Geol.

656 Isotope Geochemistry

Lecture 11 Spring 2009

ISOTOPE COSMOCHEMISTRY
INTRODUCTION
Meteorites are our
primary source of in-
formation about the
early Solar System.
Chemical, isotopic,
and petrological fea-
tures of meteorites re-
flect events that oc-
curred in the first few
tens of millions of
years of Solar System
history. Observations
on meteorites, together
with astronomical ob-
servations on the birth
of stars and the laws of
physics, are the basis
of our ideas on how
the Solar System, and
the Earth, formed.
Meteorites can be
divided into two broad
groups: primitive mete- Figure 11.1. Photograph of the meteorite Allende, which fell in Mexico in
orites and differentiated
1969. Circular/spherical features are chondrules. Irregular white patches are
meteorites. The chon-
CAI’s.
drites constitute the
primitive group: most
of their chemical, isotopic, and petrological features resulted from processes that occurred in the cloud
of gas and dust that we refer to as the solar nebula. All chondrites, however, have experienced at least
some metamorphism on “parent bodies”, the small planets (diameters ranging from a few km to a few
hundred km) from which meteorites are derived by collisions. The differentiated meteorites, which in-
clude the achondrites, stony irons, and irons, were so extensively processed in parent bodies, by melt-
ing and brecciation, that information about nebular processes has largely been lost. On the other hand,
the differentiated meteorites provide insights into the early stages of planet formation.
Chondrites are so called because they contain “chondrules”, small (typically a few mm diameter)
round bodies that were clearly once molten (Figure 11.1). The other main constituents of chondrites are
the matrix, which is generally very fine grained, amoeboid olivine aggregates (AOA’s), and refractory
calcium-aluminum inclusions (generally called CAI’s). These last two groups formed by a variety of
mechanisms, some of which appear to be complex, but we can generalize and say that all these are
grains or aggregates of grains which are also grain that equilibrated with nebular gas at high tempera-
ture through condensation and/or evaporation. Most chondrites can be divided into carbonaceous (C),
ordinary, and enstatite classes1. The carbonaceous chondrites are, as their name implies, rich in carbon
(as carbonate, graphite, organic matter, and, rarely, microdiamonds) and other volatiles and are further

1
In the last decade or two, additional classes have been added that are defined by rarer meteorites.

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Lecture 11 Spring 2009
divided into classes CI, CV, CM, CO, CR, CH, and CB. The CI chondrites lack chondrules and are con-
sidered the compositionally the most primitive of all objects. The ordinary chondrites are divided into
classes H, L, and LL based on iron content, and enstatite chondrites can be subdivided into EH and EL,
also based on iron content. Chondrites are further assigned a petrographic grade on the basis of the ex-
tent of metamorphism they have experienced in parent bodies. Grades 4, 5, and 6 have experienced in-
creasing degrees of high-temperature metamorphism, while grades 1 and 2 experienced low-
temperature aqueous alteration. Grade 3 is the least altered. Achondrites are in most cases igneous
rocks, some roughly equivalent to terrestrial basalt, others appear to be cumulates. Other achondrites
are highly brecciated mixtures. Irons, as they name implies, consist mainly of Fe-Ni metal (Ni content
around 5%), and can also be divided into a number of classes. Stony-irons are, as their name implies,
mixtures of iron metal and silicates.
In these two lectures, we focus on the question of the age of meteorites and variations in their isotopic
composition.
COSMOCHRONOLOGY
Conventional methods
Meteorite ages are generally taken to be the age of Solar System. The oft cited value for this age is
4.566 Ga. Before we discuss meteorite ages in detail, we need to consider the question of precisely what
event is being dated by radiometric chronometers. Radioactive clocks record the last time the isotope
ratio of the daughter element, e.g., 87Sr/86Sr, was homogenized. This is usually some thermal event. In
the context of what we know of early Solar System history, the event dated might be (1) the time solid
particles were removed from a homogeneous solar nebula, (2) thermal metamorphism in meteorite
parent bodies, or (3) crystallization (in the case of chondrules and achondrites), or (4) impact metamor-
phism of meteorites or their parent bodies. In some cases, the nature of the event being dated is un-
clear.
The oldest reliable high precision age is from CAI inclusions of Allende, a CV3 meteorite. These give a
Pb isotope age of 4566±3 Ma. Amelin and Krot (2007) 4566.6 ± 1.0 Ma for chondrules from Allende and
Bouvier et al. (2008) reported and age of 4567.59 ± 0.10 Ma for a single large Allende chondrule. The
matrix of Allende may be somewhat younger, although this is uncertain. Precise Pb-Pb ages of 4.552
Ga have been reported by several laboratories for the St. Severin LL chondrite. The same age
(4.552±0.003 Ga) has been reported for 2 L5 chondrites. U-Pb ages determined on phosphates in equili-
brated (i.e., petrologic classes 4-6) ordinary chondrites range from 4.563 to 4.502 Ga. As these phos-
phates are thought to be secondary and to have formed during metamorphism, these ages apparently
represent the age of metamorphism of these meteorites. Combined whole rock Rb-Sr ages for H, E, and
LL chondrites are 4.498±0.015 Ga. However, within the uncertainty of the value of the 87Rb decay con-
stant, this age could be 4.555 Ga (uncertainties normally reported on ages are based only on the scatter
about the isochron and the uncertainty associated with the analysis, they do not include uncertainty as-
sociated with the decay constant). No attempt has been made at high-precision dating of CI chondrites
as they are too fine-grained to separate phases.
Pb isotope ages of the unusual achondrite Angra dos Reis, often classed by itself as an ‘angrite’ but re-
lated to the Ca-rich achondrites, give a very precise age of 4.5578±0.0004 Ma. Ibitira, a unique un-
brecciated eucrite (achondrite), has an age of 4.556±0.006 Ga. Perhaps surprisingly, these ages are the
same as those of chondrites. This suggests that the parent body of these objects formed, melted, and
crystallized within a very short time interval. Not all achondrites are quite so old. A few other high
precision ages (those with quoted errors of less than 10 Ma) are available and they range from this
value down to 4.529±0.005 Ga for Nueve Laredo. Thus the total range of the few high precision ages in
achondrites is about 30 million years.
K-Ar ages are often much younger. This probably reflects Ar outgassing as a result of collisions.
These K-Ar ages therefore probably date impact metamorphic events rather than formation ages.

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 Geol. 656 Isotope Geochemistry
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The present state of conventional meteorite chronology may be summarized by saying that it appears
the meteorite parent bodies formed around 4.56±0.005 Ga, and there is some evidence that high-
temperature inclusions (CAI's: calcium-aluminum inclusions) and chondrules in carbonaceous chon-
drites may have formed a few Ma earlier than other material. Resolving events on a finer time-scale
than this has proved difficult using conventional techniques. There are, however, other techniques that
help to resolve events in early solar system history, and we now turn to these.
Initial Ratios
Attempts have been made to use initial isotope ratios to deduce a more detailed chronology, but
these have been only moderately successful. Figure 11.2 shows initial 87Sr/86Sr ratios of meteorites and
lunar rocks and a time scale showing how 87Sr/86Sr should evolve in either a chondritic or solar reser-
voir. The reference 'initial' 87Sr/86Sr of the solar system is taken as 0.69897±3, based on the work of Pa-
panastassiou and Wasserburg (1969) on basaltic achondrites (this value is known as BABI: basaltic
achondrite best initial). Basaltic achondrites were chosen since they have low Rb/Sr and hence the ini-
tial ratio (but not the age) is well constrained in an isochron. Subsequent high precision analyses of in-
dividual achondrites yield identical results, except for Angra Dos Reis and Kapoeta, which have slightly
lower ratios: 0.69885. This suggests their parent body(ies) were isolated from the solar system some-
what earlier. CAI's and Rb-poor chondrules from Allende have an even lower initial ratio: 0.69877±3.
Allende chondrules appear to be among the earliest formed objects. The parent body of the basaltic
achondrites appears to have formed 10 to 20 Ma later. Note there is no distinction in the apparent age
of the oldest lunar rocks and the basaltic achondrites: from this we may conclude there was little or no
difference in time of formation of the moon, and presumably the Earth, and the basaltic achondrite par-
ent body.
The initial 143Nd/144Nd ratio of the solar system is taken as 0.506609±8 (normalized to 143Nd/144Nd =
0.72190) based on the work on chondrites of Jacobsen and Wasserburg (1980). Achondrites seem to
have slightly higher initial ratios, suggesting they formed a bit later.
The initial isotopic composition of Pb is taken from the work of Tatsumoto et al. (1973) on troilite
from the Canyon Diablo iron meteorite as 206Pb/204Pb: 9.307, 207Pb/204Pb: 10.294, 208Pb/204Pb: 29.476. These
values are in agreement with the best initial values determined from chondrites, including Allende
chondrules. More recent work by Chen and Wasserburg (1983) confirms these results, i.e.: 9.3066,

Figure 11.2. Initial Sr isotope ratios plotted against a time scale for 87Sr/86Sr as-
suming a chondritic Rb/Sr ratio. After Kirsten (1978).

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Lecture 11 Spring 2009
10.293, and 29.475 respectively.
EXTINCT RADIONUCLIDES
There is evidence that certain short-lived
nuclides once existed in meteorites. This
evidence consists of the anomalous abun-
dance of nuclides, for example, 129Xe,
known to be produced by the decay of
short-lived radionuclides, e.g., 129I, and cor-
relations between the abundance of the ra-
diogenic isotope and the parent element.
Consider, for example, 53Cr, which is the
decay product of 53Mn. The half-life of
53
Mn, only 3.7 million years, is so short that
any 53Mn produced by nucleosynthesis has
long since decayed. If 53Mn is no longer Figure 11.3. Correlation of the 53Cr/52Cr ratio with
55 52
present, how do we know that the anoma- Mn/ Cr ratio in inclusions from the Allende CV3 me-
53 53 teorite. After Birck and Allegre (1985).
lous Cr is due to decay of Mn? We rea-
son that the abundance of 53Mn, when and
if it was present, should have correlated with the abundance of other isotopes of Mn. 55Mn is the only
stable isotope of Mn. So we construct a plot similar to a conventional isochron diagram (isotope ratios
vs. parent/daughter ratio), but use the stable isotope, in this case 55Mn as a proxy for 53Mn. An example
is shown in Figure 11.3.
Starting from our basic equation of radioactive decay, we can derive the following equation:
D = D0 + N 0 (1 − e− λt ) 11.1
This is a variation on the isochron equation we derived in lecture 4. Written for the example of the de-
cay of 53Mn to 53Cr, we have:
53
Cr  53 Cr   53
Mn 
= + (1 − e− λt ) 11.2
52
Cr  52 Cr  0  52 
Cr  0
where the subscript naught denotes an initial ratio, as usual. The problem we face is that we do not
know the initial 53Mn/52Cr ratio. We can, however, measure the 55Mn/53Cr ratio. Assuming that initial
isotopic composition of Mn was homogeneous in all the reservoirs of interest; i.e., 53Mn/55Mn0 is con-
stant, the initial 53Mn/52Cr ratio is just:
53 55 53
 Mn   Mn   Mn 
 = 11.3
52
Cr  0  52
Cr  0  55
Mn  0
Of course, since 55Mn and 52Cr are both non-radioactive and non-radiogenic, the initial ratio is equal to
the present ratio (i.e., this ratio is constant through time). Substituting 11.3 into 11.2, we have:
53
Cr  53 Cr   55
Mn   53
Mn 
= + (1 − e− λt ) 11.4
52
Cr  52 Cr  0  52
Cr  0  55
Mn  0
Finally, for a short-lived nuclide like 53Mn, the term λt is very large after 4.55 Ga, so the term e–λt is 0
(this is equivalent to saying all the 53Mn has decayed away). Thus we are left with:
53
Cr  53 Cr   55
Mn   53
Mn 
= + 11.5
52
Cr  52 Cr  0  52
Cr  0  55
Mn  0

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 Geol. 656 Isotope Geochemistry
Lecture 11 Spring 2009
On a plot of 53Cr/52Cr vs.
55
Mn/52Cr, the slope is propor- Table 11.1. Short-Lived Radionuclides in the Early
tional not to time, as in a conven- Solar System
tional isochron diagram, but to the Radio- Half-life Decay Daughter Abundance
initial 53Mn/55Mn ratio. Thus cor- nuclide Ma Ratio
relations between isotope ratios 10Be 1.5 β 10
B 10
Be/ Be ~ 9 × 10–4
9

such as these is evidence for the ex- 26Al 0.7 β 26

Mg 26
Al/27Al ~ 5 × 10–5
istence of extinct radionuclides. 41
Ca 0.15 β 41
K 41
Ca/40Ca 1 × 10–8
In this way, many extinct radi- 53Mn 3.7 β 53
Cr 53
Mn/55Mn ~ 4 × 10–5
onuclides have been identified in 60Fe 1.5 β 60
Ni 60
Fe/56Fe ~ 6 × 10–8
meteorites from variations in the 107Pd 9.4 β 107
Ag 107
Pd/108Pd ~ 4 × 10–4
abundance of their decay products. 129I 16 β 129
Xe 129
I/127I ~ 1 × 10–4
The most important of these are 146Sm 103 α 142
Nd 146
Sm/144Sm ~ 0.008
listed in Table 11.1. On a cosmic 182Hf 9 β 182
W 182
Hf/180Hf ~ 2.6 × 10–4
scale, nucleosynthesis is a more or 244Pu 82 α, SF Xe 244
Pu/238U ~ 0.005
less continuous process – roughly
once every second, a supernova explodes somewhere in the universe. So we might expect that inter-
stellar dust might contain some of the longer-lived of these nuclides at low concentrations. However,
such events are much rarer on a local scale (fortunately for us), and the shorter-lived of these nuclides
must have been synthesized nearby shortly before the solar system formed.
To understand why these short-lived radionuclides require a nucleosynthetic event, consider the ex-
ample of 53Mn. Its half-life is 3.7 Ma. Hence 3.7 Ma after it was created only 50% of the original number
of atoms would remain. After 2 half-lives, or 7.4 Ma, only 25% would remain, after 4 half-lives, or 14.8
Ma, only 6.125% of the original 53Mn would remain, etc. After 10 half lives, or 37 Ma, only 1/210 (0.1%)
of the original amount would remain. The correlation between the Mn/Cr ratio and the abundance of
53
Cr indicates some 53Mn was present when the meteorite, or its parent body, formed. From this we can
conclude that an event that synthesized 53Mn occurred not more than roughly 30 million years before
the meteorite formed. We will return to this issue in the next lecture.
129
I–129Xe and 244Pu
Among the most useful of these short-
lived radionuclides, and the first to be
discovered, has been 129I, which decays to
129
Xe. Figure 11.4 shows the example of
the analysis of the meteorite Khairpur.
In this case, the analysis in done in a
manner very analogous to 40Ar-39Ar dat-
ing: the sample is first irradiated with
neutrons so that 128Xe is produced by
neutron capture and subsequent decay of
127
I. The amount of 128Xe produced is
proportional to the amount of 127I present
(as well as the neutron flux and reaction
cross section). The sample is then heated
in vacuum through a series of steps and
the Xe released at each step analyzed in a
mass spectrometer. As was the case in Figure 11.4. Correlation of 129Xe/130Xe with 128Xe/130Xe.
The 128Xe is produced from 127I by irradiation in a reactor,
Figure 11.3, the slope is proportion to the
129 so that the 128Xe/130Xe ratio is proportional to the 127I/130Xe
I/127I ratio at the time the meteorite ratio. Numbers adjacent to data points correspond to
formed. temperature of the release step.

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 Geol. 656 Isotope Geochemistry
Lecture 11
In addition to 129Xe produced by decay
of 129I, the heavy isotopes of Xe are pro-
duced by fission of U and Pu. 244Pu is of
interest because it another extinct radi-
onuclide. Fission does not produce a
single nuclide, rather a statistical distri-
bution of many nuclides. Each fission-
able isotope produces a different distri-
bution. The distribution produced by U
is similar to that produced by 244Pu, but
the difference is great enough to demon-
strate the existence of 244Pu in meteorites,
as is shown in Figure 11.5. Fission tracks
in excess of the expected number of
tracks for a known uranium concen-
tration are also indicative of the former
presence of 244Pu.
These extinct radionuclides provide a orites (5). The isotopic composition of fission products of
Figure 11.6. Summary of I-Xe ages of meteorites relative to
Bjurböle. After Swindle and Podosek (1989).
125
Spring 2009
Figure 11.5. Variation of 134Xe/132Xe and 136Xe/132Xe in mete-
man-made 244Pu is shown as a star (✯). After Podosek and
Swindle (1989).
means of relative dating of meteorites
and other bodies. Of the various sys-
tems, the 129I–129Xe decay is perhaps
most useful. Figure 11.6 shows relative
ages based on this decay system. These
ages are calculated from 129I/127I ratios,
which are in turn calculated from the ra-
tio of excess 129Xe to 127I. Since the initial
ratio of 129I/127I is not known, the ages
are relative to an arbitrary value, which
is taken to be the age of the Bjurböle me-
teorite, a L4 chondrite.
The ages ‘date’ closure of the systems
to Xe and I mobility, but it is not clear if
this occurred at condensation or during
metamorphism. Perhaps both are in-
volved. The important point is that
there is only slight systematic variation
in age with meteorite types. Carbona-
ceous chondrites do seem to be older
than ordinary and enstatite chondrites,
while LL chondrites seem to be the
youngest. Differentiated meteorites are
generally younger. These are not
shown, except for silicate in the El Taco
iron, which is not particularly young.
The bottom line here is that all chon-
drites closed to the I-Xe decay system
within about 20 Ma.
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 Geol. 656 Isotope Geochemistry
Lecture 11 Spring 2009
An interesting aspect of Figure 11.6 is that the achondrites, which are igneous in nature, and the irons
are at most only slightly younger on average than the chondrites. Irons and achondrites are both prod-
ucts of melting on meteorite parent bodies. That they appear to be little younger than chondrites in-
dicates that and melting and differentiation of those planetismals must have occurred very shortly after
the solar system itself formed and within tens of millions of years of the synthesis of 129I.
107
Pd–107Ag
The existence of variations in isotopic
composition of silver, and in particular
variations in the abundance of 107Ag that
correlate with the Pd/Ag ratio in iron me-
teorites indicates that 107Pd was present
when the irons formed. The half-life of
107
Pd is 9.4 million years; hence the irons
must have formed within a few tens of mil-
lions of years of synthesis of the 107Pd. This
in turn implies that formation of iron cores
within small planetary bodies occurred
within a few tens of millions of years of
formation of the solar system.
Fractions of metal from the meteorite
Gibeon (IVA iron) define a fossil isochron
indicating an initial 107Pd/108Pd ratio of 2.4
× 10-5 (Chen and Wasserburg, 1990). Other Figure 11.7. Correlation of 107Ag/109Ag with 108Pd/109Ag
IVA irons generally fall along the same iso- in Group IVA iron meteorites, demonstrating the exis-
chron (Figure 11.7). IIAB and IIAB irons, tence of 107Pd at the time these irons formed. After Chen
as well as several anomalous irons show and Wasserburg (1984).
107
Ag/109Ag–108Pd/109Ag correlations that
indicate 107Pd/108Pd ratios between 1.5
and 2.4 × 10-5. Assuming these differ-
ences in initial 107Pd/108Pd are due to
time and the decay of 107Pd, all of
these iron meteorites would have
formed no more than 10 million years
after Gibeon (Chen and Wasserburg,
1996).
26
Al–26Mg
Another key extinct radionuclide
has been 26Al. Because of its short
half-life (0.72 Ma), it provides much
stronger constraints on the amount of
time that could have passed between
nucleosynthesis and processes that
occurred in the early solar system.
Furthermore, the abundance of 26Al
was such that its decay could have
been a significant source of heat. 26Al
decays to 26Mg; an example of the cor- Figure 11.8. Al-Mg evolution diagram for Allende CAI WA.
relation between 26Mg/24Mg and Slope of the line corresponds to an initial 26Al/27Al ratio of
27
Al/24Mg is shown in Figure 11.8. 26
Al/27Al ratio of 5.1 × 10-4. After Lee et al. (1976).

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 Geol. 656 Isotope Geochemistry
Lecture 11 Spring 2009
Because of the relatively short
half-life of 26Al and its potential
importance as a heat source, con-
siderable effort has been devoted
to measurement of Mg isotope ra-
tios in meteorites. Most of this
work has been carried out with ion
microprobes, which allow the si-
multaneous measurement of
26
Mg/24Mg and 27Al/24Mg on spa-
tial scales as small as 10 µ. As a re-
sult, there are some 1500 meas-
urements on 60 meteorites re-
ported in the literature, mostly on
CAI’s. The reason for the focus on
CAI’s is, of course, because their
high Al/Mg ratios should produce Figure 11.9. Inferred initial 26Al/27Al for all available meteoritic
higher 26Mg/24Mg ratios. data. After MacPherson et al. (1995).
Figure 11.9 summarizes these
data. These measurements show a maximum in the 26Al/27Al ratio of around 4.5 × 10-5. Significant
26
Mg anomalies, which in turn provide evidence of 26Al, are mainly confined to CAI’s. This may in part
reflect the easy with the anomalies are detected in this material and the focus of research efforts, but it
almost certainly also reflects real differences in the 26Al/27Al ratios between these objects and other ma-
terials in meteorites. The usual interpretation is that this difference reflects a difference in the timing of
the formation of the CAI’s and other materials, most notably chondrules. In this interpretation, CAI’s
would be 2 to 3 million years older than chondrules. Based on the U-Pb dating of Allende mentioned
earlier, however, chondrules appear to be just as old as CAI’s. This observation may favor an alterna-
tive hypothesis is which the chondrules and CAI’s form at the same time in different environments,
with the 26Al by produced by spallation. We’ll discuss these alternative interpretation in the next lec-
ture.
Extinct Radionuclides in the Earth
Several of the short-lived radionuclides listed in Table 11.1 have half-lives sufficiently long that they
should have been present in the early Earth. Of greatest interest are 129I, 182Hf, and 146Sm. The decay
products of these nuclides are 129Xe, 182W, and 142Nd, an atmophile, a siderophile, and a lithophile ele-
ment respectively. Their distribution can tell us about the early evolution of the Earth’s atmosphere,
core, and mantle. Here we’ll consider 182Hf and 142Sm. We’ll discuss 129I in the lecture on the origin and
evolution of the atmosphere.
182
Hf–182W and Core Formation
The Hf-W pair is particularly interesting because Hf is lithophile while W is moderately siderophile.
Thus the 182Hf-182W decay system should be useful in “dating” silicate-metal fractionation, including
core formation in the terrestrial planets and asteroids. Both are highly refractory elements, while has
the advantage the one can reasonably assume that bodies such as the Earth should have a chondritic
Hf/W ratio, but the disadvantage that both elements are difficult to analyze by conventional thermal
ionization. These observations have led to a series of measurements of W isotope ratios on terrestrial
materials, lunar samples, and a variety of meteorites, including those from Mars. The conclusions have
evolved and new measurements have become available. Among other things, the story of Hf-W illus-
trates the importance of the fundamental dictum in science that results need to be independently repli-
cated before they be accepted.

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Lecture 11 Spring 2009
Because the variations in
182
W/183W ratio are quite small, 15
they are generally presented Carbonaeous Chondrite
Chondrite
and discussed in the same ε
Achondrite (Eucrite)
notation used for Nd and Hf
isotope ratios. There is a slight 10
difference, however; εW is the
deviation in parts per 10,000
from a terrestrial tungsten stan-
!W 5
dard, and ƒHf/W is the fractional
deviation of the Hf/W ratio
from the chondritic value. As- Moon
Initial 182Hf/180Hf = 1.0 x 10-4
suming that the silicate Earth
has a uniform W isotope com- 0
Silicate Earth
position identical to that of the
standard (an assumption 182Hf/180Hf = 1.1 x 10-5 (29.5 Ma)
which has not yet been
-5
proven), then the silicate Earth 0 5 10 15
has εW of 0 by definition. The fHf/W
basic question can posed this
way: if the 182W/183W ratio in Figure 11.10. W isotope ratios in meteorites, the Moon and the
the silicate Earth is higher than Earth reported by Yin et al. (2002).
in chondrites, it would mean
that much of the Earth’s tungsten had been sequestered in the Earth’s core before 182Hf had entirely de-
cayed. Since the half-life of 182Hf is 9 Ma and using our rule of thumb that a radioactive nuclide is fully
decayed in 5 to 10 half-lives, this would mean the core must have formed within 45 to 90 million years
of the time chondritic meteorites formed (i.e., of the formation of the solar system). If on the other
hand, the 182W/183W ratio in the silicate Earth was the same as in chondrites, which never underwent
silicate-metal fractionation, this would mean that at least 45 to 90 million years must have elapsed
(enough time for 182Hf to fully decay) between the formation of chondrites and the formation of the
Earth’s core.
‘Anomalous’ W isotopic compositions were first found in the IA iron Toluca by Harper et al. (1991).
They found the 182W/183W ratio in the meteorite was 2.5 epsilon units (i.e., parts in 10,000) lower than in
terrestrial W. This value was revised to -3.9 epsilon units by subsequent, more precise, measurements
(Jacobsen and Harper, 1996). Essentially, the low 182W/183W ratio indicates Toluca metal separated from
Hf-bearing silicates before 182Hf had entirely decayed. Because of the difference between “terrestrial”
W, Jacobsen and Harper (1996) concluded the Earth’s core must have segregated rapidly. At this point,
however, no measurements had yet been made on chondritic meteorites. Chondrites are undifferenti-
ated solar system material, and therefore the reference to which other materials must be compared.
Lee and Halliday (1995) reported W isotope ratios for 2 carbonaceous chondrites (Allende and Mur-
chison), two additional iron meteorites (Arispe, IA, and Coya Norte, IIA) and a lunar basalt. They found
the iron meteorites showed depletions in 182W (εW = -4.5 and -3.7 for Arispe and Coya Norte respectively)
that were similar to that observed in Toluca reported by Jacobsen and Harper (1996). The chondrites,
however, had εw values that were only slightly positive, about +0.5, and were analytically indistin-
guishable from “terrestrial” W, as was the lunar basalt. Lee and Halliday (1995) inferred an initial
182
Hf/180Hf for the solar nebula of 2.6 × 10-4, much higher than assumed by Jacobsen and Harper. Based
on this similarity of isotopic compositions of chondritic and terrestrial W, Lee and Halliday (1995) con-
cluded that the minimum time required for formation of the Earth’s core was 62 million years.
Subsequently, Lee and Halliday (1998) reported εW values of +32 and +22 in the achondrites Juvinas
and ALHA78132. These large differences in W isotopic composition meant that metal-silicate fractiona-

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Lecture 11 Spring 2009
Karooonda
tion, i.e., core formation, oc-
curred quite early in the parent
Murray
bodies of achondritic meteorites; Nogoya
in other words, asteroids or
“planetismals” must have differ- Cold Bokkeveld
Carbonaceous
entiated to form iron cores and
silicate mantles very early, virtu-
chondrites
Murchison
ally simultaneous with the for-
mation of the solar system. This Orgueil
is consistent with other evidence
discussed above for very little
age difference between differen- Allende
tiated and undifferentiated me- a
teorites. Lee and Halliday (1998)
b
also reported εW values in the
range of +2 to +3 in 3 SNC mete-
orites thought to have come from
IGDL-GD
G1-RF Terrestrial
Mars. These data indicated that BB
the Martian core formed rela-
samples
BE-N
tively early. The heterogeneity
in tungsten isotopes indicates in
Martian mantle was never fully Toluca a
homogenized. Lee et al. (1997) b
reported that the W isotope ratio c
of the Moon was about 1 epsilon
unit higher than that of terres- -6 -5 -4 -3 -2 -1 0 1 2
trial W. !W
Thus at this point, the Earth
appeared to be puzzlingly Figure 11.11. W isotope ratios measured in chondrites, the iron
anomalous among differentiated meteorite Toluca, and terrestrial materials by Kleine et al.
planetary bodies in that silicate- (2002).
metal differentiation appeared to
have occurred quite late. Subsequently, Yin et al. (2002) reported W isotope measurements carried out
in two laboratories, Harvard University and the Ecole Normale Supérieure de Lyon, which showed that
the chondrites Allende and Murchison had W isotope ratios 1.9 to 2.6 epsilon units lower than the terres-
trial standard (Figure 11.10). In the same issue of the journal Nature, Kleine et al., (2002) reported simi-
larly low εW (i.e., -2) for the carbonaceous chondrites Allende, Orgueil, Murchison, Cold Bokkeveld, Nogoya,
Murray, and Karoonda measured in a third laboratory (University of Münster). Furthermore, Kleine et
al. (2002) analyzed a variety of terrestrial materials and found they all had identical W isotopic compo-
sition (Figure 11.11). It thus appears that the original measurements of Lee and Halliday (1995) were
wrong. The measurement error most likely relates to what was at the time an entirely new kind of in-
strument, namely the multi-collector ICP-MS.
Yin et al. (2002) also analyzed separated metal and silicate fractions from two ordinary chondrites
(Dhurmsala and Dalgety Downs) that allowed them to estimate the initial 182Hf/180Hf of the solar system
as 1 × 10-4. Yin et al. (2002) considered two scenarios for the formation of the core (Figure 11.12). In the
first, which they call the two-stage model in which the Earth first accretes (stage 1) and then undergoes
core formation (stage 2), induced by the giant impact that forms the moon. In this scenario, core forma-
tion occurs 29 million years after formation of the solar system. In the second scenario that they be-
lieved more likely, metal segregates continuously from a magma ocean. In this continuous model, the
mean age of core formation is 11 million years. In contrast, they concluded that the parent body of the

129 2/23/09
 Geol. 656 Isotope Geochemistry
Lecture 11 Spring 2009
Magma ocean Two-stage model
eucrite class of achondrites 3.0 model
(suspected to be the large as-
teroid Vesta) underwent core
formation within 3 million
years of formation of the solar
system. Klein et al. (2002) 11±1 Myr 29.5±1.5 Myr
reached similar conclusions. 2.0
146
Sm-142Nd
As we have mentioned, geo-
chemists generally assume that
rare earth and other refractory !"W
elements have the same relative 1.0
concentrations in the Earth as
they have in chondrites. If so, Lee & Halliday (1995)
the Sm/Nd ratio of the Earth
should be chondritic, and by
extention the 147Sm/144Nd ratio
of the present Earth should be 0.0
chondritic and the 146Sm/144Nd
of the early Earth should have
been chondritic. Thus the
143
Nd/144Nd and 142Nd/144Nd of
the bulk earth should also be
chondritic. However, recent -1.0
studies of the 142Nd/144Nd ratio 0 10 20 30 40 50 60 70
in chondrites and terrestrial Mean time of core formation (Myr)
materials suggest that this may Figure 11.12. Models for timing of core formation in the Earth. The
not be the case, at least that figure shows how the difference between the 182W/183W between
part of the Earth accessible to the silicate Earth and chondrites, ΔεW, declines as a function of time
sampling. This is surprising to between formation of the chondrites and separation of the Earth’s
say the least. These two ele- core. Yin et al. (2002) considered two scenarios: a two-stage model
ments are very similar to each in which Earth first accretes completely and then the core forms,
other in chemical behavior, and a model in which the core segregates progressively from a
having identical configurations magma ocean as the Earth accretes. In the first scenario, the mean
of electrons in bonding orbi- age of the core is about 30 million years, in the second it is 11 mil-
tals, and are both refractory lion years. These results are sharply different from those of Lee
lithophile elements. Indeed, and Halliday (1995) who found only a small difference in εW be-
Nd and Sm have 50% conden- tween the Earth and chondrites and consequently concluded the
sation temperatures of 1602 core formed later (at about 60 million years).
and 1590 K, respectively. It is
difficult to see how processes operating in the solar nebula could have fractionated these elements sig-
nificantly. The total range of high precision Sm/Nd ratio measurements in chondrites varies by less
than 3%, which would seem to confirm that these elements were not fractionated in the solar nebula.
142
Nd is the product of α-decay of 146Sm, a nuclide with a half-life of 103 million years. As Table 11.1
shows, the initial 146Sm/144Sm ratio of the solar system about 0.008, a value deduced from 142Nd/144Nd
variations in meteorites using procedures discussed above. 144Sm is the least abundant isotope of Sm,
comprising only 3% of natural Sm, so even initially, 146Sm would have only constituted 0.025% of Sm.
Because of this and because the range of Sm/Nd ratios in nature is small, any variations in the
142
Nd/144Nd ratio should be quite small, no more than a few 10’s of ppm. Detecting such small varia-
tions is analytically challenging, and indeed was nearly impossible before about 15 years ago. Fur-

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 Geol. 656 Isotope Geochemistry
Lecture 11 Spring 2009
thermore, because the half-life of 146Sm is short, any variation in 142Nd/144Nd must be the result of frac-
tionation occurring in at most the first few hundred million years of solar system or Earth history.
However, considerable variation in the 142Nd/144Nd ratio had been detected in SNC meteorites, which
suggested early mantle differentiation on Mars. It thus seemed reasonable to look for such variations
on Earth.
Geochemists focused their initial attention on early crustal rocks from the Isua area in Greenland.
Some rocks from this area are as old
as 3.8 Ga and have initial
143
Nd/144Nd ratios several epsilon
units above the chondritic value,
suggested there were derived from
an incompatible element-depleted
mantle with high Sm/Nd. A study
by Harper and Jacobsen (1992) re-
ported a 33 ppm excess of 142Nd in
one 3.8 Ga old metavolcanic rock
from Isua. This excess was based on
a comparison between the rock and
laboratory standards; the latter was
assumed to have the same
142
Nd/144Nd ratio as chondrites.
Other workers failed to find any ex-
cesses in other rocks from Isua, so
these results were controversial.
More recent work using advanced
mass spectrometers by Caro et al.
(2003) and Boyet et al. (2003), how-
ever, has confirmed the original find-
ings of Harper and Jacobsen. This
means that these early parts of the
crust formed from a mantle reservoir
that had Sm/Nd ratios higher than
the chondritic one – and importantly,
that this reservoir formed very early,
most likely within the first 100 Ma.
A yet more surprising result came
when Boyet and Carlson (2005) ana-
lyzed the 142Nd/144Nd ratios of mete-
orites and found that terrestrial rocks
had 142Nd/144Nd ratios that average
20 ppm or 0.2 epsilon units higher
than chondrites, and most eucrites as Figure 11.13. Variation in ε142Nd in the Earth and meteorites.
well (Figure 11.13). This implies that Gray region is the range measurements of laboratory stan-
the accessible Earth has a signifi- dards derived from terrestrial Nd. All other terrestrial mate-
cantly higher Sm/Nd ratio than rials plot within this range with the exception of some sam-
chondrites. How much higher de- ples from Isua, Greenland. Chondrites have, on average,
pends on when the increase oc- ε142Nd of -0.2 relative to the terrestrial standards. Data from
curred. If the increase occurred 5 Caro et al. (2003), Boyet and Carlson (2005), Boyet and Carl-
million years after the beginning of son (2006). SNC data from the compilation of Halliday
the solar system (taken as the age of (2001).

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Lecture 11 Spring 2009
CAI’s), the Sm/Nd ratio of the accessible Earth would have to be 8% higher than chondrites; if the in-
crease occurred at 30 million years, it would have to be 10% higher. If the increase occurred later, the
Sm/Nd ratio would have to be even higher. This increase in Sm/Nd might seem small; after all, we
have already stated that the assumption that the Earth has chondritic abundances of refractory ele-
ments is probably only valid to 10%. Yet this small difference is very important in interpretation of Nd
isotope systematics. For the two scenarios above, 5 Ma and 30 Ma, the εNd of the accessible Earth would
be +8.4 and +10.1 respectively. These values fall within the range of values of mid-ocean ridge basalts.
Recalling that the Isua samples have a 30 ppm excess in 142Nd relative to a terrestrial standard∗, this
means that the Isua samples have a 50 ppm excess in 142Nd relative to chondrites.
How might the increase in Sm/Nd come about? First, we need to recall that meteorites come from
the asteroid belt and their compositions might not be representative of the composition of the inner so-
lar nebula from which the Earth and the other terrestrial planets formed. Its possible the inner solar
nebula had a higher Sm/Nd ratio. That said, it is very difficult to see why this should be so. The ob-
servable fractionation in primitive meteorites relates to volatility and lithophile/siderophile tendency.
As we have seen, Sm and Nd have quite high and very similar condensation temperatures and neither
shows a significant siderophile tendency. Although the possibility cannot be excluded, there is simply
no good reason to believe that the Sm/Nd ratio of the Earth should be different from chondrites.
If the Earth does have the same Sm/Nd ratio as chondrites, then the Sm/Nd ratio of the accessible
Earth must be higher than that of the Earth as a whole. Since neither Sm nor Nd should be present to
any significant degree in the core, this implies there is an unsampled reservoir in the mantle with a
lower than chondritic Sm/Nd ratio. Furthermore, since 146Sm has a half-life of only 103 Ma, the differ-
entiation that produced high and low Sm/Nd reservoirs must have occurred very early in Earth’s his-
tory. Fractional crystallization of a magma ocean might seem an obvious candidate for this event. In-
deed, Boyet and Carlson (2005) suggested that crystallization of the terrestrial magma ocean left a layer
of residual melt, similar to the KREEP source on the Moon. They termed this hypothetical reservoir the
early enriched reservoir (EER) and its compliment the early depleted reservoir (EDR). The EER would be
created in the upper mantle, but since it is unsampled by volcanism and tectonism, the unsampled
mantle reservoir should be in the deep mantle. Boyet and Carlson (2005) noted that if it were rich in Fe
and Ti, as is the lunar KREEP reservoir is, once crystallized the EER may have sunk into the deep man-
tle, where it remains because if its high density. So in their scenario, the EDR forms in lower mantle but
ends up becoming the part of the mantle that produced the continental crust and continues to be sam-
pled by volcanism today. In other words, the EDR comprises the accessible mantle.
The EER could be the product of fractional crystallization of a mantle that was initial entirely or
largely molten. In that case, the principal crystallizing phases would be the deep mantle minerals, the
two perovskite phases and magnesiowüstite. Judging from partition coefficients published by Corgne
et al. (2005), a cumulate layer formed of Mg-perovskite should have a Sm/Nd ratio over twice that of
chondrites, far too high to be appropriate for the accessible mantle. This could be mixed with unfrac-
tionated mantle material. However, because Sm and Nd concentrations would be low in the perovskite
cumulate, a great deal of it would be necessary: the EDR would be composed of about 75% Mg-
perovskite cumulate. This reservoir would be quite depleted in most incompatible elements, with Sm
and Nd concentrations only about 1/3 those of the BSE and would have ratios of some refractory ele-
ments that are very different from chondritic. Another possibility is that Mg- and Ca-perovskite crys-
tallized together to form the cumulate. This requires about 70-75% fractional crystallization, judging
from the partition coefficients of Corgne et al. (2005). Interestingly, because Sm and Nd partition into
Ca-perovskite, an EDR created in this way would have concentrations of many lithophile trace ele-
ments, including the REE, U, and Th, that are close to or slightly higher than BSE. However, ratios of
some elements, such as Sc/Sr and Ba/Sm, would be very different from chondritic. This problem

∗ The two standards commonly used in Nd isotope ratios measurements are the “La Jolla” standard and
the “Ames” standard. Both are solutions created from industrially purified Nd.

132 2/23/09
 Geol. 656 Isotope Geochemistry
Lecture 11 Spring 2009
seems to preclude the possibility of creating the EDR by crystallization of a magma ocean that extended
into the deep mantle.
Boyet and Carlson (2005) suggested instead that crystallization of the magma ocean involved purely
upper mantle phases. This would be the case if the magma ocean were relatively shallow and did not
extend substantially deeper than 660 km. The problem with this idea is that region above constitutes
only 25% of the mass of the mantle and it is difficult to create an enriched reservoir within it with suffi-
ciently low Sm/Nd that the remaining mantle would have Sm/Nd 10% greater than chondritic. In the
upper mantle, the phase that is likely to fractionate Sm and Nd most is majorite garnet. However, even
majorite does not seem to fractionate Sm and Nd enough to do this. Using partition coefficients pub-
lished by Corgne and Wood (2004), no extent of fractional crystallization of majorite from an upper
mantle magma ocean produces a sufficiently enriched residual melt layer to leave the rest of the mantle
with a Sm/Nd ratio that is 10% higher than chondritic.
Yet another alterative is that a primordial crust was created by partial melting of an already solidified
mantle. That crust would have been enriched in incompatible elements just as the modern crust is. The
crust may have destabilized in some way and been recycled back into the deep mantle. Under certain
circumstances, its density might be greater than that of ordinary mantle peridotite such that if forms a
stable layer in the deep mantle, perhaps in D”. Boyet and Carlson (2005) calculated that if this Early En-
riched Reservoir (EER) occupied the volume of D”, it would have to be as nearly enriched in in-
compatible elements as the present continental crust. If the EER comprises the region deeper than 1600
km, it need be only twice as enriched in incompatible elements as the bulk silicate Earth.
There are significant problems with all of the scenarios; none seems entirely satisfactory. An addi-
tional problem with them all is that there is no seismic evidence for chemical layering in the deep man-
tle. Indeed, tomographic imaging of the mantle shows seismically fast regions extending from subduc-
tion zones at the surface to the deep mantle. These regions are presumably sinking oceanic lithosphere.
Other images show mantle plumes rising from near the core-mantle boundary to the surface. Both
suggest whole mantle convection and consequently, whole mantle mixing. It is difficult to see how any
chemical layer could survive.
Recently reported results on SNC meteorites by Caro et al. (2008) have reopened the alternative pos-
sibility – namely that the Sm/Nd ratio of the Earth, and perhaps all the terrestrial planets, is not chon-

Figure 11.14. Schematic planetary isochrons for Mars, the Moon, and Vesta (the presumed source
for eucrite meteorites). Mars and the Moon intersect the terrestrial 142Nd at 147Sm/144Nd = 0.206,
while Vesta would appear to have a chondritic Sm/Nd ratio. From Caro et al. (2008).

133 2/23/09
 Geol. 656 Isotope Geochemistry
Lecture 11 Spring 2009
dritic. The found that the shergottite meteorites (the S in SNC) define a planetary isochron yielding an
age of differentiation of 40±18 Ma (after the beginning of the solar system) for the Martian mantle.
Nakhlites and the Chassigny meteorite (the NC in SNC) do not plot on the isochron; Caro et al. argued
that was because the mantle sampled by the Nakhlites was later disturbed. The isochron does not pass
through the chondritic reference value, but instead intersects the lunar isochron at ε142Nd = 0, i.e., the ter-
restrial value (Figure 11.14). Caro et al. suggest that the Earth, Moon, and Mars share a common, non-
chondritic 147Sm/144Nd of 0.206±0.05, compared to the chondritic value of 0.1966. The Sm/Nd ratio
would produce a modern 143Nd/144Nd ratio corresponding to εNd = +5. How Sm could be fractionated
from Nd in the early solar system remains problematic. Caro et al. note that while chondrites are quite
uniform in their Sm/Nd ratios, the chondrules they contain have more variable, and on average higher,
Sm/Nd ratios. The suggest Sm/Nd fractionation might somehow be related to chondrule formation
processes. Alternatively, they suggest, it could result from collisional erosion of planetary crusts.
Thus the discovery that the 142Nd/144Nd ratio of the accessible Earth is 20 ppm higher than chondrites
presents a difficult and intricate problem for geochemistry: a true conundrum. It is certainly the result
of processes that occurred very early. If it reflects fractionation is the solar nebula, then our under-
standing of nebular chemistry is weaker than we realize. If it is the product of early differentiation of
the Earth, then our understanding of both early planetary processes and the chemistry of the Earth may
be poorer than we had thought. In particular, it potentially invalidates our estimates of the composi-
tion of the Earth, and also models of its evolution.

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