Earth and Planetary Science Letters 177 (2000) 287^300

www.elsevier.com/locate/epsl

Re^Os fractionation in eclogites and blueschists and the

implications for recycling of oceanic crust into the mantle
Harry Becker *
Isotope Geochemistry Laboratory, Department of Geology, University of Maryland, College Park, MD 20742, USA

Received 28 June 1999; received in revised form 31 January 2000; accepted 12 February 2000

Abstract

Metabasalts (eclogites, blueschists and mafic granulites) metamorphosed in paleosubduction zones show a range in
rhenium (Re) abundances between 3 and 1689 parts per trillion (ppt), with a median value of 331 ppt Re. The median
Re abundance of the metabasites corresponds to only V40% of the Re abundances expected for likely mafic protoliths.
Osmium (Os) abundances in the metabasites (2^42 ppt, with one sample at 909 ppt) are comparable to abundances in
mid-ocean ridge basalt (MORB). Re was lost from the protoliths either during dehydration, the most likely explanation,
or during alteration of the protoliths near the ocean ridges. Radiogenic 187 Os/188 Os and 206 Pb/204 Pb of HIMU ocean
island basalts (OIB) that are believed to contain a component of recycled altered MORB would require excessive
amounts ( s 80^90%) of V0.5^1 Gyr old recycled altered MORB in the mantle source, if constraints on Re/Os and
U/Pb from the metabasites are applied. The necessary amount of recycled component is only marginally lower (70%) if
equal amounts of altered and unaltered 2 Gyr old MORB are present in the mantle source. Considering the major
element abundances in alkaline OIB, these estimates appear unreasonably high. One possibility is that the simple bulk
mixing models commonly employed are not applicable. Rapid melting during the formation of alkaline basalts and
sluggish kinetics may prevent complete equilibration with Os-rich phases such as sulfides and alloys. Other possible
explanations include the shielding of Os-rich phases in peridotite by silicates from reaction with partial melts of eclogite
and the isolation of melt from peridotite by means of pyroxene-rich, Os-poor reaction zones along conduit walls. In the
case of disequilibrium, the actual fraction of recycled component in OIB sources could be much lower than in
equilibrium mixing models. ß 2000 Elsevier Science B.V. All rights reserved.

Keywords: rhenium; osmium; system; eclogite; blueschist; recycling; oceanic crust; ocean-island basalts

1. Introduction crust forms an important component in the source

Rhenium^osmium (Re^Os) isotopic systematics
of ocean island basalts (OIB) provide key argu-
ments for the hypothesis that recycled oceanic
* Tel.: +1-301-405-0084; Fax: +1-301-314-9661;
E-mail: hbecker@geol.umd.edu
of mantle plume-derived melts [1^8]. 187 Os/188 Os
in most OIB and continental £ood basalts are
higher than those of abyssal peridotites, peridotite
massifs and xenoliths that are assumed to repre-
sent the slightly subchondritic to chondritic upper
mantle (187 Os/188 Os = 0.12^0.13, [9,10]). High val-
ues for 187 Os/188 Os in most OIB with low Os
abundances ( 6 30^50 parts per trillion, ppt) likely
result from high-level crustal contamination

0012-821X / 00 / $ ^ see front matter ß 2000 Elsevier Science B.V. All rights reserved.
PII: S 0 0 1 2 - 8 2 1 X ( 0 0 ) 0 0 0 5 2 - 2

EPSL 5412 4-4-00

288 H. Becker / Earth and Planetary Science Letters 177 (2000) 287^300
[3,4,11]). Nonetheless, some OIB with high Os
abundances (several hundred ppt) also have high
187
Os/188 Os. The 187 Os/188 Os (0.13^0.15) of these
lavas are di¤cult to explain by crustal contami-
nation, since contaminants such as seawater and
oceanic crust have very low Os abundances. For
this reason, and supported by complementary Pb,
Sr and Nd isotopic data, Os isotopic compositions
of OIBs with high Os abundances (e.g. Hawaii,
Austral Islands, Canary Islands) have been in-
ferred to be derived from plume sources that con-
tain up to 30^40% of recycled, altered mid-ocean
ridge basalt (MORB) or recycled MORB plus
sediment [1^8]. Os is strongly retained in the res-
idue during mantle melting while Re is moder-
ately enriched in melts (e.g. [12]), resulting in
high Re/Os in most crustal materials. Because
MORB and sul¢de-rich metaliferous sediments
have relatively high Re and low Os abundances
[13,14], these rocks acquire very high 187 Os/188 Os
in several hundreds Myr. Lithophile radiogenic
isotope tracers in OIB, such as Sr, Nd and Pb
isotopic compositions, are predominantly derived
from recycled components in the mantle, and
hence, are not very sensitive indicators of the
mass fraction of these components in the mantle.
The compatible nature of Os makes 187 Os/188 Os a
more sensitive indicator for the proportion of re-
cycled crust [1,2]. Because Os contents in MORB
are very low [12,13,15], the 187 Os/188 Os of hybrid
mixtures of recycled crust and mantle depends
essentially on the Re content of recycled crust
and the age of the recycled component [1]. In
addition, the very low Os abundances in
MORB, yet relatively high Os abundances of
some radiogenic alkaline OIB, require speci¢c
proportions of recycled crust in the mantle sour-
ces if independent age constraints are available
(e.g. from Pb isotopic data, [2]).
It is commonly assumed that typical Re abun-
dances in MORB and pelagic sediments can be
used to constrain the evolution of 187 Os/188 Os in
subducted oceanic crust, with age estimates for
the latter provided by 206 Pb^207 Pb model ages
[2]. However, evidence for suprachondritic 187 Os/
188
Os in arc peridotites indicates the mobilization
of Os during subduction of oceanic crust [16].
Variable Re enrichment in some arc harzburgites
EPSL 5412 4-4-00
[16] may indicate that Re in subducted basalts
and sediments may also be mobilized, however,
the evidence for this is insu¤cient. Substantial
loss of Re from subducted oceanic crust would
signi¢cantly alter the e¡ect of addition of recycled
oceanic crust to plume sources and consequently
increase the amounts of recycled crust or time
necessary to generate high 187 Os/188 Os in OIBs.
In the present study, Re and Os abundances of
eclogites, blueschists and ma¢c high-pressure
granulites from high-pressure metamorphic belts
(paleosubduction zones) were determined to as-
sess possible losses of these elements relative to
likely protolith compositions. The types of rocks
analyzed represent the closest proxies available to
study element fractionation in subducted oceanic
crust, and yield an integrated record of sub-sea-
£oor alteration and metamorphic dehydration in
subduction zones.
2. Samples and analytical techniques
Most of the eclogites and blueschists analyzed
in this study represent metamorphosed basalts
that are remnants of subducted slabs and are
now exposed, along with metasediments, in
high-pressure/low-temperature metamorphic belts
[17]. One sample (A43) probably represents a for-
mer gabbro, as is indicated by its relatively Ca^
Al-rich composition and the trace element compo-
sitions [17]. The samples (Table 1) are from the
Zermatt^Saas ophiolite zone in the western Alps
(LC4A, LC4B, LC5, CEV11B, TAA6A, age of
metamorphism ca. 35^40 Ma, [18]), Adula nappe
in the central Alps (AA15, age of metamorphism
35^40 Ma, [19]), Mu«nchberg gneiss massif, Ger-
many (W1, AGR13, age of metamorphism 380^
400 Ma, [20]), Syros, Greece (BSY88, BSY87, age
of metamorphism V70 Ma, M. Broecker, person-
al communication, 1999), northern Bohemian
massif (DIET1, DIET3, age of metamorphism
ca. 340 Ma, [21]), Corsica (SAC10, age of meta-
morphism likely Alpine, 40^120 Ma?) and Nor-
way (A43, age of metamorphism presumably
500 Ma, [22]). More details can be found in
[17]. The ma¢c samples show compositional and
textural evidence for multistage histories including
 H. Becker / Earth and Planetary Science Letters 177 (2000) 287^300 289

Table 1
Re^Os data for eclogites, blueschists and ma¢c granulites
187
Sample Re Re Re blank Os Os Os blank Re/188 Osc 187
Os/188 Osc
(ppt)a (pg)b (%) (ppt)a (pg)b (%)
ORT4 Eclogite 665 1995 0.8 5.42 16 5.8 1805 þ 103 15.9 þ 0.9
W1 Eclogite 141 436 3.4 2.12 6.4 13.6 517 þ 42 4.91 þ 0.38
Dupl. 23 86 17.5 0.96 2.9 34.2 350 þ 189 15.2 þ 7.8
Dupl.d 38 107 11.2 1.32 3.3 31.3 293 þ 94 8.62 þ 2.7
AGR13 Eclogite 3.0 24 62.3 1.92 5.7 20.7 10.1 þ 13.5 2.67 þ 0.31
AA15 Eclogite 48 156 9.6 5.56 17 15.4 46.8 þ 5.1 1.16 þ 0.08
Dupl.d 49 140 8.6 3.99 10 22.4 76.3 þ 9.8 2.30 þ 0.28
CEV11B Eclogite 1108 3510 0.4 29.4 93 1.6 218 þ 2 1.66 þ 0.01
LC4A Eclogite 230 713 2.1 10.2 31 4.6 121 þ 3 0.964 þ 0.018
LC4B Eclogite 331 1068 1.4 11.4 36 4.0 154 þ 3 0.887 þ 0.014
Dupl. 282 885 1.7 11.7 36 4.0 129 þ 3 0.945 þ 0.015
Dupl.d 458 1157 1.0
LC5 Eclogite 1689 4985 0.3 28.9 85 1.7 304 þ 2 0.747 þ 0.005
A43 Eclogite 44 154 9.7 5.58 18 7.9 99 þ 11 12.3 þ 0.9
DIET1 Maf. Gran. 866 2603 0.6 4.56 14 9.9 2661 þ 282 14.8 þ 1.6
DIET3 Maf. Gran. 795 2567 0.6 5.41 17 7.9 1527 þ 95 8.99 þ 0.56
SAC10 Blueschist 757 2409 0.6 6.51 21 6.8 736 þ 24 2.53 þ 0.08
BSY88 Blueschist 331 1031 1.5 41.7 128 1.2 38.5 þ 0.5 0.1720 þ 0.001
BSY87 Blueschist 125 388 3.9 909 2717 0.06 0.661 þ 0.021 0.1279 þ 0.0005
TAA6A Blueschist 2.5 23 65.3 2.48 7.8 16.0 4.98 þ 0.32 0.277 þ 0.02
Dupl. 2.7 23 64.9 2.03 6.1 19.8 6.65 þ 0.56 0.397 þ 0.04
Dupl., duplicate; Maf., ma¢c; Fels., felsic; Gran., granulite.
a
Blank-corrected.
b
Including blank.
c 187
Errors were propagated from the uncertainties on the blank correction. In a few cases, errors on Os/188 Os are determined by
external mass spectrometric precisions.
d
Predigested in HF^HCl^ethanol.

variable ocean £oor alteration, dehydration, but
very limited retrograde metamorphic overprint
(e.g. formation of low-pressure amphiboles, [17]).
Finely-ground powders of samples (2^3 g) were
digested and equilibrated with dilute 185 Re and
190
Os spikes in reverse aqua regia (5 ml 14 M
HNO3 +2.5 ml 11 M HCl) for 2 days at 240³C
in sealed Carius tubes. Os was puri¢ed by solvent
extraction into CCl4 and back-extraction into 9 M
HBr, with a subsequent clean-up by micro distil-
lation. The Re fraction was separated in a two-
step column chemistry using 100^200 mesh AG1-
X8 anion exchange resin and HCl^HNO3 . Three
duplicates (see Table 1) were predigested together
with spike solutions in a mixture of 24 M HF, 11
M HCl and ethanol in te£on bombs at 90³C for
12 h to rule out analytical problems, such as the
incomplete decomposition of silicates. After evap-
oration, the procedure was repeated in HCl^etha-
nol at 100³C. After slow evaporation, the residues
are transferred into Carius tubes and treated like
the rest of the samples. Os was loaded on Pure-
tech1 or ESPI1 Pt ¢laments and covered with a
mixture of Ba(OH)2 and NaOH. Re was loaded
on fused Pt ¢laments with Ba(NO3 )2 . Os and Re
were run as OsO3 3
3 and ReO4 on the 12-inch, 68³
sector thermal ionization mass spectrometer at
the Isotope Geochemistry Laboratory (University
of Maryland) in pulse counting mode on the
electron multiplier. Some of the Re fractions
were run using a Faraday cup detector. Multiple
runs of 0.5^1 ng Os in the Johnson^Mattey
Os standard solution used at IGL yielded
187
Os/188 Os = 0.1140 þ 8 (2c, RSD = 0.7%, n = 19)
and 187 Os/188 Os = 0.1144 þ 6 (2c, RSD = 0.5%,
n = 11) for two di¡erent run periods. The external
precision for the standard re£ects the external
precision of 187 Os/188 Os for the samples only in

EPSL 5412 4-4-00

290 H. Becker / Earth and Planetary Science Letters 177 (2000) 287^300
the few cases where the blank contribution on
187
Os/188 Os is insigni¢cant (Table 1). Total analyt-
ical blanks were 15 þ 12 pg Re (12 þ 5 pg for sam-
ples with HF predigestion, processed in fall 1998),
and 1.5 þ 0.5 pg for Os (1.0 þ 0.3 pg for ORT4
and one of the W1 samples processed in fall
1997, and 3 þ 1 pg for samples with HF prediges-
tion processed in fall 1998). 187 Os/188 Os of the
blank was 0.175 þ 0.005. Abundances and isotopic
ratios in Table 1 were corrected for blank contri-
bution.
3. Results
Os behaves as a compatible element during
melting and fractionation in the mantle (e.g.
[12]) and consequently, it is advantageous to com-
pare it with other compatible elements, such as
Ni, that show predominantly lithophile character-
istics in the crust and mantle (Fig. 1). Os abun-
dances in the metabasites range between 1 and
42 ppt (except for sample BSY87, see below).
The median Os abundance in the metabasites is
6 ppt (n = 15) or 4.9 ppt for `common' Os (the
non-radiogenic Os component), little di¡erent
from the median of 4.2 ppt reported for modern
MORB (n = 40, [12,13,15]). Consequently, most of
Fig. 1. Ni^Os variation diagram. Shown are abundances in
MORB (+, [12,13]) and OIB (X, [2,23,11,34]). To facilitate
comparisons, the Os abundance data for metabasites were re-
calculated using a chondritic 187 Os/188 Os, because most of
the samples contain a large fraction of radiogenic Os. Nickel
data for metabasites from [17]. Symbols: F, metabasaltic
eclogites and blueschists; E, metagabbroic eclogites; O, low-
temperature blueschist (not Ca-depleted); R, Na-rich, Ca-de-
pleted blueschists; 8, ma¢c high-pressure granulites. For de-
tails on samples, see text and [17].
EPSL 5412 4-4-00
Fig. 2. Y^Re variation diagram. Symbols as in Fig. 1. Note
the di¡erent scales for Y and Re axes. Both elements are
mildly incompatible and correlate well in MORB (e.g.
[12,23]). Most of the Re data in this diagram are from [13].
Values for Y were calculated from the Tb data in [13], using
Tb/Y = 0.025 for average N-MORB [53]. Yttrium data for
metabasites from [17]. Many high-P rocks have Y abundan-
ces comparable to MORB, but signi¢cantly lower Re, indi-
cating substantial loss of the latter.
the data lie within the MORB ¢eld in the Ni^Os
diagram (Fig. 1). Re is mildly incompatible during
mantle melting [12,23] and shows good correla-
tions with other mildly incompatible elements,
such as Y (Fig. 2). Most eclogites and blueschists
(3^1689 ppt) have much lower Re abundances
than MORBs, but comparable Y abundances (Y
data from [17]). The metabasalts yield a median
Re of 331 ppt, 62% lower than the median of
MORB (860 ppt, n = 37, [12,13]). Only two ma¢c
granulites and two eclogites overlap with the
MORB ¢eld (Fig. 1b). Two very Na-rich and
Ca-depleted blueschists (TAA6A and BSY87)
that presumably underwent intense high-temper-
ature hydrothermal sub-sea£oor alteration [17]
show variable Re depletion. In sample TAA6A,
Re and Y may be depleted as a result of this
process. Part of the Ca (presumably also Y) lost
from this sample was deposited nearby, and is
preserved as epidote^clinozoisite-rich pockets.
These pockets also contain sul¢des and it is pos-
sible that the sul¢des contain some of the missing
Re. The other blueschist sample (BSY87) has high
Os, Cr and Ni abundances, and a mantle-like
187
Os/188 Os, suggesting that the low Re abun-
dance in this sample re£ects the depleted nature
of the protolith (either a cumulate or a MgO-rich
melt).
 H. Becker / Earth and Planetary Science Letters 177 (2000) 287^300 291

The results for Re and Os abundances on du-

plicates processed including predigestion in HF^
HCl^ethanol are comparable to results obtained
without predigestion, indicating either that Re in
the silicates is released during both digestion pro-
cedures, or that the silicates contain minor
amounts of Re only. The agreement between du-
plicates of the same sample varies between poor
(samples W1, LC4B) and good (AA15, TAA6A),
most likely re£ecting the heterogeneous distribu-
tion of sul¢des in these medium-grained rocks.
Rutile, a common trace mineral in eclogites, is
not or only partially dissolved by these digestion
procedures. Rutile may accommodate some Re in
its structure if Re has the proper valence (Re4‡ ).
However, it is unlikely that Re in rutile can bal-
ance the low Re abundances in samples AGR13,
AA15 or TAA6A (Table 1), because this would
require 3^6 orders of magnitude higher Re con-
tents in rutile, compared with the amounts of Re
analyzed.
Because of the high Re/Os of most of the meta-
basites relative to Re/Os of the mantle, the meta-
basites have developed high to very high 187 Os/
188
Os (up to 16, Table 1, Fig. 3). Only one sample
has high Os abundances (909 ppt, blueschist
BSY87) and an `upper mantle'-like present-day Fig. 3. (a) Re^Os isochron diagram. Symbols as in Fig. 1.
187 Error bars are shown or are smaller than symbol size. Errors
Os/188 Os (0.1279). Some metabasites, for which
include propagated uncertainties from blank corrections. Iso-
the blank correction on Os and Re was very large, chrons depict the evolution of 40, 200, 500 and 1000 Myr
have 187 Re/188 Os that are too low for their 187 Os/ old rocks evolving from upper mantle-like 187 Os/188 Os (0.13).
188
Os compared to other metabasalts (Fig. 3). (b) Expanded isochron diagram showing samples at low
187
This is particularly the case for two duplicates Re/188 Os.
of sample W1 that contain very little Os and re-
quired a large blank correction (Table 1). The roughly consistent with the ages of metamorphism
aliquot of this sample that yielded the highest and the assumption that igneous formation did
Os content lies close to the 500 Myr isochron, not precede metamorphism by more than 50^
suggesting that the two duplicates that plot to 100 Myr (Fig. 3). In Fig. 4, a model for the Os
the left of the isochron were overcorrected for isotopic evolution of a metabasite is shown with a
their Os or Re blank. Two other samples (AA15 protolith age of 480 Myr and metamorphism and
and A43) show a similar behavior, but possibly concurrent decrease in Re/Os at 400 Myr. Several
for di¡erent reasons as will be discussed further aspects of Re^Os behavior in altered basalts
below. should be noted. The decrease in Re/Os will re-
tard the increase of 187 Os/188 Os compared to the
unmetamorphosed protolith. Thus, if the proto-
4. Impact of alteration on Re^Os model ages and lith age is known, calculated initial 187 Os/188 Os
calculated initial 187 Os/188 Os will be higher (point B in Fig. 4) than the actual
initial 187 Os/188 Os (point A in Fig. 4). Conversely,
187
Most blank-corrected Os/188 Os values are if the protolith age is unknown, a Re^Os model

EPSL 5412 4-4-00

292 H. Becker / Earth and Planetary Science Letters 177 (2000) 287^300
Fig. 4. Os isotope evolution diagram showing the evolution
of 187 Os/188 Os (bold lines) in a hypothetical example of a
Phanerozoic basalt crystallized at 480 Ma and metamor-
phosed at 400 Ma with concurrent decrease of Re/Os. The
Re^Os model age of this sample would be too old. If the
age of the protolith is known from independent constraints,
the calculated initial 187 Os/188 Os at the time of protolith for-
mation would be too high. With increasing time, intervals
between protolith formation and metamorphism di¡erences
between real and calculated protolith ages and initial ratios
become much more pronounced, particularly if metamor-
phism occurred recently.
age at the intersection with the evolution of aver-
age chondrites will yield an age that is older than
the true age of the protolith (Fig. 4). These e¡ects
are increasingly ampli¢ed as the metamorphism
approaches the present. Large time di¡erences be-
tween protolith formation and metamorphism are
the likely explanation for some samples showing
high 187 Os/188 Os and low Re/Os (Fig. 3). For ex-
ample, two separate analyses of eclogite AA15
show reproducibly low Re/Os that correlate with
relatively high 187 Os/188 Os (Table 1). Given the
young age of metamorphism for this sample
(35^40 Myr), the high 187 Os/188 Os was likely ac-
quired before metamorphism and loss of Re. The
relatively high 187 Os/188 Os would require a longer
time span between formation of the igneous pro-
tolith (Variscan?) and metamorphism. The eclo-
gite sample from Norway (A43) underwent eclo-
gite facies metamorphism about 400^500 Myr ago
([22] and references therein). This sample also has
a very high 187 Os/188 Os (12.3, Table 1) for its Re/
Os, indicating that most of the radiogenic Os
EPSL 5412 4-4-00
grew before the metamorphism. The evolution
of 187 Os/188 Os in this sample can be modeled by
rapid increase in a 1200 Ma old mantle-derived
ma¢c protolith with 187 Re/188 Os of 1000 and
metamorphism, and Re loss at 500 Ma, with sub-
sequently retarded increase in 187 Os/188 Os. This
interpretation is consistent with the Svecokareli-
an^Grenville age of other eclogite protoliths in
Scandinavia [24] and suggests that the protolith
of A43 may have been a gabbro that intruded
into continental crust or accreted Proterozoic oce-
anic crust.
5. Re and Os loss in high-pressure metabasites
It is di¤cult to evaluate whether Os was lost or
gained in the metabasites because there is only a
weak correlation between the compatible elements
Os and Ni in MORB. In contrast, the low Re
abundances in most of the eclogites and blue-
schists relative to MORB suggest that substantial
amounts of Re were lost either during ocean £oor
alteration or as a result of dehydration. The e¡ect
of low- and high-temperature alteration at ocean
ridges on Re and Os abundances in MORB is
poorly constrained. Data on pyrite-rich hydro-
thermal deposits from the TAG hydrothermal
¢eld suggest that near the surface, Re may be
mobile under oxidizing conditions, but generally
immobile under reducing conditions deeper in the
mineralized zones [14]. It is also unknown
whether low-temperature weathering of MORB
results in the mobilization of Re. It is conceivable
that Re loss occurs during dehydration of altered
metabasalts in subduction zones because low-
pressure experiments at 500³C show a strong in-
crease in the solubility of ReO2 in hydrothermal
solutions with increasing chloride concentration
of the £uid [25]. Speciation and solubilities of
the PGE and Re in complex supercritical £uids
at high pressures ( s 1^2 GPa) are virtually un-
known. However, some observations provide cir-
cumstantial evidence that at least some removal
of Re and Os from altered oceanic metabasalt
occurs during dehydration in subduction zones.
First, variable Re enrichment in some depleted
arc harzburgites that also show suprachondritic
 H. Becker / Earth and Planetary Science Letters 177 (2000) 287^300
187
Os/188 Os [16] suggests that Re may be trans-
ported from the subducted slab into the subarc
mantle. Second, blueschists and eclogites often
contain sul¢des as a trace phase. These sul¢des
are likely inherited from the igneous protolith or
from previous alteration at low temperatures. The
high sul¢de^silicate partition coe¤cient for Re
(values between 43 and 1200 have been reported
[26,27]) indicates that as long as sul¢des are stable
in eclogites and blueschists, the Re budget of the
bulk rocks will be dominated by sul¢des. Sul¢de-
bearing silicate veins that formed during dehydra-
tion at high pressures were reported from eclo-
gites [28] and are evidence that sul¢des can be
mobilized in hydrous subduction zone £uids.
The heterogeneous distribution of Re and Os in
subducted altered metabasalts (Table 1) makes it
di¤cult to constrain the depletion of these ele-
ments precisely for the purpose of a general mod-
el. Some eclogites and the blueschists still contain
hydrous minerals, hence, the possibility exists that
more Re and Os could be lost upon further dehy-
dration. Because of the large variability of the
abundance data, the median abundances of the
metabasites (see Section 3) will be used to charac-
terize the subducted altered MORB reservoir. The
median values for Re (331 ppt) and Os (6 ppt)
yield a 187 Re/188 Os of 325 for subducted altered
metabasalt, signi¢cantly lower than the value for
MORB (V1000).
6. Os^Pb isotopic constraints on recycled altered
MORB in HIMU-type OIBs
The new data presented here warrant a re-eval-
uation of Os isotopic constraints on the presence
of recycled MORB in OIBs. On the basis of trace
element and Pb isotopic systematics, HIMU-type
OIBs (e.g. Tubuai, Mangaia, St. Helena, Canary
islands, Cape Verde islands) have been interpreted
to contain a distinctive signal of recycled altered
MORB (e.g. [29,30]). The discussion here will fo-
cus on HIMU OIB, because other OIBs contain
additional recycled sediment components [6,7]
that may complicate a quantitative assessment
of recycling models. In order to obtain estimates
for the proportion of recycled altered MORB in
EPSL 5412 4-4-00
293
Fig. 5. 187 Os/188 Os^206 Pb/204 Pb diagram showing OIB data
¢ltered for Os abundances v50 ppt. Ma, Mangaia; Tu, Tu-
buai; Ru, Rurutu; Ta, Tahaii; Sav, Savaii; Ra, Raratonga
[2]; Can, Canary islands [4,8]; Az, Azores [11]; Ha, various
Hawaiian volcanoes [6,7,33,34]. OIB endmember composi-
tions from [2,6,54]. UM, upper mantle (e.g. [9,10]); EPM, en-
riched plume mantle [11,31]. OIBs with high 187 Os/188 Os and
206
Pb/204 Pb are believed to be derived from a source contain-
ing recycled MORB (e.g. [2]). The low 206 Pb/204 Pb in some
Hawaiian lavas may re£ect old pelagic sediment in a recycled
component [6,7].
OIB sources, previous isotopic evolution models
used age constraints derived from Pb isotopic re-
lations and assumptions on the likely Re and Os
contents of recycled altered MORB [1^8]. From
these models, it was concluded that the mantle
sources of OIB that show the most extreme
HIMU signature (e.g. Mangaia, Tubuai, St. Hel-
ena) may contain between 20 and 30% of recycled
MORB, with a model-dependent age of ca. 2 Gyr
[2]. The 2 Gyr age constraint is based on the as-
sumption that the 206 Pb^207 Pb isotopic correla-
tions de¢ned by OIB have age signi¢cance (e.g.
[29]). Some OIBs that show less radiogenic Pb
isotopic compositions (e.g. Canary islands), but
187
Os/188 Os that are as high as those of extreme
HIMU lavas, have been interpreted to contain
either old recycled MORB with lower 238 U/204 Pb
(W) or younger recycled MORB in their sources
[4,8]. Distributions of Os and Pb isotopic data for
ocean islands that show a dominant HIMU sig-
nature require at least one or two additional
components to explain their compositions
(Fig. 5). Besides the HIMU component, a compo-
nent that may be either upper mantle or `enriched
plume mantle' (EPM, putative lower mantle with
somewhat higher 206 Pb/204 Pb and 187 Os/188 Os than
294 H. Becker / Earth and Planetary Science Letters 177 (2000) 287^300

the upper mantle, e.g. [11,31,32]) is present in the

HIMU OIB source (Fig. 5).
It has been noted previously (e.g. [6,33]) that
certain OIB suites tend to de¢ne straight correla-
tions between 187 Os/188 Os and other radiogenic
tracers (Pb, He, Sr, Nd). Because Os behaves as
a compatible element in the mantle, the linear
correlations with incompatible isotopic tracers im-
ply that equilibrium interactions between Os-de-
pleted partial melts and high-Os mantle peridotite
must be severely restricted, otherwise a decou-
pling of these tracers should be observed
[2,6,34]. Consequently, it has been proposed that
correlations of 187 Os/188 Os with other radiogenic
tracers predominantly re£ect the mixing of mag-
mas derived from isotopically distinct mantle
[2,6,34]. Most data for uncontaminated HIMU
OIB from individual islands or groups of islands
seem to form clusters in this diagram (Fig. 5).
6.1. Standard models with new data
The 187 Os/188 Os^206 Pb/204 Pb diagram in Fig. 6
shows the evolution of recycled altered MORB
and unaltered MORB for variable ages. Present-
day compositions for 350, 700, 1200 and 2000
Myr old recycled altered MORB were obtained
from evolution models using the median Re and
Os abundances from the present study and a
model W value of 37, derived from the high-pres-
sure rocks ([17], for details see Fig. 6). Initial iso-
topic compositions were based on simple evolu-
tion models for the upper mantle (see caption of
Fig. 6) and the evolution for the ¢rst 50 Myr was
calculated using 187 Re/188 Os (1000) assumed to be
typical for altered MORB (the e¡ect of a some-
what higher W is negligible). Evolution during the
remaining time was calculated using 187 Re/
188
Os = 325 and W = 37 for subducted altered
MORB. For unaltered MORB, it was assumed
that no dehydration occurs during subduction,
since the low water contents of unaltered
MORB may be accommodated in nominally an-
hydrous phases (see [17]). Re, Os, U and Pb abun-
dances of average fresh MORB were used for un-
altered MORB (see caption of Fig. 6). Mixing
lines between depleted upper mantle or EPM
and recycled altered MORB are strongly curved
Fig. 6. Evolution of 300, 700, 1200 and 2000 Myr old sub-
ducted MORB in a 187 Os/188 Os^206 Pb/204 Pb diagram. Note
logarithmic 187 Os/188 Os axis. (a) Evolution model for altered
MORB (indicated by long arrow) calculated assuming chon-
dritic 187 Os/188 Osi , radiogenic growth for 50 Ma and 187 Re/
188
Os = 1000, and retarded growth and 187 Re/188 Os = 325 for
the rest of the time (300, 650, 1150 and 1950 Myr). 206 Pb/
204
Pbi calculated assuming a single-stage evolution model
and 238 U/204 Pb = 11. Pb isotopic evolution after metamor-
phism calculated using 238 U/204 Pb = 37, derived from eclogites
[17]. Strongly curved thin lines are mixing lines between
modern upper mantle peridotite (3300 ppt Os, 187 Os/
188
Os = 0.130, 20 ppb Pb, 206 Pb/204 Pb = 18.3) and subducted
altered MORB (6 ppt Os, 196 ppt Pb, [17]). The ¢eld for
HIMU OIB is shown as a bold bar. (b) Model for 350^2000
Myr old unaltered MORB (187 Re/188 Os = 1000, 238 U/204 Pb
= 11 [35,53], 187 Os/188 Osi and 206 Pb/204 Pbi ) calculated the
same way as in (a). Also shown is a mixing line between
2000 Myr old unaltered and altered MORB (from (a)). Thick
marks represent 20% increments. A mixture of 60% altered
and 40% unaltered 2 Gyr old MORB would develop 206 Pb/
204
Pb comparable to the most extreme HIMU OIB (Fig. 5).
because of the very di¡erent Os/Pb in these end-
members (Figs. 6, 7). This e¡ect is largely caused
by the very di¡erent Os concentrations.
For a W value of 37, the 206 Pb/204 Pb of HIMU
OIB sources suggests ages between 0.5 and V1
Gyr, if the recycled component in these lavas is
indeed subducted altered MORB (Figs. 6a, 7a).
The extreme HIMU samples from Mangaia
(Fig. 5) require melting of a mixture of ca. 80%
V1 Gyr old recycled altered MORB and 20%
peridotite, if complete equilibration between par-

EPSL 5412 4-4-00

 H. Becker / Earth and Planetary Science Letters 177 (2000) 287^300
Fig. 7. (a) Expanded view of Fig. 6 at low 187 Os/188 Os.
EPM, UM and OIB data ¢elds from Fig. 5. Shown are mix-
ing lines between 350, 700, 1200 and 2000 Myr old altered
MORB and peridotite (see Fig. 6a), and mixing relationships
between hybrid 2000 Myr old MORB (60% altered, 40% un-
altered) and peridotite (from Fig. 6b). Thick marks indicate
20% intervals of the fraction of recycled altered MORB in a
mixture of eclogite and peridotite. This model assumes that
partial melting results in complete equilibration of melt with
both eclogite and peridotite. If the assumptions of the model
are correct, very high percentages (80^90%) of relatively
young ( 6 1000 Myr) recycled altered MORB are required to
explain HIMU OIB compositions (see text). If HIMU OIB
sources contain mixtures of recycled altered and unaltered
MORB, ages of recycled components may be signi¢cantly
older, but large amounts of recycled MORB are still indi-
cated. (b) Disequilibrium between partial melt of recycled al-
tered MORB eclogite and peridotite. Endmember composi-
tions are the same as in (a) except that the melt reacts only
with a fraction (300 ppt) of the Os in peridotite. Disequilib-
rium may result from e¡ective shielding of Os-bearing phases
(sul¢des, alloys) by silicate or oxide host phases that do not
react with melt because of compositional and/or kinetic ef-
fects (see text).
tial melt of eclogite and peridotite occurred (Fig.
7a). Some basalts from the Canary islands would
require more than 90% of V500 Ma old altered
MORB in their source to explain their high 187 Os/
188
Os in these simple mixing models (Figs. 5, 6a,
7a). Signi¢cantly lower estimates for the amount
of recycled crust in HIMU OIB sources were ob-
tained in previous studies, resulting from the as-
sumption of older ages of the recycled component
EPSL 5412 4-4-00
295
and high estimates of average Re abundances in
recycled altered MORB. The new metabasite data
(Table 1) and the Re data on MORB now avail-
able [12,13,15] show that many earlier estimates
of Re abundances in recycled MORB were too
high. The present results are most similar to the
770 Ma, 500 ppt Re endmember model for HIMU
basalts discussed by Hauri and Hart [2]. Even if
the average age of recycled altered MORB in OIB
sources would be 2000 Myr, this still requires 60^
70% of recycled component.
A possible way to relax the age constraints im-
posed by the high W and 206 Pb/204 Pb of recycled
altered MORB could be that HIMU OIB sources
contain mixtures of recycled altered and unaltered
MORB. It is conceivable that unaltered MORB
does not lose any water (and hence Pb and Re) in
subduction zones [17]. Consequently, subducted
unaltered MORB would develop relatively unra-
diogenic Pb isotopic compositions, but highly ra-
diogenic 187 Os/188 Os (Fig. 6b). If the sources of
HIMU OIB contain both altered and unaltered
recycled MORB, the age of the recycled material
is more di¤cult to evaluate, because such a hybrid
likely has a lower W than recycled altered MORB
(most commonly, values for W in fresh MORB
range between 8 and 13, [35]). Figs. 6b and 7a
show an example that assumes that the source
of HIMU OIB with the most radiogenic 206 Pb/
204
Pb contains altered and unaltered 2 Gyr old
recycled MORB. For a 206 Pb/204 Pb of 21.7, a val-
ue found in extreme HIMU lavas from Mangaia,
and the parameters in the caption of Figs. 6b and
7a, the proportion of altered to unaltered MORB
is 60:40% if the crust is 2 Gyr old. The Re con-
centration of such a mixture is 543 ppt, and the
present-day 187 Os/188 Os is 16.9. In this model, the
proportion of recycled crust in the source of
HIMU OIB has to be at least 70% to explain
the radiogenic 187 Os/188 Os of basalts from Man-
gaia and Tubuai (Fig. 7a). This example illus-
trates that even the presence of recycled unaltered
MORB does not su¤ciently ease the requirement
of large amounts of these materials in HIMU OIB
sources.
The high proportion of recycled altered MORB
required in the bulk mixing models in Figs. 6 and
7a poses a problem that is not easily resolved.
296 H. Becker / Earth and Planetary Science Letters 177 (2000) 287^300
Major element compositions of HIMU basalts
suggest that such high proportions of recycled
MORB in HIMU sources are unlikely. For in-
stance, MgO contents of 15^20 wt% and low
SiO2 (43^45 wt%) in some Tubuai and Mangaia
samples [23,30] are inconsistent with partial melt-
ing of a mixture of 80% MORB eclogite with 20%
peridotite. Melting modes of such a composition
will contain high proportions of clinopyroxene
and garnet (e.g. [36], and references therein) and
one might expect silica-rich rather than silica-poor
melt compositions (trondhjemitic^tonalitic
liquids, e.g. [37]). Abundances of highly incom-
patible elements such as Nb and Th are enriched
by a factor of 10^40 in HIMU OIB relative to
MORB. These enrichments have been attributed
to low degrees of partial melting of a peridotitic
mantle source [38]. If the mantle source of HIMU
OIB is dominated by eclogite, then for 60 parts
per million (ppm) Nb in alkaline OIB, and 3 ppm
Nb in a MORB eclogite source, 5% melting of
eclogite would be required to explain the trace
element enrichment in the lavas. Such low degrees
of partial melting of a clinopyroxene^garnet-rich
source should yield silica-rich melts [37] that are
not observed. On the contrary, HIMU-type OIB
are silica-undersaturated. In the past, this has
been attributed to the e¡ects of the decrease of
the stability ¢eld of olivine during melting of peri-
dotite at high pressures and in the presence of
CO2 (e.g. [39]). The behavior of hybrid clinopyr-
oxene- and garnet-rich mantle during melting in
the presence of C^H^O species is not well known.
Experiments on ma¢c compositions suggest [40]
that melting of eclogite-enriched hybrid mantle
that contains minor amounts of carbonate should
produce melts enriched in SiO2 .
These considerations suggest that the Re^Os
bulk mixing models of recycled oceanic crust
with peridotite yield results that are di¤cult to
reconcile with other evidence. Possible explana-
tions for this are : (1) the endmember in HIMU
OIB that contains radiogenic 187 Os/188 Os and
206
Pb/204 Pb may not be recycled MORB, or (2)
partial melting of mixed lithologies of eclogite (re-
cycled crust) and peridotite may either be a dis-
equilibrium process or may result in unexpected
partitioning e¡ects during melting and reaction
EPSL 5412 4-4-00
causing bulk mixing scenarios to be inappropri-
ate. These alternatives will be discussed in the
next two sections.
6.2. Radiogenic 187 Os/188 Os of HIMU OIB may
not re£ect a contribution from recycled altered
MORB
Previous studies of lithophile trace element (e.g.
Ce/Pb and Nb/U) and isotopic compositions of
HIMU lavas provide strong arguments for the
presence of recycled altered MORB in the source
of these lavas (e.g. [30]). One possibility is that the
budget of lithophile tracers in HIMU OIB is do-
minated by the recycled component while the ra-
diogenic Os isotopic composition re£ects the pres-
ence of a component with su¤ciently high Os
abundances that is not recycled MORB. Signi¢-
cant amounts of recycled pelagic sediment in
HIMU OIB are commonly ruled out as sources
of the radiogenic Os because it would dominate
the Pb budget and impose a low W, high Th/U
signal on HIMU OIB [41]. However, as for al-
tered MORB, it is likely that dehydration in sub-
duction zones will dramatically change the par-
ent^daughter ratios of lithophile isotopic
systems. The extent of this modi¢cation is un-
known. Even if the lithophile isotopic systematics
of HIMU OIB can be accommodated with old
recycled sediments, it is uncertain whether the
moderate Os abundances and relatively low Re/
Os in pelagic sediments [42] are su¤cient to ac-
count for the radiogenic Os and mixing relations
in HIMU OIB.
Walker et al. [43,44] proposed that radiogenic
187
Os in some plume-derived basalts could re£ect
contributions from either the outer core or from
the lower mantle. Elevated 186 Os/188 Os (the rele-
vant isotopic ratio for the 190 Pt^186 Os decay sys-
tem) in some OIB from Hawaii may indicate a
contribution from the outer core [32]. However,
the models for a contribution from the outer core
yield only slightly suprachondritic 187 Os/188 Os
(V0.132^0.137). These values are di¤cult to rec-
oncile with radiogenic 187 Os/188 Os of HIMU OIB
of up to 0.15. In principle, a strati¢ed mantle with
high Re/Os in the lower mantle as proposed by
Walker et al. [44] could also explain the radiogen-
 H. Becker / Earth and Planetary Science Letters 177 (2000) 287^300
ic 187 Os/188 Os of HIMU OIB. However, at
present, no direct evidence is available that the
lower mantle has a higher Re/Os than the upper
mantle.
Metasomatism of lithospheric mantle by small-
degree (e.g. carbonatitic) melts was proposed as
an alternative explanation for the high 206 Pb/204 Pb
of some HIMU basalts. Metasomatism could im-
part a high-U/Pb signal on lithospheric mantle
that would result in radiogenic 206 Pb/204 Pb in
less than 100 Ma [45]. However, studies of litho-
spheric peridotites metasomatized by small-degree
melts [46] do not indicate that this process adds
or removes signi¢cant amounts of Re and Os to
produce radiogenic 187 Os/188 Os in less than
100 Ma. In conclusion, it is di¤cult to identify
alternative materials or processes that could be
suitable to explain both the high 187 Os/188 Os and
206
Pb/204 Pb in HIMU OIB.
6.3. Are bulk mixing models appropriate?
If no source other than recycled altered crust
can produce high 187 Os/188 Os and 206 Pb/204 Pb,
then the assumptions made for the bulk mixing
models must be re-evaluated. It is commonly as-
sumed that under the conditions of partial melting
in the asthenospheric mantle, local equilibration
of melts and mantle occurs in less than 105 yr [47].
This is likely true for asthenosphere-derived large-
volume magmas such as MORB, or £ood basalts,
tholeiites, picrites and komatiites that may re£ect
higher than average mantle temperatures (Hawaii,
Iceland, Gorgona Island). It is less clear if the
equilibrium assumption is met by the smaller-vol-
ume alkali basalts, basanites and nephelinites that
show the HIMU signature. For instance, experi-
mentally determined mineral dissolution rates [48]
and assessments of xenolith settling rates [49] sug-
gest that mantle xenoliths preserved in some of
the alkali basalts require rapid ascent velocities
of these magmas from their source regions (in
the order of days or weeks). These fast ascent
velocities can be largely attributed to the low den-
sity of volatile-rich magmas and the increased vol-
ume and magma pressure relative to dry magma
during partial melting [49]. The volatile-rich man-
tle source required by the composition of these
EPSL 5412 4-4-00
297
lavas suggests that melt extraction occurs more
rapidly than under dry conditions. These circum-
stances render it likely that disequilibrium proc-
esses may be the norm rather than the exception
in the source of HIMU OIB. The high MgO, Cr,
Ni and Os contents of many HIMU OIB indicate
that peridotitic mantle must have contributed sig-
ni¢cantly to the formation of these magmas. A
scenario that could potentially explain some of
the inconsistencies encountered here involves
melting of carbon-bearing eclogite and limited
or no reaction of the melt with peridotite during
separation from the eclogitic residue. Since a sili-
ceous partial melt of eclogite is not in equilibrium
with lherzolite, once the melt leaves the eclogite
domain, reaction of melt with olivine and forma-
tion of pyroxene-bearing assemblages may be the
consequence. The reaction of siliceous melt with
olivine in peridotite likely results in a gain of Mg,
a loss of Si from the melt [37] and consequently a
decrease of viscosity and increase in silica under-
saturation of the melt. When conduits develop in
the host peridotite, it can be expected that melt^
peridotite reaction produces layers of pyroxene on
the walls of the conduit, because the alkaline ba-
salts are Ca-rich and may be saturated with py-
roxene at an early stage. The e¡ect of these pyrox-
enite layers on the next melt batches that use the
conduits would be to limit interaction of the mag-
ma with peridotite.
For the Os mixing relationships, it is important
that the melt equilibrates or interacts with only a
small fraction of the peridotitic Os. Another way
this could be achieved is if most Os is contained in
accessory sul¢des or alloys [50] that are included
in a peridotite mineral that does not participate in
the reaction with siliceous melt. If alloys are sta-
ble and the dominant host for Os in peridotite in
the presence of silicate melt, very low solubilities
of Os in silicate melts [51] could translate into
very high peridotite^melt partition coe¤cients
for Os. Several problems exist with this model.
First, it is not known how homogenously the
bulk of the Os is distributed in peridotites, and
if peridotite minerals may be excluded from dis-
solution^precipitation reactions for given P^T
conditions and melt compositions. Second is the
unknown extent of kinetic control on these reac-
298 H. Becker / Earth and Planetary Science Letters 177 (2000) 287^300
tions and on the dissolution of Os-bearing phases
in melt. Di¡usion coe¤cients of lithophile major
and trace elements in silicate melts (10310 ^10312
cm2 s31 at 1200^1300³C, e.g. [47]) suggest that for
some of these elements, cm-scale equilibration
may occur in approximately 300^30000 yr. These
time scales may be too long to reach equilibrium
if volatile-charged magmas are involved. Note,
however, that theoretical work on the physics of
melt segregation in the mantle suggests longer
time scales for melt^residue separation [52].
Fig. 7b shows an example in which a `reactive'
Os content of mantle of 300 ppt is assumed. The
mixing relationships in Fig. 7b require signi¢-
cantly lower proportions of eclogite to peridotite
in the source of HIMU OIBs and result in curves
that appear to be more consistent with data ¢elds
for HIMU OIBs. Disequilibrium models would
lessen the problem of explaining relatively radio-
genic 187 Os/188 Os and relatively high Os abundan-
ces in HIMU OIB by recycled MORB with very
low Os abundances. In the case of disequilibrium
melting and reaction, time scales as well as mag-
ma temperatures and composition likely deter-
mine how much Os from the wall rock will be
transferred into the melt. It is interesting to note
that abundances of lithophile incompatible ele-
ment abundances in HIMU OIBs are generally
assumed to re£ect low degrees of partial melting
under the assumption that the melts equilibrated
with a peridotitic residue (e.g. [38]). The main
argument supporting these models is the strong
enrichment of LREE and highly incompatible el-
ements in many HIMU basalts [30,38]. These
models are di¤cult to reconcile with a disequi-
librium scenario unless only Os does not equili-
brate with melt but the lithophile elements do, or
the enrichment of incompatible elements in
HIMU basalts re£ects the pre-enrichment of the
mantle source by metasomatic melts (e.g. [45])
and disequilibrium during melting.
7. Conclusions
Eclogites, blueschists and ma¢c granulites tend
to contain only V40% of the Re abundances ex-
pected for likely ma¢c protoliths, but comparable
EPSL 5412 4-4-00
Os abundances. The implication is that Re was
lost either during dehydration, the most likely ex-
planation, or during alteration of the protoliths
near the ocean ridges. Models for the origin of
HIMU OIB that are believed to contain a com-
ponent of recycled altered MORB would require
excessive amounts ( s 80^90%) of the latter to ex-
plain their radiogenic 187 Os/188 Os and 206 Pb/204 Pb
if constraints on Re/Os and U/Pb from the meta-
basites are used. In the light of other evidence,
these estimates appear unreasonably high. It is
suggested that the bulk mixing models commonly
employed may not be applicable and that the ac-
tual fraction of recycled component in these OIB
sources is much lower than implied by these mod-
els. Possible explanations for the `misbehavior' of
Os may include kinetic reasons and the shielding
of Os-rich phases by silicates from reaction with
melt.
Acknowledgements
Al Brandon, Sonia Esperanc°a, John Morgan
and Rich Walker provided invaluable intellectual
input through various conversations in the lab
and during lunch at China Cafe and other places.
Thanks go also to other Re^Os folks (the DTM
crew, Gerhard Bru«gmann, John Chesley, Robbie
Frey, Munir Humayun, Jon Snow, Liz Widom)
for sharing techniques and insight. A thorough
review of a ¢rst draft by Rich Walker is very
much appreciated. O¤cial journal reviews by
Chris Hawkesworth and Jan Kramers helped to
improve the manuscript signi¢cantly. I am grate-
ful to Sonia Esperanc°a and Tim Mock for their
support in the lab. Work on this project was
made possible through various NSF research
grants to Rich Walker.[AH]
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