2002 Geological Society of America. For permission to copy, contact Copyright Permissions, GSA, or editing@geosociety.org.

Geology; October 2002; v. 30; no. 10; p. 915918; 3 gures. 915

Roasting the mantle: Slab melting and the genesis of major Au and
Au-rich Cu deposits
James E. Mungall* Department of Geology, University of Toronto, 22 Russell Street, Toronto, Ontario M5S 3B1, Canada
ABSTRACT
The generation of large deposits of Au and Cu in suprasubduction-zone settings depends
upon a combination of factors, including availability of the chalcophile elements to arc
magmas in their mantle source regions, and the operation of suitable hydrothermal sys-
tems in the upper crust where the deposits eventually form. The removal of chalcophile
elements from the mantle wedge into arc magmas can only occur if sulde is absent from
the melted source rock, requiring oxidation of the mantle wedge to values of log fO
2

FMQ 2, where fO
2
is oxygen fugacity and FMQ is the fayalite-magnetite-quartz oxygen
buffer. The only agent capable of effecting this change is ferric iron, carried in solution
by slab-derived partial melts or supercritical uids. Arc magmas with high potential to
generate Au and Cu deposits will have certain geochemical characteristics; they will have
fO
2
more than two log units above FMQ and they will have either adakitic, sodic-alkaline,
or potassic-ultrapotassic afnities. Favorable tectonic settings include subduction of very
young lithosphere or very slow or oblique convergence, at subduction, and the cessation
of subduction.
Keywords: mineral deposits, genesis, subduction zones, Au, Cu, mantle.
Figure 1. Oxygen buffers in log f O
2
vs. tem-
perature space (see text). Only addition of
Fe
2
O
3
can bring mantle assemblages higher
than SSO buffer. Undersaturation of magma
in sulde requires either very high degrees
of partial melting or generation in unshaded
portion of diagram. SSOsulde-sulfur ox-
ide buffer; CCOcarbon dioxidecarbonox-
ide buffer; FMQfayalite-magnetite-quartz
oxygen buffer; MHmagnetite-hematite ox-
ygen buffer.
INTRODUCTION
Many of the worlds major deposits of Au
and Cu owe their origins to the emission of
hydrothermal uids from cooling magmas em-
placed above subduction zones; however,
most arc magmas do not produce economic
deposits. Magma associations recognized to
be particularly fertile include potassic calc-
alkaline magmas (Muller and Groves, 1993),
adakitic magmas (i.e., arc magmas with trace
element signatures of garnet and hornblende
in their source and possibly generated by slab
melting; Kay et al., 1995; Drummond et al.,
1996; Thieblemont et al., 1997; Sajona and
Maury, 1998), and alkaline arc magmas (e.g.,
Richards, 1990; McInnes and Cameron,
1994). Whereas normal subduction processes
do not appear to favor the generation of large
Au and Cu deposits, the tectonic settings rec-
ognized as favorable include the onset and
termination of periods of at subduction
(Kay and Mpodozis, 2001), the reversal of
polarity of a subduction zone (Solomon,
1990), and the cessation of subduction due to
collision (McInnes and Cameron, 1994; Sil-
litoe, 1997).
In this article I attempt to show that simple
geochemical arguments can be used to ac-
count for such disparate observations within a
single framework, elucidating and building
upon the suggestion of Sillitoe (1997) that sul-
de oxidation is the key process in the liber-
ation of chalcophile elements from the arc
mantle.
ROLE OF SULFIDE IN MANTLE
SOURCE REGIONS OF ARC MAGMAS
Sulde melt sequesters the chalcophile el-
ements during partial melting of the mantle,
*E-mail: mungall@geology.utoronto.ca.
and complete dissolution of sulde into sili-
cate melt with S solubility 1000 ppm (Mav-
rogenes and ONeill, 1999) at normal mantle
S contents of 250 ppm would require 25%
partial melting (e.g., Hamlyn and Keays,
1986). In order for a silicate magma to contain
signicant amounts of Au and Cu, sulde melt
must be absent from its mantle source. Fur-
thermore, unless the magma remains sulde
undersaturated it will lose Cu and Au during
its evolution (Wyborn and Sun, 1994). If S is
added to the mantle by the same uids that
induce partial melting in the subduction zone
(Alt et al., 1993; Metrich et al., 1999), then
the degree of partial melting required to de-
stroy residual sulde might easily exceed
40%. Such abnormally high aggregate degrees
of melting at moderate pressures generate
boninitic magmas, which contain high abun-
dances of the chalcophile elements, including
the platinum group elements (Hamlyn and
Keays, 1986). However, many deposits are as-
sociated with alkaline magmas, the composi-
tions of which reect very low degrees of par-
tial melting of the mantle (e.g., Richards,
1990; McInnes and Cameron, 1994).
Sulde can also be removed by the oxida-
tion of sulfur from S
2
to S
6
:
FeS 2O
(liq) 2(fluid)
FeO SO . (1)
(melt) 3(melt)
In mantle peridotite the main reservoir for Ca
is pyroxene, so upon anhydrite saturation
equation 1 can be rewritten as:
FeS CaFeSi O 2O
(sul) 2 6(cpx) 2(fluid)
CaSO 2FeSiO . (2)
4(An) 3(opx)
Because the activities of ferrosilite, hedenber-
gite, and FeS in their respective host phases
vary only through limited ranges, the assem-
blage anhydrite sulde melt will constitute
an oxygen buffer (here named SSO; i.e., the
sulde-sulfur oxide buffer).
OXIDATION OF THE MANTLE
ABOVE SUBDUCTION ZONES
The oxidation state of upper mantle rocks
from many settings has been assessed through
consideration of reactions like
6Fe SiO O
2 4(ol) 2(fluid)
2Fe O 3Fe Si O , (3)
3 4(sp) 2 2 6(opx)
where fayalite, magnetite, and ferrosilite ap-
pear as components in solid solution within
olivine, spinel, and orthopyroxene (ONeill
and Wall, 1987). Oxygen fugacity thus mea-
sured in mantle xenoliths not related to sub-
duction zones is generally found to fall within
one log unit of the fayalite-magnetite-quartz
(FMQ) oxygen buffer, at which it is thought
to be held by reactions like the carbon dioxide
carbon oxide (CCO) buffer (Fig. 1; Blundy et
al., 1991):
CO C O .
2(fluid) (gr) 2(fluid)
(4)
Samples of peridotite gathered from volca-
noes tapping the mantle above subduction
zones record equilibration at higher log f O
2
,
916 GEOLOGY, October 2002
Figure 2. A: Concentrations of aqueous spe-
cies as functions of pressure. Estimated
concentrations of ferric iron complexes
(FeO

aq
, HFeO
2aq
) remain well below those
of ferrous iron (FeO
aq
) at all pressures below
30 kbar. Sulfate concentration remains sev-
eral orders of magnitude higher than ferric
iron solubility at all pressures. B: Concen-
tration of Fe
2
O
3
in silicate melts as function
of fO
2
(expressed as difference from FMQ in
log units). Note scale difference between A
and B.
typically ranging from FMQ to FMQ 2
(i.e., still within the stability eld of sulde
melt; Carroll and Rutherford, 1987) due to the
action of oxidized slab-derived metsomatizing
uids or melts (e.g., Brandon and Draper,
1996; Luhr and Aranda-Gomez, 1997; Parkin-
son and Arculus, 1999).
The subducted oceanic crust has variable
but locally very high intrinsic f O
2
due to
equilibration with seawater during hydrother-
mal alteration and deposition of terrigenous
sediment. Melts or uids derived from the slab
will carry this oxidizing potential up into the
overlying mantle (e.g., McInnes and Cameron,
1994). The only elements existing in variable
oxidation states and present in sufcient abun-
dances to affect the redox state of the upper
mantle are C, H, S, and Fe.
The effect of addition of CO
2
to a mantle
assemblage containing graphite can be seen by
combining equations 3 and 4:
6Fe SiO CO
2 4(ol) 2(fluid)
2Fe O C 3Fe Si O . (5)
3 4(sp) (gr) 2 2 6(opx)
As long as the fO
2
remains below the CCO
buffer, continuous addition of CO
2
will lead
to continuous increase in the amount of both
graphite and ferric iron in the assemblage.
Once sufcient iron has been oxidized by the
reduction of CO
2
to graphite to bring the as-
semblage to the CCO buffer, further addition
of CO
2
will have no effect on fO
2
because it
coexists with stable graphite but cannot oxi-
dize graphite. The metasomatic addition of
CO
2
cannot raise fO
2
to the SSO buffer (Fig.
1).
The dissociation of water is represented by
H O H 0.5O .
2 (fluid) 2(fluid) 2(fluid)
(6)
The equilibrium constant for this reaction at
upper mantle conditions is so small that the
amount of free oxygen available to participate
in reactions like equation 4 is of the order of
10
14
molal during reduction of water from
log fO
2
of FMQ 2 to FMQ (Frost and Ball-
haus, 1998). Water alone cannot act as an ox-
idizing agent unless the ambient fO
2
of the
mantle is in the stability eld of H
2
. Sponta-
neous physical separation of H
2
and O
2
into
distinct, spatially separated, reduced, and ox-
idized reservoirs (cf. Brandon and Draper,
1996) in a formerly homogeneous system
would violate the second law of
thermodynamics.
At ambient f O
2
below SSO, 1 mol of added
sulfate would be reduced to sulde, while ox-
idizing 8 mol of iron:
13Fe SiO SO
2 4(ol) 3(fluid)
4Fe O FeS
3 4(sp) (sul)
6.5Fe Si O . (7)
2 2 6(opx)
If fO
2
is at or above the SSO buffer, SO
3
will be stable, so that continued addition of
sulfate cannot cause any further oxidation of
iron to raise the f O
2
above the stability eld
of sulde. The process of raising f O
2
from
CCO to SSO by reduction of the introduced
sulfate causes a net addition of sulde to the
mineral assemblage. The addition of slab-
derived sulfate will rmly buffer the f O
2
of
the mantle wedge exactly at SSO while in-
creasing the total amount of sulde melt pre-
sent. Sulfate metasomatism therefore effec-
tively precludes the subsequent generation of
fertile magmas rich in the chalcophile
elements.
The addition of Fe
2
O
3
will adjust the man-
tle f O
2
along a continuously sliding scale ac-
cording to reactions like the following, as long
as the mantle remains below the magnetite-
hematite buffer:
Fe O Fe SiO
2 3(fluid) 2 4(ol)
Fe O FeSiO , (8)
3 4(sp) 3(opx)
where uid is either aqueous uid or silicate
melt (Fig. 1). When Fe
2
O
3
addition brings the
f O
2
of an assemblage containing sulde melt
up to the SSO buffer, the f O
2
cannot increase
further until all sulde has been oxidized to
sulfate according to a reaction like
FeS 4Fe O 9FeSiO
(sul) 2 3(fluid) 3(opx)
SO 9Fe SiO . (9)
3(fluid) 2 4(ol)
Once sulde has been fully oxidized there
is no further bar to the continued increase in
f O
2
resulting from Fe
2
O
3
addition to the man-
tle wedge via equation 8.
METASOMATIC AGENTS
I have estimated the concentrations of sul-
fate and ferric iron in subduction uids by us-
ing thermochemical data and empirical mod-
els for aqueous solutes and minerals (Johnson
et al., 1992; E. Shock, 2000, personal com-
mun.) combined with thermochemical and di-
electric models for water (Harvey et al., 1996;
Fernandez et al., 1997) to calculate Gibbs free
energies of reaction for dissolution and com-
plexation reactions at 600 C and pressures to
30 kbar. These calculations are extrapolations
of low-pressure data and results must be re-
garded with caution.
Calculated concentrations of several aque-
ous complexes in uids equilibrated with spi-
nel (Fe species) or anhydrite (sulfate) are
shown in Figure 2A as functions of pressure.
All activity coefcients are assumed to be uni-
ty and the activity of magnetite in spinel is
assumed to be 0.1. The estimated concentra-
tion of FeO
(aq)
at 30 kbar is 250 ppm, sim-
ilar to total iron concentration measured by
Schneider and Eggler (1986) at 1520 kbar
and temperatures from 750 to 850 C.
The rst-order result of this modeling ex-
ercise is that the solubility of anhydrite re-
mains several orders of magnitude greater
than that of ferric iron over the entire pressure
range considered. Whereas aqueous uids are
able to transport signicant amounts of sul-
fate, they are exceedingly poor carriers of fer-
ric iron.
During reduction of its log f O
2
from FMQ
4 (cf. McInnes and Cameron, 1994) to
FMQ, an aqueous uid equilibrated with spi-
nel will donate 2.5 10
5
mol Fe
3
per
mole of aqueous solution to redox reactions in
metasomatized mantle. To oxidize 1 mol of
sulde to sulfate, 8 mol of Fe
3
are required;
by converting to weight fractions and assum-
GEOLOGY, October 2002 917
Figure 3. Composite sketch of convergent plate margins (SL is sea level). Scales are in
kilometers, without vertical exaggeration. Inset diagram shows elds in which breakdown
of hydrous phases produces melt, aqueous uid, or supercritical uid (SC) from subducted
oceanic crust. Smaller inset diagrams show pressure-temperature (P-T) paths associated
with various tectonic settings. Only those inset diagrams labeled with Au (i.e., B, C, D, and
E) represent tectonic settings capable of generating oxidized Au- and Cu-rich magmas.
ing that normal asthenospheric mantle initially
contains 250 ppm S, I nd that 1 g of aqueous
uid can oxidize the sulde contained in 0.4
g of mantle.
Figure 2B shows the dependence of Fe
2
O
3
concentrations on f O
2
estimated by using the
MELTS thermochemical model of Ghiorso
and Sack (1995) in two different examples of
melt thought to have been present in metaso-
matized mantle wedge peridotites above par-
tially melted oceanic plates (McInnes and
Cameron, 1994; Schiano et al., 1995). The re-
duction of silicate melts from FMQ 4 to
FMQ consumes 0.01 mol of Fe
3
per mole
of silicate melt. Following the same calcula-
tion as for aqueous uid, as previously dis-
cussed, I nd that 1 g of silicate melt derived
by slab melting can oxidize the sulde con-
tained in 160 g of mantle peridotite.
Silicate melts thus have a carrying capacity
for Fe
2
O
3
some 400 times greater than have
aqueous uids. The effectiveness of slab melt-
ing is further augmented by the fact that the
mass of aqueous uid that can be released dur-
ing slab dehydration is less than or equal to
the amount of water originally present in the
slab, whereas slab melt containing 4% dis-
solved water will have a mass 25 times the
mass of water originally present. In terms of
the total ux of Fe
2
O
3
per unit mass of water
brought into the subduction zone by the down-
going slab, slab melts will thus carry as much
as 10 000 times more Fe
2
O
3
than can dehy-
dration uids.
Metasomatism of the upper mantle by the
aqueous uid released during slab dehydration
will introduce abundant sulfate but only trace
quantities of ferric iron. Slab dehydration will
oxidize the mantle wedge while augmenting
the amount of sulde present. Melting of pe-
ridotite metasomatized by aqueous uid will
be expected to produce typical sulde-saturated,
water-rich arc magmas with intrinsic f O
2
be-
tween FMQ and SSO and minimal potential
for the generation of chalcophile element de-
posits. In contrast, the ux of Fe
2
O
3
via slab
melts can lead to sulde-undersaturated melt-
ing of fertile asthenosphere and the generation
of Au- and Cu-rich arc magmas.
It is critical to emphasize that the only plau-
sible source of highly oxidized melts or uids
in the upper mantle is the upper oceanic crust
in a subducted slab. Although melts similar to
slab melts may form by remelting of basaltic
or gabbroic crustal underplates originally
sourced in normal arc mantle, these melts will
retain the low f O
2
of their sources (Carmi-
chael, 1991). Basaltic magmas emplaced at
Earths surface with f O
2
SSO must contain
a signicant component of melt from sub-
ducted oxidized crustal rocks.
TECTONIC CONTROLS
Figure 3 is a schematic section of a conver-
gent margin showing several possible scenarios
for the generation of slab melts or aqueous uids
for both normal (solid lines) and at (dashed
lines) subduction. The inset diagram is a sim-
plied sketch of pressure- and temperature-
dependant phase relations in hydrous metabas-
altic rocks representative of the hydrothermally
altered oceanic crust on the subducted slab
(e.g., Peacock et al., 1994; Schmidt, 1996). In
the eld labeled uid, minerals such as talc,
serpentine, and actinolite undergo progressive
dehydration reactions to release aqueous u-
ids. At high pressure there are no important
dehydration reactions above the uid eld
until the mica breakdown curve is reached. At
moderate pressures the same minerals break
down to produce slab melts (melt eld). At
temperatures above the critical curve there is
no distinction between a dehydration reaction
and a melting reaction because silicate melt
and aqueous uid are a single thermodynamic
phase (Paillat et al., 1992). The critical curve
shown corresponds approximately to the mea-
sured critical end points in the haplogranite-
or dacite-water system (Bureau and Keppler,
1999). The upper left margin of the super-
critical eld marks the breakdown of phen-
gite mica to an anhydrous residue and a su-
percritical potassic uid (Schmidt, 1996).
Dense supercritical uids are capable of dis-
solving large (wt%) loads of otherwise im-
mobile elements such as Al
2
O
3
and Fe
2
O
3
.
The six small reproductions of the inset
phase diagram each show the pressure-
temperature (P-T) path followed by a sub-
ducted slab in various tectonic settings. In nor-
mal contemporary subduction zones the
subducted crust never melts (Fig. 3, box A;
see also Peacock et al., 1994), and magmas
produced by hydrous uxing of the astheno-
spheric mantle wedge will be sulde saturated
and poor in Au and Cu.
Box B shows the fate of a slab which may
be a: young and hot; b: the leading edge of a
newly formed subduction zone; or c: subduct-
ed very slowly or obliquely. It follows a P-T
path across the amphibole solidus before the
mineral assemblage has been dehydrated, per-
mitting small degrees of partial melting of the
subducted slab. Mantle peridotite uxed by
slab melts will generate adakitic magmas
(Drummond et al., 1996), which may be high-
ly oxidized and potentially fertile for Au and
Cu.
Slab P-T paths intermediate between cases
A and B will allow early, shallow dehydration
and generation of ordinary arc magmas, fol-
lowed by the release of potassic supercritical
uids at great depths of 300 km (labeled SC;
Schmidt, 1996) to generate rear-arc potassic or
ultrapotassic magmas with high f O
2
and com-
paratively high potential to host Au and Cu-
Au deposits (box D; Muller and Groves,
1993).
If a slab stalls in the subduction zone then
its temperature will increase continuously
while it remains at a constant pressure. In this
case the upper portions of the slab will pass
directly into the melt eld, whereas the deeper
portions will pass into the supercritical eld
(box C). Panguna in Bougainville, Ok Tedi in
New Guinea, Baguio in Luzon (Thieblemont
et al., 1997; Sajona and Maury, 1998), Por-
gera in New Guinea, and Ladolam on Lihir
(Solomon, 1990; McInnes and Cameron,
1994) are all deposits generated after reversal
of subduction direction led to the stalling of a
slab. The process may lead directly to eruption
of adakitic or potassic magmas, or it may
918 GEOLOGY, October 2002
cause emplacement of oxidized veins in the
mantle that do not actually melt until a later
extensional tectonic event produces small vol-
umes of alkaline magmas.
During at subduction a slab passes under
the overriding plate for great distances at con-
stant pressure. If the process has just begun or
if the slab is beginning to fall back down to a
normal angle, then it will be passing under hot
asthenospheric mantle while remaining at low
pressure for extended periods, possibly lead-
ing to slab melting under thin lithosphere (cf.
Gutscher et al., 2000). Under more realistic
lithospheric thicknesses than those modeled
by Gutscher et al. (2000), the result would be
release of oxidized supercritical uids rather
than adakitic magmas (box E). Major deposits
that have been suggested to be related to slab
melting and adakitic or potassic magmatism
in this setting include El Indio, El Salvador,
Quebrada, and Chuquicamata of the Chilean
Copper Belt, and Bingham, United States
(Thieblemont et al., 1997). If there is no as-
thenosphere present above the slab, then it
will follow a very cold path, allowing dehy-
dration to occur without uxing of the mantle,
and causing cessation of magmatism until nor-
mal steep subduction resumes (box F; Gutsch-
er et al., 2000; Kay and Mpodozis, 2001).
The importance of slab melting in subduc-
tion zones, particularly in relation to at sub-
duction, remains a contentious issue (Peacock
et al., 1994; Martin, 1999; Gutscher et al.,
2000; Kay and Mpodozis, 2002). Current geo-
chemical probes of arc magma petrogenesis
focus on differences between uid and melt
transfer from slab to mantle, and are poorly
suited to detection of small slab melt volumes
or the possible presence of supercritical melt-
uid mixtures.
I suggest here that a powerful new discrim-
inant is magma oxidation state. If an arc mag-
ma has log f O
2
SSO, then it must contain
a component of melted oceanic crust, because
no vector other than slab-derived melt or su-
percritical uid can carry such high redox po-
tential into the upper mantle. If the concepts
presented here are correct, then large Au and
Cu deposits may by their very existence pro-
vide evidence for slab melting or the release
of supercritical uids in the source regions of
their parental magmas. Conversely, the rec-
ognition of slab melting signatures in arc mag-
mas should be considered a promising rst
step in the denition of Au-Cu exploration tar-
gets at the regional scale.
ACKNOWLEDGMENTS
The author was funded by a research grant from the
Natural Sciences and Engineering Research Council of
Canada during this study. Thanks to Everett Shock for ad-
vice on high-pressure extrapolation of Supcrt92.
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Manuscript received April 2, 2002
Revised manuscript received June 20, 2002
Manuscript accepted June 25, 2002
Printed in USA