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Journal of Archaeological Science 136 (2021) 105511

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Journal of Archaeological Science


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

Provenance study of the variscite artifacts of the Sierra Nevada de Santa


Marta, Colombia and approach to routes of pre-Hispanic exchange
Natalia Acevedo a, *, Marion Weber a, Joaquín A. Proenza b, Antonio Garcia-Casco c,
Juanita Sáenz-Samper d
a
Departamento de Geociencias y Medio Ambiente, Universidad Nacional de Colombia, Carrera 80 No. 65-223, Medellín, Colombia
b
Department of Crystallography, Mineralogy and Mineral Deposits, University of Barcelona, Martí i Franquès s/n, 08028, Barcelona, Spain
c
Department of Mineralogy and Petrology, University of Granada, and IACT (CSIC-UGR), Granada, Spain
d
Banco de la República, Museo del Oro, Calle 16 No. 5-41, Bogotá, Colombia

A R T I C L E I N F O A B S T R A C T

Keywords: Variscite is a rare mineral that offers new opportunities for research on the mobility of raw materials in America
Variscite during pre-Hispanic times through the provenance study of the source material. In this article we address a
Archaeological artifacts detailed characterization of the texture, mineralogy and chemical composition of the variscite beads belonging to
Origin
the Nahuange (100–1000 AD) and Tairona (1000–1600 AD) societies of the Sierra Nevada de Santa Marta region
Pre-hispanic exchange
(northern Colombia), which we compare with the known deposit located in the Gran Roque Island, Venezuela.
The presented evidence proves the origin of the material from this location, allowing the interpretation of the
distribution models of northern South American archaeological variscite.
Indeed, different findings of beads made of variscite have shown that this mineral could have a much wider
distribution that extends to the Northern Andes, the Amazon basin and the Caribbean islands, though other not
yet discovered geological sources cannot be discarded. This is shown by the discovery of variscite beads at the
Nueva Esperanza Archaeological Site south of Bogotá and in the archaeological records of the Nariño culture
(Colombia), the Amazon basin in Brazil, Aruba and the Lesser Antilles.

1. Introduction belonging to the pre-Hispanic Nahuange and Tairona societies, where


the geological units of Gran Roque Island, Venezuela, are proposed as a
Archaeological artifacts, such as necklace beads, winged plates, or­ possible source of this material.
naments and zoomorphic and anthropomorphic figures made from The variscite mineral group comprises orthorhombic hydrated
green rocks and minerals, have been documented in the Nahuange and phosphates with the general formula MPO4.2H2O, where M = Al3+,
Tairona cultural area, in the Sierra Nevada de Santa Marta (SNSM), Fe3+, Cr3+, V3+, formed by the reaction of phosphoric acid with Al-rich
Colombia (Fig. 1), which ranges chronologically from 100 to 1600 CE rocks (Larsen, 1942). The most common minerals in this group are
(Mason, 1931, 1936, 1939; Bishof, 1968; Reichel-Dolmatoff, 1997). A variscite and strengite, and their metavariscite and phosphosiderite
large number of these artifacts have been made from semi-precious isomorphs. Variscite commonly occurs in the form of microcrystalline
stones, including serpentine, jadeite and nephrite jade, soapstone, fibrous-radiated aggregates, massive forms, nodules and concretions,
chalcedony, and rocks such as amphibolite, shale, basalt, andesite and typically filling fissures and cavities in rocks (Calas et al., 2005).
tuff (see Acevedo, 2014; Acevedo et al., 2018), whose main character­ Variscite deposits are very scarce worldwide, and the limited number
istics are the green color, the microcrystalline texture and in some of of geological formations containing variscite makes it possible to
them their semi-translucent nature. Generally, the term used to classify constrain its source, making it an important mineral for identifying
these materials has been “jade”, given not as a mineralogical but a social patterns of social exchange and interaction in prehistory (Domi­
term (“cultural jade”). nguez-Bella, 2004; Odriozola, 2012).
Recent studies (Acevedo et al., 2016) have identified for the first time In Colombia, a high proportion of the variscite archaeological arti­
in Colombia the presence of variscite as a raw material of lithic artifacts facts, mainly beads, have been recovered from the Tairona cultural area

* Corresponding author.
E-mail address: naceved@unal.edu.co (N. Acevedo).

https://doi.org/10.1016/j.jas.2021.105511
Received 21 June 2021; Received in revised form 20 October 2021; Accepted 20 October 2021
Available online 27 October 2021
0305-4403/© 2021 Published by Elsevier Ltd.
N. Acevedo et al. Journal of Archaeological Science 136 (2021) 105511

Nahuange and Tairona societies are housed in different heritage col­


lections in Colombia. Specific objects were chosen for their represen­
tativeness according to the stylistic classification of the collections, the
macroscopic and mineralogical characteristics described in Acevedo
et al. (2016), and for their availability fordestructive and
non-destructive analyzes. Table 1 lists the archaeological pieces studied,
the type of analysis carried out and the archaeological collection to
which they belong. The rock samples studied as a potential source of
supply for variscite artifacts were extracted from the Gran Roque Meta­
ignea Association (Urbani, 2018), located on the Gran Roque Island,
Venezuela. A total of 43 variscite geological samples were collected for
testing provenance of the archaeological material. The analytical tech­
niques used are described below:
Polarized Light Optical Microscopy (PLOM). The analysis was car­
ried out in the Laboratorio de Petrografía y of the Departamento de
Geociencias y Medio Ambiente of the Universidad Nacional de
Fig. 1. Regional location of the Sierra Nevada de Santa Marta in Colombia and
Colombia, Medellín campus, using an Olympus BX41 microscope with a
the Gran Roque Island in Venezuela.
transmitted light source.
X-ray diffraction (XRD). The diffractograms were obtained in the
in the SNSM. However, there is a shortage of regional geological out­
Laboratorio de Biomineralogía y Biohidrometalurgia of the Universidad
crops containing this mineral. The only likely deposit in the Caribbean
Nacional de Colombia, Medellín campus, using a Rigaku diffractometer,
realm identified so far is located on the Gran Roque Island, Venezuela
Miniflex model and Bragg-Brentano configuration. The analyses were
and was proposed as the possible source of the Tairona raw material
performed with a 2ϴ angle sweep between 2◦ and 70◦ , using a Cu source,
(Acevedo et al., 2016).
voltage of 30 kV and current of 15 mA. The XRD analyses were per­
The number of pieces made of this material in the archaeological
formed on the samples milled by hand using an agate mortar up to a 200
records housed in collections raises important questions about the origin
ASTM mesh size. The spectra were analyzed using X’Pert HighScore Plus
and distribution networks of artifacts made in variscite. In this work we
software.
characterize the archaeological material in mineralogical, textural and
Raman spectroscopy (micro-Raman). The spectra were obtained at
chemical terms in more detail, and compare it with a detailed charac­
the Centro de Investigación, Innovación y Desarrollo de Materiales
terization of rocks sampled in the Gran Roque Island, Venezuela (Ace­
(CIDEMAT) of the Universidad de Antioquia, using a HORIBA Jobin
vedo, 2019). Taking into account the geological and archaeological
Yvon LabRam HR dispersing spectrometer 800 equipped with an
evidence found we examine the source and evaluate the potential
Olympus BXFM light microscope. Non-polarized Raman spectra were
exploitation of the Gran Roque raw material during the studied
obtained by applying a 532 nm laser and using a 100× objective (beam
chronologies.
size around 2 μm), with 10 measurement repeats for 15 s each. The in­
strument was calibrated by verifying the position of the metallic Si band
1.1. Archaeological context at ~520 cm− 1.
Fourier Transform Infrared Spectroscopy (FTIR). The FTIR spectra
The SNSM was one of the last refuges of ancient pre-Hispanic cul­ were obtained in the Laboratorio de Biomineralogía y Bio­
tures, which gives us an important archaeological record exposed with hidrometalurgia of the Universidad Nacional de Colombia, Medellín,
the discovery of numerous cultural remains, corresponding to the from a Shimadzu 8400s spectrometer, using 24 scans, with a spectral
Nahuange (100–1000 AD) and Tairona (1000–1600 AD) chronological resolution of 4 cm− 1 and a spectral range between 400 and 4000 cm− 1
periods (Reichel-Dolmatoff, 1997; Langebaek, 2005; Oyuela-Caycedo, and apodization Happ-Genzel function. For this technique, pellets of
2008; Giraldo, 2010; Sáenz, 2010). The location of the region adjacent sample- KBr mixtures pulverized in agate mortar were used in a weight
to the Caribbean coast of Colombia, which connects the Caribbean, ratio of 1: 100 mg (sample/KBr). The spectra were analyzed using the
Central America, and the Andes of Colombia and Venezuela, is key to IRsolution software.
understanding social changes during the pre-Hispanic era, as recent Electron microprobe (EPMA). The analyses were carried out at the
research shows (e.g. Reichel-Dolmatoff, 1951; Bischof, 1968; Cadavid Centros Científicos y Tecnológicos of the Universitat de Barcelona
and Herrera, 1985; Langebaek, 2005; Sáenz, 2007, 2010; Oyuela-Cay­ (CCiT-UB), Spain, with a JEOL JXA-8230 electron microprobe consisting
cedo, 2008; Giraldo, 2010). of 5 WDX spectrometers (Wavelenght Dispersive X-Ray spectroscopy)
During the Nahuange period, the population settled in the coastal and an EDX spectrometer (Energy Dispersive X-Ray spectrosocpy). An
region, decreasing its density towards the mountains (Reichel-Dolmat­ acceleration voltage of 20 kV, probe current on the sample of 20 nA and
off, 1997; Giraldo, 2010), organized in small and isolated towns without diameter of the incident beam of 2 μm were used. The analyses of
stone foundations and in settlements without hierarchical differentia­ phosphates were normalized to 4 oxygens. The atomic concentration of
tions. At approximately the 10th century social and political changes elements per unit formula is abbreviated apfu. Backscattered electron
occurred, along with rapid population growth, which led to the colo­ (BSE) images and elemental X-ray maps of P, Fe, Al and Si were obtained
nization of the upper slopes of the mountain, introducing stone masonry, by WDS scans of samples using the same equipment operated at 20 kV
so that by the end of the 10th century many towns and cities with and 200 nA, a focused beam of 5 μm, size pitch (pixel) size of 3 μm and
foundations of stone were connected by roads and inhabited by people count time of 20–30 ms/pixel.
from the Tairona period, a warrior society with deep religious practices
(Wynn, 1975; Oyuela-Caycedo, 1986, 1987, 2008; Cadavid and Herrera, 3. Results
1985; Groot, 1985; Serje, 1987b; Reichel-Dolmatoff, 1997; Langebaek,
2005; Giraldo, 2010). 3.1. Characterization of beads and ornaments

2. Materials and methods The analyzed necklace beads and ornaments are shown in Fig. 2. The
beads of various sizes exhibit cylindrical, globular and rounded shapes,
The studied archaeological variscite artifacts belonging to the and the ornaments exhibit different sizes and include zoomorphic

2
N. Acevedo et al.
Table 1
Location of archaeological artifacts of pre-Hispanic cultures. General description of the shape and macroscopic classification, summary of the analyses carried out on the artifacts and mineralogical characterization using
micro-Raman and XRD. Legend: Var = variscite, St = strengite, Mv = metavariscite, Fos = phosphosiderite, Leu = leucophosphite, Qz = quartz, Chy = chalcedony, Ilm = ilmenite, Hem = hematite, SNSM = Sierra Nevada
de Santa Marta.
N◦ Collection Code Culture Location Description Macro Analysis - Archaeological artifacts Identified minerals
classification
MO Raman XRD FTIR EPMA δD/ SEM/ Raman XRD
δ18O EDS

1 Gold Museum LT854-1 Nahuange and SNSM Tabular bead Variscite x x x x Var Var + Ilm
2 LT854-2 Tairona Tabular bead Variscite x x x x St St + Qz
3 LT621 100–1600 d.C. Tabular beads and Variscite
charms
4y5 – Tabular and globular Variscite
beads
6 LT1912 Zoomorphic figure - Variscite
frog
7 LT2105 Zoomorphic figures Variscite
necklace - frog
8 – Zoomorphic figure - Variscite
frog
9 LT1911 Anthropomorphic Variscite
figure
10 – Globular bead Variscite
11 ICANH – Nahuange and SNSM Tabular bead Variscite
12 – Tairona Globular bead Variscite
13 IC-2 100–1600 d.C. Tabular bead Variscite x x x x x x Var Var + Qz +
Mv
14 a – Flat and tabular round Variscite
17 beads
3

18–20 – Tabular bead Variscite


21 a MUUA – Nahuange and SNSM Tabular and globular Variscite x Var + St
28 Tairona beads
29 a – 100–1600 d.C. Beaded necklace Variscite
39
40 – Zoomorphic figure Variscite
41 Archaeological un-1 Nahuange and SNSM Tabular bead Variscite x x x x x x Var + St St + Fos +
Laboratory - Universidad Tairona + Fos, Ilm Chy + Mv +
del Norte 100–1600 d.C. Leu + Ilm
42 un-2 Tabular bead Variscite x St + Fos
43 un-3 Tabular bead Variscite x x x x x x Var + St St + Fos +
+ Fos Qz
44 un-4 Tabular bead Variscite x x x x x x St + Fos St + Fos +

Journal of Archaeological Science 136 (2021) 105511


Chy + Mv
45 un-5 Tabular bead Variscite x x x x x x St, Ilm Var + St +
Mz + Qz
46 un-6 Tabular bead Variscite x St, Hem

47 a –
54
55 Archaeological L613 Nahuange and SNSM Tabular bead Variscite
56 Laboratory - Universidad L537 Tairona Globular bead Variscite
57 del Magdalena L528 100–1600 d.C. Flat round bead Variscite
58 L589 Tabular bead Variscite
59 L579 Tabular bead Variscite
60 L500 Tabular bead Variscite
61 L593 Tabular bead Variscite
62 L497 Tabular bead Variscite
(continued on next page)
N. Acevedo et al. Journal of Archaeological Science 136 (2021) 105511

figures representing primarily frogs and anthropomorphic figures. All


the pieces have a transverse or front hole, except artifacts 6 and 9
(Fig. 2).
The artifacts display a variety of shades of green and, to a lesser
Identified minerals

XRD

extent, white and brown. They have a glassy to resinous luster, uneven
fracture, microcrystalline texture with a homogeneous or irregular
surface. In addition, some pieces have abundant pores on their surface,
Raman

white streaks less than 1 mm thick, and opaque mineral inclusions.


Var

Var

Var
Table 1 shows a general description of the beads and ornaments and a
detailed characterization obtained using micro-Raman and DRX.
SEM/
EDS

The mineralogical and chemical characterization of the green beads

x
and ornaments confirmed the initial macroscopic classification, which
indicates a main composition of minerals belonging to the variscite
δ18O
δD/

group and variscite-strengite series ([AlPO4 ⋅2H2O] - [Fe+3PO4 ⋅2H2O]).


Representative analyzed beads are shown in Fig. 3A, C and E. From
EPMA

the deconvolution of the curves of the micro-Raman spectra, the position


of the maxima corresponding to the superimposed vibratory modes in
the region between 900 and 1200 cm− 1 were obtained. The curves
Analysis - Archaeological artifacts

FTIR

indicate that they are composed of strengite, with the most intense vi­
bration band at 992 cm− 1 (Fig. 3G and K) and variscite, with the most
intense vibration band at 1031 cm− 1 (Fig. 3I) in the green areas, and by
XRD

phosphosiderite, with main vibration bands in 992, 1009 and 1031 cm− 1
in the white areas (Fig. 3C and E). The spectra, allowed identifying the
Raman

opaque minerals as ilmenite and hematite.


x

The spectra obtained by IR (Figures 3M, N and O, black lines) show


the characteristic bands described for the minerals of the variscite group
MO

(Frost et al., 2004), whose vibrations at frequencies between 1200 and


900 cm− 1 indicate the presence of the coordination polyhedron [PO4] in
classification

the analyzed beads. The position of the vibrational modes also reveals
Variscite?
Variscite
Variscite
Variscite
Variscite

Variscite

Variscite
Variscite
Variscite
Variscite
Variscite

Variscite

the presence of water molecules present in the structure of variscite


Macro

(frequencies less than 900 cm− 1), M-OH2 and PO43− (between 500 and
600 cm− 1), O–P–O (between 550 and 400 cm− 1), adsorbed water (be­
tween 2500 and 3500 cm− 1) and superficial P–OH groups (3584 cm− 1).
Tabular and oval beads

The X-ray diffractograms indicate that the dominant phases in the


Flat and oval beads
Zoomorphic figure

analyzed beads are variscite and strengite. Other phosphates such as


Flat round bead

Flat round bead


Flat round bead

phosphosiderite, metavariscite, and leukophosphite were identified, in


Tabular bead
Tabular bead

Tabular bead
Tabular bead

Tabular bead
Round bead
Description

addition to chalcedony, ilmenite and quartz (Table 1). Ilmenite and


quartz are relicts of the original igneous rock.
The chemical characterization of the beads studied by means of
EPMA confirms that they are mainly made up of variscite and strengite,
Marie-Galante,

Amazon Basin,
575–1450 d.C.

with the presence of leucophosphite, chalcedony and relict quartz,


Lesser Antilles
Quíbor valley,

ilmenite, hematite, actinolite and spinel. Fig. 4 represents the analyses in


Venezuela
Location

the ternary diagram P–Al + V–Fe + Cr along the variscite-strengite join,


Bogotá
Nariño
Aruba

Brazil

suggesting a complete solid solution between the end-members.


The textures identified in the beads include spherulitic textures
(Fig. 4A), variscite veins along different directions (Fig. 4C), replace­
900 a.C - 800 d.C.
100 a.C. - 600 d.C

Quillacingas and
1000–1500 d.C.
900–1500 d. C.

800–1500 d. C.

ment of relict minerals (Fig. 4E), pseudomorphs of variscite after


400–1600 d.C.

Troumassoide

amphibole in tabular (Fig. 4G) and rhombohedral sections (Fig. 4I), and
Guadalupe
Boulevard

Caquetíos
Tradition

Tradition

Abades,

Herrera

banded textures (Fig. 4K). These textural relationships show several


Culture

Pastos

generations of phosphate precipitation, interspersed with numerous


irregular cavity systems, where the depositional medium records the
transport flow routes of the phosphate waters that gave rise to the for­
C67_CC_220
C72_CC_204

MG-03-004

mation of the variscite after replacement of the original metaigneous


LN113

rock.
Code

L628

509

The compositional and textural relationships of the beads were also





studied from X-ray maps in a selected area with spherulitic texture


(Fig. 5A), this being the most common among the textures of the beads
Aruba Archaeological
University of Caracas

Taken from Resque y

studied. The maps show the sequence of mineral crystallization, starting


with the Fe-richer phosphate variety and with recurrent oscillations in
Alain Queffelec
Gold Museum

Al and Fe content, ending with chalcedony precipitation within fractures


Costa, 2012
Undefined
Collection
Table 1 (continued )

and voids (Si-richer areas).


Museum

The textures and chemical characterization obtained for the beads


allow us to interpret that variscite formed through the multistage
phosphatization of a preexisting amphibole-rich quartz-bearing rock
with minor magnetite and ilmentite.
63
64
65
66

67

68

69

70
71
72

73
N◦

4
N. Acevedo et al. Journal of Archaeological Science 136 (2021) 105511

Fig. 2. Photographic representation of the studied archaeological artifacts. Artifacts 1–65 correspond to Nahuange and Tairona cultures. Artifacts 66–73 are from
other localities and cultures. The general description of the archaeological artifacts is shown in Table 1.

3.2. Comparison with Gran Roque variscite inclusions of opaque minerals, such as ilmenite and hematite (Fig. 3E
and F), which are also present in the rock samples and we interpret as
Representative beads and rock samples are compared in Fig. 3. relicts of the rock that suffered phosphatization.
Similar macroscopic textural features are observed. The comparison of In terms of the mineralogical association there are important simi­
the beads and the rocks shows a remarkable equivalence in their shades larities between beads and rock. The studied beads show a mixture of
of green, associated with the presence of intermingled white minerals phosphates and hydrogenphosphates, including variscite, strengite,
(Fig. 3C–F) that correspond to phosphosiderite. Some beads exhibit phosphosiderite, metavariscite and leucophosphite, in addition to

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N. Acevedo et al. Journal of Archaeological Science 136 (2021) 105511

Fig. 3. A. Bead un-5. B. Rock sample var-cr4. C. Bead un-3. D. Rock sample var-cr1. E. Bead un-1. F. Rock sample var-cr3. G–L. Micro-Raman spectra compared with
the reference spectra of the minerals of the variscite group from the RRUFF database (http://rruff.info/) and the spectra reported by Frost et al. (2004). M-O. Infrared
spectra between the region from 400 to 4000 cm− 1 compared with those described by Frost et al. (2004) and Farmer (1974).

chalcedony, ilmenite, quartz and spinel, an association also found in the studied according to the identified textural characteristics and according
deposits of Gran Roque (cf. Acevedo, 2019). to the associated formation process. The X-ray maps obtained in the
This is evidenced from the replacement textures found and the beads (Fig. 5A) show the same textural-mineral development and crys­
chemical analyzes carried out. The phosphatization processes of the tallization sequence as in the analyzed rocks (Fig. 5B), where crystalli­
variscite deposit on Gran Roque Island (Urbani, 2005; Acevedo, 2019) zation nuclei of the first precipitate in the spherulites, both in the bead
were triggered by the penetration of phosphate fluids formed from and in the analyzed rock corresponds to strengite, and the late precipi­
guano, which replace the underlying rocks including quartz-bearing tation to chalcedony. All these characteristics clearly point to similar
metagabbros and metadiabases. These processes formed the same rock-forming processes in both types of material.
replacement textures observed in the beads. This replacement is pro­
gressive, and relict textures of the amphiboles are observed locally in the 4. Discussion
tabular and rhombohedral cut both in the beads and in the rocks, as seen
in Fig. 4G–J. In addition, minerals such as quartz, ilmenite and hematite Variscite as an ornamental mineral is used in its massive and
are preserved, which are not affected during the phosphatization microcrystalline form. Its texture and hardness are suitable for carved
process. objects to achieve a good polishing. It is a very scarce mineral, and
Fig. 4 shows a remarkable compositional relationship (represented in therefore, it has a high potential as a tracer of exchange routes such as is
the ternary diagrams P–Al + V–Fe + Cr) between the beads and rocks for instance jadeite (Adams, 1977, 1978; Popenoe de Hatch, 2010;

6
N. Acevedo et al. Journal of Archaeological Science 136 (2021) 105511

Fig. 4. Comparison of compositional and textural characteristics of beads from the Sierra Nevada de Santa Marta and rock samples from Gran Roque Island in
Venezuela. Backscattered electron images: A-B. Spherulitic textures. C-D. Variscite veins cross-cutting earlier banded textures. E-F. Spherulitic textures replacing
tabular cut of amphibole. G-H. Pseudomorph of variscite after tabular cut of amphibole. I-J. Pseudomorph of variscite after rhombohedral cut of amphibole. K-L. The
formation of phosphates with banded texture is observed. The analyses are represented in the ternary diagrams P–Al + V–Fe + Cr (atomic units). Legend: Var =
variscite, St = strengite.

Fig. 5. X-ray element maps in selected area with spherulitic texture. A. Bead un-1. B. Rock sample var-c3. Compositional characteristics and spherulitic textures show
initial precipitation of Fe-rich phosphate (strengite) and recurrent growth of Al- and Fe-rich varieties. In A note the relic cleavage of the original amphibole crystal on
the top or the image.

García-Casco et al., 2013; García-Casco, 2017). records for the characterization of cultural exchanges of this time.
For example, in prehistorical Iberia variscite was an important For Colombia, the studied artifacts elaborated in variscite (Fig. 2)
mineral for making beads and ornaments that represented magical and suggest that this material was quarried mainly for making necklace
religious values, thus being used as a prestigious ornament and social beads, and to a lesser extent for the crafting of zoomorphic and
and economic differentiator among members of the cultural group anthropomorphic ornaments, associated with chronologies that span
(Noain, 1998; Domínguez-Bella et al., 2003; Domínguez-Bella, 2004; from 100 CE to 1600 CE in South America and the Circum-Caribbean. In
Linares-Catela and Odriozola, 2011). These green beads are believed to the archaeological sites reported in the Sierra Nevada de Santa Marta,
have been exchanged through long-distance circuits in prehistory, since the green beads appear associated with funerary contexts (Mason,
only five Iberian variscite deposits are known (Arribas et al., 1971; 1931), that also present a stylistic affiliation with the other cultures
Alonso et al., 1978; Meireles et al., 1987; Moro et al., 1995; Bosch et al., mentioned here, which suggests an important symbolic and ceremonial
1996; Nocete e Linares, 1999; Villalba, 2002; Odriozola et al., 2012; value.
Domínguez-Bella et al., 2018), hence making variscite one of the guiding During the field campaign carried out on the Gran Roque Island,

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N. Acevedo et al. Journal of Archaeological Science 136 (2021) 105511

Venezuela, representative rocks made up of variscite minerals from the process. In addition, the X-ray maps (Fig. 5) show a variation in the Al
Asociación Metaígnea Gran Roque were obtained, mainly in a quarry with and Fe content whose identified precipitation sequence coincides in the
evidence of human activity, possibly from the 19th century (Urbani, beads and rocks analyzed.
2005). To our knowledge, no record of archaeological remains of stature All this evidence implies that the rocks of the Gran Roque Island in
or production residues have been recorded so far, and none were Venezuela and the raw material of the studied artifacts were formed
observed during fieldwork. under the same geological processes under similar environmental con­
The macroscopic and mineralogical characterization (micro-Raman, ditions. The phosphatization process for beads and rocks is associated
FTIR, DRX) of the beads belonging to the Nahuange and Tairona cultures with the alteration of igneous rocks with a particular mineralogical as­
fully coincides with the characterization obtained from the rocks of the sociation. This makes it possible to rule out other variscite formation
Gran Roque Island (cf. Acevedo, 2019). By macroscopic identification of environments, such as supergenic processes in clay rocks (Díaz-Acha,
the beads and rocks (Fig. 3A–F) it is possible to correlate the main 2019).
physical characteristics, such as color, hardness and texture. Likewise, Fig. 6 presents the variscite distribution model. In the proposed
the combination of qualitative spectrographic analyzes (Fig. 3G-O) in­ model, Gran Roque Island is the source of raw material, of the archae­
dicates that the beads and rocks are mainly made up of minerals from ological artifacts used by the pre-Hispanic societies that inhabited the
the variscite and strengite series, with the presence of a mixture of SNSM in Colombia. However, we do not have evidence if either the raw
phosphate and hydrogenphosphate species (PO43− , HPO42− ; Figure 3M, material or the finished objects were exported, and therefore we do not
N, O). The diffractograms obtained in the beads and rocks show the rule out the existence of workshops on the island.
presence of other crystalline phases in addition to variscite and stren­ This interconnection between pre-Hispanic societies of the southern
gite, such as metavariscite, phosphosiderite, leucophosphite, ilmenite, margin of the Circum-Caribbean region is further evidenced by the ex­
quartz and chalcedony. istence of small variscite beads excavated at the Pura y Limpia archae­
The microscopic textural variation and the mineral chemistry ob­ ological site, located in the Quíbor Valley (Fig. 6) in the Central Coast of
tained by EPMA (Fig. 4) allowed to identify a direct relationship be­ Venezuela, associated with a funerary context (León, 2014; Franco
tween the beads and rocks studied. This relationship is associated with Urbani and Luis E. Molina, personal communication), whose mineralogy
the formation conditions through the precipitation of variscite and other identified through micro-Raman coincides with the mineralogy of the
identified phosphates, which indicate a multi-episodic mineralization beads of the Nahuange-Tairona cultural area. In addition its textural
that suggests dissolution and re-deposition processes according to the characteristics are similar (Fig. 2, bead No. 66). This site was inhabited
physical-chemical conditions that prevailed during the formation between CE 575 and 1450, which chronologically corresponds to the

Fig. 6. Variscite distribution model. The black lines


represent the proposed route for variscite distribution
in pre-Hispanic times, the dotted lines represent
probable variscite distribution along different di­
rections in South America and the red line is the route
suggested by Antczak and Antczak (2006) according
to the extraction and exchange of botuto shells in
pre-Hispanic times. (For interpretation of the refer­
ences to color in this figure legend, the reader is
referred to the Web version of this article.)

8
N. Acevedo et al. Journal of Archaeological Science 136 (2021) 105511

Nahuange (late settlement) and Tairona periods. located south of Bogotá (discovered in 2015), which contains lithic and
These connections between regions are also supported by the occu­ ceramic pieces that belonged to the Muisca indigenous people and which
pation sequence postulated by Acosta Saignes (1983) for the La Pitia chronologically coincides with the tairona period. (within the lithic
archaeological site, located in the Venezuelan Guajira Peninsula on the pieces, we also identified beads made of green turquoise).
coast of the Gulf of Venezuela (Fig. 6). At this site an extensive shell Likewise, although of uncertain provenance, we have identified
deposit was found with important archaeological remains that includes variscite beads in the archaeological collection of the Gold Museum
polychrome ceramics, lithics, shell necklaces, beads described as jade, related to the Nariño culture from southwestern Colombia. These beads
among others, which served as a starting point to propose a scheme for show a mineralogy, texture and iconography similar to those described
the old settlement of Venezuela, indicating that the people of La Pitia in the Nahuange-Tairona area. In addition, a cylindrical variscite bead
could be related to Central America, as deduced after the discovery of found in the Amazon basin and currently housed in the collections of the
beads described as made of jade (Acosta Saignes, 1953, 1983). Museus de Gemas in Brazil (Resque Meirelles and Costa, 2012) shows
Furthermore, similarities have been found in the raw material between textural characteristics, such as its intense green color, vitreous luster
artifacts from the La Pitia archaeological site with artifacts from the and porous surface, similar to the Nahuange-Tairona beads studied. This
Ranchería region in Colombia and Lake Valencia, in the central region of may indicate large-scale relations that may include
Venezuela (Acosta Saignes, 1983). Andean-Mesoamerican contacts inferred from the finding of pieces of
This interaction is reinforced with studies by Antczak and Antczak high symbolic value made in shells of tropical seas (Spondylus pictorum
(2006) that identify a trade network established by the Valencioide and Conus fergusoni) in archaeological sites in Ecuador, Peru and as far as
culture (1200–1500 CE) from the Central Coast of Venezuela towards Chile (Marcos, 1998), suggesting rather long-distance trade routes. This
the Los Roques archipelago (Fig. 6), as evidenced from botuto shells archaeological evidence makes rather possible to exchange variscite
(Strombus gigas) extracted from the islands (i.e., botuto shells, excavated artifacts further south of the Sierra Nevada de Santa Marta, though lack
at the La Mata archaeological site located in Lake Valencia, whose of a detailed mineralogical and textural characterization of the artifacts
radiocarbon dating gave approximate ages of 1200 CE; Antczak and found in Bogotá, Nariño and the Amazon basin rules out the precise
Antczak, 2006). During the approximate 300 years of pre-Hispanic definition of the area of provenance.
fishing, it is estimated that at least 5500000 shells were removed Additional geological sources of variscite identified in South America
(Antczak and Antczak, 2016). Once used as food, seashells were used for include a few localities in Brazil, Argentina, Bolivia and Chile. In Brazil,
the manufacture of personal adornments, mainly necklace beads and the variscite occurs in the state of Bahia as crusts on volcanic rocks formed
crafting of tools, such as axes and punches (Antczak and Antczak, 2006). by basalt weathering from guano (Flicoteaux and Melfi, 2000), in Minas
At the Dos Mosquises site, located in the Los Roques archipelago, 21 Gerais as secondary veins and filling cavities in pegmatites forming red
small undrilled shell discs were recovered, believed to have been precast spheroidal crystals (Cassedanne and Baptista, 1999) and in Mato Grosso
for beads production, indicating the manufacture on-site, although no as small spherical and tabular aggregates of green color associated with
specialized manufacturing tools were found (Antczak and Antczak, the formation of chalcedony (Bermanec et al., 2011). In the El Criollo
2006). However, Serrand (1997) identified prefabricated shell beads mine, Córdoba Province, Argentina, purple-pink strengite occurs asso­
associated with human burials at the Dabajuroide site in Aruba, sug­ ciated with pegmatitic bodies (Gay, 1968). In Oruro, Bolivia, variscite
gesting that these disks could be finished objects with an unknown occurs in white spherical aggregates (Arce and Nambu, 1989). And
function. finally, in the Province of Antofagasta, Chile, variscite is found in
Likewise, winged plates, representing artifacts with thin and elon­ colorless spherical aggregates (Atencio et al., 2012). These occurrences
gated shapes associated with religious or ceremonial uses, have been do not represent important mineralization and do not show the char­
reported in the Andes and western states of Venezuela, Panama, Costa acteristic color and texture to those found in the studied beads.
Rica, Puerto Rico and, in Colombia, in the Caribbean plains, La Guajira,
Sierra Nevada del Cocuy and SNSM (summarized in Acevedo et al., 5. Conclusions
2018). The winged plates found in excavations on Dos Mosquises Island
in the Los Roques archipelago and in the State of Trujillo in. Artifacts made from green rocks and minerals were highly appreci­
Venezuela (Wirz, 1948; Antczak and Antczak, 2006; Acevedo et al., ated by pre-Hispanic societies in the Caribbean - northern South
2018) show an important similarity with the plates belonging to the America realm, with an important presence in funerary contexts. Their
Nahuange and Tairona societies (e.g. winged plates made of serpentine). characteristic green color and textures possibly contributed to their
All this evidence not only suggests an interconnection between popularity during different pre-Hispanic periods, making the study of
Colombia and Venezuela, but also to other Caribbean islands. This is this type of raw material an important indicator of social expression and
reinforced by the identification by macroscopic description of the organization in prehistory.
probable variscite beads in the National Archaeological Museum of The studied beads belonging to the Nahuange and Tairona cultural
Aruba (Franco Urbani and Raymundo Dijkhoff, personal communica­ area are mainly made up of minerals from the variscite group. The
tion), where these beads show textural characteristics similar to those macroscopic, mineralogical and chemical characteristics indicate that
reported in the Nahuange-Tairona cultural area, variscite beads the raw material of the beads was sourced from the Gran Roque Island in
analyzed by Raman reported on Marie Galante Island located in the Venezuela.
Lesser Antilles (Alain Queffelec, personal communication) and the We propose the existence of a pre-Hispanic exchange routes between
similarities of early ceramic artifacts from the Antilles with those of the societies of Colombia and Venezuela, where the acquisition and
northwestern Venezuela and Colombia, indicating that there was a long-distance exchange of variscite between human communities sug­
direct interaction between these regions during the pre-Arawak era (500 gests an important part of social development and complex political
BCE) (Zucchi, 1984). structures during pre-Hispanic times.
These networks, probably connected to the Caribbean coasts of Initial archaeological evidence indicates a cultural connection that
Colombia and Venezuela, mainly by coastal and river trade (although extends further South into South America and the Circum-Caribbean.
land routes are not excluded), are inserted within the broader areas of However, defining an interaction pattern to more distant regions, to­
pre-Columbian interactions that connected the southern margin of the wards the south of Colombia and other Caribbean islands, requires
Circum-Caribbean region with the Northern Andes. This is demonstrated detailed characterization and further studies on archaeological artifacts.
by the finding of the winged plates (summarized in Acevedo et al., 2018)
and the variscite beads (Acevedo, 2019) that we have identified at the
Nueva Esperanza archaeological site in the municipality of Soacha,

9
N. Acevedo et al. Journal of Archaeological Science 136 (2021) 105511

Acknowledgments primas geológicas, 26A. Boletín de la Sociedad Española de Mineralogía,


pp. 113–114.
Domínguez-Bella, S., 2004. Variscite, a prestige mineral in the Neolithic-Aeneolithic
This research was supported by Colciencias (Project No. Europe. Raw material sources and possible distribution routes. Slovak Geol. Mag.
111866044635) and the Universidad Nacional de Colombia (Project No. 1–2, 151–158.
18819). The University of Barcelona and the University of Granada, Farmer, V.C., 1974. The Infrared Spectra of Minerals. Mineralogical Society, London.
Flicoteaux, R., Melfi, A., 2000. The phosphatic crusts from basalts of the Abrolhos
Spain, co-financed this work. We thank the Gold Museum of the Banco Archipelago (Bahia, Brazil): rocks formed from guanos during the Late Quaternary.
de la República de Colombia, the ICANH in Bogotá, the University Comptes Rendus Acad. Sci. - Ser. IIA Earth Planet. Sci. 330, 193–200.
Museum of the University of Antioquia and the Archeology Laboratories Frost, R.L., Weier, M.L., Erickson, K.L., Carmody, O., Mills, S.J., 2004. Raman
spectroscopy of phosphates of the variscite mineral group. J. Raman Spectrosc. 35,
of the Universidad del Norte and the Universidad del Magdalena. The 1047–1055.
authors thank the Biomineralogy and Biohydrometallurgy Laboratory García-Casco, A., 2017. Descifrando la “ruta del jade” en Mesoamérica-Caribe: Estudio
and the Biomaterials Laboratory of the National University of Colombia geoarqueológico de artefactos de jade pre-Colombinos en el Caribe e implicaciones
geológicas y antropológicas. Conferencia presentada en la Universidad Nacional de
and the CIDEMAT laboratory of the University of Antioquia. We are Colombia, Medellín, Colombia.
especially grateful to Professor Franco Urbani for ample support during García-Casco, A., Knippenberg, S., Rodríguez-Ramos, R., Harlow, G.E., Hofman, C.,
logistics and field-work in Venezuela, and archaeologists Paula Gallego Pomo, J.C., Blanco-Quintero, I.F., 2013. Pre-columbian jadeitite artifacts from the
golden rock site, St. Eustatius, lesser Antilles, with special reference to jadeitite
and Sergio González for allowing us access to the lithic collections of the artifacts from elliot’s, antigua: implications for potential source regions and long-
Nueva Esperanza archaeological site. distance exchange networks in the greater caribbean. J. Archaeol. Sci. 40 (8),
3153–3169.
Gay, H.D., 1968. Fosfatos en la pegmatita del cerro Blanco, Tanti, provincia de Córdoba.
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