Journal of Archaeological Science 58 (2015) 31e45

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Journal of Archaeological Science

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

Skeletal arsenic of the pre-Columbian population of Caleta Vitor,

northern Chile
Jaime Swift a, *, Matthew L. Cupper b, Alan Greig b, Michael C. Westaway c, Chris Carter a,
Calogero M. Santoro d, e, Rachel Wood f, Geraldine E. Jacobsen g, Fiona Bertuch g
a
School of Archaeology and Anthropology, Australian National University, Canberra, ACT 0200, Australia
b
School of Earth Sciences, The University of Melbourne, Melbourne, Victoria 3010, Australia
c
Environmental Futures Centre, Griffith University, Nathan, QLD 4111, Australia
d
, Arica, Chile
Instituto de Alta Investigacion, Universidad de Tarapaca
e
Centro de Investigaciones del Hombre en el Desierto, Arica, Chile
f
Research School of Earth Sciences, Australian National University, Canberra, ACT 0200, Australia
g
Institute for Environmental Research, ANSTO, Locked Bag 2001, Kirrawee DC, NSW 2232, Australia

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

Article history: Exposure to toxic arsenic has severe health consequences for past and present societies. This research
Received 26 October 2014 resolves changes in a pre-Industrial population's exposure to the toxin within an arsenic-endemic area of
Received in revised form the Atacama Desert of northern Chile over long timescales. Inductively coupled plasma mass spec-
17 March 2015
trometry (ICP-MS) trace element analysis of human bone and tooth samples from 21 burials at Caleta
Accepted 19 March 2015
Available online 28 March 2015
Vitor on the Pacific coast of northern Chile has established that the pre-Columbian inhabitants were
exposed to elevated levels of arsenic where one third of the sample population had accumulated levels in
their skeletal system indicative of chronic poisoning. Coupled with new accelerator mass spectrometry
Keywords:
Arsenic
(AMS) radiocarbon ages for the skeletal samples, spanning c. 3867 to 474 cal BP and encompassing all
Bone major cultural periods of the region, these results demonstrate the continual risk of arsenic poisoning
Trace element analysis over several millennia of occupation at one site.
Chile Numerous factors may have partially contributed to the population's inferred poisoning, due to the
Human skeletal remains complex interaction of various environmental sources of arsenic and human behaviours. Increased
Caleta Vitor exposure to arsenic could relate to climatic variability influencing sources of drinking water or anthro-
Atacama pogenic activities such as mining and metallurgy or dietary changes associated with agriculture.
Radiocarbon
Assessment of these potential sources of arsenic toxication, including evaluation of modern environ-
Arsenic poisoning
mental data from the region, suggests contaminated drinking water was the most likely cause of
arseniasis.
© 2015 Elsevier Ltd. All rights reserved.

1. Introduction levels of arsenic (As) (Cornejo-Ponce and Acarapi-Cartes, 2011;

Exposure to environmental toxins is a common hazard for
communities living on the geographical or economic fringes of
society. Humans have continuously occupied the Atacama Desert of
South America (Fig. 1) following first settlement of the continent at
least 13,000 years ago, despite it being one of the driest places on
Earth, with virtually no rainfall and scant plant and animal life
(Nún~ ez et al., 2002; Latorre et al., 2013). However, many of the
essential sources of drinking water within the desert have elevated
* Corresponding author. Tel.: þ613 8344 6521.
E-mail address: jswift@westnet.com.au (J. Swift).
Cornejo-Ponce et al., 2011; Bundschuh et al., 2012a).
Arsenic is an abundant trace element in the geology of the An-
dean Cordillera (Byrne et al., 2010). High temperature, pressure and
reducing conditions in this volcanic setting promote arsenic disso-
lution. As-laden geothermal groundwater mixes with aquifers fed by
snow melt from the Andes, which are used directly as a water supply,
and also flow into surface waters (Webster and Nordstrom, 2003;

pez et al., 2012). In addition to erosion and natural leaching,
Lo
anthropogenic sources, such as pollution and mining, also contribute
to local concentrations of arsenic (Bundschuh et al., 2012a).
The public health consequences from exposure to arsenic are
widespread. Contamination of drinking water is of critical concern

http://dx.doi.org/10.1016/j.jas.2015.03.024
0305-4403/© 2015 Elsevier Ltd. All rights reserved.
32 J. Swift et al. / Journal of Archaeological Science 58 (2015) 31e45
Fig. 1. Map of the South Central Andean region showing the Atacama Desert of northern Chile, the location of the study area, Caleta Vitor, and other places mentioned in the text.
and is particularly prevalent in Latin America, where 14 of the
continent's 20 countries record unsafe levels (Bundschuh et al.,
2012a). It is estimated that 1.8 million Chileans are living in
arsenic endemic areas, many of whom are in rural settings without
purification plants where contaminated water is used for drinking
and irrigation (Sancha and O'Ryan, 2008; Bundschuh et al., 2012a).
Arsenic is a carcinogen, with mutagenic effects capable of causing
various cancers (Hopenhayn-Rich et al.,1996; Hopenhayn-Rich et al.,
1998; Smith et al., 2006; McClintock et al., 2012). The genotoxicitiy,
DNA damage and oxidative stress induced by exposure to arsenic are
well established (Ostrosky-Wegman et al., 1991; Lerda, 1994; Moore
et al., 2002; Martínez et al., 2004; Salazar et al., 2004; Andrew et al.,
2006). Arsenic is also teratogenic, able to cross the placental barrier
and interfere with foetal development (Nordstro € m et al., 1979;
Hopenhayn-Rich et al., 2000; Ahmad et al., 2001; Centeno et al.,
2002; Hopenhayn et al., 2003; Milton et al., 2005).
Studies of endemic arsenic areas indicate up to 20% of all deaths
among exposed populations can be attributed to the effects of arsenic
toxicity (Smith et al., 1998; Argos et al., 2010). Symptoms of As
poisoning can be dependent on total dosage. Acute poisoning causes
gastrointestinal, kidney and liver disease as well as myocardial
toxicity and, in the most extreme cases, brain stem failure
(Aufderheide and Rodrígue
z-Martin,1998). Chronic arsenic poisoning
often induces peripheral neuropathy, skin lesions, respiratory ill-
nesses, cardiovascular disease and can also cause goitres, diabetes
mellitus and cancers of the skin, lungs, kidneys, bladder and liver
(Hopenhayn-Rich et al., 1996; Aufderheide and Rodrígue
z-Martin,
1998; Hopenhayn-Rich et al., 1998; Smith et al., 1998, Smith et al.,
2000; Abrahams, 2002; Centeno et al., 2002; Ferreccio and Sancha,
2006; Smith et al., 2006; Coronado-Gonza
lez et al., 2007; Marshall
et al., 2007; Yuan et al., 2007; Liaw et al., 2008; Cornejo-Ponce et al.,
2011). The increased risk of developing these illnesses is sustained for
decades even after limited exposure (Smith et al., 2006).
Prehistoric societies of the Atacama coast are proving particu-
larly useful in understanding exposure of past people to environ-
mental hazards (e.g. Sandweiss et al., 2001; Arriaza, 2005; Arriaza
et al., 2008a; Williams, et al., 2008; Arriaza et al., 2010). Such
research is possible because the arid environment leads to excellent
preservation of hard and soft human tissue, lending itself to
bioarchaeological and bone chemistry studies such as trace
element analyses. Pre-Columbian burials from Arica, Camarones
and Iquique in coastal northern Chile dating to the Archaic
(9000e4000 BP) and Late Intermediate periods (950e500 BP) in
particular have elevated concentrations of hair arsenic (Arriaza
et al., 2010; Byrne et al., 2010). Mummies from Camarones have
revealed especially high levels of arsenic poisoning (e.g. Figueroa
et al., 1988; Arriaza et al., 2010; Silva-Pinto et al., 2010). These
previous studies, however, have not examined any temporal pat-
terns of exposure to arsenic. Nor have they examined samples from
the Formative Period (c. 4000e1500 BP) to the Middle Horizon (c.
1500e950 BP) associated with the Azapa, Alto Ramírez or Tiwa-
naku/Cabuza cultural periods (see Table 1). These are periods of
significant cultural and technological change as well as increased
climate fluctuation (Nún ~ ez and Santoro, 2011; Gayo et al., 2012), all
of which may have had an impact on the risk of exposure to
environmental arsenic.
Retrospective assessments of arsenic exposure have primarily
been constructed from analyses of hair (Arriaza et al., 2010; Byrne
et al., 2010). Such determinations can be somewhat problematic,
particularly if the hair was washed in arsenic-containing water
during life, treated with cosmetics derived from arsenic minerals or
buried in arsenic rich soil after death. This is because keratinous
tissue, such as hair and also fingernails, has a high concentration of
sulphur rich amino acids, which selectively absorb exogenous
arsenic (Young and Smith, 1942; Paddock et al., 1970; Aufderheide
and Rodrígue
z-Martin, 1998; Byrne et al., 2010). Indeed, in a com-
parison of paired Late Intermediate period hair and bone samples
from Camarones mummies, the As concentrations in hair were
found to be much higher (Figueroa et al., 1988). Bones and teeth
have the advantage of being less susceptible to diagenetic uptake of
arsenic than hair and fingernails, particularly in dry environments
(Aufderheide and Rodrígue
z-Martin, 1998).
Modern studies of arsenic concentrations in humans typically
measure As in blood, urine, hair and fingernails, samples less
invasive to obtain than bone. As a consequence, there is no agreed
normal range for bone arsenic. Published analyses of both archae-
ological and modern bone from various locations around the world
suggest normal background levels of arsenic in bone should be
 J. Swift et al. / Journal of Archaeological Science 58 (2015) 31e45
Table 1
Summary of archaeological periods and cultural phases relevant to northern Chile.
Age (BP) Andean Prehistoric Periods
c. 13,000e10,000 Terminal Pleistocene
c. 10,000e4000 Archaic Period Early Archaic
(1000e8000 BP)
Middle Archaic
(8000e6000 BP)
Late Archaic
(6000e4000 BP)
c. 4000e1500 Formative Period Early Formative
(4000e2500 BP)
Late Formative
(2500e1500 B P)
c. 1500e950 Middle Horizon
c. 950e500 Late Intermediate Period
c. 500e418 Late Period
below 1.0 ppm, and quite possibly less than 0.5 ppm (e.g. Lindh
et al., 1980; Wiechula et al., 2003; Djingova et al., 2004; Bocio
et al., 2005; Aras and Ataman, 2006; Shafer et al., 2008). Figueroa
et al.'s (1988) study from Camarones demonstrated that
mummies with macroscopic soft tissue pathologies indicative of
arsenic poisoning as well as elevated levels in hair also had corre-
sponding bone As concentrations between 1 and 13 ppm. Known
modern cases of arsenic poisoning show that toxic levels in bone
can fall within the 0.5e1.0 ppm range (Young and Smith, 1942), but
are usually above 1.0 ppm (Kuo et al., 2000). Based on the available
literature, and particularly the relevant regional study by (Figueroa
et al., 1988), a minimum As limit of 1 ppm is considered to be a
conservative and appropriate level to apply for the purposes of
determining toxic exposure to arsenic for this study.
This research aims to resolve changes in exposure to arsenic
within a pre-Industrial population over long timescales. Bio-
archaeological chemistry is applied to samples of human tooth and
bone from 21 individuals recorded and collected during a field
season at the archaeological site of Caleta Vitor. These analyses
include AMS radiocarbon dating in order to establish an absolute
chronology for the series of skeletal remains sampled from the
burial sites and ICP-MS trace element analysis to determine the
level of exposure to hazardous concentrations of arsenic. The pos-
sibility of diagenetic alteration of the samples is examined through
comparing bone arsenic concentrations to those of the surrounding
burial soil. Possible sources of exposure, such as drinking water,
dietary changes and metallurgy are explored. This study is the first
to test for the presence of arseniasis during the Formative Period
(~4000e1500 BP) to the Middle Horizon (~1500e950 BP), with a
continuous sample set spanning all cultural phases from the late
Chinchorro through to the Inka (c. 3900e500 cal BP).
2. Study area
Caleta Vitor (18.73 S, 70.32 W) is one of a number of inlets that
incise the Pacific coast of the Atacama Desert in northern Chile,
some 30 km south of the border city of Arica (Figs. 1e3). It is the
mouth of Rio Vitor, which has cut a deep outlet to the sea. Seasonal
33
Local Cultural Phases Key developments
First nomadic hunterefisher-gatherers occupy the region.
Acha Specialised adaptations to coastal occupation.
Early Chinchorro
(9500e8000 BP)
Chinchorro Continued development of adaptations
to coastal occupation.
Late Chinchorro Sedentism and the emergence of incipient
agriculture with continued reliance
on marine resources.
Final Chinchorro First ceramics, metallurgy and collective political
(4000e3600 BP) structures. Increasing domestication of plants
Azapa (3600e2500 BP) and animals and the introduction of irrigation.
Alto Ramírez Consolidation of the new technologies from the Early
Formative and the emergence of complex trade networks.
Tiwanaku polities Political integration with the circum-Titicaca region,
expansion (Cabuza) urbanisation, monumental architecture.
Maitas Chiribaya Collapse of Tiwanaku state, prolonged droughts.
(850e650 BP)
San Miguel, Pocoma Continued droughts and further decline of coastal
and Gentilar (650e500 BP) settlement. Competition for resources and the
appearance of defensively walled settlements.
Inka Empire Centralised political control, collective farming,
infrastructure construction, Spanish conquest.
flows from Andean snow melt discharge into the embayment
through the steep sided Quebrada Vitor. The inlet and upstream
river valley are flanked to the north and south by steep slopes. The
ocean floor rises sharply to a broad, sandy beach, abutted by low
terraces of Rio Vitor. Prehistoric occupation and burial sites
concentrated on the narrow littoral terraces and valley flanks at the
back of the cove show where pre-Columbian people were able to
live on the edge of the desert and survive by exploiting marine
resources and freshwater from Rio Vitor.
The archaeological sites at Vitor comprise seven hunter-fisher-
gatherer habitation and burial areas (designated CV1 to CV7)
behind the beach (Fig. 4). An estimated several hundred burials at
the site range from simple interments of skeletal remains to
bundled mummies containing grave goods. Similar settings at Arica
to the north and Caleta Camarones to the south preserve the
world's oldest artificially mummified human remains, the Chin-
chorro mummies, which are up to 8000 years old (Bittmann and
Munizaga, 1976; Aufderheide et al., 1993; Arriaza, 1995; Rivera,
1995).
Relative dating of archaeological context and cultural material,
as well as four previous radiocarbon ages from the burials (Roberts
et al., 2013), suggest these sites encompass all the major cultural
periods of northern Chile (Table 1). The burials examined within
this research were often heavily disturbed, fragmentary and had
been subject to looting, making it difficult to provide confident
estimates of their contemporaneous cultural period. Thus, directly
radiocarbon dating the bone collagen from the remaining burials
permits greater chronological resolution and a more meaningful
interpretation of the arsenic trace element concentrations.
3. Materials methods
In 2010 a team from the Australian National University (ANU),
Flinders University and the University of Melbourne (UoM) in
collaboration with Arica's Universidad de Tarapaca
and Centro de
Investigaciones del Hombre en el Desierto, surveyed the sites at
Vitor and collected bone and cultural materials for further analyses.
The parameters of the field strategy and conditions of the
34 J. Swift et al. / Journal of Archaeological Science 58 (2015) 31e45

Fig. 2. The deep, narrow canyons that traverse the Atacama Desert in northern Chile carrying arsenic laden water to the ocean (Google, 2013).

excavation permit restricted examination of human remains to
preliminary description and circumscribed collection of represen-
tative bone and tooth samples for laboratory analyses. This was
achieved through surface survey and, in the case of any burials, only
limited subsurface investigation of interments that had already
been exposed or disturbed. Due to the limited nature of the
investigation, it was difficult to maintain consistency when
selecting samples and it was not possible to obtain all samples from
the same skeletal element for each burial. However, available
contextual information and relative sizes of bones were carefully
scrutinised to avoid confusing elements from different individuals.
In some instances, particularly where articulated and semi-
articulated remains were present, it was possible to make in-
ferences of sex and age at death from characteristics of cranial,

Fig. 3. Low level oblique aerial image of Caleta Vitor from the west (Google, 2013).
 J. Swift et al. / Journal of Archaeological Science 58 (2015) 31e45
Fig. 4. Caleta Vitor showing the location of archaeological sites CV1e7 and human burials.
mandibular, sacral and pelvic remains and degree of epiphyseal
fusion (see e.g. Buikstra and Ubelaker, 1994; Bass, 1995; Baker et al.,
2005).
Burials suitable for collecting skeletal samples for arsenic trace
element analysis, radiocarbon dating and other analyses were
located at five of the Vitor sites: CV1, CV2, CV3, CV6 and CV7.
Multiple samples were obtained from 21 individuals within 17
burials at these sites. Samples were preferentially obtained from
the cortical bone of the diaphysis or metaphysis of long bones,
teeth, or, when neither of these options were viable, samples were
obtained from the cortical bone of various other elements (phalanx,
clavicle).
Soil samples were obtained from each of the burial sites to
complement chemical analyses of the skeletal material. A sample of
marine mammal bone (Pinnipedia: Otaria flavescens [South Amer-
ican sea lion]) from a midden at CV6 was also collected for
comparative analysis.
3.1. Radiocarbon dating
The skeletal remains were dated by accelerator mass spec-
trometry (AMS) radiocarbon dating, with samples from 10 of the
21 burials submitted to the Australian Nuclear Science and Tech-
nology Organisation (ANSTO, lab code OZN) (Fink et al., 2004) and
a further seven samples submitted to the ANU radiocarbon labo-
ratory (lab code S-ANU) (Fallon et al., 2010) (direct ages had
already been obtained for the remaining four individuals see
Roberts et al., 2013). At the ANU samples were washed in a 2:1
mixture of chloroform and methanol for at least 1 h to remove
lipids. Beyond this point, the methodology employed by both
laboratories was fundamentally the same. Collagen was extracted
and purified using an ultra-filtration protocol similar to Brock et al.
(2010). They were air-dried and demineralised (0.5 M HCl, 5  C),
washed in NaOH (0.1 M, 30 min, room temperature) and HCl
(0.5 M, 1 h, room temperature), rinsing with ultrapure MilliQ™
water between each step, before gelatinisation (pH3 water, 20 h,
70  C), filtration (Ezee filters™) and ultrafiltration (Millipore [at
35
ANSTO] and Vivaspin™ [at ANU] VS15 30 kDa MWCO ultrafilters).
Samples were combusted in evacuated sealed quartz tubes in the
presence of silver foil or wire and copper oxide wire. The CO2
generated was cryogenically collected and purified before con-
version to graphite over an iron catalyst in the presence of
hydrogen at 600  C prior to analysis using AMS.
Stable carbon isotopes were analysed at ANSTO using a Micro-
mas IsoPrime IRMS with varioMicroCube Elemental analyser (Fink
et al., 2004) and stable carbon and nitrogen isotopes at ANU in a
Sercon 20e22 IRMS connected to an ANCAeGSL operating in
continuous flow mode. Samples were referenced to an in-house
gelatin standard, and corrected against the international stan-
dards USGS-40 and USGS-41.
In order to account for the marine reservoir effect, an estimation
of the marine input percentage for each sample was calculated
using the technique described in Roberts et al. (2013) using regional
data to determine endpoints for linear extrapolation from a 100%
terrestrial diet in northern Chile (d13C terrestrial
endpoint ¼ 20.1%) to a 100% marine diet in northern Chile (d13C
marine endpoint ¼ 8.7%). The final ages were calibrated to 95.4%
probability using Calib 6.1.0 (Stuiver and Reimer, 1993) with the
mixed SHCal04 and the Marine09 (Reimer et al., 2009) datasets. A
regional marine reservoir correction, DR of 226 ± 98 yr, was applied
as per Ortlieb et al. (2011) for northern Chile.
3.2. Arsenic trace element analysis
Skeletal arsenic was measured by ICP-MS for 20 samples of
human cortical bone from sites CV1, CV2, CV3 and CV6. The bone
samples from CV7 were insufficiently preserved and, as such, a
tooth sample (dentine from a right maxillary second molar) from
CV7 was instead analysed. The marine mammal bone from CV6 was
also submitted for analysis, as were the five samples of sightly
acidic (pH 5e6) sandy soil, from CV1, CV2, CV3, CV6 and CV7.
The samples were prepared as per Shafer et al.'s (2008)
recommendation for removing exogenous As contamination. The
outer surface of the bone samples was gently removed using a
36 J. Swift et al. / Journal of Archaeological Science 58 (2015) 31e45
Dremel rotary tool. The samples for analysis were then taken from
the cortical bone. The tooth was sampled by gently cracking it in a
sterile plastic bag with a hammer, then using a Dremel rotary tool
to remove the enamel from the dentine.
Samples were processed and analysed at the geochemistry
laboratory in the School of Earth Sciences at UoM. Between 23 and
140 mg of bone and tooth were dissolved in concentrated nitric acid
in Teflon beakers, then ultra-pure water was added. About 100 mg
of the soil samples were dissolved overnight with a mixture of HF
and nitric acid in Teflon beakers at 80  C, then evaporated to dry-
ness and refluxed with nitric acid. The residue was then dissolved
with nitric acid and ultra-pure water.
The solutions were transferred to centrifuge tubes and centri-
fuged. An aliquot of each solution was added to a second centrifuge
tube and diluted with a dilute nitric acid solution spiked with in-
ternal standards. All standards, blanks and samples were also
spiked to 4% ethanol to reduce differences due to carbon
enhancement of As ionization efficiency. The total dilution factors
were 1000 for the bone samples and 2000 for the soil samples.
Analysis followed procedures described by Eggins et al. (1997) and
Kamber et al. (2005) using an Agilent 7700x ICP-MS in cell gas
mode using He.
4. Results
4.1. Radiocarbon dating
Samples from 13 of the 17 individuals submitted were dated
successfully (Table 2). These, combined with four ages from Roberts
et al. (2013), directly date 17 of the 21 individuals studied at Vitor.
The skeletal samples range in age from 474 to 3870 cal BP. These
ages come from sites CV1, CV2, CV3 and CV6. The samples from CV7
proved to be unsuitable for dating.
The quality of the samples was assessed by their collagen yield
and the carbon to nitrogen ratio (C:N) of the extracted collagen.
Four samples were unable to be dated as they yielded insufficient
collagend. The C:N of the collagen for each sample was assessed as
an indicator of carbonaceous contamination. Modern bone collagen
has a C:N ratio within the range of 2.8e3.6 (DeNiro, 1985; Ambrose,
1990; Van Klinken, 1999).
During pre-treatment of the samples at ANU, a yellowish dis-
colouration was noticed of the solvent wash, possibly indicative of
excess lipids. If elevation of the C:N ratio was caused by lipids from
the bone, the conventional radiocarbon age should not be affected,
but the d13C values would vary and affect the calibrated ages. After
initially yielding high C:N ratios, samples CV2 B1 S2 and CV6 B1 S4
were dated again using supplementary material. The second
collagen extraction for these samples yielded acceptable C:N and
the conventional radiocarbon ages were still concordant with the
ages from the previous high C:N extractions (CV2 B1 S2 first
extraction [OZP075] ¼ 1175 ± 25 BP and second extraction
[OZP580] ¼ 1170 ± 30 BP; CV6 B1 S4 both first and second ex-
tractions [OZP072] and [OZP579] ¼ 1890 ± 35 BP). These results
support the observation that the elevated C:N may have been
caused by lipids from the bone. If this is the case, it is possible the
uncalibrated ages for the two remaining affected samples (CV6 B1
S3 and CV6 B1 S6) may be valid, but they are reported with the
caveat that they had elevated C:N ratios.
4.2. Arsenic trace element analysis
Arsenic concentrations of the human bone samples ranged from
0.124 ppm to 5.993 ppm with a mean of 1.132 ± 1.347 ppm (Table 3,
Fig. 5). This data, as with that from other regional studies, has
substantial intra-population variation (variance ¼ 1.813, standard
deviation ¼ 1.347). The dentine from the tooth had an As concen-
tration of 0.021 ppm. It is unclear whether this is representative of
arsenic accumulation during tooth formation, or accumulation
during life. Some trace elements, such as lead and calcium, are
known to continually accumulate in dentine throughout life
(Ericson et al., 1979; Hillson, 1996). There is some preliminary ev-
idence to suggest this is also the case for arsenic in dentine, but at
approximately a tenth of the concentration in bone (Rauh et al.,
2011; Dudgeon et al., in press). At any rate, the concentration of
0.021 ppm is low compared to other published data for contami-
nated teeth, averaging 0.45 ppm (Dudgeon et al., in press). With
scant data for comparison, it appears the concentration in this tooth
is not indicative of poisoning.
Seven of the 21 skeletal samples contained elevated concen-
trations of arsenic (>1 ppm), indicative of chronic arsenic
poisoning. These values ranged from 1.064 ppm to 5.993 ppm with
a mean of 2.376 ± 1.702 ppm. The South American sea lion (O.
flavescens) bone had an As concentration of 9.834 ± 0.243 ppm.
Arsenic concentrations of the soil samples ranged from
10.159 ppm to 26.008 ppm with a mean of 16.591 ± 6.005 ppm
(Table 4).
Due in part to the variance of the results, the total number of
samples from each of the burial sites at Vitor (CV1 n¼3; CV2 n¼5;
CV3 n¼3; CV6 n¼9; CV7 n¼1) is too small to determine whether
any changes between the sites are statistically significant. However,
there may have been a higher rate of inferred poisoning among
those who were buried at CV2. The burial sites at CV1, CV3 and CV6
all maintain a possible poisoning ratio close to one-third, however,
three out of the five burials (60%) sampled from CV2 have elevated
levels of arsenic. The burials from CV2 are amongst the more recent,
dating from the Middle Horizon (~1500e950 BP) through to the
Late Intermediate Period (~950e500 B P). When the results are
examined by cultural period, the Tiwanaku phase (Middle Horizon;
~1500e950 BP) burials proportionally have the greatest number of
instances of increased arsenic exposure (four out of the nine),
representing two-thirds of all the suspected cases of arseniasis
within this study.
The sole case of possible poisoning from CV1 (Late Chinchorro to
Azapa phase) was only slightly above 1.0 ppm and the sole case
from CV3 (Alto Ramírez) between 1.0 and 2.0 ppm, whereas cases
from CV6 and CV2 (Tiwanaku through to Inka) reached much
higher concentrations, with a mean of 2.736 ppm for those indic-
ative of arseniasis from these sites. However, this is only reported
with the caveat that the number of samples from each site is too
small to produce significant results (F¼0.726, p¼0.551; ANOVA when
data is grouped by site).
Nonetheless, out of the seven individuals who pre-date
2000 cal BP, there is only one, borderline (1.064 ppm) case of
possible poisoning. All other instances of inferred arseniasis post-
date 2000 cal BP. Half (seven out of 14, with a mean As concen-
tration of 2.597 ppm) of the post-2000 cal BP section of the sample
set exhibit elevated arsenic and indicate a possible trend towards
higher frequencies of exposure as well as increasingly high con-
centrations over time. However, linear regression analysis of the
relationship between skeletal arsenic concentrations and age
shows the negative correlation is weak (r¼ 0.245) and not signif-
icant (p¼0.284).
There is no apparent relationship between estimated age at
death and likelihood of suffering arseniasis for any of the in-
dividuals studied (t ¼ 1.77, p>0.05). It was not possible to deter-
mine whether there was any correlation between arsenic levels and
sex; while one of the suspected poisoned individuals was a male,
sex could not be determined for the remaining six out of the seven
inferred poisoned individuals due to the fragmentary and dis-
articulated nature of the remains.
 J. Swift et al. / Journal of Archaeological Science 58 (2015) 31e45 37

Table 2
Radiocarbon results and bone quality indicators for human skeletal samples from Caleta Vitor.

Site Burial Sample Sample Laboratory ID Collagen Collagen Collagen Conventional radiocarbon Marine proteina Calibrated Age cal BP
number type (Lab) yield % (wt) C:N d13 C (‰) Age BP ± 1s % (95.4% probability range)b

CV1 1 CV1B1S1 Bone OZN921 3403e3770c

2 CV1B2S2 Tooth S-ANU3341 4.0 3.2 12.0 3815 ± 41 71 3456e3870
3 CV1B3S3 Bone S-ANU8872 0d e e e e e
CV2 4 CV2B1S1 Bone OZP076 13.76 3.5 12.6 1310 ± 25 66 679e934
5 CV2B1S2 Bone OZP075 10.0 4.3e 13.7 1175 ± 25 56 655e887e
CV2B1S2 OZP580 3.7 3.3 11.7 1170 ± 30 74 526e786
6 CV2B2aS2 Bone OZN923 1103e1408c
7 CV2B2bS1 Bone OZN924 1081e1370c
8 CV2B3S1 Bone OZP074 13.64 3.4 11.1 1255 ± 25 79 559e876
CV3 9 CV3B1S2 Bone S-ANU8873 1d e e e e e
10 CV3B2S1 Bone OZN919 1821e2200c
11 CV3B3S2 Bone OZP073 9.68 3.6 13.3 2525 ± 30 60 2008e2325
CV6 12 CV6B1S1 Bone S-ANU33420 19.4 3.2 12.7 990 ± 39 65 474e668
13 CV6B1S3 Bone S-ANU30739 3.9 3.7e 12.8 1848 ± 25 64 1260e1522e
14 CV6B1S4 Bone OZP072 5.76 4.4e 14.2 1890 ± 35 52 1320e1593e
OZP579 0.8 3.3 12.0 1890 ± 35 71 1234e1540
15 CV6B1S5 Bone OZP071 2.59 3.6 13.3 1850 ± 30 60 1277e1526
16 CV6B1S6 Bone OZP070 5.55 3.9e 13.6 1845 ± 30 57 1288e1529e
OZP578 4.3 5.0e e e e e
17 CV6B3S1 Bone S-ANU30232 18.2 3.2 11.3 1560 ± 25 77 820e1188
18 CV6B4S1 Bone OZP068 0d e e e e e
OZP577 0d e e e e e
19 CV6B5S2 Bone S-ANU30233 15.9 3.2 12.6 1000 ± 25 66 487e665
20 CV6B6S1 Bone OZP069 19.0 3.3 12.3 1940 ± 30 68 1292e1584
CV7 21 CV7B1S1 Tooth OZP576 0d e e e e e
Bone OZP067 0d e e e e e
a
Estimation of percentage of marine input calculated using the technique described in Roberts et al. (2013) using regional data to determine endpoints for linear
extrapolation from a 100% terrestrial diet (d13C terrestrial endpoint ¼ 20.1%) to a 100% marine diet (d13C marine endpoint ¼ 8.7%).
b
The ages were calibrated to 2s using Calib 7.0.4 (Stuiver and Reimer, 1993) using the mixed southern hemisphere SHCal13 (Hogg et al., 2013) and the Marine13 (Reimer et
al., 2013) datasets with DR ¼ 226 ± 98 yr (Ortlieb et al., 2011).
c
Previously published in Roberts et al. (2013).
d
Insufficient collagen preserved for dating. Sample CV3B1S2 did have some collagen, but high-precision measurements required to obtain C:N and stable isotope data from
such a small proportion of collagen was not available in time for inclusion in this report.
e
Collagen extracted from these samples had a C:N > 3.6. Enough material was available from the original samples of CV2 B1 S2, CV6 B1 S4 and CV6 B1 S6 for additional
material to be submitted for a second round of collagen extraction. After a second round of extractions for CV2 B1 S2 (OZP580) and CV6 B1 S4 (OZP579), both samples yielded
collagen with acceptable C:N and the radiocarbon ages derived from these extractions are reported in preference to the ages obtained from the first extractions. The additional
extraction of collagen from extra material for CV6 B1 S6 (OZP578) still yielded collagen with C:N > 3.6.

Table 3
Arsenic concentrations (ppm) of tooth and bone samples from Caleta Vitor.

Site Burial Sample Sample Sex Age Calibrated Age cal BP Period (Cultural Phase) As mg/g (ppm)
number type (95.4% probability)

CV1 1 CV1B1S1 Bone Male Young adult 21þ 3403e3770 [OZN921]a Formative (Late Chinchorro/Azapa) 0.588
2 CV1B2S3 Bone Male Young adult 18e22 3456e3870 [S-ANU33419] Formative (Late Chinchorro/Azapa) 0.272
3 CV1B3S3 Bone na Adult na Formative (Late Chinchorro/Azapa) 1.064
CV2 4 CV2B1S1 Bone na Adult 679e934 [OZP076] Late Intermediate (Maitas Chiribaya) 0.292
5 CV2B1S2 Bone na Infant 1 526e786 [OZP580] Late Intermediate 5.993
(Maitas Chiribaya/San Miguel & Gentilar)
6 CV2B2aS2 Bone na Adult 1103e1408 [OZN923]a Middle Horizon (Tiwanaku/Cabuza) 1.530
7 CV2B2bS1 Bone na Adult 1081e1370 [OZN924]a Middle Horizon (Tiwanaku/Cabuza) 1.305
8 CV2B3S1 Bone na Adult 559e876 [OZP074] Late Intermediate 0.314
(Maitas Chiribaya/San Miguel & Gentilar)
CV3 9 CV3B1S2 Bone na Infant/Child 1 to 6 na Formative (Alto Ramirez) 0.708
10 CV3B2S1 Bone Male Adult 1821e2200 [OZN919]a Formative (Alto Ramirez) 1.818
11 CV3B3S2 Bone Male Young Adult 2008e2325 [OZP073] Formative (Alto Ramirez) 0.814
CV6 12 CV6B1S1 Bone na Adult 474e668 [S-ANU33420] Late Intermediate/Late 0.128
(San Miguel & Gentilar/Inka)
13 CV6B1S3 Bone na Infant 1260e1522 [S-ANU30739] Middle Horizon (Tiwanaku/Cabuza) 0.542
14 CV6B1S4 Bone na Infant 1234e1540 [OZP579] Middle Horizon (Tiwanaku/Cabuza) 0.497
15 CV6B1S5 Bone na Infant 1277e1526 [OZP071] Middle Horizon (Tiwanaku/Cabuza) 0.856
16 CV6B1S6 Bone na Juvenile/adolescent 1288e1529 [OZP070] Middle Horizon (Tiwanaku/Cabuza) 2.829
17 CV6B3S1 Bone na Adult 820e1188 [S-ANU30232] Middle Horizon (Tiwanaku/Cabuza) 0.124
18 CV6B4S1 Bone na Adult na Middle Horizon (Tiwanaku/Cabuza) 2.021
19 CV6B5S1 Bone na Adult 487e665 [S-ANU30233] Late Intermediate/Late 0.685
(San Miguel & Gentilar/Inka)
20 CV6B6S1 Bone na Adult 1292e1584 [OZP069] Middle Horizon (Tiwanaku/Cabuza) 0.268
CV7 21 CV7B1S1 Tooth Female Adult (~45e55) na Archaic (Chinchorro) 0.021
a
Ages from Roberts et al. (2013).
38 J. Swift et al. / Journal of Archaeological Science 58 (2015) 31e45
Fig. 5. Arsenic concentrations (ppm) within human tooth and bone samples from Caleta Vitor.
Overall, the elevated exposure to arsenic inferred for some of
the pre-Columbian inhabitants from Vitor accords with the known
effects of increased environmental arsenic upon modern and
ancient populations of northern Chile. However, the prevalence of
elevated skeletal arsenic (one-third of the population) is lower than
the levels observed in other studies from northern Chile, which
found poisoning in over 90% of the populations at Azapa, Morro,
Yungay, Camarones and Iquique by analysing hair samples (Arriaza
et al., 2010; Byrne et al., 2010).
5. Evaluation
5.1. Diagenesis
Assessing the impact of post-mortem processes on the
elemental concentrations of bone is an essential precursor to
evaluating the results of any trace element analyses. Determining
the preservation quality of bone in regards to trace element con-
centrations can be problematic. Attempting to assess diagenetic
uptake of one element by examining the concentrations or ratios of
other elements is unreliable as the pathways for absorption,
diffusion and resultant contamination of bone by trace elements is
element specific (Pike and Richards, 2002; Dudgeon et al., in press).
Previous research on the diagenetic uptake of arsenic in bone
has shown that contamination occurs via surface contact, and up-
take in cortical bone is superficial, restricted to the outer 500 mm of
the periosteum and outer cortex (Shafer et al., 2008; Dudgeon et al.,
in press). However, it is possible to remove the contaminating
arsenic by cleaning or removing the outer surface of samples, which
was done during the sample preparation for this research (Oakberg
et al., 2000; Shafer et al., 2008; Dudgeon et al., in press).
Burial conditions are the principle factor influencing diagenetic
alteration of bone and the degree of alteration is highly variable
depending on the site and environmental conditions (Shafer et al.,
2008). A number of investigations measuring As concentrations in
archaeological bone have concluded the skeletal samples were
Table 4
Arsenic concentrations (ppm) within soil samples from Caleta Vitor and bone:soil ratios on a site by site basis.
Site Sample numbers Sample depth (m)
CV1 VR-13 0.17
CV2 VR-16 0.44
CV3 VR-06 0.40
CV6 VR-08 0.85
CV7 VR-01 0.23
diagenetically altered (e.g. Zapata et al., 2006; Rasmussen et al.,
€
2009; Ozdemir et al., 2010; Güner et al., 2011). However, all of
these studies were from environments substantially different to
that of northern Chile; they all reported significant ground or
meteoric water, in contrast to the extreme aridity of the Vitor study
area with no groundwater or rainfall at the burial sites. These
conditions were maintained throughout the late Holocene (see
Nún~ ez et al., 2002) and the burial sites are well elevated above the
Rio Vitor and local water table to preclude the possibility of
contamination even if surface- or groundwater levels had been
higher in the past.
The presence of water is an important factor to consider when
evaluating the possibility of diagenesis because groundwater is the
means by which various elements, including arsenic, are mobilised
and then able to contaminate bone. The environmental setting of
the study area lends weight to the validity of the results from Vitor.
Indeed, the hyperarid conditions of the Atacama as well as the low
acidity of the soil have been shown to provide optimal conditions
for unaltered preservation (Feldmann and Charnock, 2006; Arriaza
et al., 2010; Byrne et al., 2010).
Another method for examining the likelihood of diagenetic
arsenic uptake in bone is to compare the results with the arsenic
concentrations of the surrounding burial soil. Previous studies
affected by diagenesis show bone:soil ratios of As of at least 2.5:1
€
(Oakberg et al., 2000; Ozdemir and Erdal, 2010; Güner et al.,
2011). Contaminated bone samples often have a greater concen-
tration of As than the surrounding burial soil as the bone tissue
continues to accumulate the element in what is described as a
sink effect until it reaches an equilibrium whereby the As content
of the bone is several orders of magnitude higher than the sur-
rounding soil (Pike and Richards, 2002). The As concentrations in
bone from Vitor (X¼1.132 ppm) were less than that of the sur-
rounding soil (X¼16.591 ppm), with a bone:soil ratio of 0.068:1.
This was also true when the mean skeletal As concentrations were
compared to the soil As concentrations on a site-by-site basis (see
Table 4).
1 1
As soil mg g (ppm) Mean As (bone/tooth) mg g (ppm) Bone:Soil
17.728 0.641 0.036
10.159 1.887 0.186
13.046 1.113 0.085
26.008 0.883 0.034
16.013 0.021 0.001
 J. Swift et al. / Journal of Archaeological Science 58 (2015) 31e45
Higher arsenic concentrations in juveniles and infants are
another possible indicator that bones have been diagenetically
altered, due to the greater porosity of these bones (Wiechula et al.,
2003; Aras and Ataman, 2006). At Vitor, there was no apparent
relationship between age at death and As concentrations in bone.
The difference in mean As concentration between adult and sub-
adult remains was not significant (t ¼ 1.77, p>0.05).
The possibility of post-depositional uptake of As cannot be
categorically dismissed without further understanding of the pro-
cesses of diagenesis of human bone, particularly a more robust,
specific test for diagenetic arsenic, but based on the current un-
derstanding of these processes and the evidence and tests pre-
sented above, the results of arsenic poisoning within the
population at Vitor appear valid. Given the high endemic levels of
arsenic in northern Chile, the health consequences known to have
been experienced by inhabitants in recent times, the soft tissue
evidence of arseniasis in other pre-Columbian mummies from the
area, the extreme aridity of the environment and the apparent lack
of any significant diagenetic alteration, it is reasonable to infer that
these results are a reflection of some of the inhabitants of Vitor
having suffered from chronic arsenic poisoning.
6. Discussion
The accumulation of toxic elements such as arsenic in humans
may be a reflection of both changing environmental exposure and
anthropogenic behaviours. For example, variability in the level of
arsenic exposure within and between burial assemblages from
other studies in the Atacama has been attributed to regional
mobility, possibly related to exogamous marriages and mortuary
practices (Arriaza et al., 2010; Byrne et al., 2010).
Humans can be exposed naturally to arsenic through soil, water,
food and air, and anthropogenically through metallurgical practices
and the use of chemical compounds containing arsenic for indus-
trial waste disposal, pesticides, fungicides, preservatives and some
traditional and herbal medicines (Garry, 1986; Cornejo-Ponce and
Acarapi-Cartes, 2011; Cornejo-Ponce et al., 2011; Graef and Lovejoy,
2012). Possible sources and mechanisms of arsenic exposure for the
past inhabitants of Vitor may have included agricultural practices,
diet, metallurgy and drinking water.
6.1. Agriculture and diet
Intensification of human activities in the Atacama from around
2000 B P may have increased the local inhabitants' exposure to
arsenic. Changes from this time included the full emergence of
intensive farming societies, and corresponding increases in popu-
lation size (Nester et al., 2007; Gayo et al., 2012). Lowland valleys
had irrigated pastures and inland farming contributed agricultural
produce to the staple marine diet (Kelley et al., 1991; Rivera, 1991;
Nún ~ ez and Santoro, 2011).
In general, plants are “geochemical barriers”, only passing on to
their consumers a limited amount of As from the soil in which they
have been grown (Abrahams, 2002 p.23, Smith et al., 2009). While
in most cases plant absorption may be a fraction of the total arsenic
in soil, absorption through the stomach wall after consumption of
the plants by humans is a fraction of the total arsenic taken up by
the plants (Bundschuh et al., 2012b).
A previous study of the bioavailability of arsenic from soil in the
neighbouring valleys determined that despite high total arsenic
content in the soil from the region, it was largely associated with
the least mobile fractions bound to iron oxides, and therefore un-
likely to pose a health risk to those consuming locally grown
agricultural products (Cornejo-Ponce and Acarapi-Cartes, 2011).
Using the soil As concentrations for the Vitor sites from this study
39
with the regression equation ([As]bioavailable to humans ¼ 0.0114
[As]Soil þ 1.5824) proposed by Cornejo-Ponce and Acarapi-Cartes
(2011) to determine the bioavailability of arsenic directly from
contaminated soil of northern Chilean valleys to local residents
reveals a soil arsenic bioavailability of 1.77 ± 0.06 ppm for Vitor. In
spite of the high total arsenic content of the soil, this level of
bioavailability of arsenic from soil is considered to be within a safe
range for humans (Cornejo-Ponce and Acarapi-Cartes, 2011).
Previous studies of llama meat from As afflicted areas have also
found it did not exceed the maximum safe As concentration limit
(Bundschuh et al., 2012b), another indication that local soil and
natural vegetation are not the cause of the human arsenic tox-
ication in the region. It thus seems unlikely that either direct
interaction with the soil or the introduction of agricultural products
to the diet were the cause of poisoning at Vitor.
6.1.1. Marine food
Dietary intake of As is strongly influenced by the amount of
seafood in the diet as it typically contains much higher As con-
centrations than terrestrial based foods (Underwood, 1977; Aras
and Ataman, 2006). Previous C and N stable isotope results along
with the archaeological material and middens at Vitor suggest the
inhabitants had economies almost entirely based upon the
extraction of marine resources (Roberts et al., 2013). The coastal
seawaters of northern Chile are contaminated by discharge of
sediment and water from rivers with elevated As. Marine plants
and animals readily bio-accumulate As dissolved in water
(Bundschuh et al., 2012b). Exposure to As through seafood con-
sumption can be significant and several studies have noted a cor-
relation between seafood consumption and elevated As exposure in
coastal populations around the world (Heinrich-Ramm et al., 2001;
Becker et al., 2003; Hysong et al., 2003; Heitland and Ko € ster, 2006;
Link et al., 2007; Fillol et al., 2010; Bundschuh et al., 2012b).
Seaweed is known to be very high in arsenic, with reported
concentrations ranging from 18 to 135 ppm (Feldmann et al., 2000;
McSheehy and Szpunar, 2000; Kohlmeyer et al., 2003; Wei et al.,
2003; Rasmussen et al., 2009). The consumption of seaweed by
past and present Chilean populations has been recorded elsewhere
(Aaronson, 1986; Dillehay et al., 2008). While no prior analysis of
the seaweed at Vitor has been conducted, one edible genus of
seaweed, Porphyra, which is abundant in Chile, and one of the most
commonly consumed seaweeds worldwide, is known to contain
high concentrations of As (Kohlmeyer et al., 2003; Wei et al., 2003).
Various fish and mollusc species from northern Chile have
recorded elevated As levels (Lavanchy Dougnac, 1999). Cornejo-
Ponce et al. (2011) analysed arsenic content of three species of
non-migratory marine fish and seven species of marine molluscs
from the bays of Vitor and Camarones. In general, arsenic concen-
trations accumulated by non-migratory marine life at Camarones
were higher than those at Vitor. Fish and molluscs from Vitor largely
had arsenic concentrations within a safe level for human con-
sumption. The only exception was the Chilean abalone (Concholepas
concholepas) (Cornejo-Ponce et al., 2011), the shells of which are
found in abundance within the archaeological middens of Vitor.
These localised studies do not take into account the potential As
concentrations of larger, migratory species of fish and marine
mammals which were also widely consumed at Vitor. Middens
from the study area have an abundance of marine mammal re-
mains, particularly sea lion (O. flavescens), but also unidentified
species of whale, as well as large predatory fish, such as the dol-
phinfish (Corpyhaena equiselis). Notably, previous C and N stable
isotope analysis from Vitor suggested the inhabitants' marine diet
was derived from the upper trophic levels (Roberts et al., 2013). The
analysis of the sea lion (O. flavescens) bone within this study
recorded an As concentration of 9.834 ± 0.243 ppm, suggesting that
40 J. Swift et al. / Journal of Archaeological Science 58 (2015) 31e45
marine animals at higher trophic levels might have accumulated
dietary As. The arsenic concentration in the pinniped bone,
collected from a CV6 midden (Middle Horizon to Inka; c.
1500e418 B P), shows this component of the diet could have been a
substantial source of As, albeit based on one sample.
Certain marine foods from coastal northern Chile may contain
elevated concentrations of arsenic and, indeed, other studies from
the Atacama have similarly found elevated rates of arsenic exposure
among communities reliant on marine resources (Arriaza et al.,
2010; Byrne et al., 2010). However, arseniasis has also been recor-
ded in populations more heavily dependent on terrestrial based
food sources (Feldmann and Charnock, 2006). Additionally, some of
the individuals from Vitor (e.g. CV1B1) inferred to have a high ma-
rine diet from previous stable C and N studies (Roberts et al., 2013)
had low skeletal arsenic. It is, therefore, difficult to conclusively
attribute elevated skeletal arsenic at Vitor to a marine diet.
6.1.2. Cooking and food preparation
The processes involved with cooking and preparing food must
also be considered as they can cause a significant increase in As
content due to the solubilisation of arsenic when heated (Vahter
et al., 1995; Del Razo et al., 2002; Mun ~ oz et al., 2005; Bastías
et al., 2010; Bundschuh et al., 2012b). An increase in total arsenic
content, some by as much as 500%, has been observed in some
foods, including garlic, maize, spinach, cauliflower, beans and
pumpkin, when prepared with As contaminated water (Díaz et al.,
2004). Concentrations of As further increase depending on cooking
time, temperature and the volume of water (Díaz et al., 2004;
Bundschuh et al., 2012b). Frying, grilling or baking seafood also
dramatically increases As content, particularly at temperatures of
150  C and higher (Devesa et al., 2001a, Devesa, et al., 2001b,
Devesa, et al., 2001c, Devesa, et al., 2005).
The people at Vitor were certainly heating food, as evidenced by
charred animal and plant remains in discrete hearths, which have
been noted at CV1, CV2, CV3, CV4 and CV6. The abundance of
ceramic vessels at the sites means that it is possible food prepa-
ration included boiling. This evidence, coupled with elevated con-
centrations of arsenic in the local water supply (see Section 6.3 e
Drinking Water, below), suggests the elevated skeletal arsenic
levels in some of the population at Vitor could be attributable to
cooking processes concentrating arsenic in food. Nevertheless, the
overall evidence for significant dietary arsenic input is inconclusive.
6.2. Metallurgy
Geologically, arsenic is hosted within igneous and sedimentary
rock and most commonly mineralised in association with copper,
lead and gold (Cornejo-Ponce et al., 2011). Arsenic-rich minerals
often naturally occur alongside copper-rich minerals and as an
impurity within copper ores (Merkel et al., 1992; Goffer, 2007). Of
notable relevance to Chile is the mining of copper, which results in
exposure to arsenic. Smelting of copper to create alloys, such as
bronze in particular, produces highly toxic arsine gas (Aufderheide
and Rodrígue
z-Martin, 1998).
Presently, industrial exposure is a common source of arsenic
poisoning (Garry, 1986; Lagerkvist and Zetterlund, 1994; Simonato
et al., 1994; Graef and Lovejoy, 2012). Modern studies have
demonstrated anthropogenic exposure to metals is reflected in the
trace element concentrations of hair and bone (Wiechula et al.,
2003; Jurkiewicz et al., 2004). Studies of lead and copper smelters
in Canada, the United States, Zaire and Sweden have noted increased
exposure, including elevated arsenic concentrations in hair and
bones, in the smelter workers and nearby residents (Jervis et al.,
1977; Lindh et al., 1980; Polissar et al., 1990; Tshiashala et al., 1990).
Over the past 2000 years, copper, copperearsenic alloys and
bronze (an alloy of copper and tin) were readily used by the people
of the South Central Andes. Both the Tiwanaku and Inka utilised
arsenical-copper alloys sourced from their outlying settlements.
Tiwanaku and Inka expansionist strategies also targeted new areas
for their mineral wealth. The subjugated communities of these
empires were required to mine local resources to be conveyed back
to the heartland. It is believed northern Chile was the major source
of copper for the Tiwanaku and Inka states (Graffam et al., 1996;
Zori, 2011; Figueroa et al., 2013; Salazar et al., 2013).
Much of northern Chile, including Quebrada Vitor, is rich in
copper ores, including atacamite (Letchman and Klein, 1999). There
is a modern, inactive copper mine at the foot of Vitor's northern
headland and another active mine, the Santo Domingo, on the
northern slopes a short way up the valley. The geological outcrop at
the northern end of the bay contains visible seams of copper ore,
which could have been directly exploited by the past inhabitants.
Indeed, copper artefacts, primarily fishhooks, have been located at
site CV6. Burial inclusions of copper have also been recorded in
neighbouring sites at Morro, Quiani and Pisagua and sheets of
copper and clay moulds for casting have been identified in
Camarones Valley (Schiappacasse and Niemeyer, 1984). Copper ore,
slag, metal and smelting furnaces have also been discovered within
archaeological contexts in northern Chile, with evidence of copper
smelting from at least 2050 cal BP (Graffam et al., 1996). X-ray
fluorescence analysis of copper slags of this antiquity in northern
Chile has revealed accessory arsenic (Graffam et al., 1996).
Copperearsenic alloys (arsenical bronze and arsenical copper)
replaced unalloyed copper as one of the most common metal
products produced during the Middle Horizon to the end of the Late
Intermediate Period (from about 1150 to 500 years BP) (Letchman,
1991; Merkel et al., 1992; Letchman and Klein, 1999; Stanish, 2003;
Goffer, 2007). While the initial discovery may have been uninten-
tional, it is believed the continued addition of arsenic bearing
minerals in copper smelting charges was deliberate as the cop-
perearsenic alloy is superior to pure copper in that it is more easily
worked, harder, holds a sharper edge, melts more easily and is
better for casting and forging (Goffer, 2007).
Metallurgical sites from the region suggest smelting of cop-
perearsenic alloys took place in coastal settlements, rather than the
highlands (Letchman, 1991). Artefacts recovered from Peruvian
sites show a blow-tube method of smelting may have been utilised.
Ceramic tobera (blow-tube tips) were attached to cane blow tubes
and used to increase the temperatures within crucibles or furnaces
(Letchman, 1991). If a similar method had been employed for co-
smelting copper and arsenic at Vitor, the smelters would surely
have inhaled arsine gases. Indeed, the bone samples from Vitor
contain higher concentrations of As than those of modern copper
smelter workers (see Lindh et al., 1980). However, the high As levels
in some juvenile individuals is unlikely to have been derived from
their direct involvement in smelting.
Only limited archaeological excavation has been undertaken at
Vitor to date, but further investigations to determine the presence
or absence of artefacts associated with metal casting and process-
ing, such as crucibles, furnaces, moulds and slag, may reveal
whether the inhabitants mined and processed metals.
6.3. Drinking water
Accidental arsenic poisoning from consumption of contami-
nated water is well documented (Zaldívar, 1980; Smedley and
Kinniburgh, 2002; Bhattacharya et al., 2007; Steinmaus et al.,
2013). Modern analysis of the aquifers in Vitor has revealed un-
safe levels of arsenic in the groundwater, with three out of four
wells tested containing higher concentrations than the WHO safe
 J. Swift et al. / Journal of Archaeological Science 58 (2015) 31e45
Fig. 6. Regional water arsenic concentrations in northern Chile.
limit of 0.01 ppm (10 mg L 1) (Cornejo-Ponce et al., 2011; WHO,
2011). As concentrations in the wells at Vitor (7.83 ± 0.13 mg L 1,
36.98 ± 0.38 mg L 1, 30.02 ± 0.24 mg L 1 and 16.78 ± 0.65 mg L 1
[Cornejo-Ponce et al., 2011]) are somewhat comparable to those
from the city of Arica (12e88 mg L 1 [Arriaza et al., 2010]), but
generally lower than many other settlements in the region,
particularly the extreme levels recorded in the river at Camarones
(700e1300 mg L 1 [Arriaza et al., 2010]) (see Fig. 6).
The harsh, arid environment of Vitor means it is subject to
fluctuating availability of water. No surface water was present
during the winter 2010 field season. Nowadays, local inhabitants of
Vitor source water from arsenic contaminated wells. However,
ephemerally available surface water can also be drawn directly
from Rio Vitor within the valley floor when available.
Sources of freshwater in the Atacama vary seasonally. In the
austral summer, the rivers and aquifers of the coastal valleys are
typically higher due to rainfall and snowmelt in the highlands
recharging underground springs. However, flow is minimal during
the rest of the year (Arriaza et al., 2008b). Variability of water
availability may also mean exposure to arsenic in antiquity was
somewhat dependent on seasonal and longer term changes in
climate, and thus water availability, over time.
The El Nin ~ o-Southern Oscillation (ENSO) can have a significant
effect on the habitability of the Atacama Desert. Flooding rains of El
Nin~ o events increase stream flow and recharge aquifers, whereas
water tables and discharge wane during dry La Nin ~ a. An exami-
nation of ENSO cycles (Moy et al., 2002) for the past 4000 years
reveals increased interannual and sub-decadal climate variability
over the late Holocene. Fluctuating climatic conditions would have
placed increased stress on the inhabitants of an already extreme
environment and caused them to vary their sources of drinking
water and food supply. Resorting to the consumption of ground-
water in particular would have almost certainly exposed the past
inhabitants of Vitor to elevated levels of arsenic (see Cornejo-Ponce
et al., 2011).
41
Historical accounts from the area indicate varying states of
water availability and a number of potential sources. Spanish ex-
plorer Pedro de Cieza de Leon (1864 [1553]) recounts observing
coastal villagers drawing their drinking water from very deep wells.
Nearly 200 years later, another explorer navigating the coasts of
Peru and Chile remarks that Vitor was the only location in the
immediate region with a source of water, specifically noting Vitor as
a place “where there is wood and freshwater: it is the only place
where the ships anchoring at Arica can be supplied with them”
(Fre

zier, 1717, p.148).
Reconstructions of the Atacama's palaeohydrology reveal pe-
riods of increased surface water availability from 2500 to 2040,
1615e1315 and 1050e680 cal BP, but these were preceded by and
interspersed with drier phases (Nester et al., 2007; Gayo et al.,
2012). These intermittent periods of fluctuating water availability
may have necessitated the relocation of sources of drinking water;
for example, during periods of increased surface water, the in-
habitants of the valley could obtain their drinking water directly
from Rio Vitor, but during drier periods would have had to rely
upon drawing drinking water from wells.
Not only fluctuating climatic conditions, but also other anthro-
pogenic factors may have impacted upon the availability of water at
Vitor. For example, during the agricultural intensification of the
Formative period, the settlement of Codpa, some 60 km upstream
from Vitor, began diverting flows to irrigate their fields (Mun ~ oz
et al., 1987; Ajata, 2004; Madaleno, 2006). Upstream diversion of
the watercourse would have certainly impacted upon the avail-
ability and quality of surface water in downstream settlements
such as Vitor.
Given the high concentrations of arsenic in water from modern
wells at Vitor, multiple times above what is considered to be safe,
and the assessment of other sources such as diet and metallurgy, it
seems that contaminated drinking water was the most likely cause
of inferred arseniasis among the pre-Columbian inhabitants at the
site.
42 J. Swift et al. / Journal of Archaeological Science 58 (2015) 31e45
7. Conclusions
The pre-Columbian inhabitants of Caleta Vitor were exposed to
elevated arsenic, with one third of the sample population, spanning
c. 3900 to 500 cal BP, accumulating levels in their skeletal system
indicative of chronic poisoning. In the face of ongoing public health
concerns relating to arsenic exposure, this study adds to the
growing evidence of arseniasis in ancient northern Chile and con-
firms, for the first time, the incidence of arsenic toxication in the
Formative and Middle Horizon Periods, demonstrating an ongoing
risk of exposure from the late Chinchorro through to the Inka.
The new radiocarbon chronology has confirmed the continual
risk of poisoning over several millennia of occupation at one site.
While there was no significant correlation between the arsenic
concentrations and time, this requires robust evaluation with a
larger sample size. The new ages also provide a more accurate
chronological resolution of the patterns of occupation at the site.
As with any study utilising trace element analysis, the potential
for diagenetic contamination cannot be entirely dismissed. How-
ever, the hyperarid environment of Vitor represents one of the most
favourable settings possible for preservation. The complete absence
of any groundwater, the essential mechanism for mobilising
arsenic, at the burial sites and low bone:soil arsenic concentration
ratios are a positive indication that arsenic within the skeletal re-
mains is biogenic.
Environmental arsenic concentrations in northern Chile were
(and still are) influenced by numerous factors including geology,
hydrology and climate, creating a variable spatial and temporal
distribution. This environmental heterogeneity, coupled with var-
iations in human behaviour, means the relative exposure of resi-
dent populations was geographically and temporally complex.
Mining and amalgamation may have contributed to the elevated
levels of skeletal arsenic in this population, but further archaeo-
logical investigation is required to determine the extent of any
metallurgy practised at Vitor. The heavy marine diet may have also
had some contribution to the intake of arsenic. However, the single
most significant variable was likely to have been the consumption
of contaminated drinking water. Heightened climatic variability in
the late Holocene may have prompted greater reliance on high-
arsenic groundwater and marine resources. The adoption of agri-
culture may have similarly affected water quality, with irrigation
higher up the catchment also potentially reducing surface flows.
The contamination of groundwater with geogenic arsenic is an
ongoing public health concern in Chile. Given the harsh environ-
ment in which the past inhabitants had to carve out their existence,
it is a cruel irony that the scant water sources that were the very
lifeblood for habitation of the hyperarid Atacama Desert were also
slowly poisoning its human populations.
Acknowledgements
We are grateful to all those involved in the Flinders University
Advanced Archaeological Field School and greatly benefited from
the input of two anonymous reviewers, to whom we are also
thankful. Christopher Carter directed the excavations and Calogero
Santoro arranged all local permissions for archaeological survey
and sampling with support from Universidad de Tarapaca
and
Centro de Investigaciones del Hombre en el Desierto (CIHDE),
CONICYT-REGIONAL R07K1001. Ten of the radiocarbon ages for this
research were funded by an AINSE research grant (ALNGRA12131).
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