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Geology

Oxidation state of subarc mantle

K.A. Evans, M.A. Elburg and V.S. Kamenetsky

Geology 2012;40;783-786
doi: 10.1130/G33037.1

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Oxidation state of subarc mantle

K.A. Evans1, M.A. Elburg2,3, and V.S. Kamenetsky4
1
School of Applied Geology, Curtin University, GPO Box 1987, WA 6845, Australia
2
Department of Geology and Soil Science, Ghent University, Krijgslaan 281 S8, 9000 Ghent, Belgium
3
School of Geological Sciences, University of KwaZulu-Natal, Private Bag x54001, 4000 Durban, South Africa
4
School of Earth Sciences, and CODES Centre of Excellence in Ore Deposits, University of Tasmania, Hobart, Tasmania 7001,
Australia

ABSTRACT fractionation or degassing (Burgisser and Scail-

The subarc mantle is a primary control on the composition of arc magmas and the forma- let, 2007).
tion of arc-related ore deposits. Elevated ferric iron contents in arc lavas have been interpreted The data presented here compose a uniquely
as a record of subarc mantle that is oxidized relative to mid-oceanic ridge basalt (MORB), but large and consistent database; all the data were
this conclusion is controversial. Measurements of spinel compositions in primitive arc lavas obtained by a single operator with a consistent
imply an arc magma source 1–4 log units more oxidized than MORB and ocean island basalts method. The MnO/FeO ratio of selected olivine
analyzed using the same technique. Samples from seven arcs show a significant correlation (P phenocrysts was measured and plotted against
< 0.0005) between redox budget, subduction zone convergence rate, and subduction zone age. ΔQFM (quartz-fayalite-magnetite). MnO
These results support the notion of oxidized arc lavas in the mantle source zone, but resolution behaves very similarly to FeO, except that the
of contradictory evidence regarding subarc mantle redox state requires further work. oxidation reaction of tephroite (Mn2SiO4) to
hausmannite (Mn3O4) occurs at significantly
INTRODUCTION primitive olivine and spinel crystals in near- higher oxygen fugacities (fO ) than for the QFM
2
The oxidation state of a magma controls primary arc, MORB, and ocean island basalts buffer (Brusnitsyn, 2007), so Mn2+/Fe2+ ratios in
the crystallization, separation, and composi- (OIB). This strategy minimizes the effects of magmas increase with increasing fO . Therefore,
2
tion of magmatic fluids, element transport, fractionation and volatile exsolution on magma olivine from more oxidized magmas should
and ore deposition (Snyder et al., 1993; Sun et oxidation state. The results are discussed in the display higher Mn/Fe ratios than those from
al., 2004). Mid-ocean ridges and subduction- context of relationships between redox budget magmas that formed at lower fO , so long as the
2
related volcanic arcs are the two major contrib- and arc characteristics such as convergence rate. original melts had similar Mn/Fe ratios.
utors to the global magma budget, and previous
work has suggested that arc lavas have a signif- METHODS RESULTS
icantly higher oxidation state than mid-oceanic The spinel-olivine oxybarometer (Ballhaus The calculated fO of arc basalts is 2–4 log
2
ridge basalt (MORB) (e.g., Christie et al., 1986; et al., 1991) was applied to olivine + olivine- units above the QFM buffer, whereas MORBs
Wood et al., 1990; Eggins, 1993; Kelley and hosted spinel pairs in basalts from volcanic arcs, show a ΔQFM between 0 and +1 (Fig. 2A). The
Cottrell, 2009). However, the oxidation state mid-ocean ridges, and ocean islands (Fig. 1; high-K arc samples show an average ΔQFM
of magma can change during crystallization Kamenetsky et al., 2001; see the GSA Data (2.9 ± 0.7) somewhat higher than the low- to
and volatile exsolution (Burgisser and Scaillet, Repository1 for locations and details of analyti- medium-K arc samples (2.1 ± 0.6). Data for
2007), which may obscure the signature of the cal techniques). The chosen olivines were the OIBs and arc-related boninites show fO inter-
2
magmatic source. most primitive (forsterite content > 85 mol%) mediate between arc basalts and MORBs. These
The mantle beneath island arcs is thought to in each sample, minimizing potential effects of results compare well with those obtained using
resemble the mantle source for MORB, apart
from a significant enrichment in water and fluid-
mobile elements such as B, Cs, Rb, Sr, and K Subduction zone
Other plate boundary
(the subduction zone component; Gill, 1981; Analyzed island arc samples
Pearce and Peate, 1995). Evidence from spinel Aleutians

compositions, Fe-Ti-oxide stability, the mag- Kamchatka

Kurile
nitude of the Eu anomaly, Cr-Ga systematics, ATLANTIC
and the speciation of sulfur (Gill, 1981; Turner Izu Bonin

et al., 1997; Parkinson and Arculus, 1999; Dare Marianas

Antilles
et al., 2009; Rowe et al., 2009) has been used Yap
Equator
as a basis for the proposal that the oxidation 90oE 180o 90oW
state of the subarc mantle is higher than that of INDIAN
the mantle underlying mid-ocean ridges. How- OCEAN PACIFIC OCEAN
OCEAN
ever, the perceived high oxidation state of the
subarc mantle compared to mid-ocean ridge
mantle has been challenged on the basis of V/
AUSTRAL OCEAN
Sc systematics of basalts (Lee et al., 2005; Mall-
AUSTRAL OCEAN
mann and O’Neill, 2009), Zn/Fe ratios (Lee et
al., 2010), and iron isotope evidence (Dauphas
et al., 2009). Here we present oxygen fugacity Figure 1. Location map showing arcs and sample sites.
data derived from the composition of the most
1
GSA Data Repository item 2012223, description of the sample sites and methods, is available online at
*E-mail: [email protected]; elburg@ukzn. www.geosociety.org/pubs/ft2012.htm, or on request from [email protected] or Documents Secretary,
ac.za; [email protected]. GSA, P.O. Box 9140, Boulder, CO 80301, USA.

GEOLOGY, September 2012; v. 40; no. 9; p. 783–786; Data Repository item 2012223 | doi:10.1130/G33037.1 | Published online 29 June 2012
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Tomkins, 2011). Results indicate that sufficient gence rate, V/Sc (n = 57), V/Ga (n = 24), Zn/Fe
oxidized material is subducted to significantly (n = 49), total Fe, the age of subduction zone,
oxidize subarc mantle on time scales shorter than and the product of subduction zone age and con-
the lifetime of a subduction zone (105–107 yr); vergence rate.
that the limit on the extent of subarc mantle oxi- Redox budget is correlated at a significant
dation is the solubility of oxidized iron, carbon, level (Fig. 3; Table 1) with convergence rate,
and sulfur in fluids that leave the subducting the age of the subduction zone, and the proxy
slab; and that the redox budget of subarc mantle for the total length of oceanic crust subducted.
increases with the age of the subduction zone. In This result is robust whether the average of
addition, the extent of oxidation should be sensi- results for each subduction zone or the full data
tive, to some extent, to convergence rate, since set is considered. V/Sc is not correlated with
the depth of fluid release affects the solubility the redox budget or the total length of crust
and efficiency of transfer of oxidized iron, car- subducted. V/Sc ratios vary from 3 to 10; based
bon, and sulfur in fluids. on the assumption of 10% melting of a spinel
If convergence is slow, then fluid release or garnet peridotite, this indicates a source
occurs at relatively shallow depths, which zone with an fO of QFM ±~1 (Mallmann and
2
reduces the chance of sulfate release (Newton O’Neill, 2009), lower than that estimated for
and Manning, 2005), and fluids may escape up arc regions (Fig. 2). V/Ga and Zn/Fe produce
the slab-mantle interface instead of migrating similar results. Total Fe correlates to some
into the subarc mantle. If convergence is fast, extent with redox budget (σ = 0.38), and to a
then fluid release will occur at greater depths; lesser extent with convergence rate (σ = 0.26)
fluids are likely to be more silica rich, and may and subduction zone age (σ = 0.28).
Figure 2. A: Oxidation state of olivine-spinel carry higher concentrations of sulfate (Newton The strong correlation between redox budget
pairs versus forsterite content of olivine and Manning, 2005) than fluids produced at and arc parameters suggests a causal relation-
from contrasting basalts. Calculations per- shallower depths. Fluids released from the slab ship between increased redox budget in arc
formed following Ballhaus et al. (1991). Black at depth may also infiltrate and interact with basalts and subduction zone age and/or conver-
circles—mid-oceanic ridge basalts (MORB);
triangles—boninites; squares—ocean is-
the subarc mantle more effectively than fluids gence rate. This relationship is robust so long as
land basalts (OIB); white circles—low-K arc derived from shallower depths. It is possible the redox budget has not been affected by degas-
magmas; gray circles—high-K arc magmas. that there is a critical convergence rate such that sing or fractionation processes during basalt
Calculated differences in oxygen fugacities convergence rates greater than the critical value ascent and eruption, or by oxidation processes
between groups are independent of spinel lead to transfer of oxidized elements to the deep subsequent to eruption. The effects of degas-
compositions (see the Data Repository [see
footnote 1]). B: Average MnO/FeO ratio of ol- mantle rather than release by devolatilization. sing and fractionation on the data set were mini-
ivine per sample suite versus average calcu- To explore these ideas, a database was con- mized by choosing the most primitive basalts,
lated ΔQFM (quartz-fayalite-magnetite) from structed that contains ferric:ferrous ratios of and it seems unlikely that degassing and/or
olivine-spinel pairs. basalts from a range of different arcs, taken fractionation processes would produce the
from the GeoRoc database (http://georoc.mpch observed correlations. Post-eruption alteration
-mainz.gwdg.de/georoc/). Criteria for inclusion could also cause oxidation, and, if old basalts
the Cr-Ga oxybarometer proposed by Dare et al. of an arc in the study were (1) a lack of recent are more altered than young basalts, then the
(2009), but cannot be compared directly with subduction history related to arcs other than observed correlation between redox budget and
the results of Kelley and Cottrell (2009) because those studied; (2) a lack of continental crust subduction zone age could be caused by altera-
they did not calculate fO . The calculated differ- in the arc region; and (3) reasonable age con- tion. However, alteration would increase water
2
ence in fO between the sample groups is not a straints on convergence rates and arc age. Data content, and there is no correlation between this
2
function of spinel composition (Fig. DR1 in the for convergence rates and arc age were taken parameter and redox budget, so a role for altera-
Data Repository). from Jarrard (2003). Redox budgets (Evans, tion seems unlikely.
Mn/Fe ratios correlate with calculated fO for 2006; see the Data Repository) were calculated The cause of the relationship between redox
2
MORB and arc samples, including boninites for the more primitive basalts (MgO > 8%). budget, convergence rate, subduction zone age,
(Fig. 2B); this supports the validity of trends in Redox budget is an extensive variable that can and the convergence rate–subduction age prod-
the calculated fO . OIB olivines are not on the be used to measure the oxidizing capacity of a uct is difficult to identify because each pair
2
trend defined by the MORB and arc samples; material; high values indicate high levels of oxi- of these four parameters is significantly cor-
this may relate to the mantle source’s residual dized elements. This variable was used because related. Thus it is impossible to state whether
mineralogy (Sobolev et al., 2007). it depends on the quantity of material consid- the increased redox budget of basalts from old,
ered, and is therefore appropriate for studies of fast-converging arcs is a result of the increase
DISCUSSION element fluxes and mass balances. in the depth of fluid release associated with
Results (Fig. 2) imply that subarc mantle is Redox budgets were plotted against conver- increased convergence rate, or the cumulative
1–4 log units more oxidized than mid-ocean gence rate, time since initiation of subduction, input of oxidized material into the subduction
ridge mantle. Potential oxidants include water, and the product of convergence and subduction zone. Higher correlation coefficients are cal-
oxidized iron, sulfur, and carbon (e.g., Kelley zone age, which is a proxy for the total length culated for convergence rate and redox budget
and Cottrell, 2009) from subducting slab, sedi- of ocean crust subducted. V/Sc, V/Ga, and Zn/ than for subduction zone age and redox budget.
ments, and mantle lithosphere. Fe ratios, which are proposed proxies for subarc This may indicate that convergence rate is the
Quantitative estimates of the relationship mantle fO (e.g., Mallmann and O’Neill, 2009; more influential parameter, or it may indicate
2
between the oxidizing capacity of subducted Lee et al., 2010), were also calculated. Correla- that subarc mantle reaches a steady-state redox
material and increases in subarc mantle redox tion coefficients were calculated for seven arcs budget after a certain time so that inclusion
state have been made (Evans, 2012; Evans and between the redox budget (n = 158), conver- of arcs older than a critical age degrades the

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0.6 0.8 subduction zone age–redox budget correlation.

This view is supported by the fact that younger
0.7
0.5
subduction zones (younger than 100 Ma) are
Kamchatka more strongly correlated with redox budget than
Kurile 0.6

RB (moles kg–1)
Izu-Bonin arcs older than 100 Ma. However, the older arcs
RB (moles kg–1)

0.4 also show significant variability, so the steady

0.5
state for each arc may be different (cf. Evans
0.3 Marianas 0.4 and Tomkins, 2011).
Lesser Antilles
Greater Antilles The correlation between redox budget and
Aleutians 0.3
Yap
convergence rate is consistent with the olivine-
0.2 spinel data, in which the high-K arcs display the
0.2
highest oxygen fugacities. Transfer of K from
0.1 0.1 the subducted slab into the mantle wedge is

0
0

10

20

30

40

50

60

70

80
more efficient in silica-dominated than water-
10

20

30

40

50

60

70

80
Convergence Rate (mm yr-1) Convergence Rate (mm yr-1) dominated fluids (Hermann and Spandler,
0.6
0.8
2008), and deep dehydration caused by rapid
convergence could lead to fluid release in silica-
0.7 rich supercritical fluids (Mibe et al., 2011).
0.5
Kamchatka Kurile
In addition, the lower water contents of such
Izu-Bonin
0.6 melts compared to aqueous fluids may induce
RB (moles kg–1)
RB (moles kg–1)

0.4 smaller degrees of melting in the mantle, which

0.5
would also increase the potassium contents
Marianas of the magmas (Elburg et al., 2002). Water is
0.3 Lesser Antilles 0.4
Greater Antilles incompatible in mantle rocks, so the H2O content
Aleutians 0.3 of magmas generated from melt-metasomatized
Yap
0.2 mantle need not be much lower than magmas
0.2 from fluid-fluxed mantle. Fe3+ may also be more
0.1
soluble in silica-rich than aqueous fluids (see
0.1
following discussion).
20

40

60

80

100

120

140

160

20

40

60

80

100

120

140

160
Age (Ma) The data provided here support and help to
Age (Ma)
explain the notion of oxidized subarc mantle.
0.6 0.8
However, contradictory evidence from Zn/
0.7 Fe, V/Sc, and iron isotope data remains
0.5 Kamchatka Kurile unexplained. It may be that there are factors that
0.6 are not yet accounted for that affect the results
RB (moles kg–1)

Izu-Bonin
of the relatively new trace element and isotopic
RB (moles kg–1)

0.4
0.5 techniques. For example, the data investigated
here were obtained via a range of methods, and
Marianas 0.4
0.3 Lesser Antilles it is possible that the lack of a single consistent
Greater Antilles
0.3
method and database has obscured relationships.
Aleutians
0.2
Yap Alternatively, it must be considered if high
0.2 subarc mantle fO is the only possible cause of
2
high Fe3+/Fetot in primitive arc basalts.
0.1 0.1 Water in the arc magma source zone cannot
4
4

0
0

2000

4000

6000

8000
2000

4000

6000

8000

1 10
1 10

cause oxidation directly (Frost and Ballhaus,

Total km subducted
1998). However, water has a strong effect on
Total km subducted
the position of the eutectic in silicate systems
Figure 3. Summary of relationships between redox budget (RB), convergence rate, and time (e.g., Inoue, 1994), and should alter the relative
since initiation of subduction. melt/residue partition coefficients of ferric and
ferrous iron. Fe2+/Fe3+ in silicate melts is linearly
correlated with the degree of polymerization
(Mysen et al., 1985), and the addition of water
TABLE 1. SUMMARY OF CORRELATION COEFFICIENTS
is thought to depolymerize melts (e.g., Zotov
et al., 1996; Zotov and Keppler, 1998). Thus,
Redox budget Convergence Age of Total length V/Sc
(RB) all subduction (n = 57) Fe3+/Fe2+ in a dry melt should be less than in a
(n = 158) wet melt derived from a parent rock with the
RB (average, n = 8) n.a. 0.96 0.79 0.96 n.a. same redox budget, and would produce a lower
RB (all, n = 158) - 0.66 0.55 0.67 0.1 apparent calculated fO , as the effects of water
2
Convergence - - 0.82 n.a. 0.25 in the source are not accounted for in current
Age of subduction - - - n.a. 0.24 oxybarometers, which are based on experiments
Total length - - - - 0.21
on dry systems. Thus mantle that has undergone
Note: Bold—probability that there is no relationship is <0.0005; italics—probability that there is no relationship prolonged addition of subduction components
is >0.05; n.a.—not applicable.
that include water and potassium might produce

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melts with higher apparent fO values than melt sution, A., 2002, Geochemical trends across an Mysen, B.O., Virgo, D., Neumann, E.R., and Seifert,
2
from water-poor mantle. arc-continent collision zone: Magma sources F.A., 1985, Redox equilibria and the structural
and slabwedge transfer processes below the states of ferric and ferrous iron in melts in the
Pantar Strait volcanoes (Indonesia): Geochi- system CaO-MgO-Al2O3-SiO2-Fe-O—Rela-
CONCLUSIONS mica et Cosmochimica Acta, v. 66, p. 2771– tionships between redox equilibria, melt struc-
Olivine-spinel oxybarometry on primitive arc 2789, doi:10.1016/S0016-7037(02)00868-2. ture and liquidus phase-equilibria: American
basalts shows that these basalts are more oxi- Evans, K.A., 2006, Redox decoupling and redox bud- Mineralogist, v. 70, p. 317–331.
dized than MORBs or OIBs, with the implication gets: Conceptual tools for the study of earth sys- Newton, R.C., and Manning, C.E., 2005, Solubility
tems: Geology, v. 34, p. 489–492, doi:10.1130 of anhydrite, CaSO4, in NaCl-H2O solutions at
that subarc mantle is 1–4 log units more oxidized /G22390.1. high pressures and temperatures: Applications
than the MORB or OIB source. Redox budgets Evans, K.A., 2012, The redox budget of subduction to fluid-rock interaction: Journal of Petrol-
of primitive arc basalts correlate strongly with zones: Earth-Science Reviews, v. 113, p. 11–32, ogy, v. 46, p. 701–716, doi:10.1093/petrology
the age of subduction zones and convergence doi: 10.1016/j.earscirev.2012.03.003. /egh094.
Evans, K.A., and Tomkins, A., 2011, The relationship Parkinson, I.J., and Arculus, R.J., 1999, The redox
rate. These observations support a causal link between subduction zone redox budget and arc state of subduction zones: Insights from arc-
between subduction and the increased ferric iron magma fertility: Earth and Planetary Science peridotites: Chemical Geology, v. 160, p. 409–
content of minerals and whole rocks in primitive Letters, v. 308, p. 401–409, doi:10.1016/j.epsl 423, doi:10.1016/S0009-2541(99)00110-2.
arc outputs. However, resolution of the current .2011.06.009. Pearce, J.A., and Peate, D.W., 1995, Tectonic im-
controversy regarding subarc mantle redox state Frost, B.R., and Ballhaus, C., 1998, Constraints on plications of the composition of volcanic arc
the origin of the oxidation state of mantle over- magmas: Annual Review of Earth and Plan-
requires further work. lying subduction zones: An example from Sim- etary Sciences, v. 23, p. 251–285, doi:10.1146
coe, Washington, USA: Comment: Geochi- /annurev.ea.23.050195.001343.
ACKNOWLEDGMENTS mica et Cosmochimica Acta, v. 62, p. 329–331. Rowe, M.C., Kent, A.J.R., and Nielsen, R.L., 2009,
Evans acknowledges research funding from a Gill, J.B., 1981, Orogenic andesites and plate tecton- Subduction influence on oxygen fugacity and
Curtin Research and Teaching Fellowship, The In- ics: Berlin, Springer Verlag, 401 p. trace and volatile elements in basalts across the
stitute for Geoscience Research (TIGeR publication Inoue, T., 1994, Effect of water on melting phase- Cascade Volcanic Arc: Journal of Petrology,
411), and Australian Research Council Discovery relations and melt composition in the system v. 50, p. 61–91, doi:10.1093/petrology/egn072.
Grant DP1094075. We thank Ron Frost, Bruce Yard- Mg2SiO4-MgSiO3-H2O up to 15 GPa: Physics of Snyder, D., Carmichael, I.S.E., and Wiebe, R.A.,
ley, Jim Mungall, Hugh O’Neill, and Roger Powell the Earth and Planetary Interiors, v. 85, p. 237– 1993, Experimental study of liquid evolution
for discussions. 263, doi:10.1016/0031-9201(94)90116-3. in an Fe-rich, layered mafic intrusion—Con-
Hermann, J., and Spandler, C.J., 2008, Sediment melts straints of Fe-Ti oxide precipitation on the
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