Fitch, Grauer, Augustine

Lead Isotope Ratios: Tracking the
Migration of European-Americans to
Grafton, Illinois in the 19th Century
A. FITCH,
a
* A. GRAUER
b
AND L. AUGUSTINE
c
a
Department of Chemistry, Loyola University Chicago, Chicago, IL 60626, USA
b
Department of Anthropology, Loyola University Chicago, Chicago, IL 60626, USA
c
Department of Drug Enforcement, Loyola University Chicago, Chicago, IL 60626, USA
ABSTRACT Lead isotope analysis was conducted using inductively coupled plasma mass spectrometer (ICP-MS)
instruments on local soil samples and human premolar tooth enamel from a 19th century population from
Grafton, Illinois, USA. The goal of the study was to determine if lead isotope analysis could be used to infer
place of birth and patterns of 19th century migration into the city of Grafton. Five soil core samples from a
location near Grafton, Illinois, ve grave soil samples fromthe city cemetery and the tooth enamel of 19 human
premolars were analysed. The results of the soil core analysis indicated that the lead isotopic signature of
Grafton differs signicantly fromisotope ratios of other geographic areas associatedwith recordedplaces of birth of
19th century Jersey County residents. Elemental and isotope analysis of the soil samples indicated that diagenesis
was not a factor in the analysis of lead isotopic signatures of enamel. From the lead isotope analysis of human
premolars, the geographic origin of 13 of the remaining 15 individuals could be inferred. The inferred geographic
origin was supplemented by an analysis of 1860 mortality and census records and demonstrated the utility of using
lead isotope analysis in bio-archaeological investigations. Copyright 2010 John Wiley & Sons, Ltd.
Key words: diagenesis; human migration; lead isotope ratios
Introduction
A growing body of research suggests that the study of
lead contained in human tissues (bones and teeth in
particular) can provide answers to anthropological
questions concerning human life in the past. While
early studies focused primarily on determining the
presence and amount of lead in human tissues (Jarcho,
1964; Becker et al., 1968; Jaworowski, 1968; Grandjean &
Homa, 1973; Mackie et al., 1975; Waldron et al., 1976),
more recent studies have explored the association
between lead exchange between tissues (Gulson &
Gillings, 1997), the potential for lead exchange between
mother and offspring (Gulson & Wilson, 1994; Gulson,
1996; Gulson et al., 1999; Gulson et al., 2003) and effects
and controls for diagenesis (Budd et al., 2000b). It is
through these more nuanced studies that questions
regarding human migration have been tackled. Chiaradia
et al. (2003) and Budd et al. (2000b), for instance, report
on detectable differences between diagenic sources of
lead and those acquired in vivo. This, in conjunction with
measures of Sr isotope ratios, has allowed for the study of
mobility and possible geographic origin of Neolithic
populations (Montgomery & Budd, 2000). The detection
of varying lead sources (natural and anthropogenic) has
been used to differentiate cultural groups such as Native-
Americans and European fur traders. Others (Carlson,
1996; Muller et al., 2003) have applied lead isotopic
analysis in an effort to determine the geographic origin of
the Alpine Iceman who lived in a period with minimal
environmental lead contamination. Montgomery et al.
(2005) have used lead in tooth enamel to study
movement of Anglo-Saxons into West Heslerton,
England. More recently, Bower et al. (2005) examine
lead isotope ratios derived from dentin, cortical bone
and knitting bone of individuals buried in a 19th
century Colorado mental asylum cemetery. The
authors use these measures as indicators of mobility
and migration, especially during the intermediate and
nal years of the lives of their population.
The goal of our study was to synthesise and expand
previous research using lead isotope ratios derived from
archaeological contexts as means of exploring aspects
International Journal of Osteoarchaeology
(wileyonlinelibrary.com) DOI: 10.1002/oa.1207
* Correspondence to: Department of Chemistry, Loyola University Chi-
cago, Chicago, IL 60626, USA.
e-mail: atch@luc.edu
Copyright # 2010 John Wiley & Sons, Ltd. Received 21 December 2009
Revised 15 July 2010
Accepted 27 July 2010
Int. J. Osteoarchaeol. 22: 305319 (2012)
Published online 4 October 2010 in Wiley Online Library
of historical human migration. Specically, this study
sought to determine whether dental enamel, extracted
from permanent dentition, could be clearly associated
with reported lead isotopic ratios worldwide, and
whether this information could shed light on 19th
century migration paths into the city of Grafton,
Illinois, located in the Mississippi Valley of central
United States. This would be accomplished by using
stringent measures to control for diagenesis, by incorpor-
ating an analysis of soils indigenous to the geographical
area and within the precise archaeological context of the
burials, by testing our data against previously published
lead isotope data using robust measures and by using
multiple lines of evidence in our analysis which included
both primary and secondary historical sources.
A number of aspects of 19th century migration
across the United States (and specically into the
Mississippi Valley region of Illinois) has been evaluated
using historical records. For instance, according to
written accounts, migration of Europeans into the city
of Grafton (Figure 1) occurred from several different
directions. One predominate set of migrants, moving
north, originated in Kentucky, or from southern
seaboard states via Kentucky (Davis, 1998). Another
set of migrants arrived via the port of New Orleans at
the convergence of the Mississippi River with the Gulf
of Mexico. These migrants moved north directly along
the Mississippi River. A third set of migrants moved
west from the northern states via the Erie Canal (opened
in 1825), further travelling down the Ohio River or via
Figure 1. Geographic location of the city of Grafton. Grafton is located approximately 120miles north of the Old Lead Belt mining region
which was in operation as early as the late 1700s. The cross-hatched region represents the settlement pattern as of 1830.
Copyright # 2010 John Wiley & Sons, Ltd.
A. Fitch, A. Grauer and L. Augustine 306
the national road towards the west. Other easterners
continued across the Great Lakes to Chicago and then
south via the Illinois River. A fourth population of
individuals were original hunters, trappers and miners
who roamed the valley in the 1700s and early 1800s
(Ekberg, 2000). While recognising these general
migration routes is an essential component towards
understanding the history of this mining region, it remains
unclear whether migrating adults were accompanied by
children, or whether, as alluded to by Schoolcraft (1819:
234), migration was practiced primarily by males, with
children being born later (and locally) as men settled and
started families. Davis suggests that most of the
settlements were established by younger male migrants
followed by chain migration of family units.
The sample
In the summer of 1993, after a devastating ood of the
Mississippi River, a cemetery was discovered in Grafton,
Illinois, located at the conuence of the Illinois and
Mississippi Rivers (Buikstra, 2000; Figure 1). Although
the grave records for the site were lost in a re, other
historical records indicate that the cemetery, known as
the Grafton Cemetery, was in use from approximately
1832 to 1873 (Sutton et al., 2000).
Excavation of the Grafton Cemetery site yielded 164
individuals from 252 unmarked graves (Houdek et al.,
2000). Of these individuals, 88 contained a minimum
of one premolar in good condition.
The decision to use tooth enamel exclusively in this
study was based on enamels incorporation of elements,
such as lead, into the tissue structure. Since elements
remain xed within enamel throughout an individuals
life, enamel serves as a means towards understanding
the environment within which the individual lived
during the years of enamel crown formation. Human
premolar enamel develops between 2 and 6 years of age
(/1 year) (Moorees et al., 1963; Ubelaker, 1989;
Hillson, 1996). Hence, it is likely that the uptake of
lead into the enamel tissue of this tooth is derived from
the childs environment, and not acquired in utero or
from maternal sources (Gulson & Wilson, 1994;
Gulson, 1996; Gulson & Gillings, 1997; Gulson et al.,
1999; Gulson et al., 2003). Equally important is the fact
that 96%of enamel tissue is apatite with a crystal size larger
than 32nm (less reactive surface area). With large
crystallinity (Lee-Thorp et al., 1991), tooth enamel is
relatively inert to diagenesis (Lambert et al., 1982; Lambert
et al., 1984; Lambert et al., 1985; Purchase &Fergusson, 1986;
Sillen & LeGeros, 1991).
As this study focused on determining the geographic
locations of individuals during their childhood as a
means of understanding migration into the city, two
subsamples were created. The rst consisted of individuals
with a recovered premolar in good condition (absence of
caries or pre/post mortem damage and yielding >100mg
of enamel for analysis) under the age of 10 years. In total,
seven of the eight juveniles recovered with dentition met
these criteria. Since premolars are some of the last teeth to
develop, all juveniles within this sample were between the
ages of 5 and 10 years. The second subsample was
composed of individuals over the age of 55 years with
premolar enamel in good condition. Fifteen individuals
met these criteria, of which eight were randomly selected
for this study. Also included in this study were previously
reported results (Augustine, 2002) obtained from two
adult skeletons (between the ages of 20 and 35 years)
containing the requisite teeth in good condition.
Materials and methods
Soil core samples
Five cores (no. 1no. 5) were taken from different
locations (Figure 2) within the town of Grafton relocation
site to a depth of 137 cm (54) in three sections of
45.7 cm(18). Seven sections were taken fromcores no.
1 and no. 2 at depths of 0, 23, 46, 84, 91, 130 and
137 cm. Three sections were taken from cores no. 3
no. 5 at depths of 0, 91 and 137 cm. Each section of soil
was subdivided into four parts.
Figure 2. Aerial photograph of Jersey County including the town
of Grafton, Grafton Cemetery, the town relocation site, and
location of soil core samples. Photo: USGS 01 April 1998.
Available 4 March 2002 http://terraserver.homeadvisor.msn.-
com/default.asp
Tracking the Migration of European-Americans 307
Lead was extracted from soils by hot HNO
3
mixture
using procedures outlined by Farmer (Farmer et al.,
1996). Four samples of 100500 mg of soil from
each section were analysed, with one of the samples
being used as a control for moisture content. The other
three samples were used for digestion. The lead
concentration analysis of the soil cores (no. 3no. 5)
was performed by inductively coupled plasma mass
spectrometry (ICP-MS) using standard curve analysis.
Quality control samples [reagent blanks, spiked blanks
(reagent blank spiked with National Institute of
Standards and Technology (NIST) standard reference
materials (SRM) 981 common lead isotopic standard))
and SRM 2704 (Buffalo River sediment)] were run to
validate the procedure. Instrumental mass bias was
corrected using NISTSRM997 in conjunction with the
power law (Begley and Sharp, 1997). The relative
deviation of the average of three replicate samples of
SRM981 standard fromthe certied value (
208
Pb/
206
Pb of
2.168 and
207
Pb/
206
Pb of 0.9146) was 0.09% for
208
Pb/
206
Pb ratio and 0.04% for
207
Pb/
206
Pb ratio. The
recovery rate associated with SRM 2704 was 94%.
Burial soil samples
Soil samples were collected by the archaeologists
during the original excavation from 115 randomly
selected graves (Powell & OGorman, 2000). Samples
from within the southwest corner of each cofn, along
with control samples taken outside the grave shaft ll
on the southwest corner of the excavation grid, were
used by the archaeologists to explore possible factors
responsible for differential preservation of wood and
bone across the site (Powell & OGorman, 2000). For
this study, the burial soil (collected within the cofn)
from ve randomly chosen graves was used to test for
diagenesis through the determination and analysis of
elemental ratios (Ba/Ca, Sr/Ca and Pb/Ca). Three sample
replicates were analysed from each burial soil sample by
extraction of 50100mg of soil with 5 ml of pH2 HNO
3
(10ppb In) as discussed in detail in Augustine (2002).
Tissue samples
The premolar tooth enamel (one per individual) was
separated from the dentin using a Cavitron-Parkell
Clean Machine (vibrating metal pick) or Star Dental
Diamond Saw. Amodied version of a solubility prole
procedure (Price et al., 1992) was performed. 3060 mg
of enamel chips were placed in a 1.5 ml polypropylene
centrifuge tube with 1 ml of pH 2 HNO
3.
The tube
containing acid and enamel was placed in an ultrasonic
bath for 2 min. The supernatant was decanted and
saved. The residue was washed 14 more times while
saving the supernatant each time. Elemental analysis
(Ba, Ca, Sr and Pb) on ICP-MS was conducted on
selected supernatant washes (washes 15, 7, 9, 11, 13,
15). Any sample with a blank reagent value greater than
3% of the total measured lead was eliminated from the
population. The total propagated uncertainty for each
elemental ratio value was calculated incorporating the
uncertainties in the analyte concentrations. The average
enamel mass loss for seven enamel samples was 4.1%.
Washes selected for lead analysis were combined, placed
in a Teon container, dried down, redissolved in 50ml of
concentrated HBr and dried down again (Strelow, 1978;
Humayun, pers. comm.). These two steps were repeated,
and the residue was redissolved in 1 ml of 0.5 NHBr. 1 ml
of AG1-X8 200-400 mesh resin was loaded onto a 10 ml
poly-prep chromatography column and then washed
with 4 ml of 4 NHNO
3
, 8ml of deionised water and 2 ml
0.5 N HBr successively to clean and convert the resin
from chloride to bromide form. 1ml of 0.5N HBr
containing sample was loaded onto the column. After the
column was washed with 2ml of 0.5N HBr, the lead was
eluted with 4ml of both 0.5N and 4N HNO
3
and saved
for isotope analysis. The average sample and column
procedural blank content for lead was 8.3ng and 47pg.
Tooth enamel samples were eliminated from nal analysis
when total recovered lead was not sufcient for lead isotope
analysis, bringing the nal sample population to 15.
Cleaning procedures were carried out in clean rooms
at University of Chicago and University of Illinois at
Chicago. Teon containers, polypropylene centrifuge
tubes and poly-prep chromatography columns were
acid cleaned (Patterson and Settle, 1974). At Loyola
University Chicago, all glassware and polypropylene
containers were acid cleaned (Patterson and Settle, 1974).
A VG Elemental Plasma Quad (PQ2-ICP-MS) and
a Perkin-Elmer 5000 Atomic Absorption Spectropho-
tometer (FAA) at Loyola University Chicago, a VG PQ
Ex Cell (PQE-ICP-MS) at Northwestern University
and a Finnegan Mat Element (HR-ICP-MS) at
University of Chicago were used for lead isotope
and elemental analysis of all samples.
Results and discussion
Assessing contamination, soil isotopic signature
and diagenesis
The lead concentration of the soil at 60130 cm below
the topsoil was compared to literature values to
determine if the soil was representative of uncontami-
nated soil. The soil lead concentration below the
topsoil was relatively constant (12 1 ppm) (Figure 3).
This value is similar to uncontaminated subsoil
(>60 cm) lead concentrations of 10.412.4 ppm taken
from Poland (Kabala & Singh, 2001). The topsoil
concentration increases only slightly. The lack of
apparent contamination is consistent with environ-
mental sampling of sediment core samples. Lead
concentration and isotope ratios are relatively constant
in sediment core samples at depths corresponding to
the mid-17th to mid-18th centuries from Northeastern
United States (Great Lakes region) (Graney et al.,
1995), the United Kingdom (Farmer et al., 1996) and
Thompson Canyon near Yosemite National Park
(Sirihata et al., 1980). For example, in a Lake Erie
core, the variation was 6% for the lead concentration,
0.02% for
207
Pb/
206
Pb ratio and 0.07% for
208
Pb/
206
Pb ratio, respectively, at depths corresponding
to between 1798 and 1860 (Graney et al., 1995).
Similarly, the Grafton soil lead isotope proles are
relatively constant with depth. The lack of change in the
isotope ratios throughout the soil prole correlates with
the lack of change in the lead concentration. The
variation in the isotope ratios from core samples no. 1 to
no. 2 over the whole soil prole was less than 0.4% for
either isotope ratio and is in agreement with the variation
in the Lake Erie sediment prole (Ritson et al., 1994). The
soil proles indicate that little contamination of the soil
occurred within the relevant historical time period.
The isotope ratios determined from soil proles
were used to calculate the Grafton isotopic signature.
The Grafton isotopic signature (
208
Pb/
206
Pb and
207
Pb/
206
Pb) was calculated by taking the average
isotope ratio (1s) of all the cores at different depths
(1.98 0.01 and 0.797 0.005). This is acceptable
because of the lack of variation of the isotope ratios
with depth (Figure 3).
Ba/Ca and Sr/Ca elemental ratios derived from the
soils associated with burial (soils) and enamel sample
rinses were evaluated to test for diagenesis (Figure 4).
The Ba/Ca and Sr/Ca ratios for the soil (see boxed
range Figure 4) were consistent with values obtained
for Wisconsin soil samples derided in a temperate
woodland climate (Burton et al., 1999). If the enamel
was contaminated by diagenesis, the rst several acid
rinses collected fromthe enamel should have elemental
ratios similar to the soil values. Ba/Ca and Sr/Ca
elemental ratios were slightly higher in the initial wash
compared to the steady state rinse value (washes 10
15) but substantially lower than the elemental values
for the soils. This type of rinse pattern has been
reported by other researchers (Sealy et al., 1991; Sillen
& LeGeros, 1991).
The change (%C
e
) from rst wash value (W
1
) to the
steady state value (S
e
) was calculated in Equation (1):
%C
e

W
1
S
e
S
e
100 (1)
A 29166% elemental change was observed. This
change in the elemental ratios was greater than other
reported studies (540%) (Budd et al., 2000a) indicating
Figure 3. Lead concentration,
207
Pb/
206
Pb, and
208
Pb/
206
Pb soil proles from core samples from town relocation site.
both the presence and the substantial removal of some
diagenetic and/or procedurally acquired contamination
containing barium and strontium. Statistical analysis
indicates a difference between W
1
and S
e
and S
e
and
burial soil values for all enamel samples.
Determining childhood origins
Pb/Ca ratios as a test for diagenesis were evaluated in a
similar fashion as the other elemental ratios. Again, the
per cent change between the initial and steady state
acid rinses of the enamel was monitored. There was no
statistical difference in the initial wash value compared
to the steady state value for all Grafton enamel samples.
In addition, Pb/Ca steady state ratio values of the
Grafton enamel were statistically different from burial
soil value. These two observations suggest that
diagenesis did not affect the enamel lead content
and that the lead present can be attributed to in vivo
biological processes. Similar conclusions were drawn
from measurements of lead isotope ratios as a function
of wash number.
Assessing childhood origins
Assessing childhood origins as a means of under-
standing migration patterns rst requires the determi-
nation of lead isotope ratios of the enamel samples and
then comparison of the results with known soil and
mineral values. Combining data (
207
Pb/
206
Pb vs.
208
Pb/
206
Pb ratios) derived from two literature data-
bases of 206 U.S. and European soil and mineral lead
isotope ratios (Doe, 1976) and 97 U.S., Australia,
Africa and European mineral (Sangster et al., 2000) as
well as selected individual publications (Russell & Farquhar,
1960; Brown, 1966; Foley et al., 1981; Brannon et al.,
1991; Monna et al., 1997; ODay et al., 1998; Townsend
et al., 1998) with those derived from tooth enamel
samples from the Grafton Cemetery indicates that the
tooth and soil data lie roughly in three clusters
(labelled 1, 2 and 3) along the larger data set (Figure 5).
Values for the tooth enamel and Grafton soil are
represented by the larger diamonds and squares.
Careful evaluation of Clusters 1, 2 and 3 provides
insight into Graftons past. An expansion of Cluster 1 of
the lead isotope ratio graph displayed in Figure 5 can be
found in Figure 6. Data points containing the ve
Grafton soil samples and four tooth enamel samples are
found in Cluster 1. Propagated error bars for the
enamel and soil data are provided when available. No
error bars are shown for the Doe geologic data, as they
are derived in large part from a compilation lacking
methodological error bars (Doe, 1976). Two points
from the Sangster database appear with very large error
bars (Sangster et al., 2000) for central and eastern
Tennessee.
Three of the enamel samples within Cluster 1 are
derived from adults (212A, 230A and 233A) and one is
from a child (157C). Lead isotope ratios derived from
child 157C are close to those obtained from our
Grafton soil samples (diamonds with error bars). The
possibility that such a strong association is due to soil
contamination of the sample is ruled out by analysis of
the elemental ratios (Ba/Ca, Sr/Ca and Pb/Ca) and the
isotope ratios as a function of sample washing (see
Figure 4), leaving the most likely cause of the isotopic
ratio being in vivo systemic uptake of local ore during
childhood. Hence, our results suggest that individual
157C was raised in Grafton throughout early child-
hood.
Analysis of Pb ratios derived from adults 233A and
230A suggests that the values are most closely
associated with those from Cave-In-Rock literature
values. Those sites are found in the Illinois-Kentucky
Fluorspar District (lead mining from 1835 to 1865
(Goldstein, 1997)) found at the southern tip of Illinois
Figure 4. Log of Ba/Ca and Sr/Ca ratios of Grafton burial soil and
enamel samples as a function of dilute acid washes. ^157C,
172A, 19A, 132A, * 140A, ^ 208A and 82C. The total
uncertainty for the enamel sample measurements is smaller
than symbol marker. The range of measurements for the burial
soils is indicated by the box in the upper portion of each graph.
bordering Kentucky (Figure 7). There are several
mining sites in that region as noted in Figure 7. In
particular, the Rosiclare mine (found within the Cave-
in Rock district) was active from 1835 to 1865
(Goldstein, 1997). It has the closest association with
individual 233A. This suggests that these older
individuals may have migrated from the Kentucky
region. Since individual 212As isotopic signature lies
below the main set of lead ore body data, the location
of childhood origin for this individual cannot be
inferred.
As Figures 5 and 6 show, the isotopic signature of
Graftons soil is different from that of the Old Lead Belt
(Missouri), Galena (North West Illinois), the Tri-State
Figure 5. Lead isotope ratio map of 206 U.S. and Western European literature values (blue circles) with Grafton soil and tooth enamel
(diamonds and squares) superimposed. The tooth and soil isotopic values appear to lie in three clusters (circled and labelled 1, 2 and 3).
The box labelled North West Il/South West Mo. consists of data associated with the Tri-State and Galena Mines (Figure 1, inset). The box
labelled Northern Ky/Southern IL consists, primarily, of data from the Illinois Kentucky Fluorite Mining District. This gure is available in
colour at wileyonlinelibrary.com.
Figure 6. Expanded lead isotope map of Cluster 1, showing literature values, ve Grafton soil samples, and four Grafton tooth enamel
samples. Tooth enamel samples are designated as C for the 510 year age class, A for the 55 age class, (Error bars are one sigma).
This gure is available in colour at wileyonlinelibrary.com.
lead mining regions (Figure 5) and those from the more
eastern regions of Tennessee and Kentucky (Figure 6).
It might be anticipated that the Grafton site should
have an isotope ratio similar to Central Illinois soils,
based on the very large geologic region known as the
Illinois Bowl. However, because Grafton lies along the
bluffs of the Mississippi River, there are a large number
of geologic strata contributing to its isotopic signature
(Willman, 1967; Lineback, 1979; Treworgy, 1979;
Willman et al., 1989; Grimley, 1999). Grafton shares
some similarity in geology with the southern tip of
Illinois. Both regions lie along river bluffs (Grafton
along the Mississippi River and Cave-In-Rock and
Rosiclare along the Ohio River) which expose strata
underlying the Illinois bowl. Consequently, one nds
alignment of lead isotopic ratios with those obtained
from the Illinois-Kentucky Fluorite District.
The expanded data for Cluster 2 are shown in
Figure 8. Values derived from ve adult premolar
enamel samples (19A, 84A, 116A, 129A, 132A) clearly
fall within this Cluster. All plotted geographic/
geologic values within this Cluster are derived from
literature data and pertain to two different lead ore
strata that were utilised at different historical periods.
The solid symbols represent various mines from the
Old Lead belt, including the Mine La Motte which has
been exploited semi-continously since the late 1700s to
the early 1900s. The open symbols represent isotope
ratios associated with the Viburnum Trend (see
Figure 1) which began production in 1960. Grafton
lies approximately 120 miles from these ore bodies. It
will be observed that the enamel samples more closely
match the data associated with the Old Lead belt
(solid symbols), as compared to the Viburnum (open
symbols), which came into production much later.
According to Davis (1998), chain migration was a
common 19th century settlement pattern in the U.S. It
was characterised by the rst, or earliest, settlers being
Figure 7. Map of Illinois-Kentucky Fluorite Mining District with some associated lead isotope ratios.
adult males who would establish a place of residence
and then would move the more vulnerable members of
the family (women and the elderly) to their new
residence. Children would subsequently be born in the
new family location. Hence, it was anticipated that
tooth enamel derived from children buried in the
Grafton Cemetery would correlate most closely with
the Grafton soils. Surprisingly, four children (75C,
82C, 140C, 180C) had tooth enamel associated with
the Old Lead belt.
There are three possible explanations for the match
of eight individuals with the lead of SE Missouri. The
rst possibility is that lead isotope ratios associated
with the Old Lead belts result from aerial contami-
nation caused by smelters spanning the distance
(120 miles) from the lead mines to Grafton. This
possibility was ruled out by the soil prole data clearly
distinguishing Grafton soil from surrounding areas.
The second possibility is that individuals, during
childhood, consumed leaded products whose lead
source was the Old Lead Belt. Historic records
indicate that the most probable sources of lead
consumption would have come from alcoholic stills,
pottery glazes, leaded paints and/or tinned food/lead
contaminated tin. For this study, lead ingestion from
the consumption of alcohol seems improbable given
that premolar crown development occurs between the
ages of 2 and 6 years. While the use of pottery glazes
derived fromOld Lead Belt ore, which were shipped up
the Ohio River for use by the pottery industry, could
serve as a possible explanation (Henry Schoolcraft, in
his 1819 mineralogical and geographical description of
the area indicates that red lead and cerusse were
nished products transported down the Ohio River),
the actual extent of use of leaded glazes and paints on
the frontier during this period remains unknown. The
tin can food processing industry as a conduit for lead
uptake into children is unlikely, as industrial canning
and distribution of food containers with lead solder did
not become common until 1869 (McMahon, 1994).
Hence, it is unlikely that the ingestion of canned goods
was the source of lead. In adults, however, the use of
leaded pewter and lead solder for tin vessel repair
cannot be ruled out, particularly as the 1850 census of
Grafton (N1276) contains two individuals with
tinning listed as their occupation.
The third explanation for the association of eight
individuals buried within the Grafton Cemetery with
enamel lead isotope ratios similar to those of the Old
Lead Belt focuses on employment opportunities in the
region and patterns of migration into the city. Records
from the 1850 census of Grafton indicate that some
residents might have resided in lead mine rich areas of
Missouri (Old Lead Belt, or south along the
Mississippi River in port town Sainte Genevieve)
through which lead was transported, prior to making
their way to Grafton. For example, Henry Barrett, a
tinsmith who was born in England, according to the
1850 Grafton Census, lists children aged 16, 14, 11
born in England, a child aged 4 born in Missouri, and a
child aged 2 born in Illinois. It should be noted that
substantial shipments of lead were simultaneously sent
from Galena, North-West Illinois to St. Louis, Missouri
in this time period (18231848; Petersen, 1930). The
isotope signature, however, for Galena, does not match
the measured lead isotope ratio in tooth enamel.
Schoolcraft (1819) enumerates 34 major lead mines
in areas in SE Missouri and estimated that 1130 persons
were employed as independent diggers and/or were
involved in lead processing in the region (p. 127). The
town of Herculaneum, located south of Grafton along
the Mississippi River, according to Schoolcraft, saw3.2
million pounds of Missouri lead from the Old Lead
Belt moving through its city limits within an 18-month
period. Similarly, south of Herculaneum along the
Mississippi River, the town of St. Genevieve had all
been more or less engaged in the storage, purchase, and
trafc of lead. Every dwelling house thus became a
store-house for lead. . . (Schoolcraft, 1819).
The important point abstracted from Schoolcrafts
observations is that all 300 homes in St. Genevieve
would have been contaminated with lead with an
isotopic signature corresponding to one of the citys
nearby mines such as Mine La Motte. As seen in
Figure 8, individuals in Cluster 2 have the closest
isotopic match to that of Mine La Motte (Figure 9).
Thus, a very probable scenario is that individuals in
Figure 8. Expanded lead isotope map for Cluster 2. All plotted
geographic points within this cluster are derived from the Old
Lead Belt (solid symbols) and Viburnum (open symbols) ore
bodies in Southeastern Missouri. The Old Lead Belt (includes
the Mine La Motte region) was in production from the 1700s on.
The Viburnum trend came into production in the early 1900s.
Cluster 2 resided in the port town of St. Genevieve as
children prior to making their way up the Mississippi
River to Grafton.
There is one last individual represented within Cluster
2: 132A. The isotope ratio of 132A lies signicantly
above the values for the remaining individuals. The
location is not within a range of any given set of literature
values which could be averaged to obtain the isotopic
value associated with 132A. No probable place of origin
can be assigned to 132A.
Cluster 3 is shown in the expanded form in
Figure 10. Here it can be seen that individual 61A
lies close to the literature value for Strontian, Scotland
and it is, therefore, reasonable to hypothesise a
Scottish origin for 61A. Note that this assignment is
based solely on isotope ratios within the database. That
is, places represented within the database can be ruled
out as a point of origin if the isotope ratios do not
match. Places within the database that match the tooth
enamel can be hypothesised, but not absolutely
conrmed, to be a place of origin. Individual 172A
appears to be at the end of a cluster of values associated
with the Austinville-Ivanhoe Pb-Zn district in Virginia
(Foley et al., 1981). The Austinville-Ivanhoe region lies
in Wythe County of Virginia. The mines were opened
in 1756, after discovery by the British colonial ofcer
Colonel John Chiswell. Lead was produced in these
mines continuously from that time forward to the U.S.
Civil War (Whisonant, 1996). Another possibility is
that individual 172A may be from the general Eastern
Tennessee area. The Eastern border of Tennessee is
approximately 150 miles in length and runs along the
Great Smokey Mountains. The Eastern scarp of the
mountain is Precambrian and within 10 miles of the
Precambrian border runs a second, parallel phanerzoic,
geologic strata. These strata account for the different
isotopic regions of Flatgap and Ducktown, TN. (See
circled isotope ratios in Figure 10 and inset geologic
map). As a result, inhabitants of Eastern Tennessee
could be exposed to both sources of lead. Assuming
that an individual living in this region consumed equal
amounts of lead from both sources, their lead isotope
ratios should be an average of theses values as marked
in Figure 10. As shown in Figure 10, the averaging of
Figure 9. Southeastern Missouri mine sites located by the mineral database of Missouri. The isotopic ratios reported are the average of
all literature values reported for a particular mine. The rst number reported is the Pb207/Pb206 value. The second number reported is
the Pb208/Pb206 value. The shading on the graph indicates regions of similar geology.
both potential sources is consistent with the measured
isotopic signature for sample 172A. We assert that
individual 172A immigrated from the region of
Western Virginia/East Tennessee.
Based on the information and analyses above, the
areas of childhood origin for 15 individuals from the
Grafton Cemetery are summarised in Table 1.
Historical comparisons
The assessment of place of childhood origin can be
further enhanced by comparison to regional historical
data. Data derived from the 1860 Grafton Census are
shown in Figure 11. Here, the most frequent locations
listed for Place of Birth in the 1860 Census, for
individuals between the ages of 5 and 10 years and over
55 years, is reported as per cent of the total number of
individuals recorded within those age groups living in
Grafton at that time. A recognisable trend is present.
According to the Census, children between in the ages
of 5 and 10 years were likely to have been born in
Illinois (the census does not record the towns or cities
of birth), followed by Germany, Ohio and Indiana,
Kentucky, Missouri, Virginia and Louisiana and
followed distantly by England, New York, Iowa,
Figure 10. Expanded lead isotopic map expansion for Cluster 3 of Figure 2. The inset is a geologic map of the eastern portion of the state
of Tennessee and those states bordering it. Within the inset the location of Flatgap and Ducktown, Tennessee are indicted. The distance
between the two towns is approximately 10 miles. As can be noted numerous strata incline to the surface in eastern Tennessee due to the
uplift of the Appalachian mountains. This gure is available in colour at wileyonlinelibrary.com.
Table 1. Pb isotope ratios of Grafton tooth enamel (CChild; AAdult)
Age-at-death Tooth enamel
207
Pb/
206
Pb
208
Pb/
206
Pb Location of similar soil/ore Pb ratios
510 157C 0.798 1.984 Grafton, Illinois
510 75C 0.755 1.880 Old Lead Belt
510 82C 0.754 1.873 Old Lead Belt
510 140C 0.758 1.885 Old Lead Belt
510 180C 0.752 1.881 Old Lead Belt
2025 132A 0.759 1.938 Unknown
2025 212A 0.793 1.941 Unknown
2535 172A 0.828 2.045 Eastern Tennessee
55 230A 0.786 1.965 Illinois Kentucky Fluorite District
55 233A 0.784 1.969 Illinois Kentucky Fluorite District
55 19A 0.765 1.897 Old Lead Belt
55 84A 0.759 1.894 Old Lead Belt
55 116A 0.755 1.882 Old Lead Belt
55 129A 0.762 1.891 Old Lead Belt
55 61A 0.832 2.017 Strontian, Scotland
55 208A 0.798 1.980 [Incomplete Data]
Tennessee and Pennsylvania. Individuals over the age
of 55 years most frequently listed Kentucky as the
Place of Birth, followed by North Carolina and
Pennsylvania.
At rst glance, it appears that the 1860 Census
snapshot of Grafton residents differs from the child-
hood origins we determined for the 15 individuals
whose premolar enamel was analysed for lead isotope
values (Figure 12). While the 1860 Census indicates
that most individuals between the ages of 5 and 10
years were born in Illinois, our analysis of the skeletal
sample (n 5) from this age group indicates that lead
isotope ratios are most similar to the area known as the
Old Lead Belt, which lies immediately southwest of
Grafton. For individuals over the age of 55, the
southern part of the United States was most commonly
listed as place of birth in the 1860 Census, while our
analysis suggests that the human remains (n 7) aged
55spent their early childhood somewhere within the
Old Lead Belt (n 4), Northern Kentucky/Southern
Illinois (n 2) or Scotland (n 1). A number of factors
may contribute to these differences. First, these
differences might be the result of assessing different
samples: the 1860 Census recorded individuals living in
the city on one particular day during that particular
year, and the Grafton Cemetery Sample represents 40
years of accumulated death in the city. Data on the
chronological use of the Grafton Cemetery are severely
limited, thus associating particular burials with a
decade, let alone the year of death, is impossible.
The differences, however, might also be due to
sampling bias, as the skeletal sample in this evaluation
is only a small portion of the cemetery population.
Conclusions
This study demonstrates that lead isotope measure-
ments of the permanent premolars derived from
archaeological populations can successfully provide
new information about the recent past. Building upon
previous research, and recognising a need to develop
stringent measures for the detection of bias and
contamination, this work sought to take a synthetic
Figure 11. Place of birth listed in the 1860 Grafton Census.
0
0.1
0.2
0.3
0.4
0.5
0.6
0.7
0.8
0.9
1
I
l
l
i
n
o
i
s
E
a
s
t

o
f

I
l
l
i
n
o
i
s
W
e
s
t

o
f

I
l
l
i
n
o
i
s
S
o
u
t
h
U
S
N
o
n
-
U
S
U
n
d
e
t
e
r
m
i
n
e
d
P
e
r
c
e
n
t

o
f

P
o
p
u
l
a
t
i
o
n

S
a
m
p
l
e
d
1860 Census Ages 5-10
Grafton Sample Ages 5-10
1860 Census Over 55
Grafton Sample Over 55
Figure 12. Comparison of Place of Birth derived from the 1860
Census and Grafton tooth samples.
approach towards the use of lead isotope ratio analysis
in an archaeological context. Using permanent
premolars to eliminate the possibility of maternal
contamination, carefully controlling for diagenesis
through analysis of archaeological soil samples
associated with the specic burials under investigation,
evaluating soil composition from undisturbed areas not
associated with the burials and incorporating data
derived from historical documents have contributed to
a robust exploration of migration into the city of
Grafton during the 19th century.
The lead isotope ratio data add new insight into the
history of Grafton and the region. The rst insight
from this study is the prevalence and importance of
geographic areas immediately southwest of Illinois,
known as the Old Lead Belt. Although Graftons
economy was closely associated with river-commerce,
due to its location on the shore of the Mississippi River,
it appears that for some eventual Grafton residents,
mining rst drew them west of the Mississippi and then
later to the river town of Grafton to the northeast. For
individuals who would eventually die in Grafton,
Illinois, the Old Lead Belt was a stopping point where
they found work and began families. This is evident
from the strikingly similar isotopic signatures derived
from the skeletons and the published signatures of the
Old Lead Belt. Of equal interest is that in our sample
both the majority of children and the majority of
individuals over the age of 55 who were buried in
Grafton Cemetery spent substantial time during their
young lives (at least living there between the ages of 2
and 6 years) in the Old Lead Belt region. While
Schoolcraft (1819, p. 234) mentions the towns of St.
Genevieve and Kaskaskia as points of temporary
residence in this region, it is in the context of single
young males. Our research indicates that migration was
likely a family event, and that temporary residence in
small mining towns southwest of Grafton might have
been measured in years, rather than by seasons.
Acknowledgements
The authors thank Dr Jane Buikstra, Center for Amer-
ican Archeology, for permission to use the skeletal
material; Dr Torma and Dr Lauterbach at Quality
Family Dentistry, for use of the Cavitron-Parkell Clean
Machine; Dr Munir Humayun for use of the Finnigan
Mat Element (HR-ICP-MS) at the University of Chi-
cago; David Goldblatt of Loyolas Center for Urban
Environmental Research and Policy for assistance with
GIS mapping and the University of Illinois, Chicago
and Northwestern University for permission and access
to the ICP-MS and clean room.
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