Science of the Total Environment 490 (2014) 861–870

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Science of the Total Environment

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

The Pb isotopic record of historical to modern human lead exposure

George D. Kamenov a,⁎, Brian L. Gulson b
a
Department of Geological Sciences, University of Florida, 241 Williamson Hall, Gainesville, FL 32611, USA
b
Graduate School of the Environment, Faculty of Science, Macquarie University, Sydney, NSW 2109, Australia

H I G H L I G H T S

• We present high-precision Pb isotope data for historical and modern human teeth.
• Human teeth reflect human Pb exposure since historical times.
• Modern teeth show distinct signal compared to historical teeth.
• Modern USA teeth are distinct isotopically from modern teeth from other countries.
• Pb isotopes allow for identification of place of origin of an individual.

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

Article history: Human teeth and bones incorporate trace amounts of lead (Pb) from the local environment during growth and
Received 4 March 2014 remodeling. Anthropogenic activities have caused changes in the natural Pb isotopic background since historical
Received in revised form 13 May 2014 times and this is reflected in the Pb isotopes of historical European teeth. Lead mining and use increased expo-
Accepted 19 May 2014
nentially during the last century and the isotopic compositions of modern human teeth reflect the modern
Available online xxxx
anthropogenic Pb. USA teeth show the most radiogenic Pb and Australian teeth show the least radiogenic Pb, a
Editor: Daniel A. Wunderlin result of different Pb ores used in the two regions. During the last century the Australian Pb was exported to
Europe, Asia, South America, and Africa, resulting in swamping of the local environmental Pb signal by the
Keywords: imported Pb. As a result, the modern human teeth in Europe show a significant drop to lower isotopic values
Pb isotopes in human teeth compared with historical times. Similarly, modern human teeth in other regions of the world show similar Pb
Human Pb exposure isotopic ratios to modern European teeth reflecting the Pb imports. The specific pattern of human Pb exposure
Pb as geo-referencing tool allows us to use the Pb isotopic signal recorded in the skeleton as a geo-referencing tool. As historical
European teeth show a distinct Pb signal, we can identify early European skeletal remains in the New World
and likely elsewhere. In modern forensic investigations we can discriminate to some extent Eastern Europeans
from Western and Northern Europeans. Australians can be identified to some extent in any region in the
world, although there is some overlap with Western European individuals. Lead isotopes can be used to easily
identify foreigners in the USA, as modern USA teeth are distinct from any other region of the world. By analogy,
USA individuals can be identified virtually in any other region of the world.
© 2014 Elsevier B.V. All rights reserved.

1. Introduction
1.1. Lead in the environment and Pb isotopes
Lead is composed of one non-radiogenic (204Pb) and three radiogen-
ic stable isotopes 206Pb (a product of 238U decay), 207Pb (a product of
235
U decay), and 208Pb (a product of 232Th decay). The abundances of
these isotopes vary depending on the age and original amount of U
and Th and Pb present in a given rock and/or mineral (e.g., Dickin,
2005). As a result, different rocks, minerals, ores, and soils tend
to have different Pb isotope abundances depending on their initial Pb,
⁎ Corresponding author.
E-mail address: kamenov@ufl.edu (G.D. Kamenov).
U/Th/Pb ratios, and the time elapsed since their formation. Geologically
old rocks with high U/Pb and Th/Pb will have radiogenic Pb isotopic
ratios (i.e., high ratios of 206Pb/204Pb, 207Pb/204Pb and 208Pb/204Pb).
Soils and biota developed over such lithological units will be expected
to inherit the radiogenic Pb from the underlying rocks. Similarly,
geologically old rocks with low U/Pb and Th/Pb will have less radiogenic
Pb isotopic ratios (i.e., lower 204Pb-based ratios) which will be incorpo-
rated in soils and biota in the given area. At present, however, the natu-
ral Pb isotopic composition virtually everywhere on Earth tends to be
altered due to anthropogenic activities ultimately related to mining
and use of Pb ores. This ore Pb is usually distinguishable isotopically
from the natural Pb background. This is because geologically old Pb
ores tend to have much less-radiogenic Pb isotopes at present when
compared with the local surrounding rocks. This is due to the fact that

http://dx.doi.org/10.1016/j.scitotenv.2014.05.085
0048-9697/© 2014 Elsevier B.V. All rights reserved.
862 G.D. Kamenov, B.L. Gulson / Science of the Total Environment 490 (2014) 861–870
galena, the main Pb ore mineral, is composed of 86.6% Pb by weight and
has extremely low concentrations of U and Th. Therefore the galena Pb
isotopes will be “frozen” at the moment the ore is formed and will not
change due to U–Th decay regardless of the time elapsed since the de-
posit formation. At the same time the Pb isotopes will continuously
grow in the rocks and soils in the region of the deposit due to U–Th
decay. During mining and subsequent smelting and lead usage this “fro-
zen in time” Pb is released into the environment and can be identified
by its distinct isotopic signature when compared with uncontaminated
local rocks and soils. In most cases lead mining and subsequent use will
release less-radiogenic Pb to the environment and typical examples are
the Broken Hill and Mt. Isa deposits in Australia formed approximately
1700–1800 million years ago (Gulson, 1986). In other cases, lead min-
ing can release highly radiogenic Pb, which is typical for the Paleozoic
ores in the Mississippi Valley Type (MVT) deposits in the USA
(e.g., Kesler et al., 1994). In the rest of the text the Pb released to the en-
vironment as a result of human activities will be referred to as “anthro-
pogenic Pb”.
1.2. Anthropogenic and natural lead pathways in the human body
Almost 3000 years ago Pb mining began in Europe. Although this
early mining activity was minor compared with modern standards, it
began to cause small but identifiable changes in the natural Pb isotope
background (Fig. 1) (e.g., Hong et al., 1994; Shotyk et al., 1998;
Brännvall et al., 2001). The Pb burden on the environment and human
health increased drastically in the last century mainly due to the leaded
gasoline usage (e.g., Nriagu, 1990; Patterson et al., 1991). This new,
major addition of modern industrial anthropogenic Pb to the environ-
ment is easily identifiable in the changes in the Pb isotopes observed
in environmental archives in Europe and USA (Fig. 1) (Shotyk et al.,
1998; Kamenov et al., 2009). Leaded gasoline was introduced in the
1920s in the USA and in the 1930s in Europe; it peaked in the 1970s
and was phased out in early 1990s in the USA and early 2000s in
Fig. 1. Peat core records of changes in the Pb isotopic background through time in Europe
(Shotyk et al., 1998) and USA (Kamenov et al., 2009). Note the distinct Pb isotopic back-
grounds in the last 500 years in the two regions. The two major shifts in the Pb isotopic
background in Europe correspond to the onset of mining during the Romano-British peri-
od and the introduction of Australian Pb (Shotyk et al., 1998). The USA data comprise ap-
proximately the last 500 years, providing record from the discovery of the New World to
present. The Pb isotopic shifts identified in the USA during the last 100 years correspond to
the use of different Pb ores (Kamenov et al., 2009).
Europe (Mielke et al., 2010). However, different ores were used in
both regions. In Europe tetra-alkyl Pb additive was manufactured with
Pb imported mainly from Broken Hill and Mt. Isa deposits in Australia,
which is characterized with distinct, low 204-based Pb isotopic ratios
(Gulson, 1986). The introduction of Australian Pb in Europe caused a
sharp drop in the regional Pb isotopic compositions and completely
swamped the local natural background values (Fig. 1). In contrast,
tetra-alkyl Pb used in USA was primarily sourced from the MVT deposits
characterized with distinct, high Pb isotopic ratios (Kesler et al., 1994).
As a result, both regions display markedly different regional Pb isotopic
signatures during the last 100 years or more (Fig. 1). There was a de-
cline in the Pb isotopic ratios in the USA in the 1950–1960 interval
(Kamenov et al., 2009), due to usage of relatively less-radiogenic Pb
from the Idaho ore deposits, however, the ratios still remain elevated
compared with Europe (Fig. 1). After the 1960s the use of relatively
radiogenic Pb from the MVT deposits continued, reflected in the sharp
increase in the Pb isotopic ratios after the 1960s (Fig. 1).
Estimates show that Pb emissions in the 20th century increased
hundreds of times compared with pre-industrial levels (Hong et al.,
1994; Shotyk et al., 1998). As a result, no region in the world today
can be really regarded as pristine and not polluted to some degree by
anthropogenic Pb, even the Antarctic (Rosman et al., 1994). During
the leaded gasoline usage period Pb in air aerosols was mainly con-
trolled by Pb released from motor vehicle emissions (Gulson et al.,
1983; Bono et al., 1995) and as this Pb falls on the ground it becomes
part of the local soil and dust. During the last several decades legislative
measures, such as elimination of leaded paint and gasoline, have been
enforced to reduce the lead burden on the environment and human
health. Regardless of these measures, the already released lead has
accumulated in the soil and dust and can be identified in the local pop-
ulation years after termination of leaded gasoline usage (Kurkjian and
Flegal, 2003; Gulson et al., 2006; Kamenov, 2008; Mielke et al., 2010).
Seasonal fluctuations in the blood Pb concentrations have been ob-
served (Gulson et al., 2000 and references there in). Recent works
with children from several large cities in the USA showed correlation
between elevated blood Pb levels and periods of low soil moisture indi-
cating that the main Pb exposure was from inhalation and/or ingestion
of soil and dust (Laidlaw et al., 2005; Zahran et al., 2013).
Every day we inadvertently ingest soil/dust via soil-born dust inha-
lation and ingestion of soil/dust particles stuck on food, objects, or
hands. Estimations of daily ingestion and/or inhalation of soil and dust
by humans vary widely, on average between 23 and 625 mg/day
(Davis and Mirick, 2006) to several grams or more in extreme cases
(Simon, 1998). In particular, soil and dust contacts and resultant inges-
tion/inhalation are usually higher in younger children because of hand-
to-mouth activity during periods of growth and adolescence (Simon,
1998) and lead to elevated blood Pb levels (Bornschein et al., 1985;
Laidlaw et al., 2005; Zahran et al., 2013). In vitro soil digestion experi-
ments indicate that Pb will be mobilized from the soil/dust and will be-
come bioavailable in the human gastrointestinal tract (Oomen et al.,
2002). Maddaloni et al. (1998) conducted in vivo experiments for Pb
bioavailability from ingested soil and showed that a significant amount,
on average 26% (+/−8%) of the soil Pb will be absorbed if ingestion oc-
curs during fasting conditions. A much lower amount, on average 2.5%
(+/−1.7%), is absorbed if soil is ingested immediately after a standard-
ized breakfast (Maddaloni et al., 1998). The latter figure is in agreement
with studies that show that much Pb is reabsorbed by food, therefore
limiting its availability to membrane absorption sites (Chaney et al.,
1998) and can explain observations by Gulson et al. (2003) that dietary
intake is not a major source of Pb in blood. The in vitro and in vivo
experiments essentially show that lower pH increases the soil/dust Pb
bioaccessibility. The Pb released from the soil/dust in such experiments
is “leachable Pb”, which at present is dominated by anthropogenic Pb
(Hamelin et al., 1989; Teutsch et al., 2001; Kamenov, 2008). It is well
documented that the anthropogenic Pb in soils is associated mainly
with labile fractions such as halides and sulfates (Hamelin et al.,
 G.D. Kamenov, B.L. Gulson / Science of the Total Environment 490 (2014) 861–870
1989), and/or carbonates (Teutsch et al., 2001), and/or organic mat-
ter (Haack et al., 2003). As this leachable Pb enters the human organ-
ism it substitutes for Ca and accumulates in bones and teeth.
Excellent correlation was found between the Pb isotopic composi-
tions of soil leachates and local residents in Sofia, Bulgaria,
confirming the local soil and soil-born dust as a major source for
human Pb exposure (Kamenov, 2008). Other studies have concluded
that lead-contaminated house dust is the most important factor for ele-
vated Pb blood level in children (Lanphear et al., 1996). However, an-
thropogenic Pb should still dominate the modern house dust,
regardless of whether it is coming from contaminated soil (i.e., outside
soil-born dust entering the house) or from in-house sources such as
leaded paint. Furthermore, Mielke and Reagan (1998) also demonstrat-
ed that the most important Pb source for children is the soil, and it can
even dominate lead-based paint. Recent work by Robbins et al. (2010)
showed that Pb accumulated in human teeth is dominated by Pb re-
leased from leaded gasoline, even in people living in old houses with
leaded paint. Overall, food is not an important Pb source, as a number
of studies conclude that ingestion/inhalation of soil and dust is the dom-
inant pathway of human Pb exposure at present (Mielke and Reagan,
1998; Zhang et al., 1998; Gwiazda et al., 2005; Laidlaw et al., 2005;
Gulson, 2008; Kamenov, 2008; Mielke et al., 2010; Zahran et al., 2013).
In addition to the above described pathway for ambient environ-
mental Pb incorporation in the human body, individuals can also be ex-
posed to high doses of Pb from “point-sources”, such as Pb objects or
artisan Pb mining. Short-term exposure to high levels of Pb will affect
the blood Pb concentration and subsequently the nervous system and
may even cause death, but unlikely to have major effect on bones and
teeth isotopic composition. This is because bones and teeth form and re-
model on multi-years to decadal time scales and tooth enamel becomes
isolated from the blood supply after formation, as we will discuss in de-
tail in the next section. Long-term (years) exposure to Pb from a “point
source”, however, will be expected to affect the skeletal Pb. Depending
on the age of the individual and the duration of the exposure, different
parts of the skeleton such as trabecular and cortical bone and teeth
can incorporate the “point source” Pb. For example, in 2010 around
400 children were killed and thousands affected by Pb poisoning in
Nigeria due to exposure to Pb contaminated dust and soil from local
artisanal mining (Plumlee et al., 2013). It is plausible to expect that
the surviving exposed children incorporated the local Pb from the
artisanal mining in their growing bones and teeth. Such exposure to a
specific “point-source” Pb can also provide useful information for geo-
referencing as it may allow us to trace the place of origin of an individual
to a very specific area, possibly even down to several square kilometers.
1.3. Pb isotopes in human teeth and bones
Lead substitutes for Ca in the human skeleton and so teeth and bones
can be used as an archive of lead exposure. Permanent teeth enamel will
mineralize during early childhood, from 3–4 months to 12–16 years
age. Once the enamel formation is completed, it will lock in the child-
hood Pb signal and will not change throughout life as it is isolated
from the blood supply. Post-eruption Pb exchange in the mouth is also
highly unlikely as the Pb concentration in saliva is many orders of mag-
nitude lower compared with surficial enamel (Costa de Almeida et al.,
2011). Furthermore, studies using high-precision Pb isotopic data
show that the enamel preserves the childhood signal and does not
change through life (Gulson and Gillings, 1997; Budd et al., 2004).
As different teeth mineralize at different times, Pb isotopes recorded
in the enamel can be used as time-series for childhood migration. Per-
manent first molar enamel begins to form at birth and it is completed
by the age of 3 (Reid and Dean, 2006). Thus, the first molar enamel
will give information about the place of birth and toddler years,
i.e., the place of residence to the age of 3. Incisor and canine enamel
formation begins later, several months to a year after birth and is
completed around the age of 5–6 (Reid and Dean, 2006), and so will
863
provide information about early childhood. Third molar enamel does
not begin to form until around 8 years of age, and is completed in the
early-mid teenage years, so will provide information about late child-
hood place of residence. In contrast, dentine and bones can continually
exchange Pb circulating in blood and in adults will represent a long-
term averaged Pb source. Gulson and Gillings (1997) estimated that
the Pb turnover in dentine is around 1% per year, therefore, even after
decades the dentine will still retain significant part of the initial child-
hood Pb. Trabecular bone, in contrast, has a faster turnover and will
possibly completely equilibrate with the local Pb within a decade or
so (Hu et al., 1998). Therefore, lead isotopic compositions in teeth and
bones can be used as time-series to trace individual migration.
A complication with this is that once Pb is deposited in the skeleton
it can be mobilized, especially during pregnancy and lactation and so
can be passed onto children (e.g., Gulson et al., 2000; Gulson, 2008;
Manton et al., 2003). In such a scenario, the early-forming teeth in a
newborn will be influenced to some degree by the isotopic composition
of the mother's skeletal Pb. Thus in the case of a recent immigration and
pregnancy, the infant may show a mixed isotopic signal between the
new environment and the mother's previous environment. Therefore,
deciduous teeth may contain some of the mother's home-land Pb. How-
ever, the formation of even the earliest permanent tooth enamel is not
completed by the age of 2–3 (1st molar enamel) and therefore will like-
ly show a significant contribution from the new environment. Sampling
other teeth such as incisors or third molars will only provide informa-
tion on the new environment Pb. Further information about the previ-
ous place of residence can be obtained from bones as they slowly
exchange elements continuously throughout life. Although bones can
be sampled from modern individuals, such as cold case victims, and
this should provide chronological information for possible migration,
use of bones from historical remains is complicated as the isotopic signal
may be affected by diagenetic changes.
1.4. Post-mortem diagenesis and historical human teeth
Although diagenetic alteration is not typically an issue for modern
human teeth and bones, it can complicate the interpretation of isotopic
data in fossil skeletal material. Bones in particular, are characteristically
porous and contain high organic contents and are therefore prone to
diagenetic alterations. Studies have demonstrated rapid (0–30 kyr),
progressive uptake of rare-earth elements in bones during diagenesis
(Trueman et al., 2004). In contrast to bones, tooth enamel has dense
crystal structure and is very resistant to diagenesis even on geological
time-scales (e.g., MacFadden et al., 2010 and references there in).
Numerous studies have shown that tooth enamel faithfully preserves
biogenic Sr and Pb isotopic compositions (Bower et al., 2007; Budd
et al., 2000, 2004; Chiaradia et al., 2003; Montgomery et al., 2005,
2010; Valentine et al., 2008; Turner et al., 2009). In particular, Budd
et al. (2004) and Montgomery et al. (2010) showed much lower Pb con-
tent in enamel data from pre-historic people (0.003 to 0.68 ppm) com-
pared with Romano-British and Medieval people (0.02 to 30.1 ppm)
from Britain. If progressive diagenesis was controlling the Pb content
in the enamel, we would expect much higher Pb concentrations in the
older pre-historic enamel samples, which is not the case. Furthermore,
the Pb isotopic data for pre-historic human enamel showed a much
higher spread compared with the “culturally focused” historical sam-
ples (Montgomery et al., 2010). Similarly, Pb isotopic data presented
in Valentine et al. (2008) and Turner et al. (2009) showed a much
higher spread compared with local soil. In Turner et al. (2009) the
local Pb isotopic signal is mid-range in the spread of the Pb isotopic
data indicating that the local soil cannot be an end-member. Perhaps
the most striking example pertinent to resistance of the human enamel
to post-mortem changes is the finding of a young female buried in a Pb
coffin, dated 4th century A.D. Regardless that the remains have been in
the Pb coffin for almost 1700 years, the tooth enamel still preserved the
original in vivo Pb isotopic signal, very distinct from that in the Pb coffin
864 G.D. Kamenov, B.L. Gulson / Science of the Total Environment 490 (2014) 861–870

(Montgomery et al., 2010). Therefore, human tooth enamel should be teeth extracted during normal dental procedures from contemporary
representative of the in vivo Pb exposure and so will be useful for geo- individuals. The data are presented in several traditional plots of
206
referencing people in modern, historical, and pre-historical times. Pb/204Pb vs 207Pb vs 204Pb vs 208Pb/204Pb (Figs. 2 to 6). On Fig. 2 we
compare historical teeth Pb isotopic data from European and South
2. Required methodology American individuals. The historical European teeth data cluster around
206
Pb/204Pb = 18.44 +/− 0.10, 207Pb/204Pb = 15.61 +/− 0.04, and
208
Obtaining high-precision Pb isotopic data requires strict preparation Pb/204Pb = 38.40 +/− 0.16. The dotted boxes on Fig. 2 represent
protocol and access to TIMS (Thermal Ionization Mass Spectrometry) or the above limits of the Pb isotopic data. Compared with Europe, histor-
MC-ICP-MS (Multi-Collector Inductively Coupled Plasma Mass Spec- ical data for South American teeth show elevated average 206Pb/204Pb
trometry). As Pb is a common environmental contaminant, sample = 18.73 +/− 0.20 and overlapping 207Pb/204Pb = 15.64 +/− 0.02
preparation must be conducted under a clean lab environment with and 208Pb/204Pb = 38.47 +/− 0.19 (green boxes). Although there is
strict blank Pb control. All reagents used for sample preparation must some overlap, historical data for Europe and South America show statis-
be ultra-pure Optima-grade. Lead is typically isolated from the tooth tically distinct 206Pb/204Pb ratios. On Fig. 3 the same historical European
matrix by digestion in concentrated HNO3 followed by purification in and South American data are compared with historical USA teeth data
a HBr medium by ion-exchange chromatography using Dowex 1X8 from 19th century. Several of the USA data plot within the Europe
resin (e.g., Valentine et al., 2008; Kamenov, 2008; Turner et al., 2009). field but the majority plot at much higher ratios (Fig. 3). Similarly, the
To obtain Pb concentrations on the same sample on which Pb isotopic majority of the 19th century USA teeth show more radiogenic Pb isoto-
ratios are measured, a purified tracer (‘spike’) such as 202Pb can be pic compositions compared with historical South American teeth (com-
added to the digest. Once the Pb fraction is isolated from the tooth pare Figs. 2 and 3).
matrix, it is ready for isotopic analyses. In the modern multi-collector Data for modern teeth, extracted from contemporary individuals, are
TIMS technique, the Pb fraction is loaded on Re-filament, heated to shown on Figs. 4 and 5. The data for modern European teeth extend to
about 1100 °C and signals from the 208Pb, 206Pb, 207Pb, and 204Pb record- much lower Pb isotopic ratios when compared with historical teeth
ed simultaneously in static mode in four separate Faraday detectors (compare Figs. 2 and 4). The highest 206Pb/204Pb observed in modern
(e.g., Dickin, 2005). Correction for mass-bias is typically done relative European teeth is around 18.4–18.5, overlapping with the average
to data for the NIST 981 Pb isotopic standard that is analyzed together European historical data, but a significant proportion of the modern
with the samples. The ultimate precision and accuracy for Pb isotopic data plot at much lower Pb isotopic ratios. The Europe field is arbitrarily
analyses can be achieved by utilizing the double or triple spike Pb
TIMS method (e.g., Abouchami et al., 2000). The 2nd generation
MC-ICP-MS (Nu-Plasma and Neptune) introduced in the early 2000s
allowed for rapid Pb isotopic analyses with better precision and accura-
cy compared with traditional TIMS methods (Kamenov et al., 2004;
Thibodeau et al., 2013). The Pb fraction isolated from the tooth matrix
is dissolved in nitric acid and spiked with Tl before introduction in the
MC-ICP-MS. Using 205Tl/203Tl for mass-bias correction in fresh Pb–Tl
mixtures Kamenov et al. (2004) demonstrated precision and accuracy
for Pb isotopic ratios measured on MC-ICP-MS comparable to a double
or triple spike Pb TIMS method. Typical 2δ errors for MC-ICP-MS for
206
Pb/204Pb, 207Pb/204Pb and 208Pb/204Pb are around 0.025% (Kamenov,
2008) and for TIMS are around 0.1% (Gulson et al., 1997).
Although high-precision Pb isotope measurements are essential in
any investigation (e.g., Gulson et al., 1996, Gulson, 2008; Manton
et al., 2000; Ellam, 2010) a number of studies utilized Pb isotopic data
obtained by single-collector ICP-MS (e.g., Alexander et al., 1993;
Prohaska et al., 2005). A major problem, however, is that single-
collector ICP-MS Pb isotopic analyses can be inaccurate and often ac-
companied by random errors (Barbaste et al., 2001; Kylander et al.,
2009; Thibodeau et al., 2013). Furthermore, such studies typically did
not report 204Pb abundances, the only non-radiogenic isotope in the
Pb system, and therefore important geochemical information is lost.
Ellam (2010) clearly showed that the only reliable test for multiple
sources identification and possible mixing relationships can be obtained
from plots involving 206Pb/204Pb, 207Pb/204Pb and 208Pb/204Pb. There-
fore, the measurement and reporting of the minor 204Pb are essential
for any attempt to use Pb isotopes for pinpointing human lead exposure
and geo-referencing humans.

3. Results

In this work we compiled only TIMS and MC-ICP-MS data presenting

data for all four Pb isotopes for human teeth from historical to modern
times. We also present new Pb isotopic data for modern humans. All
of the Pb isotopic data used in this work and their sources are presented
in the on-line supplement. For the historical period we consider Pb iso-
topic data for teeth from individuals that lived before the modern times,
from the 19th century to the beginning of written history. In the modern
time period (20th and 21st centuries) we consider Pb isotopic data for
Fig. 2. Comparison of Pb isotopic data for historical teeth from Europe and South America.
Data for Europe from Budd et al. (2004), Montgomery et al. (2010), and Åberg et al.
(1998). Data for South America from Turner et al. (2009). The dotted box represents the
extent of the average 206Pb/204Pb = 18.44 +/− 0.10, 207Pb/204Pb = 15.61 +/− 0.04,
and 208Pb/204Pb = 38.40 +/− 0.16 for the historical Europe data. The green field represents
the extent of the average historical data for South American teeth with 206Pb/204Pb =
18.73 +/− 0.20, 207Pb/204Pb = 15.64 +/− 0.02, and 208Pb/204Pb = 38.47 +/− 0.19. (For
interpretation of the references to color in this figure legend, the reader is referred to the
web version of this article.)
 G.D. Kamenov, B.L. Gulson / Science of the Total Environment 490 (2014) 861–870
Fig. 3. Comparison of Pb isotopic data for historical teeth from USA with Europe and South
America. The dotted (Europe) and green (South America) fields are the same as in Fig. 2,
note the different scales for the Pb isotopic ratios. Data for USA from Bower et al. (2007),
for Europe and South America same as Fig. 2. (For interpretation of the references to
color in this figure legend, the reader is referred to the web version of this article.)
divided into two parts (“EU few teeth” and “EU most teeth”), based on
the relative abundance of samples shown in Fig. 4. “EU few teeth” field
comprises samples showing 206Pb/204Pb below 17.70. As can be seen
from Fig. 4, there are relatively few (10.9%) of the modern European
teeth that plot within the “EU few teeth”, which is the lower radiogenic
end of the European field. Very distinct Pb isotopic compositions are
observed between modern European and USA teeth when all isotope
ratios are considered (Fig. 4). There is overlap between the few
highest European (Romania) and lowest USA teeth in 206Pb/204Pb
vs 207Pb/204Pb. However, the USA data plot at lower 208Pb/204Pb
(Fig. 4). The Pb isotopic relationships on Fig. 4 highlight the importance
of using all 4 Pb isotopes for geo-referencing people. Modern South
American data overlap with the modern European data and show
much lower values compared with historical data (compare Figs. 2
and 5). Similarly, available data for Asian and Middle Eastern modern
teeth also show overlapping values with modern European teeth
(Fig. 5). Modern Australian teeth show the lowest Pb isotopic ratios
with almost all data having 206Pb/204Pb ratios less than 17.7 (Fig. 5). Al-
though there is some overlap, the least radiogenic Pb isotopes observed
in the Australian teeth are distinct from majority of the teeth from the
rest of the world (compare Figs. 4 and 5, and 6). There is no overlap
between modern Australian and USA teeth (Fig. 6). A MANOVA test
was performed on all of the modern teeth data using the package
stats in R (R Core Team, 2013). The regions considered for the statistical
analysis of the modern teeth were USA, Europe 1 (northern and western
European countries, including Poland, Norway, Switzerland, Italy
and UK), Europe 2 (eastern European countries, including Bulgaria,
Romania, Croatia, Former Yugoslavia and Czechoslovakia), Middle
East (Lebanon, Syria, Egypt, Turkey), South America (Chile and
865
Fig. 4. Comparison of Pb isotopic data for modern teeth from Europe and USA. Dotted line
divides the European data on “EU few teeth” (10.9%) and “EU most teeth” (89.1%) based
on the relative abundance of teeth samples plotting in each region. Data for Europe from
Åberg et al. (1998), Gulson et al. (1997), Gulson and Gillings (1997), Chiaradia et al.
(2003), Rauch et al. (2007), Kamenov (2008), and this work. USA data from Regan
(2006) and this work. All data and sources are presented in the on-line supplement. Coun-
try abbreviations: CZ — Former Czechoslovakia, YU — Former Yugoslavia; HR — Croatia;
NO — Norway; CH — Switzerland; IT — Italy; UK — United Kingdom.
Uruguay), Asia (India and South Korea), and Australia (data in the
on-line supplement). The analysis of variance showed that, overall,
the three Pb ratios of all of the above regions were significantly
different (F6,367 = 247.71, p b 0.0001). However, as can be seen in
Figs. 4 and 5 the Pb isotopic data for Middle East, South America,
and Asia overall overlap in Pb–Pb space with Europe and to some ex-
tent with Australia. Thus regardless of the distinct statistical results
we would not consider it possible to distinguish modern individuals
from the Middle East, South America, and Asia from European indi-
viduals. Overall, there is excellent distinction in a number of cases
and overlap in others in Pb–Pb isotope space from historical to mod-
ern times. In the following section the reasons behind the observed
Pb isotopic systematics and potential uses for geo-referencing peo-
ple are discussed.
4. Discussion
4.1. Pb isotopes in historical human teeth in Europe and the Americas
Lead mining in Europe began around 3000 years ago and European
human teeth as far back as the Iron Age show elevated Pb in the enamel
(0.02 ppm to 30.1 ppm) compared with data from pre-historic people
(0.003 ppm to 0.68 ppm) (Budd et al., 2004; Montgomery et al.,
2010). This elevated Pb concentration is also accompanied by Pb isoto-
pic clustering or “cultural focusing” due to exposure to anthropogenic
Pb (Montgomery et al., 2010). The observed Pb isotopic ratios in the
866 G.D. Kamenov, B.L. Gulson / Science of the Total Environment 490 (2014) 861–870
Fig. 5. Comparison of Pb isotopic data for modern teeth from Australia, Middle East, South
America, Asia, and Europe. European field is outlined based on data presented in Fig. 4 and
is divided based on the relative abundances of samples. Data for Australia from Gulson
et al. (1994a, 1994b), Gulson et al. (2004b) and this work. Middle East and South
America from Gulson et al. (1997) and Gulson and Gillings (1997), Indian and South
Korean data from this work, details in the on-line supplement.
historical European teeth (Fig. 2) are very similar to galena isotopic
compositions from English and Welsh mines (Budd et al., 2004;
Montgomery et al., 2010). The British ores were heavily exploited
since the Romano-British period, dating back to 49 AD, with local minor
mining starting likely as far back as the Bronze Age (Montgomery et al.,
2010). This Pb was widely used and recycled throughout the vast
Roman Empire, which apparently is recorded in the Pb isotopic “cultural
focusing” in the historical European teeth (Montgomery et al., 2010).
Almost all of the Pb isotopic data for the “culturally focused”
European human teeth from the Iron Age to late Medieval times
(ca. 1000 BC to 1500 AD) have 206Pb/204Pb ratios b18.6, with only 3
individuals showing elevated ratios (Fig. 2). In contrast, historical
South American teeth have an average 206Pb/ 204 Pb ratio of
18.73 +/− 0.20, with relatively few individuals showing values
less than 18.6. Although there is some overlap, the European teeth
show markedly less radiogenic 206 Pb/204 Pb ratios compared with
the South American samples. Therefore, it should be possible to dis-
tinguish human remains in archeological sites whether they are from
European or South American origin based on their Pb isotopic signature.
Although this is not likely to be of any practical use in archeological sites
dating before ca. 1500 AD, there is potential for use in colonial
archeological sites in South America. The South American teeth plotted
on Fig. 2 are from individuals buried at Machu Picchu, Peru. Turner et al.
(2009) showed that almost all of the individuals interred at Machu
Picchu came from different areas of the Inca Empire. The data set of
Turner et al. (2009) is a representative sample of the South American
population living during the apogee of the vast Inca Empire (Late
Horizon, ca. 1438–1532 AD), just before the onset of the Colonial Period.
Therefore, the distinct Pb isotopic composition between the historical
Fig. 6. Large-scale comparison of Pb isotopic data for modern teeth from USA, Australia,
and Europe with ores from Broken Hill (Australia) and MVT (Mississippi Valley Type de-
posits) (USA). Data sources same as Figs. 4 and 5. Broken Hill data after Gulson et al.
(1994a, 1994b) and MVT data after Kesler et al. (1994) and Sangster et al. (2000).
European and South American teeth can be used as a tool to distinguish
early European from local human remains in South American
archeological sites.
The historical European teeth clearly show “cultural focusing” since
the Iron Age, but it is not clear if this is also the case for the South
American historical teeth data. Exposure to anthropogenic Pb may be
plausible, given the wealth of major ore deposits in the Andes and the
Inca extensive use of gold and silver ornaments. Cook et al. (2009) iden-
tified increased Pb concentrations and changes in Pb isotopes in lake
sediments in Peru dating as far back as 600 AD. The changes in the Pb
background in the lake sediments were attributed to Pb–Ag mining
from the Central Peruvian Cerro de Pasco deposit (Cook et al., 2009).
Cerro de Pasco ores have 206Pb/204Pb ratios of 18.78, 207Pb/204Pb ratios
of 15.66, and 208Pb/204Pb ratios of 38.89 (Sangster et al., 2000). The
historical South American teeth (206Pb/204Pb = 18.73 +/− 0.20,
207
Pb/204Pb = 15.64 +/− 0.02, and 208Pb/204Pb = 38.47 +/− 0.19)
show overlapping values in 206Pb/204Pb and 207Pb/204Pb, but somewhat
lower 208Pb/204Pb. Therefore, it is not clear if any of the individuals bur-
ied at Machu Picchu were exposed to Cerro de Pasco Pb. Non-exposed
individuals worldwide tend to have enamel Pb concentration below
0.7 ppm (Patterson et al., 1991; Budd et al., 2000; Montgomery et al.,
2010). However, as Pb concentrations were not measured in the histor-
ical South American teeth (Turner et al., 2009), it is not possible to eval-
uate whether or not the individuals were exposed to anthropogenic Pb.
We were not able to locate Pb isotope data for historical teeth from
native North Americans. The available historical data for teeth from
North America are from a 19th century site in Colorado, USA, most likely
from individuals that were exposed to anthropogenic Pb (Bower et al.,
2007). Although none of the 19th century teeth were from indigenous
 G.D. Kamenov, B.L. Gulson / Science of the Total Environment 490 (2014) 861–870
North Americans, a comparison of these data with the European data set
is useful because at least some of these teeth are likely from people that
were born and grew up in the USA, and therefore, will carry the “local”
Pb isotopic signal at the time. As can be seen on Fig. 3, the majority of the
USA 19th century teeth show much more radiogenic Pb isotopic ratios.
There are few individuals that overlap with the European teeth, but this
may be simply due to European origin of these individuals. The rest of
the 19th century USA teeth show 206Pb/204Pb ratios around 19.2 and
higher. Similarly, 207Pb/204Pb and 208Pb/204Pb ratios are much higher
compared with Europe. In fact, the majority of the USA 19th century
teeth are much more radiogenic when compared also with the South
American teeth (compare Figs. 2 and 3). Therefore, the distinct Pb isoto-
pic signal in the USA suggests that it should be possible to distinguish
between European or local origin for archeological human remains. Po-
tential applications can be distinction of 1st generation immigrants that
were born and spent their childhood in Europe, from 2nd-and above
generation immigrants that were born in the USA. In addition, the “cul-
tural focusing” in the European individuals should allow for distinction
of European from local, indigenous skeletal remains in archeological
sites. Also, historical skeletal remains with really high Pb isotopic ratios
will potentially indicate a North American origin and may be useful for
distinguishing individuals in South American archeological sites.
4.2. Pb isotopes in modern human teeth
4.2.1. Europe and USA teeth
The available high-precision Pb isotopic data from modern human
teeth from USA and Europe form distinct fields in Pb isotopic space
(Fig. 4). Europe teeth extend from 206Pb/204Pb around 18.5 to lower
values due to usage of Australian Pb in Europe. As can be seen on
Fig. 6, Broken Hill Pb ore is characterized with very non-radiogenic Pb
isotopes. In contrast, MVT deposits, characterized with relatively radio-
genic Pb isotopes, were a significant source of Pb used in the USA. As can
be seen on Fig. 6, the available data for modern USA teeth form a trend
extending towards the MVT Pb ores. As a result, all USA teeth (with ex-
ception of one sample) have 206Pb/204Pb ratios greater than 18.50. In
contrast, almost all of the European teeth have 206Pb/204Pb ratios less
than 18.50. There are a few teeth from Bulgaria that have 206Pb/204Pb
ratios of about 18.5 but exhibit higher 207Pb/204Pb and much higher
208
Pb/204Pb ratios compared with the USA teeth (Fig. 4). Romanian
teeth show the highest 206Pb/204Pb ratio in Europe (as high as 18.59,
Rauch et al., 2007) and although the data overlap with the lowest end
of the USA field on a 206Pb/204Pb vs 207Pb/204Pb diagram, they have a
distinctly higher 208Pb/204Pb ratio (Fig. 4). There is virtually no overlap
between the USA and Europe when the three 204Pb-based isotopic ratios
are considered and this is a valuable tool for distinguishing modern
human remains if they were from local individuals that were born and
spent their childhood in USA or foreigners and/or immigrants to the
USA.
When it comes to individual countries within Europe, it is more
difficult to make distinctions based solely on the Pb isotopes (Gulson
et al., 1997). Although Romania appears to be distinct, the majority of
the Pb isotope data are from only 1 individual (Rauch et al., 2007) so
may not be representative of the whole country. In contrast, the Pb iso-
topic data from Bulgarian teeth (Kamenov, 2008) show a significant
spread in 206Pb/204Pb ratio, comprising almost a third or more of the
range observed in the rest of the European teeth (Fig. 4). However, care-
ful examination of the modern teeth data from Norway, Switzerland,
Poland, UK and Italy reveals that Northern and Western Europe data
show in general lower 206Pb/204Pb compared with Eastern Europe.
The MANOVA test of the data confirmed the statistical difference be-
tween the two regions. The elevated Pb isotopic ratios in Eastern
Europe may be due to less Australian Pb imports to the region, utiliza-
tion of local or former Soviet Union ores in the manufacturing of the
leaded gasoline, or simply less gasoline usage due to socioeconomic
factors.
867
The USA data set plotted on Fig. 4 is based on teeth from more than
20 different states (Regan, 2006). However, the teeth data available
from Florida show a significant spread suggesting that similar to
Europe, it may be difficult to further constrain the geographical origin
of individuals within the continental USA based solely on Pb isotopes.
Gasoline was made with Pb additive manufactured mainly from MVT
deposits during the most recent decades, and so the widespread con-
tamination is possibly obscuring any “local” Pb signal from individual
states.
A complication with the Pb isotopic data is the possibility of tempo-
ral variations due to the extent of contamination and/or changes in the
Pb ore used for manufacturing the Pb additive for gasoline (Gulson et al.,
1983). The European teeth data plotted on Fig. 3 are for individuals of
widely varying ages. For example, the Bulgarian teeth are from individ-
uals who were 14 to 65 years old at the time of tooth extraction
(Kamenov, 2008). Therefore, the Europe Pb field should be useful for
distinguishing individuals born between 1940s and the present day.
The USA data set, however, is limited to individuals born between
1964 and 1987, therefore the American teeth data are mainly useful
for individuals born from the 1960s to the present day. These Pb isotope
fields are likely useful to the “present day” due to the fact that although
the leaded gasoline has been phased out, soil and blood studies show
that children still acquire Pb from the legacy of leaded gasoline usage
(e.g., Kurkjian and Flegal, 2003; Laidlaw and Filippelli, 2008). The
high-precision Pb isotope data for the USA are from individuals with a
relatively limited range of ages compared with Europe, but we can
look at other environmental archives for clues as to what the Pb isotopes
were in people born before the 1960s. Fig. 1 shows the changes in the Pb
isotopic background in the USA since the arrival of the first Europeans
(ca. 500 years) versus the longer record in Europe (ca. 12,000 years).
As can be seen from the plot, there is a distinct Pb isotopic signal during
the 20th century in the two regions. Although there is a trend to
lower values in 206Pb/207Pb ratio in the USA, the overall trend is to
much higher values compared with Europe. Lead concentrations
and 206Pb/207Pb and 208Pb/206Pb ratios (MC-ICP-MS data, but 204Pb
was not measured, Robbins, personal communication) for 127 human
teeth extracted from individuals from the Cleveland area show concom-
itant changes corresponding to changes in the leaded gasoline usage
(Robbins et al., 2010). Based on the Cleveland individuals' ages the 127
teeth were formed between 1936 and 1993 thus representing around
60 years of USA teeth record (Robbins et al., 2010). The Cleveland
teeth 206Pb/207Pb of 1.202 +/− 0.018 is similar to the high-precision
Pb isotopic data from the younger USA individuals plotted on Fig. 4
(206 Pb/ 207 Pb 1.197; +/− 0.007). For comparison, the 206 Pb/207Pb
ratio for all European teeth (excluding the Romanian data) is
1.155 +/− 0.023. Therefore, the Pb isotope range in USA teeth is dis-
tinct compared with the European data for the last 70–80 years or so.
This is indicating that Pb isotopes even in individuals born before
1960s in the USA should retain distinct Pb signal compared to Europe.
The described Pb isotopic discrimination in this section can easily
distinguish modern USA-born individuals from an immigrant or for-
eigner, but more precise geo-referencing is complicated. The complica-
tion stems from the fact that a number of other countries in the world
used gasoline additives made with Australian Pb and as a result, their
populations show Pb isotopes similar to modern Europeans.
4.2.2. Australia and the rest of the world teeth
Modern teeth from Australian individuals show the least radiogenic
Pb isotopes extending to values similar to Broken Hill (Figs. 5 and 6).
This is mainly due to use of Pb from the geologically-ancient Broken
Hill and Mt. Isa deposits, characterized by very low Pb isotopic ratios
(Gulson, 1986; Gulson et al., 1994a, 1994b). In particular, modern decid-
uous teeth from the Broken Hill region, Australia, show the least radio-
genic Pb isotopes compared with all modern individuals worldwide
(compare Figs. 4 and 5). This is expected and is due to Pb exposure
from the large-scale Pb production in the Broken Hill region (Gulson
868 G.D. Kamenov, B.L. Gulson / Science of the Total Environment 490 (2014) 861–870
et al., 1994a, 1994b). Pb data for adult Australian teeth from different re-
gions show slightly elevated ratios, with 206Pb/204Pb as high as 17.8,
when compared to Broken Hill (Figs. 5 and 6). This is due to mixing of
the anthropogenic Pb from Broken Hill used in gasoline with variable
amounts of more radiogenic local environmental Pb. The most radio-
genic Pb from Australia is observed in deciduous teeth from Boolaroo,
which is due to the presence of smelter that was smelting a mix of
Broken Hill and younger Australian ores with elevated 206Pb/204Pb ra-
tios (Fig. 5). On Fig. 5 the Australian data are compared with Europe.
Very few Australian teeth plot in the more-radiogenic European field
“EU most teeth”, suggesting that modern Australian individuals can be
distinguished from Europeans to some extent based on their teeth Pb
isotopic signature (Gulson et al., 1997). This isotopic distinction is
more pronounced when compared with Eastern European teeth, char-
acterized by somewhat elevated ratios compared with Western and
Northern Europe as discussed above (Fig. 4). There is significant overlap
between the Australian and the European teeth plotting within the “EU
few teeth” (or lower radiogenic field), which is expected given that both
regions were using Pb in gasoline additives from the same Australian
deposits. Regardless of the partial overlap, we should be able to discrim-
inate between modern European and Australian individuals in certain
cases.
There is overlap between Europe and Asian, South American, and
Middle Eastern modern teeth (Fig. 5). This is due to the use of imported
leaded gasoline additives made with Australian Pb. In India Gulson et al.
(2004a) compared blood Pb isotopes with major Indian deposits and
discovered that there is no match, suggesting that Indian blood Pb,
and by analogy Pb incorporated in the teeth of the local population is
inherited largely from the leaded gasoline. Middle East data plot entirely
in the European field (Fig. 5) suggesting that the same Pb additive was
used in the area and so we cannot really discriminate between the
two regions based solely on Pb isotopes. Although there is some overlap,
Australian teeth are significantly less radiogenic when compared with
the modern Asian (India and South Korea) and South American teeth
(Fig. 5) thus allowing for potential discrimination between these re-
gions in certain cases.
We were not able to locate published data for teeth from Canada.
However, Pb in leaded gasoline in Canada has been sourced exclusively
from ores from New Brunswick and British Columbia characterized with
206
Pb/207Pb ratios of 1.16 or lower (Sturges and Barrie, 1987) that
should correspond to a relatively low 206Pb/204Pb and potentially
would overlap with the European field. In contrast, modern USA teeth
compared with Australia and the rest of the world are very distinct,
with much more radiogenic Pb (compare Figs. 4 and 5). This will
allow for easy distinction of foreigners in the USA or USA individual in
any other region in the world.
4.2.3. Modern vs historical teeth
Where available, comparison between modern and historical teeth
in the same region shows significantly different Pb isotopic signatures,
reflecting the widespread modern Pb pollution that occurred during
the era of leaded gasoline usage. In the USA historical teeth show a
very large spread in the Pb isotopes (Fig. 3), but as stated above, these
19th century data are likely from individuals exposed to anthropogenic
Pb, and also people possibly coming from Europe. This 19th century ex-
posure was likely more “point-source” compared with the modern re-
gional scale focusing effect of the leaded gasoline. Compared with
19th century data, modern USA teeth show much less spread
confirming the strong focusing during modern times due to the usage
of leaded gasoline (compare Figs. 3 and 4). Note that the USA teeth
form a trend towards the MVT ores (Fig. 6). As we show on Fig. 1 and
discuss above, not only MVT ores but also ores with less radiogenic Pb
were used for the leaded gasoline manufacturing in the USA. Therefore,
the isotope signal is a mixture of MVTPb and Pb from other sources.
Similar relationships are observed in Europe between historical and
modern teeth. Although the Pb isotopes in the European population
show exposure to anthropogenic Pb since the Iron Age, the recent
Australian Pb imports caused a major shift in the modern teeth. As a re-
sult, the majority of the modern human teeth, in particular from North-
ern and Western Europe, show a shift to much less radiogenic ratios
(compare Figs. 2 and 4). It is worth noting that the historical data show-
ing cultural focusing since the Iron Age are mainly from Britain and
Western Europe, and the shift towards Australian Pb with very low
ratios is well-defined in the modern population in this region. In com-
parison, the modern Eastern and Southern Europe teeth show some
overlap with the historical Europe data (compare Figs. 2 and 4). Howev-
er, we do not have data for historical teeth from Eastern Europe to eval-
uate this in more details.
In South America a similar shift to much less radiogenic values is ob-
served when comparing modern versus historical teeth data (compare
Figs. 2 and 5). As can be seen on Fig. 5, the available data for modern
South American teeth have a 206Pb/204Pb ratio around 18.0 or less. In
contrast, the historical South American data have 206Pb/204Pb ratios
typically above 18.5, with only 3 samples showing values between
18.2 and 18.4. This is clearly showing that new Pb was introduced re-
cently and this Pb swamped the historical background in the region.
The similarity of the South American and European teeth suggests that
Australian Pb was used as additive in the leaded gasoline in the region.
5. Conclusions and geo-referencing applications
The isotopic composition of Pb incorporated in human teeth and
bones reflects the local environmental Pb and can provide useful infor-
mation for geo-referencing individuals. The local environmental Pb can
be controlled by natural (i.e., local bedrock, soil, dust) and/or anthropo-
genic factors. Once Pb mining and usage begins in a given region, the
local natural Pb background is rapidly altered by the addition of anthro-
pogenic Pb. This new anthropogenic Pb readily finds its way into the
human body and is recorded in teeth and bones. Historical human
teeth in Europe show Pb isotope focusing as early as the Iron Age
reflecting the addition of anthropogenic Pb to the environment as a re-
sult of Pb mining and usage during the Romano-British period (Budd
et al., 2004; Montgomery et al., 2010). During the last century, the wide-
spread Pb usage, mainly in leaded gasoline, completely altered the nat-
ural background in virtually any region in the world and this is clearly
recorded in modern human teeth. Lead from ores with highly radiogen-
ic Pb isotopic compositions from MVT deposits was mainly used in the
USA. In contrast, many other countries in the world used Australian Pb
characterized with less radiogenic Pb isotopes. This created a “silver lin-
ing” in the modern lead pollution as we can easily identify “foreigners”
in the USA or USA born-individuals elsewhere in the world based on
their Pb isotopic signature.
Comparison between available Pb isotope teeth data from different
regions of the world from historical to modern times provides some in-
teresting applications for geo-referencing of humans. In archeological
sites, in particular throughout the New World, it should be possible to
distinguish early European from local human remains. Also, there is a
significant spread in the historical South American teeth suggesting
that it may be possible to assign individual locations and so assist in
reconstructing historical human migration (Turner et al., 2009). In com-
parison, modern South American data are distinct from historical South
American data and this should allow distinguishing if skeletonized
human remains with unknown context are modern or historical. Simi-
larly, modern European individuals tend to have less radiogenic Pb iso-
topes compared with historical individuals and this also should allow
distinguishing if skeletonized human remains in a cold case are modern
or historical. Overall, this should be possible in virtually any region of
the world due to the modern Pb isotope focusing. Such information
will help the law enforcement as valuable resources won't be wasted
on investigating skeletonized human remains that may be centuries
old. In modern forensic investigations we can use different bones and
teeth, and even other tissues such as blood to provide chronological
 G.D. Kamenov, B.L. Gulson / Science of the Total Environment 490 (2014) 861–870
information about possible migration throughout the life of the victim
as different tissues form at different times. For modern investigations,
the Pb isotopes can be used to identify “foreigners” in the USA, as mod-
ern USA teeth are distinct from any other region of the world. By analo-
gy, USA individuals can be identified virtually in any region of the world.
Similarly, Australians can be identified in more or less any region in the
world, although there is some overlap with Western Europe and Middle
East. In Europe, there is some distinction with less radiogenic Pb in
Western and Northern Europe versus more radiogenic Pb in Eastern
Europe. The available data for the rest of the world show overlap with
Europe indicating that it is difficult to distinguish contemporary individ-
uals from Europe based solely on Pb isotopes.
Conflict of interest
We do not have any financial or other conflict of interest associated
with the submitted manuscript entitled “The Pb isotopic record of
historical to modern human lead exposure”.
Acknowledgments
We thank Norman Robbins for providing Cleveland Pb isotope data.
G.K. is thankful to John Krigbaum and Ben Valentine for numerous dis-
cussions about isotopes in human teeth and bones and to Erin Kimmerle
for the introduction to cold case investigations. We are indebted to
Melania Lopez-Castro for performing the statistical analyses of the mod-
ern teeth data in R. We would like to thank two anonymous reviewers
for their constructive comments that greatly improved the manuscript.
Appendix A. Supplementary data
Supplementary data to this article can be found online at http://dx.
doi.org/10.1016/j.scitotenv.2014.05.085.
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