Quaternary International 375 (2015) 13e26

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Quaternary International
journal homepage: www.elsevier.com/locate/quaint

Mud-clay banks and regional geochemistry: The provenance of

ceramic raw materials (Department Tinogasta, catamarca, Argentina)
Norma Ratto a, *, Valeria Gogni b, Mariano Bonoli Escobar b, Rita Pla

c
a
Museo Etnogra
fico Juan B. Ambrosetti, Facultad de Filosofía y Letras de la Universidad de Buenos Aires, Argentina
b
Facultad de Ingeniería de la Universidad de Buenos Aires, Argentina
c
Departamento Química Nuclear, Gerencia de Química Nuclear y Ciencias de la Salud-GAATEN, Comisio
n Nacional de Energía Ato

mica, Buenos Aires,
Argentina

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

Article history: In this paper, we carry out the multielement geochemical characterization of the different geological
Available online 2 September 2014 provinces existing in our study region (southwestern Tinogasta Department in the province of Cata-
marca, Argentina). We compare the regional geochemical profile with the profile of the sampled mud-
Keywords: clay banks that exist in different environments (valley, foothills, mountains, transitional puna) located
Multielement geochemical characterization in our region. In order to fulfill these goals, we use the geochemical information coming from the
Mud-clay banks
2769-IV. Then, we apply different multivariate sta-
georeferenced database topographic map Fiambala
Multivariate statistics
tistical techniques to compare both types of samples. We consider that it is important to understand the
Southwestern catamarca
Argentina
geochemical diversity and variability that the study area naturally provides, in order to more accurately
calibrate the cultural inferences made in studies of provenance of prehispanic pottery.
Statistical analysis shows a clear difference in the chemical profiles of the mud-clay samples and the
stream sediment ones located in the cordilleran transitional zone (“Cordillera Frontal”) respect to other
areas geological provinces (Famatina System and “Sierras Pampeanas”). However, we could not
demonstrate that mud-clay samples of the archaeological area of La Troya alfar (Famatina System)
presented a chemical profile that distinguishes them from others coming from similar environments, but
in other geological provinces. However, their profile is more homogeneous than that of other samples
from the Famatina System. The study demonstrates the high geochemical variability of the Abauca
n
extensive river basin, because of its geological history and the characteristics of its hydrographic
network.
© 2014 Elsevier Ltd and INQUA. All rights reserved.

1. Introduction approaches. These began with analysis with trinocular micro-

Studying the provenance of ceramic pieces in archaeology re-
quires analyzing the raw materials with which they are manufac-
tured. The various actions performed for the production of pottery
(cleaning, sieving, mixing raw materials obtained from different
deposits, incorporating added inclusions or temper, etc.) can alter
the characteristics of the sources exploited. This creates a dynamic
and changing process, according to the cultural conventions of
every moment and region. Therefore, in order to understand the
relationship between the ceramic piece, as a finished product, and
the source of its raw material, it is necessary to use different
* Corresponding author.
E-mail addresses: nratto@filo.uba.ar, norma_ratto@yahoo.com.ar (N. Ratto),
valeria.gogni@gmail.com (V. Gogni), mbonoli@fi.uba.ar (M. Bonoli Escobar), rpla@
cae.cnea.gov.ar (R. Pl

a).
scopes; followed by mineralogical and petrographic characteriza-
tions through thin sections, and concluded with the application of
nuclear analytical techniques such as neutron activation analysis
(Ratto et al., 2013).
Instrumental Neutron Activation Analysis (INAA) meets the
basic requirements of sensitivity, precision, accuracy and selectivity
needed to address the discussion of archaeological problems such
as origin, trade, exchange and production of objects, as well as to
reconstruct economic relationships among past populations
(Bishop, 1980; Bishop et al., 1982a,b; Bishop and Neff, 1989; Neff,
1992, 1998; D'Altroy et al., 2000; Falabella and Andonie, 2003; Pla

and Ratto, 2003, 2007; Pla
, 2009; Ratto et al., 2009, 2013; among
others). The application of this technique allows the quantification
of the concentration of the elements that have a strong geochem-
ical differentiation during crystallization of igneous rocks. The
weathering of these rocks originates the materials used for the

http://dx.doi.org/10.1016/j.quaint.2014.07.018
1040-6182/© 2014 Elsevier Ltd and INQUA. All rights reserved.
14 N. Ratto et al. / Quaternary International 375 (2015) 13e26
Fig. 1. Orography and hydrography of Southwestern Tinogasta (Catamarca, Argentina).
manufacture of ceramic vessels. Elements such as rare earths (RE),
chromium (Cr), thorium (Th), scandium (Sc) and iron (Fe), among
others, are useful for mud-clay banks differentiation. Alkaline ele-
ments such as sodium (Na), potassium (K), rubidium (Rb), cesium
(Cs), calcium (Ca) and barium (Ba) are in feldspar structure, the
most abundant mineral in earth crust. High concentration of
transition elements such as cobalt (Co), iron (Fe), hafnium (Hf),
among others, can indicate the presence of metallic inclusions
coming from oxidized sediments.
With the support of this technique, it is possible to identify the
sources of the raw materials exploited by ancient potters, to locate
production facilities by integrating the results with those coming
from other artifacts or features, and to model the extension and
routes of distribution systems. INAA is a useful tool for the char-
acterization and differentiation of mud-clay banks and the goods
(vessels) made with them. This relationship, however, is not linear,
since the process of ceramic manufacturing is a complex practice
in which the added material (volcanic rocks and potsherds,
mixture of mud or other cultural conventions) for the preparation
of ceramic pastes can alter the chemical signature of the fragments
analyzed. Despite these precautions, archaeological ceramics can
be considered as “metamorphosed sedimentary rocks” (Glascock,
1992:11).
In the Chaschuil-Abauca
n Archaeological Project, we have
analyzed 73 regional samples by INAA at the Nuclear Analytical
Techniques Laboratory of the Ezeiza Atomic Center (Argentine
National Atomic Energy Commission-CNEA). These samples come
from potential mud-clay banks (pottery) that exist in different
environments (valley, foothills, mountains, transitional puna)
located at the southwest area of Catamarca province. Furthermore,
we have also analyzed 980 sherds using the same analytical tech-
nique. These sherds were recovered during the prospection of
archaeological sites, emplaced in the environments mentioned
above. The multielemental analysis of the samples of mud-clay
banks and sherds, together with technological analysis, conform
the database that allows us to discuss the regional social relation-
ships maintained over time (Pla
and Ratto, 2007; Ratto et al., 2007,
2013; among others). One of the problems we found was that the
incorporation of new samples to the analysis sometimes changed
the predicted groups, generated by multivariate numerical treat-
ments. At the current state of research, we can say that La Troya
alfar was exploited over time, by the societies of both the first and
second millennium (Ratto et al., 2004).Therefore, we consider that
it is important to understand the geochemical diversity and vari-
ability that the study area naturally provides, in order to more
accurately calibrate the cultural inferences. This will also allow us to
identify those distinguishing features that make it possible to
differentiate one environment from another, based on their
geochemical characteristics. In this way we will be able to deter-
mine if the mud-clay banks of La Troya can be differentiated from
other sampled banks in the region, taking into account their spe-
cific geochemical characteristics. It is important to note that the
area of La Troya presents other evidence of ceramic production in
addition to the abundance of raw material, such as kilns for firing
pottery, fuel resources and climatic conditions (Ratto et al., 2002,
2004, 2010; De La Fuente, 2007; Feely, 2011; among others).
 N. Ratto et al. / Quaternary International 375 (2015) 13e26 15

Fig. 2. Geological provinces within the territory of the province of Catamarca (Argentina). Identification of the study area within the Department Tinogasta province of Catamarca.
Adapted of www.atlas.catamarca.gov.ar.

In this context, we first propose to carry out the geochemical
characterization of the different geological provinces existing in our
study region. We will then compare the regional geochemical
profile with the profile of the sampled mud-clay banks. In order to
fulfill these goals, we use the geochemical information coming
from the georeferenced database of topographic map Fiambala

2769-IV (SEGEMAR, 1998), and apply different multivariate statis-
tical techniques. This database contains the results of the analysis of
1129 stream sediment samples, coming from different areas within
the regions of Chaschuil and Fiambala
, situated in western Tino-
gasta Department (Fig. 1). Both regions are located in different
geological provinces within the province of Catamarca (Fig. 2).
Samples were analyzed for a set of 48 elements at Canadian labo-
ratories, applying Instrumental Neutron Activation Analysis (INAA)
(29:48) and Inductively Coupled Plasma Emission Spectroscopy
(ICP- ES) (19:48) (SEGEMAR, 1998).
2. Geological setting
A geological province is a region characterized by a particular
stratigraphic succession, a structural style of its own and specific
geomorphic features. Together, all these characteristics constitute
the expression of a particular geological history.
16 N. Ratto et al. / Quaternary International 375 (2015) 13e26
The province of Catamarca consists of four geological provinces:
Puna, “Cordillera Frontal”, “Sierras Pampeanas” and Famatina Sys-
tem (Ramos, 1999a; Varela, 2014). Of all these, only the last three
are located principally within the Department of Tinogasta (Fig. 2)
and present specific geological features.
The northern sector of the Cordillera Frontal geological province
is located to the west of the department of Tinogasta and presents a
wide prevalence of volcanics and pyroclastics, both rhyolitic in
composition (Ramos, 1999a,b). The structure of the Andean Cycle is
a strong contractional reactivation, forming a tectonic relief of high
mountains and some sedimentary basins and presenting moun-
tains with heights above 6000 m at the Argentine-Chilean border
(Varela, 2014). The area is a geological and orographic transition
between the two major sectors of the Andean massif (the Puna and
Andes Mountain Range). It is also called Volcanic Landscape of
Southwest Catamarca or Mountainous Transition Zone (Argerich,
1976). It is characterized by a landscape of mainly volcanic origin
that is not included in any of the surrounding morpho-structural
units. The limits are: the Puna (on the north), the Famatina Sys-
tem (on the northeast) and the “Sierras Pampeanas” (on the
southeast). The area still presents undefined aspects because the
extensive and thick outcrops of young volcanic rocks cover the
underlying geologic column, preventing accurate knowledge
(Papetti, 2003). While the volcanic landscape makes this area
similar to the Puna Province, it is topographically excluded from the
Puna plateau and presents both endorheic (internal, similar to the
Puna) as well as exorheic drainage, connected to the ocean. Vol-
canic processes prevail in the area (polygenic stratovolcanos-
formed by alternating outpourings of lava flows and pyroclastic
flows, formation of large domes, cinder cones and scoria). These
associations have been formed since the middle-upper Miocene,
and their products form the higher elevations of the region, where
the highest volcanoes of the world are located. The only depression
is the Laguna Verde “Bolson”, which presents the characteristics of
a saline beach. The whole area is above 4000 m a.s.l.
On the other side, the geological province “Famatina System” is
bordered by the Puna to the north, with “Cordillera Frontal” or
cordilleran transition zone to the northwest, and by the “Sierras
Pampeanas” to the southwest and east (Fig. 2). Its origins are in the
southern edge of the San Buenaventura mountain range, located in
the central sector of the Department of Tinogasta, ending in the
province of La Rioja, outside of the study area. The “Cordillera de
Narv
aez” extending north-south, constitutes the northern section
of the Famatina System (Fig. 2). In the Department of Tinogasta, it
covers a range of mountain blocks where the “Cordillera de
Narv
aez” stands out. The Guanchín River bisects it at “Quebrada La
Angostura”. This mountain range constitutes an orographic entity
primarily represented by outcrops of sedimentary and igneous
rocks (both volcanic and intrusive) of Paleozoic age. The volcanic-
sedimentary sequence consists of ignimbrites, pyroclastic flows
and re-deposited tuffs. Acidic and basic lavas, alternating with
epiclastic volcanic deposits that contain fossils, also are present
(Turner, 1967; Cisterna et al., 2010; Varela, 2014).
The “Sierras Pampeanas” Province constitutes the largest
igneous-metamorphic unit of Argentina, as well as of the province
of Catamarca (Fig. 2). Geologically, these hills are formed by a
crystalline basement consisting of metamorphic rocks, granites and
mixed rocks of Precambrian to lower Paleozoic age. This is the
fundamental unit of the system and represents 90% of the outcrops.
The “Sierras Pampeanas” are divided in two according to Caminos
(1979): Eastern and Northwestern. In the study region, the north-
western sector is divided into two areas (Fig. 2). The first opens as a
small wedge at the same latitude as Chaschuil, and is surrounded
by the “Cordillera Frontal” and the Famatina System; in addition,
the Pillahuasi River bisects the “wedge” (west to east). The second
area is limited to the west by the Famatina System, in the depres-
sion formed by the valleys of Fiambala
and Tinogasta, and to the
north is limited by the Puna. The “Sierras de Fiambal
a” and a small
section of the of the San Buenaventura mountain range are located
within the latter area (Fig. 2). It consists of a basement integrated by
a sequence of Precambrian meta-sedimentary rocks, including
schists, gneisses, migmatites and calc-silicate rocks affected by
episodes of metamorphism and deformation in the lower Paleo-
zoic, with the formation of syntectonic granitoids. Then, discordant
granitic stocks of post tectonic characteristics were intruded. It also
has dykes made of rhyolitic rocks (Gonza
lez Bonorino, 1972; Toselli
et al., 2003; Morello et al., 2011; among others). The San Buena-
ventura mountain range is composed of granitic and metamorphic
rocks of middle and low grade, with important volcanic
contributions.
This topography of alternating valleys and mountains is crossed
by rivers that form the basin of Abauca
n (Fig. 1). This river basin is
complex and receives tributaries that pass through different
geological provinces from its sources to its mouth in the Abauca
n
River (Argerich, 1976; Tineo, 1999). In the northern sector, the
Abauc
an receives inputs from rivers originating in the high peaks of
the Famatina System (“Las Papas”, “Chuquisaca”, “Rio Grande”,
“Colorado”, “Río de Abajo”) and the northwestern “Sierras Pam-
peanas” (“Tato
n”, “Agua del Me
dano”). In addition, it also receives
the waters of the Chaschuil or Guanchín River at the town of
Fiambala
. This river has a long course since it receives inputs from
tributaries originating in the geological province “Cordillera Fron-
tal”, then crosses the “Cordillera de Narv
aez” (Famatina System)
which also receives tributaries and finally drains into the Abauca
n
River. The rivers “La Troya” and “El Puesto” are also tributaries of
the main river. La Troya River is born in the Narva
ez mountain
range but receives the waters of the Tambería River, born in the
northwestern “Sierras Pampeanas” (western sector). Thus, the
rivers of the Abauca
n basin run through different geological prov-
inces. In this regard, Argerich (1976) said that the course of Guan-
chín or Chaschuil River establishes a hydric connection between
the basins of the “Sierras Pampeanas” and the highest mountain
range in the transition zone through the “Cordillera de Narva
ez”
(Famatina System).
3. Material and methods
3.1. Regional geochemistry
The relationship between the fields of geochemistry, mineralogy
and petrography can be understood when it is said that, “ … of the
various combinations of chemical elements, three thousand
different minerals existing on earth are formed (quartz, salt, feld-
spar, etc.). The aggregation of mineral particles forms what we call
rocks (eg. granite, limestone, basalt, sand, etc.). The science that
studies minerals is called mineralogy, the one that describes rocks,
Petrography, and the one that studies its own little bricks and their
“peregrinations” by nature, Geochemistry … ” (Fersman, 1971:15)
(translation of authors).
Particularly, mineral exploration geochemistry, or geochemical
prospection, applies the principles of element distribution in na-
ture to find indicators to locate mineral deposits of economic value.
Multi-elemental geochemistry allows the analysis of patterns of the
spatial distribution of elements and their geochemical associations.
The geochemical data of surface materials permits conclusions,
according to the general trends of geochemical mapping, that are
applicable and relevant to the geological and environmental
knowledge of the territory, as well as to mineral exploration
(Locutura et al., 2002). A geochemical anomaly is a variation in the
abundance of an element in comparison to its normal abundance in
 N. Ratto et al. / Quaternary International 375 (2015) 13e26 17

a defined area. For a general geochemical exploration, samples are
taken through an irregular pattern with large spacing between
sampling points. The samples are generally the sediments of rivers,
soils and rocks.
Part of the database used in this paper comes from the technical
data of the Regional Geochemistry Data topographic map Fiambal
a-
2769-IV (SEGEMAR, 1998). This contribution was part of the NOA
(Northwest Argentina) I -Geological Mining Prospecting Plans. At
each sampling point, samples of 100e200 g were taken. These
points were digitalized on satellite images. For the multi-elemental
geochemical analysis, mesh fraction <80 was selected. Samples
were ground to impalpable dust in tungsten carbide mortars,
following specific instructions to prevent contamination among
samples (SEGEMAR, 1998). A total of 1129 samples collected by the
Argentine Mining Geological Service (SEGEMAR) were analyzed by
Activation Laboratories Ltd. (ACTLABS) of Canada. Twenty-nine (29)
elements were determined (Au, As, Ba, Br, Ce, Co, Cr, Cs, Eu, Fe, Hf,
Hg, Ir, La, Lu, Na, Nd, Rb, Sb, Se, Sc, Sm, Sn, Ta, Tb, Th, U, W, Yb) by
INAA. However, Co and W results are not considered here, because
they were incorporated as contaminants by the grinding process.
Other elements were analyzed at the same laboratories using
Inductively Coupled Plasma Emission Spectroscopy (ICP e ES) but
are not considered in this paper. Only those elements also analyzed
by INAA at the Nuclear Analytical Techniques Laboratory, are re-
ported in Table 1, together with their detection limits (SEGEMAR,
1998). There is no other published information on quality control
for these elemental concentration results, although the analytical
data were considered as having high quality (SEGEMAR, 1998).
Thus, the number of elements is reduced from 29 to 20, excluding
Co measured by both laboratories.
3.2. Regional mud-clay banks: environmental and geochemical
characteristics
A clay material is any fine-grained, natural, earthy, argillaceous
material. Clay minerals are hydrous aluminum silicates and, in
some, iron and magnesium substitute for the aluminum, or alkaline
and alkaline earth elements are present as essential constituents
(Murrey, 2007). Clay minerals are divided into four major groups:
Kaolinite, Montmorillonite/Smectite, Illite or Clay-mica, and Chlo-
rite. These minerals occur under a fairly limited range of geologic
environments which include soil horizons, continental and marine
sediments, geothermal fields, volcanic deposits, and weathering
rock formations. In general, they occur where rocks are in contact
with water, air, or steam but the type of clay however is controlled
by the composition of pre-existing rock mineralogy. Prolonged and
extensive weathering alters the primary rock transforming min-
erals into clay minerals and under favorable conditions, leads to the
development of clay deposits. The weathering processes involve
physical disaggregation and chemical decomposition that changes
the original minerals in the rock forming clay minerals.
The sampled mud-clay banks are located at different altitudinal
levels (1465 to 4000 m a.s.l.) within our region of investigation (De
La Fuente, 2007; Pla
and Ratto, 2007; Ratto et al., 2009; among
others). In this paper, we consider only the samples of mud-clay
banks of the rivers flowing through different geological provinces.
At La Troya River (1475e1600 m.a.s.l.) and its tributary Tambería
River (3200 m.a.s.l.) 29 samples of mud-clay banks (27:29 and 2:29,
respectively) were taken. The first river is located in the Famatina
System geological province (“Cordillera de Narva
ez” e south
sector), and the others lie in the northwestern “Sierras Pampeanas”

Table 1
Samples collected by SEGEMAR (N ¼ 1129). Detection limit and descriptive statistics for the elements analyzed by INAA at ACTLABS of Canada (mean, standard deviation (SD)
and coefficient of variation (CV).

Element Detection limit (mg/g except Fe) Mean (mg/g) SD (mg/g) CV

As 0.5 17.9 34.8 194%

Ba 50 664 192 29%
Ce 3 97.5 45.0 46%
Cr 5 55.8 33.5 60%
Cs 1 9.2 12.0 130%
Eu 0.2 1.82 0.68 37%
Fe 0.01% 59,303 40,836 69%
Hf 1 8.73 3.75 43%
La 0.5 50.5 23.4 46%
Lu 0.05 0.460 0.250 54%
Rb 5 102.0 67.6 66%
Sb 0.1 0.871 1.460 167%
Sc 0.1 11.8 4.0 34%
Sm 0.1 7.63 3.45 45%
Ta 0.5 1.140 1.220 107%
Tb 0.5 0.583 0.544 93%
Th 0.2 16.4 9.13 56%
U 0.5 4.91 6.31 129%
Yb 0.2 2.87 1.580 55%

The samples (N ¼ 1129) collected by SEGEMAR and
represented in Fig. 3 come from points located within
different geological provinces (“Cordillera Frontal” 518:1129-;
Famatina System 344:1129-; Northwestern “Sierras
Pampeanas” 267:1129). The 344 samples from the Famatina
System correspond to points at both north and south of the river
Guanchín. Therefore, for the analysis we consider separately the

ez” (268:344 and
northern sector of southern “Cordillera de Narva
76:344, respectively). Samples from the “Sierras Pampeanas”
(western sector 133:267- and eastern sector 134:267) are
considered in a similar way.
(western sector). La Troya river samples from both its lower
(N ¼ 22) and upper (N ¼ 5) courses have secondary clays, altered
and transported by fluvial agents in a sedimentary environment. In
general, the region has high availability of ceramic raw material,
with excellent plasticity and workability for ceramic manufacture.
For the lower course samples, XRD showed all samples having good
quality, high clay (17e45%), low calcite (2%e5%) and feldspar (10%e
25%) and high quartz (24e45%), indicating that these mineral in-
clusions are a natural result of the deposit genesis.
The four samples from El Puesto river (1465 m a.s.l.) are similar
to the La Troya ones (lower course) and are also located within the
18 N. Ratto et al. / Quaternary International 375 (2015) 13e26

Famatina System geological province (“Cordillera de Narva
ez” e
south sector).
Mud-clay banks from the Guanchín river area (N ¼ 21) were
sampled from 1500 to 3000 m a.s.l. Deposits from higher altitudes
have significant sandy fractions and low plasticity. Macroscopic
characteristics of low altitude deposits are similar to those from the La
Troya river area, 25e40 km distant. All samples from Guanchín River
are located within the Famatina System, particularly, at the limit fixed
for dividing the “Cordillera de Narvaez” into southern and northern
sectors. As these samples were taken from the left bank of the river,
they correspond to the “Cordillera de Narva
ez” northern sector.
The eight samples from the Colorado River (1900 to
2200 m.a.s.l.) presented macroscopic characteristics similar to
those from the La Troya area, approximately 50 km distant. XRD
analysis indicated the presence of quartz, plagioclase, muscovite,
calcite and clays in all samples. Other minerals (dolomite, hematite,
gypsum, amphibole, clinoptilolite, etc.) with lower relative abun-
dance are present only in some samples. The clay fraction is present
in similar proportions in each sample. It was observed that samples
collected in the same area had different mineral loads. All these
samples (n ¼ 8) are located within the Famatina System geological
province but in the northern part of the “Cordillera de Narva
ez”.
The nine samples collected at higher elevations
(3500e4200 m a.s.l.) belong to the geological provinces of
“Cordillera Frontal” (6) and Northwestern “Sierras Pampeanas”
(western sector) (3). They correspond to secondary clays, altered
and/or transported and deposited according to the geomorpho-
logical and geological characteristics of the area. These deposits
have low availability but high plasticity and workability. Textural
analyses show high proportion of sandy textures, without differ-
ences among basins. XRD showed 50% good quality clays for
ceramic manufacture, low clay (10e25%), high calcite and high-
medium feldspar. Descriptive statistics of the multi-element
composition of the 73 samples is presented in Table 2.
reactor (current thermal flux 6.1013 cm2 s1, 8.5 Mw) for 3 h.
Two measurements were performed after approximately seven
and thirty-day decay respectively, for the determination of
twenty two elements: As, Ba, Ce, Co, Cr, Cs, Eu, Fe, Gd, Hf, La, Lu,
Nd, Rb, Sb, Sc, Sm, Ta, Tb, Th, U and Yb. However, not all elements,
such as As, Gd and Nd, were considered due to absence or low
concentrations, under the detection limit values, in some
samples.
The measurements were done using Ortec HP Ge detectors (30%
efficiency and resolution 1.8 keV for the 1332.5 keV Co-60 peak)
coupled to an Ortec 919 buffer multichannel analyzer module
(using Gamma Vision software for data acquisition). For concen-
tration calculation, software developed at the laboratory was used,
NIST standard reference material 1633b Coal Fly Ash was used as a
calibration standard, and NIST SRM 2709 San Joaquin Soil, China
National Research Centre CRM GBW07405 (GSS-5 soil) and inter-
laboratory standard andesite for quality assessment. The repro-
ducibility of the method was tested analyzing standard reference
materials NIST SRMs 2709 San Joaquin Soil and 699 Brick Clay
(Munita et al., 2001) and USGS AGV. Since 2001, the NAT laboratory
has been accredited under ISO/IEC 17025 standard by the Argentine
national accreditation body (OAA) and the current accredited scope
for geological and related matrices includes Ce, Cs, Co, Eu, Fe, La, Sc,
Sm, and Th.
3.3. Statistical methodology
Centered log ratio transformation was applied to compositional
data. This transformation allows us to work with relative rather
than absolute terms without losing information. Log ratios also
provide a simple and effective way of capturing the natural cur-
vature that is often found in compositional data sets. Log ratios are
admirably suited to investigating the ideas importance or irrele-
vance of single components (Aitchison, 1999).

Table 2
Samples of mud-clay deposits (N ¼ 73). Detection limit, descriptive statistics (mean, standard deviation (SD) and coefficient of variation (CV)) of the elements analyzed by INAA
at the Nuclear Analytical Techniques Laboratory (CNEA, Argentina)

Element Detection limit (mg/g except Fe) Mean (mg/g) SD (mg/g) CV

As 0.8 15.9 30.2 190%

Ba 60 506 133 26%
Ce 1.8 65.5 23.1 35%
Cr 3.1 33.8 12.8 38%
Cs 0.3 8.2 15.5 190%
Eu 0.089 1.24 0.40 32%
Fe 0.03% 31,148 10,143 33%
Hf 0.4 4.56 1.51 33%
La 0.5 35.0 14.3 41%
Lu 0.031 0.413 0.163 40%
Rb 6 99.1 38.0 38%
Sb 0.1 0.740 0.717 97%
Sc 0.05 10.9 4.9 44%
Sm 0.04 6.25 2.59 41%
Ta 0.23 0.941 0.375 40%
Tb 0.19 0.749 0.314 42%
Th 0.2 10.6 3.91 37%
U 0.4 3.52 1.52 43%
Yb 0.15 2.43 0.870 36%

The samples were prepared and analyzed by INAA at the
laboratories of the Nuclear Analytical Techniques Group of the
Ezeiza Atomic Center (Argentine Atomic Energy Commission)

and Ratto, 2007; Ratto et al., 2009; among others). Sample
(Pla
masses of about 100 mg were sealed in high purity quartz am-
poules and put into aluminum capsules, together with reference
materials for their irradiation. Irradiations were done at the RA-3
In order to determine whether geochemical information is
important in defining the geologic province, we use linear
discriminant analysis (LDA). In LDA, the groups are taken as given
and the aim may be to investigate whether defined groups are
chemically distinct (Baxter, 2004). Additionally, LDA indicates the
main chemical elements that discriminate each geological province
and their sectors.
 N. Ratto et al. / Quaternary International 375 (2015) 13e26 19

Fig. 3. Location of sediment samples from streams in Southwestern Tinogasta, Catamarca, Argentina (SEGEMAR, 1998).

Fig. 4. Biplot mud-clay deposits (N ¼ 73) classified by their location at the Geological Provinces.
20 N. Ratto et al. / Quaternary International 375 (2015) 13e26

The idea behind LDA is to find a linear function that maximizes
the group separation. The ratio of between-groups sum of squares
to the within-groups sum of squares is used as a measure of sep-
aration between groups. This linear function generates the first
canonical axis; a second discriminant function was generated in the
same way, searching for the best function to separate groups and
adding the condition of this second canonical axis, orthogonal to
the first one. The procedure is repeated until the discriminant G-1
axis is reached, where G is the total number of groups to
discriminate.
Analysis was performed on two different sets of data: first on
the analytical data of samples collected by SEGEMAR (N ¼ 1129),
and then on the mud-clay results (N ¼ 73). Infostat software (Di
Rienzo et al., 2012) was used to perform the analysis. The total
number of groups (G) was 5, according to the considered geological
provinces and their sectors (see Table 3).
4. Results and discussion
4.1. Mud-clay banks samples (N ¼ 73)
Each sample of mud-clay deposits was classified within a
particular geological province according to its sampling place. The
first multivariate statistical analysis was done to correlate the 73
mud-clay deposits samples to the groups representing the
geological provinces and their sectors. A 74% success rate was ob-
tained in the classification of these samples using the geological
provinces as the dependent variable. The multi-elemental con-
centration quantification of mud-clay deposits by INAA (N ¼ 73)
clearly shows the differentiation between the chemical profiles of
the cordilleran transition zone (“Cordillera Frontal”) and valley
samples (rivers Guanchín, La Troya, Colorado, etc). The valley
samples come from different altitudes (1465 m a.s.l. to
3000 m a.s.l.) and from the geological provinces of the “Sierras
Pampeanas” (eastern and western sectors) and the Famatina Sys-
tem (“Cordillera de Narv
aez”).
The first canonical axis is defined by the load of Lu, Cs and Sm,
while the second is mainly defined by Sc, Rb and Th. Fig. 4 shows
that the samples that came from the “Cordillera Frontal”
geological province (6), with elevations between 3800 and
4000 m a.s.l, are clearly different from the rest (67). This is due to
the loads of Lu and Cs, clearly different from Sm. The second
canonical axis differences the northern area of “Cordillera de
Narva
ez” (Famatina System) from the southern sector. The arbi-
trary limit was set on the Guanchín River which bisects the
geological formation. In this case, the different loads of Sc and Rb
together with Sm, are the ones that show the greatest differen-
tiation. The “Sierras Pampeanas” samples (eastern and western
sectors) are located on the surroundings of the coordinate axis
and do not present any element that discriminates them clearly
from the rest. However, their frequency is very low and weakens
the statistical analysis.
Multivariate statistical analysis was only able to correctly clas-
sify 74% of the cases. Therefore, it is interesting to analyze in which
geological provinces classifications mistakes happen. Table 3 shows
the location of each sample (mud-clay deposits) and the classifi-
cation obtained as a result of discriminant analysis. Nineteen cases
were classified within geological provinces that do not correspond
to the sampling location.
The 19 misclassified samples are located in the “Cordillera de
Narva
ez” (north and south sector) and the “Sierras Pampeanas”
(western sector). We believe that in some cases, this situation is
related to the location of the sampling site at the course of rivers.
For example, the Guanchín river samples were collected at different
altitudes along its course (3000 and 1500 m a.s. l.). It is also sig-
nificant that La Troya and El Puesto rivers show a high percentage of
wrongly classified cases. We also believe that this is related with
the rivers' dynamics, as both of them have tributaries originating in
the “Sierras Pampeanas” (western sector), crossing the “Cordillera
de Narv
aez” (southern sector) and finally flowing into the Abauca
n
river (“Sierras Pampeanas”-eastern sector). Finally, the samples of
Cazadero Grande River located in a ecotonal zone between three
geological provinces “Cordillera Frontal” Famatina System and
“Sierras Pampeanas” (western sector) also represent a wrongly
classified case.
The chemical profiles of the mud-clay banks allow us to differ-
entiate those from “Cordillera Frontal” respect to other geological
provinces. They also show the chemical variability of the Famatina
System, as the chemical profile of the northern sector of the
“Cordillera de Narvaez” is different from the southern one (arbi-
trary limit set by the Guanchín River). However, in the last case, we
recorded 26% mistakes in the classification. Samples located in the
“Sierras Pampeanas” show a low frequency. However, we obtained
more wrongly classified cases in the western sector.

Table 3
Discriminant analysis results for samples of mud-clay banks (log-ratio model). Highlighted in gray: (i) the frequency of samples correctly classified and (ii) the correct
classification rate.

Geological province the sampling Place of sampling Geological provinces (predicted) Total
area of mud-clay banks 
“C Narva
ez” 
“C Narvaez” “Sierras Pampeanas” “Sierras Pampeanas” “Cordillera
(northern sector) (southern sector) (western sector) (eastern sector) Frontal”

Famatina System.“Cordillera de Colorado River 6 1 0 1 0 8

Narv
aez” Guanchín River 15 3 3 0 0 21
(northern sector) (29:73) Subtotal 21 4 3 1 0 29
Percentage 72.41 13.79 10.34 3.45 0.00 100.00
Famatina System. “Cordillera La Troya River(lower course) 2 17 2 1 0 22
de Narvaez” La Troya River (upper course) 1 4 0 0 0 5
(southern sector) (31:73) El Puesto River (lower course) 2 1 1 0 0 4
Subtotal 5 22 3 1 0 31
Percentage 16.13 70.97 9.68 3.23 0.00 100.00
Northwestern “Sierras Tambería River (tributary 0 1 1 0 0 2
Pampeanas” La Troya River)
(western sector) (5:73) Cazadero Grande River 0 1 2 0 0 3
Subtotal 0 2 3 0 0 5
Percentage 0.00 40.00 60.00 0.00 0.00 100.00
 N. Ratto et al. / Quaternary International 375 (2015) 13e26 21

Table 3 (continued )

Geological province the sampling Place of sampling Geological provinces (predicted) Total
area of mud-clay banks
“C Narv

aez” “C Narvaez” “Sierras Pampeanas” “Sierras Pampeanas” “Cordillera
(northern sector) (southern sector) (western sector) (eastern sector) Frontal”

Northwestern “Sierras Abauca
n River 0 0 0 2 0 2

Pampeanas” Subtotal 0 0 0 2 0 2
(eastern sector) (2:73) Percentage 0.00 0.00 0.00 100.00 0.00 100.00
“Cordillera Frontal” (6:73) Las Lozas River 0 0 0 0 2 2
San Francisco Area 0 0 0 0 4 4
Subtotal 0 0 0 0 6 6
Percentage 0.00 0.00 0.00 0.00 100.00 100.00

Fig. 5. Biplot stream sediments (N ¼ 1129) classified by their location at the Geological Provinces.

4.2. Samples SEGEMAR (N ¼ 1129)
Each sample of stream sediment was classified within a
particular geological province according to their place of location.
In addition, river and/or sampled areas were identified with the
help of satellite images (Google Earth). The second statistical
analysis was to compare the multielemental composition of the
1129 stream sediment samples. A success of 74% was obtained in
the classification of these samples using the geological provinces as
the dependent variable. The multielemental characterization of
stream sediments by INAA (N ¼ 1129) show us the differentiation
between the chemical profile of the geological province “Cordillera
Frontal” respect to the other provinces (Famatina System and
Northwestern “Sierras Pampeanas”).
The first canonical axis is defined by the load of Fe and Yb, while
the second involves Eu, Sc and Ce. Fig. 5 shows that samples located
in the cordilleran transition zone (“Cordillera Frontal”, 518), with
elevations between 3800 and 4000 mas.l, are clearly different from
the rest (611). This is the result of the different Fe and Yb loads for
samples of the cordilleran transitional zone.
The analysis does not differentiate between the southern and
northern sectors of the “Cordillera de Narvaez”. However, there is a
tendency for Eu and Sc to predominate in the northern sector, while
Ce and Sb do that for the southern one. Fig. 5 shows a strong overlap
of the samples. A similar situation is found for the samples of “Sierras
Pampeanas” (east and west sectors) overlapping principally with the
samples from the “Cordillera de Narv
aez” (southern sector).
Multivariate statistical analysis was only able to correctly classify
71% of the cases. Therefore, it is interesting to analyze in which
geological provinces the mis-classifications happen. Table 4 presents
the geological province where each sample of stream sediments is
located and the classification obtained as the result of the discrimi-
nant analysis. A number of 331 cases were classified within geolog-
ical provinces that do not correspond to the sampling location.

Table 4
Discriminant analysis results for samples of stream sediments (SEGEMAR, 1998) (log-ratio model). Highlighted in gray: (i) the frequency of samples correctly classified and (ii)
the correct classification rate.

Geological province the Place of sampling Geological provinces (predicted) Total

sampling area (estimated)
“C Narv

aez” “C Narvaez” “Sierras Pampeanas” “Sierras Pampeanas” “Cordillera
stream sediments
(northern sector) (southern sector) (western sector) (eastern sector) Frontal”

Cortadera Area 0 0 3 20 1 24
El Quemado River 3 5 1 6 0 15
(continued on next page)
22 N. Ratto et al. / Quaternary International 375 (2015) 13e26

Table 4 (continued )

Geological province the Place of sampling Geological provinces (predicted) Total

sampling area (estimated)
“C Narv

aez” “C Narvaez” “Sierras Pampeanas” “Sierras Pampeanas” “Cordillera
stream sediments
(northern sector) (southern sector) (western sector) (eastern sector) Frontal”

Famatina System Anchoca River 8 3 1 1 2 15

“Narv
aez” e northern Colorado River and tributaries 6 7 0 0 1 14
sector (268:1129) de Abajo River 13 8 0 0 4 25
Río Grande and tributaries 59 1 3 4 3 70
Guanchín River (left bank) 3 7 4 4 2 20
Las Champas River 4 6 1 0 6 17
Punta de Agua River 8 0 0 0 0 8
Ranchillo River 31 2 1 0 0 34
Zanjo
n Apocango 12 3 5 0 6 26
Subtotal 147 42 19 35 25 268
Percentage 54.85 15.67 7.09 13.06 9.33 100.00
Famatina System. Serranía El Calvario 6 27 5 0 4 42
“Narvaez” e southern La Troya River (upper) 2 16 1 1 0 20
sector (76:1129) Guanchín River (right bank) 0 4 0 0 0 4
Southern Chaschuil 1 0 3 6 0 10
Subtotal 9 47 9 7 4 76
Percentage 11.84 61.84 11.84 9.21 5.26 100.00
Northwestern Campo de la Ojota 0 1 2 4 0 7
“Sierras Pampeanas” El Matambre 1 0 2 3 0 6
(western sector) (133:1129) La Troya River (upper) 0 1 2 5 0 8
Las Coipas River 3 2 7 3 12 27
Pastos Amarillos 0 0 7 7 0 14
Pillahuasi River and tributaries 1 21 24 5 1 52
Tambería River 1 3 14 0 1 19
Subtotal 6 28 58 27 14 133
Percentage 4.51 21.05 43.61 20.30 10.53 100.00
Northwestern “Sierras Antinaco River 1 2 0 19 0 22
Pampeanas”(eastern Chuquisaca River and tributaries 0 0 1 13 0 14
sector) (134:1129)
naga River
La Cie 0 0 0 7 0 7
Mesada Z
arate River 0 0 0 22 0 22
Tato
n River and tributaries 3 1 0 4 1 9
“Sierras de Fiambal
a” 9 22 6 23 0 60
(southern town Fiambal
a)
Subtotal 13 25 7 88 1 134
Percentage 9.70 18.66 5.22 65.67 0.75 100.00
“Cordillera Andes Mountain Range 7 0 3 1 175 186
Frontal” (518:1129) Area Aparejo lagoon 1 1 1 0 24 27
Area Frías lagoon 1 0 1 0 17 19
Area Negra lagoon 3 1 8 1 154 167
Las Lozas River 9 0 1 0 13 23
Las Peladas River 16 0 0 0 13 29
Cazadero Grande River (upper) 1 0 1 0 59 61
Vega San Francisco 2 0 1 0 3 6
Subtotal 40 2 16 2 458 518
Percentage 7.72 0.39 3.09 0.39 88.42 100.00

There is a high mis-classification percentage of the samples
(Table 4). Both the Famatina System and Northwestern “Sierras
Pampeanas” are distinct units regarding their geological history.
Therefore, the analysis fails when trying to differentiate those
units into sectors. Furthermore, there may also be other sources of
error such as errors while loading data, georeferencing, and defi-
nition of geological provinces, among others. The drainage
network might also be another factor to be considered in
conjunction with the abrupt terrain relief. The rivers in the area
define exorheic and endorheic basins. The wide catchment area of
the rivers and the vast expanses of the Abauca
n basin
(28,300 km2) affect the results.
Argerich (1976) said that the course of Guanchín or Chaschuil
River establishes a hydric connection between the basins of the
“Sierras Pampeanas” and the highest mountain range in the tran-
sition zone (“Cordillera Frontal”) through the “Cordillera de
Narv
aez” (Famatina System).
Interestingly, samples taken at the course of a river change their
geochemical characteristics depending on the altitudinal level of
the sampling point. Another error source might be the ecotonal
areas between geologic provinces. Regardless of these limitations,
the results allow some insights:
a. The cordilleran transition zone (“Cordillera Frontal”) is where
we recorded the lowest percentage of wrongly classified sam-
ples and where the chemical profile of the province is best
characterized. In this case, there are both exorheic and endo-
rheic basins.
b. Samples from the Famatina System (“Cordillera de Narvaez”) are
well ordered within the geological province but not in their
differentiation between northern and southern sectors of the
ridge. The rivers of this system flow towards both east and west,
a situation that can result in large geochemical variability. The
area is geologically constituted of volcanic and sedimentary
outcrops.
c. The “Sierras Pampeanas” (western sector) is the one that presents
the greatest geochemical “noise”. The area is enclosed between
two geological provinces (“Cordillera Frontal” and Famatina Sys-
tem). This situation creates high geochemical diversity, especially
because of the sampling scale used in this work.
 N. Ratto et al. / Quaternary International 375 (2015) 13e26
Fig. 6. Comparison of canonical discriminant functions (1 and 2) obtained in the analysis of mud-clay samples and stream sediment samples (SEGEMAR, 1998).
d. Samples from the “Sierras Pampeanas” (eastern sector) are the
second best classified after the “Cordillera Frontal” ones. The
geochemical diversity is related to the contribution of the
Famatina System and its relationship to the large Abauc

an river
basin.
4.3. Comparison between stream sediment samples and mud-clay
banks
The results presented above show that the loads of the elements
that discriminate the mud-clay samples and stream sediments are
very different (Fig. 6). This reduces the potential of multivariate
statistical analysis. In the previous section, we mentioned possible
misclassification sources and also added that the samples were
analyzed in different laboratories. As the samples from “Cordillera
Frontal” were discriminated from the rest in the analysis of both
types of samples (mud-clay and SEGEMAR samples), we decided to
repeat the analysis excluding them from the database. With a
sample reduced to 678 cases, both mud-clays banks (N ¼ 67) and
stream sediment (N ¼ 611), located within the geological provinces,
overlap. Statistical analysis was able to correctly classify only 65% of
23
the cases. In Table 5, we present the results of the statistical anal-
ysis. To facilitate the table reading, the sampling areas were clas-
sified considering their location within each geological province.
Furthermore, we differentiate mud-clay banks samples from
stream sediment ones.
The results are not encouraging for the goal proposed in this
paper. However, they show the high geochemical variability of the
Abauca
n river basin. Samples from a specific area (geological
province) share chemical profiles with other areas of other prov-
inces. Some miss-classifications are related to the sector as they are
correctly classified considering the geological province (Table 5).
However, there are also cases where the samples are classified
within other geological provinces. This shows some relevance and
justification when the samples come from ecotonal areas, for
example, in the case of the arbitrary boundary separating the
northern and southern sectors of Cordillera de Narva
ez. The
analytical data from the regional geochemistry (SEGEMAR, 1998)
and mud-clay banks do not allow us to differentiate mud-clay
samples located in different sectors of the geological provinces.
The tendency is to place them mainly within the Famatina System
(“Cordillera de Narva
ez” northern and southern sectors) whether
they belong to that province or not.
24 N. Ratto et al. / Quaternary International 375 (2015) 13e26

Table 5
Classification results of the statistical analysis integrating mud-clay samples (67:678:1129) and stream sediments (611:678:1129) from areas within the geological provinces
Famatina System and “Sierras Pampeanas”. Highlighted in gray: (i) number of samples of mud-clay sediments of rivers within the predictive model per geological province and
(ii) number and percentage of samples (stream sediments and mud-clay river) correctly classified.

Geological province the Location of the sampling areas Samples (muds-clay Geological provinces (predicted) Total
sampling area of regarding to geological provinces and stream sediments) 

“C Narvaez” “C Narvaez” “Sierras Pampeanas” “Sierras Pampeanas”
mud-clay deposits
(northern (southern (eastern sector) (western sector)
sector) sector)

Famatina system. Ecotonal Area “C Narva
ez” Guanchin River 1 20 0 0 21

“Cordillera de (northern and southern sectors) Segemar 7 10 8 10 35
Narv
aez” (northern Ecotonal Area “Sierras Segemar 0 1 18 5 24
sector) Pampeanas” (western sector)
and“C Na
rva

ez” (northern)
“C Narv
aez” (northern sector) Segemar 56 7 3 4 70
“C Narv


aez” (northern Colorado River 4 2 0 2 8
sector) - eastern slope Segemar 117 10 2 10 139
Subtotal 185 50 31 31 297
Percentage 62.29 16.84 10.44 10.44 100.00
Famatina System. Ecotonal Area “C Narv
aez” Segemar 2 1 0 1 4
“Cordillera de (northern and southern sectors)
Narv
aez” (southern Ecotonal Area “Sierras Segemar 1 0 5 4 10
sector) Pampeanas” (western sector)
and “C Na
rva

ez” (southern sector)
“C Narv
aez” (southern El Puesto River 0 4 0 0 4
sector) -eastern slope La Troya River (lower) 0 20 0 2 22
La Troya River (upper) 1 4 0 0 5
Segemar 8 35 0 19 62
Subtotal 12 64 5 26 107
Percentage 11.21 59.81 4.67 24.30 100.00
“Sierras Pampeanas” “Sierras de Fiambala
”
n River
Abauca 1 1 0 0 2
eastern sector (southern section) Segemar 9 19 27 5 60
“Sierras de Fiambala
” Segemar 4 1 68 1 74
(northern section)
Subtotal 14 21 95 6 136
Percentage 10.29 15.44 69.85 4.41 100.00
“Sierras Pampeanas” Ecotonal Area “Sierras Cazadero Grande River 1 2 0 0 3
western sector Pampeanas” (western sector) Segemar 0 4 7 36 47
and “C Na
rva
ez” (northern sector)
Ecotonal Area “Sierras Segemar 1 11 14 60 86
Pampeanas” (western sector) Tambería River 0 2 0 0 2
and “C Narva
ez” (southern sector)
Subtotal 2 19 21 96 138
Percentage 1.45 13.77 15.22 69.57 100.00

Mud-clay samples from the La Troya and El Puesto rivers show
better agreement, as 91% of them were classified in the south sector
of the “Cordillera de Narvaez”. Only 50% of the Colorado River
samples were well classified within the northern sector of the
“Cordillera de Narva
ez”, and the rest were divided between the
southern sector and the “Sierras Pampeanas” (western sector). The
possibility of geochemically distinguishing the northern sector of
“Cordillera Narva
ez” is very important for the purposes of our work.
However, there are few samples from this location, and sampling
should be expanded. Furthermore, Guanchín River samples were
assigned to the southern sector although they were collected at the
northern one. This discrepancy may be due to samples being
located in an ecotonal area, as the river was the limit established to
divide both sectors. Finally, the mud-clay samples located in the
“Sierras Pampeanas” (east and west sectors) were misclassified in
all cases, as they were assigned to the Famatina System.
5. Conclusion
The goal of quantitative analysis of the chemical data is to
identify compositionally homogeneous groups within the analyt-
ical database. Such groups are assumed to represent geographically
restricted sources or source zones. The location of these may be
inferred by comparing the unknown groups with known ones (raw
materials source) or by indirect means. Examples of indirect means
are the “criterion of abundance” (Bishop et al., 1982a,b) and argu-
ments based on geological and sedimentological characteristics
(Steponaitis et al., 1996).
We began this paper by saying that the various actions per-
formed for the production of pottery (cleaning, sieving, mixing
raw materials obtained from different deposits, incorporating
added inclusions or temper, etc.) can alter the characteristics of
the sources exploited. However, our work demonstrated that
besides cultural variation in provenance studies, variations
imposed by the environment in the formation of clay banks have
to be considered. This variability and their geographical distri-
bution are often conditioned by large-scale patterns of geology
and drainage.
Particularly, our study contributes evidence indicating the high
geochemical variability of the Abauc
an extensive river basin, due its
geological history and characteristics of its hydrographic network.
It also shows the difficulties of working with raw material resources
and finished ceramic products made by past populations.
Statistical analysis shows a clear difference in the chemical
profiles of the mud-clay samples and the stream sediment ones
located in the cordilleran transitional zone (“Cordillera Frontal”)
respect to other areas of the region, particularly the intermountain
valleys. However, we could not demonstrate that mud-clay samples
of La Troya have a chemical profile that distinguishes them from
others coming from similar environments, but in other geological
 N. Ratto et al. / Quaternary International 375 (2015) 13e26 25

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