathered, a raw materialsite near to the original, physically unweathered rock outcrop has tobe assumed. However, for some subgroup I/C samples it has to bementioned that: on the one hand, the grain size and the quantity ofcertain lithic clast types does not always correlate, while on theother hand, the quantity and the unweathered condition of theclasts directly correlates.

As was already discussed by others (Bray et al., 2005), it is veryprobable that it was not only the shape and decoration that rep-resented value in the classical Inka imperial pottery but thematerial itself (and its source) too. In addition to this, it isa common feature throughout the Andes in space and time thatvolcanic and tuff rocks were used as temper of the ceramics (Ixerand Lunt, 1991; Velde and Druc, 1999a) and this can be traced inthe present-day traditional handicraft too (Arnold, 1972). Based onthese suggestions, it is possible that in the case of Paria the usage ofvolcaniclastic rocks was not a chance of the Inka ceramic makingpotters but a conscious selection of a more highly esteemedmaterial.

Combining archaeometrical results with the basic archaeolog-ical data on the ceramic artefacts leads to new insights. It is veryprobable that the material used relates rather to the vessel styles(quality and stylistic features) and e in this way e to the age of theartefacts than to the function. This idea is supported by the fact thatpotteries of Inka and Inka-Colonial Period are entirely classifiedinto the petrographic group I, while potteries of the Late Interme-diate Period are only from the petrographic group II. Anotherimportant observation relates to the Inka Period ceramic assem-blage. On the one hand, Inka style (high-quality Inka Imperial andInka pacaje) potteries can almost entirely (96%) be connected to thepetrographic group I (and about two-third to subgroup I/B). On theother hand, lower-quality Inka-imitating local potteries, artefactswith a mixed style (of both Late Intermediate and Inka) and LateIntermediate Period ceramics excavated from Inka buildings arealmost entirely (93%) classified into the petrographic group II.

These observations suggest that the local alluvial sediments ofthe Paria Basin were utilized for pottery manufacturing from theearlier periods (Late Intermediate) and stayed in use during theInka Period for the making a local product imitating the imperialfashion (i.e. the Inka local style). In addition, this raw material is

basically used for lower quality coarse ware production. In contrast,pyroclastic rocks of the surroundings of the Paria Basin becamecommonly used as tempering materials of fine wares during theInka period and especially for the Inka Imperial style pottery.

6.2. Technology

Information on the manufacturing technology of pottery couldbe obtained from the fabric investigations by petrographic micro-scope and phase analysis by XRD. The results of the former methodhave shown a basic difference concerning the three petrographicgroups of ceramics. The first group of ceramics was formed froma mixture of artificially added temper and a relatively pure(elutriated?) clay paste which proved to be a high quality, fine tomedium-grained raw material. The pumiceous clasts of subgroupI/A are artificially added (temper) since fresh, angular grains couldnot survive as natural components of a clayey sediment (weath-ering product). Unweathered, angular clasts of subgroup I/B are alsoadded to the paste as temper. The only exceptions are the repre-sentatives of subgroup I/D (these samples have an almost serialfabric, so it is not very probable that it was created intentionally).The utilization of unweathered rock fragments has modern analo-gies (Velde and Druc, 1999b; Ixer and Lunt, 1991). The method ofthe preparation could be e similarly to the present-day techniquese the exploiting, crushing, sieving and mixing with the clay paste.

The second ceramic group contains fragments of vessels man-ufactured from untempered silty clay which was a natural mixtureand potters used this lower quality, coarser grained materialwithout any significant elaboration (e.g. elutriation).

Clastic components of group III are natural parts of the mixture,and the fabric suggests the usage of the primary weatheringproduct near to the rock outcrop as the raw material. It means thatthe third group of pottery was made from a natural (untreated),coarse grained, sandy-silty clay which could be exploited from theimmediate vicinity of the rock outcrop.

The XRD technique provided information on the firing condi-tions of the ceramic production. In contrast with the case of the rawmaterial preparation types, it is not possible to make significantdistinctions between the first and second petrographic groups ofceramics. Characterizing these pottery groups together, it can besaid that the majority of the ceramics of Paria was fired at the sameor similar circumstances, namely at 700e900 �C maximum firingtemperature and in a dominantly oxidizing but varying atmosphere.

These statements are just partly in agreement with the formerconclusions on Inka pottery. For coastal and Lake Titicaca regionceramics Wagner et al. (1989) suggested a higher, 850e1000 �Cfiring temperature by Mössbauer spectroscopic investigations. Theatmosphere of the pottery firing in Paria is similar to the typicalInka imperial ceramic style, which is hard reduction fired withsurface oxidation (sandwich structured) or oxidized throughout incross section (Menzel and Riddell, 1986).

In contrast, the third petrographic group of pottery can bedistinguished from the former ones concerning even the firingconditions. The presence of the neoformed, high-temperature phase(mullite) suggests a higher (850e950 �C) maximum firing tempera-ture. The final surface colour is white and in cross sectionwhite, lightgrey or pale rose. These differences e together with the foreignmaterial utilization e suggest a pottery making technology isolatedfrom the Inka imperial fashion or the typical highland traditions (Ixerand Lunt, 1991). However, the vessel shapes and principally theirdecorations are typical Inka forms (plates) which can rather indicatea separated, well defined Inka pottery manufacturing workshop.

The above estimated firing temperatures do not contradict theidea of open pit firing suggested by others (Ixer and Lunt, 1991;Hayashida, 1998; Sillar, 1997). Although some pottery workshop

V. Szilágyi et al. / Journal of South American Earth Sciences 36 (2012) 1e17 15

Author's personal copy

sites have been identified by finding equipments of manufacturing(e.g. Hayashida, 1998; Donnan, 1997), no actual Inka kiln remnantshave ever been found.

7. Conclusions

The first detailed archaeometrical investigations on InkaPeriod ceramics from the territory of Bolivia were carried out onexcavated and surface finds of the Paria Basin (Dept. of Oruro). Toget information on the raw material usage and the manufacturingtechniques applied by the potters, we made a comparative anal-ysis of the ceramic fragments, other archaeological artefacts(adobes/plasters, building stones) and potential raw materials(fine grained sediments for the clay paste and clastic materials forthe temper).

Applying classical geological methodology (petrology, instru-mental mineralogical and chemical investigations), answers to thethree main questions raised in this paper are the followings:

(1) Raw materials and sources used during the Late IntermediatePeriod continued to be utilized during the Inka Period.However, some additional raw materials, sources and tech-niques also came in fashion. The reason of the introduction ofthe “new” materials and techniques could be the demand fora larger amount and higher quality of vessels in the imperialsystem.

(2) Neither Inka Imperial nor other Inka Period ceramics e exceptfor the special white ware e proved to be an import product.Their raw material sources could be identified in thesurroundings of the archaeological site of Paria or the PariaBasin. This statement supports the idea that e instead oftransporting vessels e imperial handicraft techniques and/orartisans were brought to Paria from other regions of the Empireto supply the demands of the high level standardized potterymanufacture, as also occurred in the region of Lake Titicaca(Murra, 1978; Spurling, 1992).

(3) Inka Imperial and local-style vessels show clear differences intheir material. For Inka local pottery manufacturing, the near-est (max. 5 km distant), local raw material sources (petro-graphic group II) were used. These sources had functionedalready in the Late Intermediate Period and the tradition stayedalive even after the Inka conquest of the Paria Basin, and duringthe standardization process which influenced the local ceramicmanufacture. For Inka Imperial pottery making, two additionalnear (10e30 km distance) sources supplied tempering mate-rials (petrographic group I). These volcanic related materials(just like the tempering technique itself) gained an importantrole in the ceramic handicraft during the Inka period mostprobably because of the quality requirements and/or thequantity demand of the newly introduced, Empire-relatedceramic style.

An important result is that the limited group of pottery withunique outlook (group III of ceramics) proved to have foreign origin,suggesting a long distance connectionwith a different region of theInka Empire. Taken altogether, we find that the pottery supplysystem of the Paria region is rather complex. Our applied geologicalstudy provided useful and fundamentally new information aboutInka Period pottery making system of the Paria Basin for thearchaeological research.

Acknowledgements

The archaeological project was carried out with the permissionof the Dirección Nacional de Arqueología, Bolivia, and was

financially supported by the OTKA Hungarian Scientific ResearchFund (Grant T 047048), the Curtiss T. & Mary G. Brennan Founda-tion and the Heinz Foundation. The PGAA experiments have beendone at the Budapest Neutron Centre, with the support of NAPVENEUS05 Contract No. OMFB 00184/2006. The geological fieldwork was supported by the Hungarian Geological Society. Theauthors are thankful to Carola Condarco (project Co-Director),Alvaro Condarco Castellón and Mile Vargas Rosquellas (Oruro,Bolivia). A special thank to Margit Csömöri (Dept. of Petrology andGeochemistry, Eötvös Loránd University of Budapest) for givingefficient help in the sample preparation. For the careful reading andlinguistic corrections of the manuscript, many thanks to dr. Jesse L.Weil and dr. Katalin Gherdán.

References

Alden, J.R., Minc, L., Lynch, T.F., 2006. Identifying the sources of Inka period ceramicsfrom northern Chile: results of a neutron activation study. Journal of Archae-ological Science 33, 575e594.

Arnold, D.E., 1972. Mineralogical analyses of ceramic materials from Quinua,Department of Ayacucho, Peru. Archaeometry 14/1, 93e102.

Arnold, D.E., 2005. Linking society with the compositional analyses of pottery:a model from comparative ethnography. In: Livingstone Smith, A., Bosquet, D.,Martineau, R. (Eds.), Pottery Manufacturing Processes: Reconstruction andInterpretation. BAR International Series, vol. 1349. Archaeopress, Oxford,pp. 15e21.

Belgya, T., Révay, Zs, 2004. Gamma-ray spectrometry. In: Molnár, G.L. (Ed.), Hand-book of Prompt Gamma Activation Analysis with Neutron Beams. KluwerAcademic Publisher, Dordrecht, pp. 71e111.

Bertolino, S.R., Fabra, M., 2003. Provenance and ceramic technology of pot sherdsfrom ancient Andean cultures at the Ambato valley, Argentina. Applied ClayScience 24, 21e34.

Bray, T., 2004. La alfafería imperial Inka: una comparación entre la cerámica estataldel area de Cuzco y la cerámica de las provincias. Chungará e Revista deAntropología Chilena 36, 365e374.

Bray, T.L., Minc, L.D., Ceruti, M.C., Chávez, J.A., Perea, R., Reinhard, J., 2005.A compositional analysis of pottery vessels associated with the Inca ritual ofcapacocha. Journal of Anthropological Archaeology 24, 82e100.

Choi, H.D., Firestone, R.B., Lindstrom, R.M., Molnár, G.L., Mughabghab, S.F., Paviotti-Corcuera, R., Révay, Zs., Trkov, A., Zerkin, V., Chunmei, Z., 2007. Database ofPrompt Gamma Rays from Slow Neutron Capture for Elemental Analysis.International Atomic Energy Agency, Vienna.

Cieza de León, P., 1973. La crónica del Perú [1553]. Promoción Editorial Inca S.A.,Lima.

Cieza de León, P., 1985. Crónica del Perú. Segunda parte [1553]. Pontificia Uni-versidad Católica, Lima.

Costin, C.L., 2001. Production and exchange of ceramics. In: D’Altroy, T.N.,Hastorf, C.A. (Eds.), Empire and Domestic Economy. Kluwer Academic/Plenum,New York, pp. 203e240.

D’Altroy, T.N., 1992. Provincial Power in the Inka Empire. Smithsonian InstitutionPress, Washington, D.C., 272 pp.

De Corte, F., 1987. The k0-standardization method e a move to optimization of NAA.PhD Thesis, University of Gent.

Donnan, C.B., 1997. A Chimu-Inka ceramic-manufacturing center from the northcoast of Peru. Latin American Antiquity 8, 30e54.

Fazekas, B., Östör, J., Kis, Z., Molnár, G.L., Simonits, A., 1997. The new features ofHypermet-PC. In: Molnár, G., Belgya, T., Révay, Zs (Eds.), Proceedings of the9th International Symposium on Capture Gamma-Ray Spectroscopy andRelated Topics, Budapest, Hungary, October 8e12. Springer Verlag, Budapest,pp. 774e778.

Fazekas, B., Révay, Zs., Östör, J., Belgya, T., Molnár, G., Simonits, A., 1999. A newmethod for determination of gamma-ray spectrometer nonlinearity. NuclearInstruments and Methods A 422, 469e473.

GEOBOL, 1992. Carta Geológica de Bolivia, Hoja Oruro (1:100 000) Publicación SGBSerie I-CGB-11 (Página 6140).

GEOBOL, 1994. Carta Geológica de Bolivia, Hoja Bolivar (1:100 000) Publicación SGBSerie I-CGB-27 (Página 6240).

Govindarau, K., 1989. Compilation of working values and sample description for 272geostandards. Special Issue of Geostandards Newsletter, XIII.

Guaman Poma de Ayala, F., 1980. El primer nueva corónica y buen gobierno. [1613].In: Murra, J.V., Adorno, R., (Eds.), Vol. 3, Siglo XXI, México D.F.

GUM, 1993. Guide to the Expression of Uncertainty in Measurement. ISO, Geneva.Gutiérrez Osinaga, D.J., 2005. Avances en la arqueología de caminos precolombianos

en Bolivia tramo: Paria-Tapacarí (Sitios asociados y características formales deconstrucción del camino). Nuevos Aportes 3, 93e114.

Gyarmati, J., Varga, A., 1999. The Chacaras of War. An Inka State Estate in theCochabamba Valley, Bolivia. Museum of Ethnography, Budapest.

Hahn-Weinheimer, P.F., Hirner, A.V., Weber-Diefenbach, K., 1984. Grundlagen undpraktische Anwendung der Roentgenfluorezenzanalyse (RFA). Vieweg-Verlag,Braunschweig.

V. Szilágyi et al. / Journal of South American Earth Sciences 36 (2012) 1e1716

Author's personal copy

Hayashida, F., 1998. New insight into Inka pottery production. MASCA ResearchPapers in Science and Archaeology, Supplement to vol. 15(Andean Ceramics),pp. 313e335.

Hayashida, F., 1999. Style, technology, and state production: Inka pottery manu-facture in the Leche Valley, Peru. Latin American Antiquity 10, 337e352.

Hayashida, F., Glascock, M., Häusler, W., Neff, H., Riederer, J., Wagner, U., 2002.Technology and organization of Inka pottery production: archaeometricperspectives. In: Jerem E.T., Biró K., (Eds.), Proceedings of the 31st Interna-tional Symposium on Archaeometry, Central European Series 1, II, BARInternational Series 1043, Archaeopress-Archaeolingua, Oxford, pp.573e580.

Hayashida, F., Häusler, W., Wagner, U., 2003a. Technology and organisation of Inkapottery production in the Leche Valley. Part I: study of clays. Hyperfine Inter-actions 150, 141e151.

Hayashida, F., Häusler, W., Riederer, J., Wagner, U., 2003b. Technology and organi-sation of Inka pottery production in the Leche Valley. Part II: study of firedvessels. Hyperfine Interactions 150, 153e163.

Hyslop, J., 1984. The Inka Road System. Academic Press, Orlando.Ixer, R.A., Lunt, S., 1991. The petrography of certain pre-Spanish pottery from Peru.

In: Middleton, A., Freestone, I. (Eds.), Recent Developments in CeramicPetrology. Occasional Paper 81. British Museum Publications, London,pp. 137e164.

Jamieson, R.W., Hancock, R.G.V., 2004. Neutron activation analysis of colonialceramics from Southern Highland Ecuador. Archaeometry 46, 569e583.

Lindstrom, R.M., Révay, Zs, 2004. Beams and facilities. In: Molnár, G.L. (Ed.),Handbook of Prompt Gamma Activation Analysis with Neutron Beams. KluwerAcademic Publishers, Dordrecht, pp. 31e58.

McLennan, S.M., 1989. Rare earth elements in sedimentary rocks: influence ofprovenance and sedimentary processes. In: Lipin, B.R., McKay, G.A. (Eds.),Geochemistry and Mineralogy of Rare Earth Elements. Reviews in Mineralogy21, 169e200.

McLennan, S.M., 2001. Relationships between the trace element composition ofsedimentary rocks and upper continental crust. Geochemistry, Geophysics,Geosystems 2, 2000GC000109, 24 pp.

Menzel, D., Riddell, F.A., 1986. Archaeological Investigations in Tambo Viejo, AcaríValley, Peru 1954. Institute for Peruvian Studies, Sacramento.

Molnár, G.L., Révay, Zs., Paul, R.L., Lindstrom, R.M., 1998. Prompt-gamma activationanalysis using the k0 approach. Journal of Radioanalytical and Nuclear Chem-istry 234, 21e26.

Molnár, G.L., Révay, Zs., Belgya, T., 2002. Wide energy range efficiency calibrationmethod for Ge detectors. Nuclear Instruments and Methods A 489, 140e159.

Morgan, G.B., London, D., Luedke, R.G., 1998. Petrochemistry of Late Miocene Per-aluminous Silicic volcanic rocks from the Morococala field, Bolivia. Journal ofPetrology 39, 601e632.

Morris, C., 1978. The archaeological study of Andean exchange systems. In:Redman, C.L. (Ed.), Social Archaeology: Beyond Subsistence and Dating.Academic Press, New York, pp. 289e310.

Murra, J.V., 1972. El “control vertical” de un máximo de pisos ecológicos en laeconomía de las sociedades andinas. In: de Iñigo Ortíz de Zuñiga (Ed.), Visitasde la Provincia de León de Huánuco en 1562, Tomo II, pp. 429e468.

Murra, J.V., 1978. Los olleros del Inka: hacia una historia y arqueología del Qolla-suyu. In: Quesada, F.M.F., Pease, D. (Eds.), Historia Problema y Promesa:Homenaje a Jorge Basadre Sobrevilla. Pontificia Universidad Católica del Perú,Lima, pp. 415e423.

Murra, J.V., 1983. La organización económica del Estado Inca, third ed. Siglo XXI,México D.F.

Nance, W.B., Taylor, S.R., 1976. Rare earth patterns and crustal evolution e I.Australian post-Archean sedimentary rocks. Geochimica et Cosmochimica Acta40, 1539e1551.

Phillips, G.W., Marlow, K.W., 1976. Automatic analysis of gamma-ray spectra fromgermanium detectors. Nuclear Instruments and Methods 137, 525e536.

Plá, R., Ratto, N., 2003. Provenance archaeological studies of ceramic raw materialsand artefacts using instrumental neutron activation analysis: the cases ofChaschuil and Bolsón de Fiambalá (Catamarca, Argentina). In: Nuclear Tech-niques in Archaeological Investigations. IAEA, Technical Reports Series No. 416,Vienna, pp. 45e69.

Ratto, N., Orgaz, M., De La Fuente, G., Plá, R., 2002. Ocupación de pisos de altura ycontexto de producción cerámica durante el Formativo: El caso de la regiónpuneña de Chaschuil y su relación con el Bolsón de Fiambalá (Depto. Tinogasta,Catamarca, Argentina). Estudios Atacameños 24, 51e69.

Ratto, N., Orgaz, M., Plá, R., 2004. La explotación del alfar de La Troya en el tiempo:causalidad o memoria (Departamento Tinogasta, Catamarca, Argentina).Chungará e Revista de Antropología Chilena 36 (2), 351e363.

Ratto, N., De La Fuente, G., Plá, R., Orgaz, M., Moreno, M., 2005. Compositionalcharacterization of ceramic artefacts and clays: the utility of INAA to evaluatethe prehispanic integration between the Puna and the Bolsón de Fiambalá Area,Northwestern Argentina. In: Kars, H., Burke, E. (Eds.), Geoarchaeological and

Bioarchaeological Studies 3, Proceedings of the 33rd International Symposiumon Arcaheometry. Amsterdam, pp. 245e248.

Redwood, S.D., 1987. The Soledad caldera, Bolivia: a Miocene caldera with associ-ated epithermal Au-Ag-Cu-Pb-Zn mineralization. Geological Society of AmericaBulletin 99, 395e404.

Repartimiento de Tierras por el Inca Huayna Capac [1556]. Versión Paleográfica deDon Adolfo de Morales, 1977. Universidad Mayor de San Simon, Cochabamba.

Révay, Zs, 2006. Calculation of uncertainties in prompt gamma activation analysis.Nuclear Instruments and Methods A 564, 688e697.

Révay, Zs, 2009. Determining elemental composition using prompt gamma acti-vation analysis. Analytical Chemistry 81, 6851e6859. doi:10.1021/ac9011705.

Révay, Zs, Belgya, T., 2004. Principles of PGAA method. In: Molnár, G.L. (Ed.),Handbook of Prompt Gamma Activation Analysis with Neutron Beams. KluwerAcademic Publishers, Dordrecht, pp. 1e30.

Révay, Zs., Belgya, T., Ember, P.P., Molnár, G.L., 2001a. Recent developments inHypermet-PC. Journal of Radioanalytical and Nuclear Chemistry 248, 401e405.

Révay, Zs., Molnár, G.L., Belgya, T., Kasztovszky, Zs, Firestone, R.B., 2001b. A new g-ray spectrum catalog and library for PGAA. Journal of Radioanalytical andNuclear Chemistry 248, 395e399.

Révay, Zs., Belgya, T., Molnár, G.L., 2005. Application of Hypermet-PC in PGAA.Journal of Radioanalytical and Nuclear Chemistry 265, 261e265.

Révay, Zs., Belgya, T., Szentmiklósi, L., Kis, Z., 2008. Recent developments in promptgamma activation analysis in Budapest. Journal of Radioanalytical and NuclearChemistry 278, 643e646.

Révay, Zs., Firestone, R.B., Belgya, T., Molnár, G.L., 2004. Catalog and atlas of promptgamma rays. In: Molnár, G.L. (Ed.), Handbook of Prompt Gamma ActivationAnalysis with Neutron Beams. Kluwer Academic Publishers, Dordrecht,pp. 173e364.

Révay, Zs., Molnár, G.L., 2003. Standardisation of the prompt gamma activationanalysis method. Radiochimica Acta 91, 361e369.

Révay, Zs., Molnár, G.L., Belgya, T., Kasztovszky, Zs, Firestone, R.B., 2000. A newgamma-ray spectrum catalog for PGAA. Journal of Radioanalytical and NuclearChemistry 244, 383e389.

Rowe, J.H., 1944. An Introduction to the Archaeology of Cuzco. Papers of the Pea-body Museum of American Archaeology and Ethnology, Vol. XXVII, No. 2.Harvard University, Cambridge, Massachusetts.

Sillar, B., 1997. Reputable pots and disreputable potters: individual and communitychoice in present-day pottery production and exchange in the Andes. In:Cumberpatch, C.C., Blinkhorn, P.W. (Eds.), Not So Much a Pot, More a Way oflife: Current Approaches to Artefact Analysis in Archaeology. Oxbow Mono-graph Series, vol. 83, Oxford, pp. 1e20.

Spurling, G., 1992. The Organization of Craft Production in the Inka State: ThePotters and Weavers of Milliraya. Ph.D. Thesis, Department of Anthropology,Cornell University, Ithaca.

Szilágyi, V., Szakmány, Gy., . Comparison of volcaniclastic-tempered Inca Imperialceramics from Paria, Bolivia with potential sources. In: Quinn, P.S. (Ed.), Inter-preting Silent Artefacts: Petrographic Approaches to Archaeological Ceramics.Archaeopress, Oxford, pp. 211e225.

Szilágyi, V., Szakmány, Gy, Gyarmati, J., 2005. Inka kori kerámiák petrográfiaivizsgálatának el}ozetes eredményei (Paria, Bolívia). (Preliminary results of thepetrographic investigation of Inka Period ceramics (Paria, Bolivia)). Arche-ometriai M}uhely 2005/2, 42e47 (in Hungarian).

Szilágyi, V., Szakmány, Gy., Gyarmati, J., Tóth, M., 2007. Preliminary comparativearchaeometric results of colonial and Inka pottery in Paria (Oruro, Bolivia). In:Waksman, Y.S. (Ed.), Archaeometric and Archaeological Approaches toCeramics: Papers Presented at EMAC’05, 8th European Meeting on AncientCeramics, Lyon 2005. BAR International Series, vol. 1691. Archaeopress, Oxford,pp. 195e199.

Taylor, S.R., McLennan, S.M., 1985. The Continental Crust: Its Composition andEvolution. Blackwell Scientific Publications LTD, Oxford.

Vaca de Castro Cavallero, C., 1908. Ordenanzas de tambos. [1543]. In: Revista His-tórica, 3, pp. 427e492.

Valera Guarda, V., 2002. Enseñanzas de alfareros toconceños: tradición y tecnologíaen la cerámica. Chungará e Revista de Antropología Chilena 34, 225e252.

Velde, B., Druc, I.C., 1999a. Prehistoric Peru. In: Velde, B., Druc, I.C. (Eds.), Archaeo-logical Ceramic Materials e Origin and Utilization. Springer, Berlin, pp. 225e237.

Velde, B., Druc, I.C., 1999b. Modern ceramic production in the Andes. In: Velde, B.,Druc, I.C. (Eds.), Archaeological Ceramic Materials e Origin and Utilization.Springer, Berlin, pp. 237e247.

Wagner, U., Brandis, S.V., Marticorena, B., Salazar, R., Schwabe, R., Riederer, J.,Wagner, F.E., 1989. Mössbauer studies of ceramics from the Inca period. In:Maniatis, Y. (Ed.), Archaeometry: Proceedings of the 25th InternationalSymposium on Archaeometry. Elsevier, Amsterdam, pp. 159e168.

Williams, V.I., Vargas, C.S., Romero, A., Speakman, R.J., Glascock, M.D., 2006. InkaPottery Production and Consumption in NW Argentina, Northern Chile, andBolivia. In: Abstract for the 71st Annual Meeting of the Society for AmericanArchaeology, San Juan, Puerto Rico, 26e30 April 2006.

V. Szilágyi et al. / Journal of South American Earth Sciences 36 (2012) 1e17 17