Geochemistry

Geophysics
Geosystems

Article
Volume 5, Number 4
7 April 2004
Q04J10, doi:10.1029/2003GC000660

AN ELECTRONIC JOURNAL OF THE EARTH SCIENCES

Published by AGU and the Geochemical Society

ISSN: 1525-2027

Tracing magma sources in an arc-arc collision zone:

Helium and carbon isotope and relative abundance
systematics of the Sangihe Arc, Indonesia
Lillie A. Jaffe and David R. Hilton
Fluids and Volatiles Laboratory, Scripps Institution of Oceanography, University of California San Diego, La Jolla,
California 92093-0244, USA (ljaffe@ucsd.edu; drhilton@ucsd.edu)

Tobias P. Fischer
Department of Earth and Planetary Sciences, University of New Mexico, Albuquerque, New Mexico 87131, USA
(fischer@unm.edu)

Udi Hartono
Geological Research and Development Centre, Jl. Diponegoro 57, Bandung 40122, Indonesia

[1] The Sangihe Arc is presently colliding with the Halmahera Arc in northeastern Indonesia, forming the
worlds only extant example of an arc-arc collision zone. We report the first helium and carbon isotopic and
relative abundance data from the Sangihe Arc volcanoes as a means to trace magma origins in this
complicated tectonic region. Results of this study define a north-south trend in 3He/4He, CO2/3He, and
d13C, suggesting that there are variations in primary magma source characteristics along the strike of the
arc. The northernmost volcanoes (Awu and Karangetang) have higher CO2/3He and d13C (up to 179
109
and 0.4%, respectively) and lower 3He/4He (5.4 RA) than the southernmost volcanoes (Ruang,
Lokon, and Mahawu). Resolving the arc CO2 into component structures (mantle-derived, plus slab-derived
organic and carbonate CO2), the northern volcanoes contain an unusually high (>90%) contribution of CO2
derived from isotopically heavy carbonate associated with the subducting slab (sediment and altered
oceanic basement). Furthermore, the overall slab contribution (CO2 of carbonate and organic origin)
relative to carbon of mantle wedge origin is significantly enhanced in the northern segment of the arc.
These observations may be caused by greater volumes of sediment subduction in the northern arc, alongstrike variability in subducted sediment composition, or enhanced slab-derived fluid/melt production
resulting from the superheating of the slab as collision progresses southward.
Components: 9627 words, 3 figures, 2 tables.
Keywords: arc geochemistry; carbon isotopes; helium isotopes; mantle cycling; Sangihe Arc; volatiles.
Index Terms: 1030 Geochemistry: Geochemical cycles (0330); 1040 Geochemistry: Isotopic composition/chemistry; 1025
Geochemistry: Composition of the mantle; 8499 Volcanology: General or miscellaneous.
Received 6 November 2003; Revised 25 February 2004; Accepted 3 March 2004; Published 7 April 2004.
Jaffe, L. A., D. R. Hilton, T. P. Fischer, and U. Hartono (2004), Tracing magma sources in an arc-arc collision zone: Helium
and carbon isotope and relative abundance systematics of the Sangihe Arc, Indonesia, Geochem. Geophys. Geosyst., 5,
Q04J10, doi:10.1029/2003GC000660.

Theme: Trench to Subarc: Diagenetic and Metamorphic Mass

Guest Editors: Gray Bebout, Jonathan Martin, and Tim Elliott
Copyright 2004 by the American Geophysical Union

1 of 17

Geochemistry
Geophysics
Geosystems

jaffe et al.: tracing magma sources

1. Introduction
[2] The study of helium and carbon in arc-related
volcanic emissions has provided a wealth of information on the subduction process and its involvement in geochemical cycling between the terrestrial
mantle and the crust, hydrosphere and atmosphere.
For example, the flux of various volatile species
(including CO2) from subduction zones can be
estimated through knowledge of the arc-related
primordial 3He flux [Torgersen, 1989; Allard,
1992] and measurement of the relevant elemental
ratio (xi/3He) where xi = element of interest (see
review by Hilton et al. [2002]). In the case of CO2,
it is possible to resolve the output flux into constituent components (slab-related versus mantle
wedge contributions) through the use of modeled
end-member compositions with specific He and
CO2 isotopic and relative abundance characteristics
[Marty et al., 1989; Varekamp et al., 1992; Sano
and Marty, 1995]. Helium and carbon (isotopes
and/or relative abundances) can also be used to
identify regional tectonic controls on magma genesis, as in the case of the Sunda-Banda arcs of
Indonesia [Hilton and Craig, 1989; Hilton et al.,
1992; Varekamp et al., 1992], including recognizing crustal influences and their contribution to arcrelated magmatism [Gasparon et al., 1994].
[3] In this contribution, we apply the He-C approach to geothermal fluids collected at active
volcanic centers along the Sangihe Arc of northeastern Indonesia. The Sangihe Arc is unusual
because it is part of a conjugate pair of arcs, located
on either side of the Molucca Sea Plate, which are
in the process of colliding (Figure 1). The Sangihe
and Halmahera arcs are the only extant example of
an arc-arc collision zone. Although data are available on major element chemistry of arc rocks in
this region [e.g., Tatsumi et al., 1991; Elburg and

10.1029/2003GC000660

Foden, 1998; Macpherson et al., 2003], there is

little information on the composition of subducted
components. For example, there are no major or
trace element studies on Molucca Sea sediment,
nor is there any record of the composition of the
Molucca Sea basement (as it has been subducted).
Therefore, to identify various contributions to
magmagenesis in the region, prior studies have
had to approximate the composition of (a) Molucca
Sea sediments (major and trace elements and isotopes), using sedimentary analogs from the Philippines, SW Pacific and Banda Arc, and (b) crustal
basement, using material from the Celebes Sea [see
Elburg and Foden, 1998]. In this work, we target
He and CO2 characteristics in the volcanic arc
output of this remote arc setting, with the aim of
characterizing slab-related sources by considering
the gross (volatile) systematics of the subducted
components (both the oceanic crustal basement and
its sedimentary veneer). In this respect, the present
study represents an attempt to utilize geothermal
fluids of the Sangihe Arc to reveal the characteristics of volatiles from the underlying source region. A related aim is to assess if along-strike
variations exist in the He-C characteristics. Such
variations may reflect heterogeneity in the composition of slab-related inputs, and thus provide
information related to the tectonic development
of the region.

2. Geological and Tectonic Background

[4] There are four major lithospheric plates which
interact in the Molucca Sea region of northern
Indonesia: the Eurasian Plate to the west, the
Philippine Plate to the east, the Australian Plate
to the south, and the Molucca Sea Plate trapped in
the center (Figure 1a). The Molucca Sea Plate is
highly unusual in that it is being subducted beneath
both the Eurasian and Philippine Sea plates giving

Figure 1. Map of the Molucca Sea region, southeast Asia (modified from Macpherson et al. [2003]). Small, solid
triangles are active volcanoes from the Smithsonian Institutions database. Bathymetric contours are at 200, 2000,
4000, and 5000 m. (b) Detailed map of the Sangihe Arc. Open triangles representing volcanoes sampled during
the course of this work. (c) Cross section of the collision zone [from Macpherson et al., 2003]. Note that in subfigures
(a) and (b), barbs on each side of the Molucca Sea represent (1) direction of thrust in the Sangihe fore-arc region and
(2) direction of subduction of the Halmahera Arc beneath the Sangihe Arc (see section 2 and Macpherson et al.
[2003] for further explanation).
2 of 17

Geochemistry
Geophysics
Geosystems

jaffe et al.: tracing magma sources

10.1029/2003GC000660

Figure 1.
3 of 17

Geochemistry
Geophysics
Geosystems

jaffe et al.: tracing magma sources

rise to two converging, subparallel volcanic arcs: the

Sangihe Arc in the west and the Halmahera Arc in
the east (Figures 1b and 1c). Seismic data indicate
that the Benioff-zone extends as much as 600 km
below the Sangihe Arc, at an approximate dip angle
of 45, and up to 250 km below the younger
Halmahera Arc subducting in the opposite direction
at approximately 40 [Hatherton and Dickinson,
1969; Silver and Moore, 1978; Lallemand et al.,
1998]. The mean convergence rates of the Sangihe
and Halmahera arcs are 4 cm/yr and 3 cm/yr,
respectively, on the basis of seismic and chronological constraints [Lallemand et al., 1998].
[5] The origin of the Molucca Sea Plate can be
traced to the collision of the Philippine Sea Plate
with the Australian Plate approximately 25 Ma
ago, trapping a piece of Indian Ocean lithosphere
that attached to, and moved with, the Philippine
Sea Plate: this fragment became the Molucca Sea
Plate [Hall, 1996]. Subduction on the western
side, forming the Sangihe Arc, probably began
soon after collision. Eastward subduction of the
Molucca Sea Plate began about 15 Ma ago when
collision of the Snellius Plateau with the SangihePhilippine Arc system forced a subduction reversal, breaking the Molucca Sea Plate away from the
Philippine Sea Plate and forming the Halmahera
Arc [Hall and Nichols, 1990; Hall, 1996].
[6] There is presently no surface remnant of the
Molucca Sea Plate basement other than the thick
collision complex consisting of the melange wedges
of the two arcs [Silver and Moore, 1978]. This
wedge of unconsolidated and deformed Tertiary
sediments, up to 15 km in thickness, is composed
of volcaniclastic and continental debris, including
peridotite, serpentinite, gabbro, basalt, chert, limestone, and greywacke [Silver and Moore, 1978;
Hamilton, 1979; Sukamto, 1979], generated primarily by the continuous and ongoing collision of the
Halmahera and Sangihe arcs [Silver and Moore,
1978; McCaffrey et al., 1980].
[7] The Sangihe Arc is the oldest extant subduction
zone in the Philippine-Indonesia region: subduction-related rocks about 25 Ma old [Dow, 1976;
Effendi, 1976; Apandi, 1977; Priadi, 1993] have
been reported in the northeastern arm of Sulawesi.

10.1029/2003GC000660

Whereas the southern portion of the arc ends at the

left-lateral Sorong Fault (Figure 1a), the northern
termination is marked by the collision of eastern
and western Mindanao about 45 Ma ago [Pubellier et al., 1991]. The present-day active arc ceases
at 4N; however, the extinct margin extends to
5.5N [Lallemand et al., 1998; Widiwijayanti et al.,
2003], with lavas in central Mindanao thought to be
of Sangihe origin [Pubellier et al., 1991]. This
northern collision region is further complicated by
back-arc thrusting along the Cotobato Trench in the
west and the Philippine Trench in the east, leaving
dissected remnants of the Sangihe (and Halmahera)
arcs on Mindanao Island and the Talaud Ridge
[Morrice et al., 1983]. Post-collisional volcanism
remains active in central Mindanao (i.e., the relic
Sangihe Arc) as a result of the continuing subduction of portions of the Halmahera Arc [Pubellier et
al., 1991, 1999]. While the active portions of the
Sangihe and Halmahera arcs are currently several
hundred kilometers apart, the northern collision is
propagating southward and will continue until the
Halmahera Arc accretes onto the Eurasian margin
[Hall and Nichols, 1990].
[8] The active Sangihe Arc can be divided into two
segments: four volcanic islands north of the large
island province, Sulawesi, and eight volcanoes in
northeastern Sulawesi (see Figure 1b). The active
volcanoes in the northern segment of the arc (Awu,
Banua Wahu, Karangetang, and Ruang) occur about
50 km apart along a north-south transect. The
onshore active Sangihe Arc volcanoes (Tongkoko,
Mahawu, Lokon-Empung, and Soputan) are spaced
less regularly. Four other volcanoes, morphologically young and hydrothermally active (Duasudara,
Klabat, Manado Tua, and Ambang), also lie along
the southern portion of the arc. Lavas erupted along
the chain are mostly typical island arc volcanics
(basaltic andesite to andesite) with the exception of
Soputan that produces olivine-rich basalt [Morrice
et al., 1983]. The active Sangihe Arc is bounded by
Awu volcano in the north and Ambang in the south.

3. Sampling and Analytical Protocols

[9] In order to characterize the helium and carbon
systematics of the Sangihe Arc, we collected geo4 of 17

Geochemistry
Geophysics
Geosystems

jaffe et al.: tracing magma sources

thermal fluids (fumaroles, gas emanations from

bubbling springs, and thermal spring waters), and
olivine- and/or pyroxene-rich lavas from seventeen
different localities covering seven active volcanic
centers along the north-south strike of the arc.
Collection of geothermal samples was facilitated
by use of a Ti-tube or inverted plastic funnel [after
Giggenbach and Goguel, 1989], and samples were
stored in either AR-glass bottles or cold-welded
annealed copper tubes for transfer back to the
laboratory. Normal sampling precautions were
taken to minimize the possibility of air contamination [see Hilton et al., 2002].
[10] In the laboratory, samples were extracted using instrumentation and procedures described previously [Kulongoski and Hilton, 2002; Shaw et al.,
2003]. Briefly, all fluid samples were released into
an ultra-high vacuum system consisting of a series
of traps held at different temperatures, thus separating water vapor from the condensable (mainly
CO2) and noncondensable gases. The noncondensable fraction was aliquoted into an AR-glass breakseal for transfer to a noble gas mass spectrometer
(MAP215) for He isotopic and He and Ne relative
abundance analyses. The condensable fraction was
transferred to a separate vacuum line for further
purification, and the total amount of CO2 was
measured manometrically. A fraction of the purified CO2 was then collected in another breakseal
for isotopic analysis (using a VG Prism mass
spectrometer).
[11] Rock samples were prepared by crushing and
sieving into various grain sizes. Olivine and pyroxene mineral grains, ranging in diameter from
8501700 mm, were hand-picked from the appropriate size fraction, and ultrasonically cleaned
using a 50/50 methanol/acetone solution. Olivine
and pyroxene grains were loaded separately into
on-line, electro-magnetic crushers (see description
by Scarsi [2000]) attached to the MAP215 to
release volatiles for measurement.
[12] Prior to inlet into the noble gas mass spectrometer, all samples underwent a purification procedure designed to isolate the He and Ne fractions
by a combination of active gas gettering, sorption
onto charcoal at liquid nitrogen temperatures and

10.1029/2003GC000660

cryogenic separation using a liquid He cooled trap.

Isotopic measurements were made in static mode,
and either an air or a 3He-rich standard (Murdering
Mudpots (Yellowstone) = 16.45 RA where RA = air
3
He/4He) was used for normalization.

4. Results
[13] Helium and carbon isotopic and relative abundance characteristics of 28 samples (26 geothermal
fluids and 2 phenocrysts) from the Sangihe volcanic arc are given in Table 1. Samples cover
7 distinct volcanic centers (3 offshore and 4 onshore). Results from each volcanic center, listed
from north to south, are discussed in turn.

4.1. Awu Volcano (Sangihe Island)

[14] Two different crater localities were sampled.
The fumarole samples (from location 1) have airlike 3He/4He (1 RA) and low He/Ne values (X  2,
where X is the air-normalized He/Ne value multiplied by the ratio of the Bunsen coefficients; see
Table 1 footnote). The second locality (location 2)
was a bubbling spring located in the crater lake
close to the shore: this gas sample has a He isotope
value of 6.2 RA with an X value of 55. The CO2/3He
value of the spring is 117
109. Its d13C value is
0.4%.

4.2. Karangetang Volcano (Siau Island)

[15] Two coastal volcano flank thermal spring
localities were sampled, with both Temboko
(6.4 RA) and Lehi (5.4 RA) showing a dominantly
magmatic He input, albeit with a significant air
correction (X  12). One sample (IND-17) has an
anomalously high d13C value of +1.3%; however,
the other two samples have CO2/3He values between
6.4 and 17.9 (
109) and have similar d13C values
of 2%. The pyroxene mineral separate from
Sang01-40 has a 3He/4He ratio 4.9 RA; slightly
lower than the thermal spring samples.

4.3. Ruang Volcano (Tagulandang Island

Group)
[16] Two summit fumarole localities were sampled,
with one characterized by a 3He/4He ratio of 7.0 RA
(X = 470). The other locality has a greater degree
5 of 17

fm
fm
sf
sf
sf

fm
fm
fm
fm
ol

sf
sf
sg
sg
sg
sg

0 44.9060
"
"
"
0 42.9400

1 7.1220
"
1 7.5290
"
"

1 20.8710
"
1 16.1490
"
1 15.9710
"

124 25.2800
"
"
"
124 22.1820

124 44.2880
"
124 44.6460
"
"

124 50.8750
"
124 49.3230
"
124 49.0580
"

124 47.9820
"

1 21.8270
"

1317
"
"
"
494

1708
"
1426
"
"

897
"
832
"
777
"

1109
"

691
688

0
0
"
"

1278
"
"
"

Elev,
m

97.6
"
89.7
"
46.9

72.9
"
86.9
"
"

35.9
"
101.1
"
61.9
"

96.1
"

97.9
140

68.7
48.8
"

96.6
"
"

T, C

0.06
0.06
0.07
0.39

0.01
0.01
0.02
0.07

4.63
4.59
3.68
3.27
3.97

1.07
1.04
0.95
1.02
5.33

7.33
7.11
7.32
7.04
7.23
6.90

0.07
0.04
0.09
0.10
0.06

0.02
0.01
0.02
0.01
0.15

0.11
0.08
0.07
0.08
0.09
0.09

7.11 0.06
7.27 0.06

3.55 0.03
6.97 0.07

5.49
4.73
4.99
4.42

1.00
1.22
1.08
6.12

RM/RAc

924
713
30.0
349
27.8

2.66
2.38
2.59
2.50
78.7

37.7
68.9
2741
2159
2557
1062

833
885

6.41
470

5.77
11.8
11.3
8.72

2.42
2.27
2.18
55.0

Xd

0.08
0.07
0.08
0.50

0.01
0.02
0.02
0.08

0.12
0.08
0.10
0.10
0.14
0.10

4.64
4.60
3.77
3.27
4.08

0.07
0.04
0.10
0.22
0.06

1.11 0.02
1.07 0.01
0.93 0.02
1.03 0.01
5.39 0.34

7.50
7.20
7.33
7.04
7.23
6.91

7.12 0.07
7.27 0.06

4.02 0.04
6.99 0.07

6.43
5.08
5.37
4.86

1.00
1.39
1.14
6.22

RC/RAe,f

5.7 0.1
6.45 0.08
590 20
140 10
292 5

0.69 0.01

0.113 0.002
0.143 0.002

53.8 1
6.44 0.08
5.07 0.09
5.37 0.09
5.8 0.1
5.8 0.1

4.41 0.05
8.4 0.1

1.49 0.08
2.83 0.04

63.8 0.9
27.5 0.4
179 3

31.3 0.4
108 1
96 2
117 2

CO2/3He (
109)f

= Copper tube, others are rock samples.

fluid phase; sg, thermal spring gas phase; fm, fumarole; sl, solfatara fumarole; ol, olivine; px, pyroxene.
RM/RA = measured He/ He (RM) in sample relative to air 3He/4He (RA). Error is 1s.
d
X = [(He/Ne)sample/(He/Ne)air]
1.209 (i.e., the air-normalized He/Ne ratio multiplied by bNe/bHe = 1.209 - the ratio of the Bunsen coefficients at 17C).
e
RC/RA = air-corrected 3He/4He (RC) in sample relative to air (RA). RC/RA = [(RM/RA)X  1]/(X  1).
f
Values in italics have been removed from the discussion; they are considered unrepresentative of primary magmatic source (see section 5.1).
g
Errors on d13C are less than 0.5%, based on replicate analyses.
h 4
[ He] per gram of water in fluid samples, and per gram of mineral in rock samples.

a
IND-## = AR-glass bottle, I-###
b
Abbreviations: sf, thermal spring
c
3
4

Bonkurai

IND-9
I-198
IND-10
I-193
IND-11

IND-12
I-016
IND-13
IND-14
SOP-1

I-150
IND-3
IND-4
IND-5
IND-6
IND-7

fm
fm

IND-1
I-159

125 22.1150
125 22.1000

125 22.1110
125 22.6030
"
"

2 46.3370
2 45.4870
"
"
2 18.1870
2 18.2200

125 27.2320
"
"
"

Long, E

3 40.4890
"
"
"

Lat, N

5.2
4.5
2.3
4.3
4.7

3.5

19.9
20.1

6.8
5.7
3.5
3.4
3.0
3.3

3.6

3.3
3.1

2.0
1.3
2.0

2.0
1.5
1.3
0.4

d13C, %f,g

88.5
97.3
252.7

3.05

256.0
2190

309.1
312.2
206.2
0.28

[4He]/gh
(
109 cm3 STP)

jaffe et al.: tracing magma sources

Crater Loc. 2

Ambang
Crater Loc. 1

Aeseput
(flank cone)

Soputan
Crater

Lahendong 2

Lahendong 1

Mahawu
Kakaskasen

sl
sl

sf
sf
sf
px

IND-18
IND-17
I-021
Sang01-40

IND-19
IND-20

fm
fm
fm
sg

Typeb

IND-15
IND-16
I-048
I-043

Samplea

Ruang
Crater Loc. 1
Crater Loc. 2
Lokon
Crater

Crater Loc. 2
Karangetang
Temboko
Lehi

Awu
Crater Loc. 1

Volcano

Table 1. Helium and Carbon Results Along the N-S Strike of the Sangihe Arc (Sampled in 2001)

Geochemistry
Geophysics
Geosystems

10.1029/2003GC000660

6 of 17

Geochemistry
Geophysics
Geosystems

jaffe et al.: tracing magma sources

10.1029/2003GC000660

of air contamination (X = 6.41) and its 3He/4He

ratio is significantly lower (3.6 RA). Although the
air-corrected 3He/4He ratios are dissimilar (4.0 and
7.0 RA), there is good agreement between d13C
values (3%) for the two localities. In addition,
the two CO2/3He ratios 1.52.8 (
109) fall within
a narrow range.

summit thermal fluid locality gave lower 3He/4He

ratios (3.3 RA and 3.8 RA), and higher d13C
(4.3% and 2.3%) and CO2/3He (140
109
and 590
109) values. The flank thermal spring
locality at Bonkurai has intermediate 3He/4He (4.1
RA), CO2/3He (292
109) and d13C (4.7%)
values.

4.4. Lokon Volcano (North Sulawesi)

5. Discussion

[17] He/ He values of duplicate samples from a

single fumarole locality at Lokon volcano showed
excellent agreement (7.2 0.1 RA). Air contamination in each case was negligible (X > 800).
CO2/3He ratios are 48 (
109) and the single d13C
value is 3.6%.

4.5. Mahawu Volcano (North Sulawesi)

[18] Two different localities in the vicinity of
Mahawu volcano were sampled: the Lahendong
geothermal complex (including thermal resort) and
a remote thermal spring locality at Kakaskasen.
Consistent results were obtained for all samples
with the exception of one duplicate from Kakaskasen (see below). 3He/4He ratios are 6.97.5 RA and
CO2/3He values lie between 5 and 6 (
109). One
sample from Kakaskasen has an anomalously high
CO2/3He ratio of 54
109. d13C values for
Lahendong are tightly constrained at 3.3%,
whereas Kakaskasen values are significantly lower
(5.8 to 6.8%).

4.6. Soputan Volcano (North Sulawesi)

[19] All fumarole samples from the summit of
Soputan have air-like values (3He/4He  1 RA;
X  2.5). The flank cinder cone Aeseput samples
also had air-like He isotopes (3He/4He  1 RA;
X  2.5). The olivine crystals, separated from the
ash sample, gave a 3He/4He ratio of 5.4 RA.

4.7. Ambang Volcano (North Sulawesi)

[20] Two localities were sampled on the summit of
Ambang Volcano, and one on the volcano flank.
The summit fumarole locality gave consistent
3
He/4He ratios of 4.6 RA for 2 samples, with good
agreement in both CO2/3He (5.7
109 and 6.4

109) and d13C values (4.5% and 5.2%). The

[21] There are three principal contributors to the

inventory of magmatic volatiles at arc-related settings: the subducted crustal basement, its overlying
sedimentary veneer and the mantle wedge above
the slab. The atmosphere as well as the arc lithosphere through which magma erupts are also potential sources of volatiles; although these sources
are generally regarded as contamination and unrelated to the magma source of volatiles. Therefore,
in order to quantify the various contributors of
volatiles to these magmas, and to recognize any
extraneous additions to, or modifications from,
source characteristics, it is essential to adopt various criteria that differentiate samples that possess
intrinsic magma characteristics from those that
have been modified by air contamination, crustal
assimilation, degassing, and/or sampling error. To
this end, we adopt a number of criteria in the
following section aimed at assessing the integrity
of each individual sample to preserve its primary
source signature. Only after we have applied this
filter can we relate the He-C systematics of the
Sangihe Arc to the tectonic framework of the
region.

5.1. Identifying Samples With Modified

He-C Characteristics
5.1.1. Air-Like 3He//4He and He//Ne Values
[22] There are a total of 7 geothermal samples with
air-like 3He/4He and He/Ne values (Table 1). These
are: all three samples from Awu crater fumaroles
(location 1; IND-15, IND-16, I-048) and all four
samples from Soputan fumaroles (from the main
crater and the Aeseput flank cone; IND-12, I-016,
IND-13, IND-14). In both cases, the diffusely flowing fumaroles could have entrained air through the
7 of 17

Geochemistry
Geophysics
Geosystems

jaffe et al.: tracing magma sources

highly altered (Awu) or porous and blocky (Soputan) material covering the fumarole discharge sites.

5.1.2. Low 3He//4He: Indications of

Radiogenic Crustal Influence
[23] Helium isotopic ratios in arc-related settings
around the circum-Pacific region generally fall
between 68 RA [Poreda and Craig, 1989]. A
more recent compilation of arc 3He/4He data
[Hilton et al., 2002] has produced an average value
of 5.4 RA for all arcs worldwide. As He isotopes
are a sensitive tracer of volatiles of crustal provenance [Hilton et al., 1993; Gasparon et al., 1994],
we suspect that 3He/4He less than the average value
cited above may have incorporated a significant
radiogenic He contribution, thus masking the magmatic source ratio. For this reason, we reject all five
Ambang samples (IND-9, IND-10, IND-11, I-198,
and I-193), as their 3He/4He are less than 4.6 RA.
We reject the pyroxene separate from Karangetang
(Sang01-40), and the olivine sample from Soputan
(SOP-1) as they also have low 3He/4He values.

5.1.3. High CO2/ 3He Values: Indications of

Fractionation in the Hydrothermal System
[24] The average CO2/3He ratio of arc-related volcanism is 15 11 (
109) [Sano and Marty, 1995;
Sano and Williams, 1996]. Significant deviations
from this value are usually indicative of fractionation of He from C [van Soest et al., 1998; Hilton
et al., 2002]. In the case of geothermal (aqueous)
fluids, the greater solubility of C relative to He [see
Stephen and Stephen, 1963] can lead to higher
CO2/3He values in the residual phase following
vapor formation or other gas loss event. Both van
Soest et al. [1998] and Shaw et al. [2003] report
significantly higher CO2/3He ratios in gases dissolved in thermal waters compared to gas phase
samples collected at the same locality. This observation is consistent with the notion that free gas
samples provide a more robust means of sampling
the intrinsic CO2/3He value of a degassing magma
body whereas gases dissolved in waters may represent (fractionated) volatiles residual from a
degassing event. The current data set allows us to
make the same comparison between liquid and gas
phase CO2/3He values.

10.1029/2003GC000660

[25] Unusually high CO2/3He ratios are measured

in Ambang and Karangetang geothermal fluid
samples. Three Ambang geothermal fluid phase
samples (IND-10, I-193, and IND-11; average
CO2/3He  340
109) had significantly higher
CO2/3He values than their gas-phase counterparts
from the same locality (IND-8, IND-9, and I-198;
average CO2/3He  4.5
109). Likewise, one
Karangetang thermal spring fluid phase sample (I021) has a high CO2/3He value (179
109) when
compared with the other fluid phase sample from
the same locality (IND-17 CO2/3He = 27.5
109).
These differences between gas and fluid phase
CO2 /3 He values suggest that the fluid phase
CO2/3He represents volatiles that have been modified due to fractionation most likely by vapor
formation in the geothermal fluid system. Therefore we omit four samples with anomalously high
CO2/3He values from further consideration.

5.1.4. Atypical D13C Values: Additional

Indications of Alteration in the
Hydrothermal System
[26] Although agreement in d13C between duplicate samples is generally good (see Table 1), there
is one locality (Karangetang volcano) with samples
showing markedly different d13C values. One sample (IND-17) has an unusual d13C value of +1.5%
that is very different from its duplicate (I-021)
(d13C = 2.0%). We can find no analytical reason
for the discrepancy. However, we note that given
the observation [e.g., Sano and Williams, 1996]
that almost all arc-related d13C values are negative
(reflecting end-member mixtures of CO2 which are
all 0%) then this positive value is clearly anomalous. Consequently, we reject it from further
consideration.
[27] Likewise, we measure exceptionally low d13C
values in two samples from Soputan volcano: the
two Aeseput samples (IND-13 and IND-14) have
exceptionally low d13C values of 20%. This
observation, coupled with air-like He-isotope
ratios, leads us to believe that these samples have
been compromised. Interestingly, the carbon is not
air-like (air CO2 has a d13C 8% [Keeling,
1984]). Prolonged outgassing may be responsible
for these extraordinarily light C isotope ratios
8 of 17

Geochemistry
Geophysics
Geosystems

jaffe et al.: tracing magma sources

[Gerlach and Taylor, 1990]. Again, we remove

these values from further consideration.

5.1.5. Poor Agreement Between Duplicate

Samples
[28] There are a number of samples that show poor
agreement between duplicate samples. For example, the 3He/4He ratio of IND-19 from location 1 in
Ruang crater is rejected as a result of its low He/Ne
and 3He/4He ratios compared to a duplicate sample
(IND-20) collected at the same locality. Similarly,
sample I-150 from Kakaskasen (Mahawu volcano)
has an anomalously high CO2/3He value (53.8

109), approximately ten times that of a duplicate
from the same locality (6.4
109), and other
samples from the same volcano (5.5
109).
Additionally, its d13C value, and the d13C value
of its duplicate (IND-3), is much lower than other
samples from Mahawu (average d13C = 3.3%). It
seems reasonable therefore to assume that both
samples from Kakaskasen do not reflect the primary magma sources in the region.

5.1.6. Summary
[29] Out of a total of 26 geothermal fluid samples
that were collected along the strike of the Sangihe
Arc, 15 samples have experienced sufficient modification that both their He and C systematics no
longer reflect primary magma characteristics.
These samples are: IND-15, IND-16, I-048
(Awu); IND-17 (Karangetang); I-150, IND-3
(Mahawu); IND-12, I-016, IND-13, IND-14
(Soputan); and IND-9, I-198, IND-10, I-193,
IND-11 (Ambang). Of the remaining 11 samples,
there is no evidence of modification for either He
or C for the following nine: I-043 (Awu); IND-18
(Karangetang); IND-20 (Ruang); IND-1, I-159
(Lokon); IND-4, IND-5, IND-6, IND-7 (Mahawu).
The remaining 2 samples have unmodified data for
either He or C (CO2/3He and d13C) but not both.

5.2. Along-Strike Variations in He-C

Characteristics
[30] In this section, all interpretations are based
on the filtered data from section 5.1. Figure 2
shows 3He/4He, CO2/3He and d13C as a function
of latitude along the Sangihe Arc. Here, we

10.1029/2003GC000660

consider both variations along-strike as well as

the magnitude of the absolute values in relation to
averages of arc-related volcanism and MORB
worldwide.

5.2.1. The 3He//4He Variations

[31] The majority of arc-related volcanism is characterized by 3He/4He values coincident with that
found in MORB mantle [Poreda and Craig, 1989;
Hilton et al., 2002]. Some localities, however,
record the addition of radiogenic He, either through
slab-derived contributions [Hilton and Craig,
1989; Hilton et al., 1992; Marty et al., 1994]
and/or contamination by arc crust [Hilton et al.,
1993; Gasparon et al., 1994]. If the filtered database (section 5.1) allows consideration of magmatic 3He/4He characteristics only, then the Sangihe
Arc comprises relatively low values in the northern
section of the arc (Awu and Karangetang; 5.4
6.4 RA) versus more typical arc-like values in the
southern segment (Ruang, Lokon and Mahawu;
6.97.5 RA). Addition of a small radiogenic He
component to magmas of the northern Sangihe Arc
may reflect contributions from either the subducted
sedimentary veneer, its underlying oceanic basement or the overlying arc crust. It seems unlikely
that sediments have the transport capacity (due to
diffusional losses) to subduct He [Hilton et al.,
1992; Hiyagon, 1994] so we can discount this
possibility with a fair degree of confidence. Preliminary trace element and Sr-Nd-Pb data do not
show any evidence for upper-crustal contamination
along the entire strike of the Sangihe Arc [van der
Meer et al., 2002]. This observation is in contrast
to the southern Lesser Antilles Arc where low
3
He/4He ratios are accompanied by radiogenic Sr
and Pb isotope ratios [van Soest et al., 1998, 2002].
In the absence of any other constraints, therefore,
we conclude that the source of radiogenic He in
northern Sangihe Arc magmas may be the subducted crustal basement which modifies 3He/4He
values to below typical arc values (see further
discussion in section 5.4).

5.2.2. The CO2/ 3He Variations

[32] In a manner similar to the He isotope distribution, CO2/3He values of geothermal samples
9 of 17

Geochemistry
Geophysics
Geosystems

jaffe et al.: tracing magma sources

10.1029/2003GC000660

Figure 2. Latitudinal variations (from south to north) in (a) air-corrected He-isotope ratios (RC/RA notation),
(b) CO2/3He ratios, and (c) C-isotope ratios (% relative to PDB) for geothermal fluids and phenocrysts from the
Sangihe Arc, Indonesia. All errors fall within symbols except where indicated by error bars. Worldwide arc 3He/4He
average of 5.4 RA (dotted line) and MORB range (8 1 RA) from Hilton et al. [2002]. Worldwide arc average
CO2/3He value (15.7 11.0
109) from Sano and Williams [1996] and average MORB d13C of 6.5 2.3% from
Sano and Marty [1995]. Volcano location listed by letter: Am, Ambang; S, Soputan; M, Mahawu; L, Lokon; R,
Ruang; K, Karangetang; Aw, Awu. Large (colored) symbols represent data points considered representative of
primary magmatic values, whereas small (gray) symbols are deemed modified by crustal, geothermal, and/or other
processes (see discussion in section 5.1).

from Mahawu and Lokon 48 (
109) are typical

of arc-related volcanism: all samples fall close to
the worldwide arc average of 15 11
109 [Sano
and Williams, 1996]. Ruang has a slightly lower
than average value (CO2/3He  2 1
109);
nevertheless, its value is close to the lower range of

arc lavas. Therefore the three southern volcanoes

show similar, arc-like CO2/3He characteristics.
[33] In contrast, the northern arc samples (Awu and
Karangetang) have CO2/3He values significantly
higher than the southern arc (Figure 2). The
10 of 17

Geochemistry
Geophysics
Geosystems

jaffe et al.: tracing magma sources

CO2/3He values are 64180 (
109), or between 1

and 2 orders of magnitude greater than the southern
segment of the arc. Higher CO2/3He values in the
northern arc would suggest a diminished mantle
3
He input, a greater subducted slab influence, or
both. A diminished mantle 3He input and/or a
greater slab flux might also be expected to result
in a lower 3He/4He ratio, as observed for this
section of the arc.

5.2.3. The D13C Variations

[34] Although d13C values of all samples are higher
than typical mantle values (6.5% [Sano and
Marty, 1995]), there is a marked distinction in d13C
values between the northern and southern segments
of the arc. The two volcanoes in the northern arc
(Awu and Karangetang) have d13C values 2%,
whereas all three southern segment volcanoes
(Ruang, Lokon and Mahawu) are characterized by
d13C values 3%. It is interesting to note that if
some of the rejected data from Soputan and Ambang
are included, then the pattern between the northern
and southern segments remains unchanged as these
two volcanoes also have low values of d13C.

5.2.4. Along-Strike Variations in He-C:

Summary
[35] Along-strike profiles in 3He/4He, CO2/3He and
d13C of Sangihe Arc volatiles show a consistent
pattern: the southern Sangihe Arc volcanoes
(Ruang, Lokon, and Mahawu) show typical arc
values in all three He-C parameters whereas the
northern volcanoes (Awu and Karangetang) have
higher CO2/3He and d13C, and lower 3He/4He
ratios relative to the southern segment. The results
are consistent with either addition of a strong
crustal input (presumably slab-derived) in the
northern segment of the arc or a reduction in
the mantle contribution. The boundary between
the two segments lies between the islands of Ruang
and Karangetang.

5.3. Differentiating CO2 Sources in

Sangihe Arc Magmas
[36] Following the methodology of Marty et al.
[1989] and Sano and Marty [1995], we can
resolve the total CO2 observed in any particular

10.1029/2003GC000660

Sangihe Arc sample into its component structures.

We adopt the same end-member compositions of
previous workers: namely, MORB mantle
(CO2/3He = 2
109; d13C = 6.5%); limestone
(sedimentary carbonate and altered oceanic basement) (CO2/3He = 1013; d13C = 0%); and organic
sediment (CO2/3He = 1013; d13C = 30%). In
Figure 3 we plot He-C results from the present
study along with the end-member compositions
joined by two binary mixing trajectories with
mantle-derived carbon common to both mixtures.
It is clear that Sangihe Arc samples do not fall on
either of the binary mixing trajectories. This would
imply that all three end-members must contribute
to the total CO2. As the majority of samples lie
close to the M-L binary mixing line, an alternative
explanation is that the Sangihe samples are indeed
binary mixtures of mantle- and limestone-derived
carbon with some samples experiencing isotopic
fractionation to lower d13C [Snyder et al., 2001].
Dewatering of metabasalts at the slab interface
and/or precipitation of calcite within the hydrothermal systems are two possibilities that may lead
to lower d13C values [Snyder et al., 2001]. Given
the observation that some samples (e.g., Lehi and
Temboko) appear to plot subparallel to the M-L
mixing line (Figure 3), then the extent of isotopic
fractionation must be approximately equal in all
cases irrespective of possible along-strike variations in thermal regime at the slab interface (see
next section) or differences in fluid chemistry at
the various volcanic geothermal systems. Both of
these possibilities seem unlikely. A more compelling argument comes from the N-isotope systematics which show some volatile contributions from
organic sedimentary material along the entire
strike of the Sangihe Arc (L. E. Clor et al., Volatile
and N-isotopic chemistry of colliding island arcs:
Tracing source components along the Sangihe
Arc, Indonesia, submitted to Geochemistry Geophysics Geosystems, 2004) (hereinafter referred to
as Clor et al., submitted manuscript, 2004). We
conclude therefore that addition of sedimentaryderived C is responsible for d13C values lower
than predicted by simple binary M-L mixing.
[37] In this case, the contribution of each endmember to the total CO2 can be quantified by use
11 of 17

Geochemistry
Geophysics
Geosystems

jaffe et al.: tracing magma sources

10.1029/2003GC000660

Figure 3. Plot of CO2/3He versus d13C showing (a) data points considered unmodified from primary magmatic
values (see section 5.1 and caption to Figure 2) and (b) binary mixing trajectories involving representative endmember compositions of mantle wedge (M), and slab-derived organic sediment (S) and limestone (L). End-member
compositions are from Sano and Marty [1995]: namely, MORB mantle (CO2/3He = 1.5
109; d13C = 6.5 2.5%),
limestone (CO2/3He = 1013; d13C = 0 2%), and organic sediment (CO2/3He = 1013; d13C = 30 10%).
Uncertainties in CO2/3He values are as shown. The box denotes the worldwide average for arc-related geothermal
fluids [Sano and Marty, 1995].

of the following equations [Sano and Marty,

1995]:


13








C=12 C fM 13 C=12 C fL 13 C=12 C fS 13 C=12 C
o

1






1= 12 C=3 He fM = 12 C=3 He fL = 12 C=3 He
o
M
L


fS = 12 C=3 He
S

fM fS fL 1

2
3

where o = observed and f is the fraction contributed

by L, S and M to the total carbon output.
[38] In Table 2, we detail the fractional contributions of the L-, M- and S-components to the total
CO2 inventory as well as the ratios of (a) limestone
(carbonate) to organic sediment carbon input (L/S),
and (b) slab-derived carbon (L + S) to carbon of
mantle derivation (M). The first and most obvious
point to note is that carbon is predominantly of
carbonate derivation throughout the Sangihe Arc.
This could reflect contributions from both sedi-

mentary carbonate in subducted sedimentary

sequences as well as carbonate contained within
the oceanic basement (e.g., as calcite veins). It is
not unusual for arc-type lavas to be dominated by a
carbonate component [Sano and Marty, 1995;
Hilton et al., 2002]. However, it is significant that
the proportion of carbonate-derived carbon is consistently >90% in the northern section of the arc,
and considerably lower in the southern segment.
Indeed, the southern Sangihe arc has a carbonatederived carbon contribution similar to the average
value seen at arcs worldwide (75%).
[39] Although there is an enhanced contribution of
carbonate-derived carbon to the total carbon inventory in the northern Sangihe Arc, there is (with
the exception of Awu volcano) little difference in
the ratio of L/S in the volcanic output, i.e., the
fraction of carbon of carbonate derivation versus
organic (sedimentary) carbon. We note that the
same observation characterizes the Nicaragua segment of the Central America Arc compared to the
adjacent Costa Rica sector [Shaw et al., 2003].
This may simply reflect uniformity in this param12 of 17

Geochemistry
Geophysics
Geosystems

10.1029/2003GC000660

jaffe et al.: tracing magma sources

Table 2. Limestone-Mantle-Sediment Contributions to CO2 Inventory of Sangihe Arc Geothermal Fluids

Samplea

Typea

Lb

Sb

Mb

L/S

(L + S)/M

I-043

sg

97.6

1.1

1.3

87.4

74.4

Karangetang
Temboko
Lehi

IND-18
I-021

sf
sf

91.4
92.7

6.2
6.4

2.4
0.9

14.8
14.4

39.9
114.9

Ruang
Crater Loc. 2

IND-20

sl

46.4

55.4

0.81

I-159

fm

73.3

7.9

18.8

9.2

4.3

IND-4
IND-5
IND-6
IND-7

sg
sg
sg
sg

64.2
65.7
68.7
67.6
75 10

4.8
5.1
4.0
5.1
13 8

30.9
29.2
27.3
27.3
13 6

13.3
13.0
17.1
13.3
5.8

2.2
2.4
2.7
2.7
6.8

Volcano
Awu
Crater Loc. 2

Lokon
Crater
Mahawu
Lahendong Loc.1
Lahendong Loc.2
Worldwide Averagec

a
See Table 1 footnote for explanation.
b
L, S, and M (in %) are calculated using
c

the same end-members compositions as Sano and Marty [1995] (see text for details).
Average values for arcs worldwide [from Sano and Marty, 1995].

eter in the sedimentary input. In the case of Central

America, organic carbon is dispersed throughout
the subducted sedimentary pile so that it is insulated against thermal loss during early stages of
subduction [Shaw et al., 2003, and references
therein]. The same may hold true in the Sangihe
Arc input.

plus other alternative explanations for along-strike

differences in relative carbon contributions, is discussed in more detail in the following section.

[40] Finally, the Sangihe Arc presents a consistent

picture of an enhanced slab-derived input in the
north relative to carbon from the mantle wedge.
The ratio (L + S)/M is considerably higher in the
northern volcanoes (>40) compared the southern
section of the arc (<4.3). Again, the same observation was made for the Nicaragua segment of the
Central America Arc compared to the adjacent
Costa Rica sector [Shaw et al., 2003]. In Central
America, the difference in (L + S)/M was ascribed
to differences in thermal regime along the strike of
the arc with steeper subduction in Nicaragua leading to a colder slab retaining its carbon inventory
until subarc depths. In contrast, the warmer thermal
regime in Costa Rica leads to loss of carbon from
the slab at shallower (fore-arc) depths thus lowering the relative amount of available slab-derived
carbon. This possibility, i.e., a thermal control on
the relative contribution of slab-derived carbon,

[41] In this section, we explore the possibility that

differences in the volatile systematics observed
between the northern and southern sections of
Sangihe Arc ultimately have a tectonic origin and
are related to the collision and development of the
arc. In this context, we note that the Sangihe and
Halmahera arcs have already collided in the north
causing volcanism to cease north of 4N [e.g.,
Pubellier et al., 1991], and that the collision is
propagating southward. This has caused the subduction rate to decrease along the active arc
[Elburg and Foden, 1998]. Therefore we might
anticipate that any variability in volatile chemistry
related to the collision may be more noticeable in
the northernmost section of the arc, closer to the
locus of collision. We speculate that the observed
along-strike variations in He-C characteristics
could therefore reflect (1) an increase in the
volume of subducted sediment in the northern

5.4. Implications for Tectonic

Development of the Sangihe Arc

13 of 17

Geochemistry
Geophysics
Geosystems

jaffe et al.: tracing magma sources

arc; (2) variability in the composition of subducted

sediment chemistry; or (3) a change in thermal
regime experienced by the subducting slab related
to the onset of collision. These possibilities are
discussed in turn.
[42] 1. Volume of subducted sediment: The massive accretionary wedge (15 km thick) formed by
the collision of the Sangihe and Halmahera arcs is
thickest in the northern Molucca Sea where collision is oldest [e.g., Hall, 1996]. These sedimentary
sequences represent the fraction of the total sediment load involved in the collision that have
obducted onto the fore-arc region. Studies at other
accretionary arcs worldwide [von Huene and
Scholl, 1991] estimate that only 20% of the
sediment on the incoming plate forms the prism,
whereas 80% is subducted into the mantle. Although the He-C systematics of this work are
consistent with recycling of sediment-derived carbon through the entire arc system, we speculate
that the thicker incoming sequences in the northern
arc translates into a greater absolute volume of
sediments that is subducted. Under these circumstances, then it is conceivable that the contribution
of mantle wedge derived carbon could be overwhelmed by the large sediment-derived carbon
contribution in the north, and this would lead to
the enhanced CO2/3He and (L + S)/M ratios
observed at Awu and Karangetang.
[43] 2. Variability in sediment composition: Given
the relatively high C isotopic ratios measured in the
northern arc, we suggest that the subducted sediment in this region contains little hemi-pelagic,
organic-rich sediment. This conclusion is reinforced by nitrogen isotope data from the same
Awu locality that was sampled for the present
sample suite. The d15N value of 3.3% (Clor
et al., submitted manuscript, 2004) indicates that
there is some but not much organic-derived sedimentary N contributing to the volatile flux in this
region (organic N is characterized by d15N values
+6 to +7% [Peters et al., 1978; Kienast, 2000]).
Thus N in the northern arc has a predominantly
upper mantle origin. Carbonate is essential devoid
of N [see also Fischer et al., 2002], and therefore
slab carbonate addition would not mask a mantlelike N isotope signature. In combination with the

10.1029/2003GC000660

high CO2/3He and (L + S)/M, it is reasonable to

conclude that there is a strong slab contribution in
the north, dominated by pelagic or crustal carbonate. In contrast, the southern arc samples have
heavier N isotope signature (average d15 N
2.5%) and higher N2/He, consistent with a
more pronounced contribution of hemipelagic
sediment derived N2 (Clor et al., submitted manuscript, 2004). Thus there is geochemical evidence for some degree of heterogeneity in the
slab composition between the two segments of
the arc.
[44] One possibility to account for the heterogeneity in sediment composition along the strike of the
Sangihe Arc is the process of off-scraping; i.e., loss
of the uppermost sedimentary veneer during subduction. Fischer et al. [2002] interpreted variations
in d15N between Costa Rica and other segments of
the Central America Arc by loss of hemipelagic
(N-bearing) and shallow subducted sediments by
accretion to the over-riding plate. If this scenario is
applicable to the Sangihe Arc, then loss of the
hemipelagic sediment would have to be greater in
the northern segment of the arc, consistent with the
increased thickness of the accretionary wedge
toward the collision. In support of this possibility
is the observation that the L/S ratio is extremely
high at Awu volcano (L/S = 87.4) and then
becomes more constant to the south (L/S  13).
The relatively large distance between Awu and
Karangetang volcanoes may account for the fact
that the effect of off-scraping is not yet observed at
volcanoes other than Awu.
[45] 3. Enhanced fluid/melt generation: An enhanced slab signature (i.e., high (L + S)/M) may
result from more efficient heating of the slab rather
than the addition of larger volumes or different
compositions of sediment. In this scenario, the
slow-down or cessation of collision in the northernmost arc (as seen from seismic evidence [e.g.,
McCaffrey, 1983; Pubellier et al., 1991]) would
lead to enhanced heating of the slab [Peacock et
al., 1994], thereby promoting greater production
of melt and/or fluid. Additionally, on the basis
of mineral chemistry, Morrice and Gill [1986]
propose a northward increase in the depth of
melting.
14 of 17

Geochemistry
Geophysics
Geosystems

jaffe et al.: tracing magma sources

[46] Along the northern extension of the Sangihe

Arc (central Mindanao, The Philippines), there is
extensive volcanic activity formed by post-collisional magmatism. Sajona et al. [2000] describe
these magmas as subducted basaltic crust-derived
melts, or adakites. Their study attributes the slab
melting to thermal rebound of previously depressed
geotherms upon cessation of subduction. In the
northernmost Sangihe Arc (south of Mindanao),
where subduction-related volcanism is still active
but where the subduction rate is slowing [e.g.,
Pubellier et al., 1991], an analogous situation of
more efficient heating of the subducting slab would
be expected to enhance the slab contribution relative to the (mantle) wedge input. Elburg and Foden
[1998] have suggested that the Sangihe Arc has
evolved from a system of fluid-derived contributions to magmagenesis to a system dominated by
sediment-derived melts. They indicate that this
temporal change in apparent source composition
is due to the reduced rate of subduction and
therefore superheating of sediments on the slab.
The CO2/3He and (L + S)/M values in both Awu
and Karangetang geothermal fluids, 12 orders of
magnitude higher than average volcanic arcs, are
consistent with the notion of a much more efficient
transfer of a slab component to the northern Sangihe volcanics. Furthermore, the anomalously high
L/S value of Awu could indicate that the thermal
regime is sufficiently hot so that a significant
fraction of CO2 is derived from a marine carbonate
component within the oceanic basement (i.e., the
source of the L-component). Kerrick and Connolly
[2001] show that significant slab decarbonation is
limited to localities with high-T geotherms; therefore an enhanced CO2 flux in the northern segment
of the arc may indicate initiation of slab melting, as
proposed by Sajona et al. [2000]. In this scenario,
the helium-carbon results are tracing changes in the
thermal regime of the subducted slab as the collision complex propagates south along the Molucca
Sea Plate margin.

6. Conclusions
[47] This work presents the first He and C results
of geothermal fluids from the Sangihe Arc, Indonesia, giving insight into how volatiles are mobi-

10.1029/2003GC000660

lized in an arc-arc collision zone. The following

conclusions are emphasized:
[48] 1. The 26 geothermal and 2 mineral samples
collected along the north-south strike of the
Sangihe Arc contain air-, crustal-, subducted-slab
and/or mantle-derived volatiles. Samples showing
either air contamination (throughout the arc) or
a significant crustal signature (e.g., Ambang
volcano) are identified using a number of criteria
(low 3He/4He, low He/Ne values, high CO2/3He, and
extreme d13C), and are distinguished from samples
that characterize the parental source magmas.
[49] 2. He-C isotope and relative abundance results
of this investigation suggest that the oblique collision of the Halmahera and Sangihe arcs has defined a distinctive pattern of variability in these
parameters along the north-south strike of the
Sangihe Arc. The northern volcanoes (Awu and
Karangetang) show higher CO2/3He and d13C, and
lower 3 He/ 4 He than the southern volcanoes
(Ruang, Lokon and Mahawu): the transition in
He-C systematics occurs between Karangetang
and Ruang volcanoes.
[50] 3. Resolving the CO2 output into primary
source component structures (mantle- carbonateand organic-derived carbon) indicates that there is
a dominant carbonate influence (>90%) in magmas
supplying the northernmost volcanoes (Awu and
Karangetang). In contrast, the southern arc volcanoes (Ruang, Lokon, and Mahawu) contain carbonate contributions (63%) more typical of
average arc magmas (75%).
[51] 4. The northern arc volcanoes record an enhanced slab contribution to the carbon inventory
relative to that derived from the mantle wedge. We
discuss three possible reasons for this observation:
(1) increase in sediment volume contributing to arc
volcanism; (2) variations in sediment composition;
and (3) enhanced heating of the slab resulting from
cessation of collision in the northernmost portion
of the arc.

Acknowledgments
[52] This work was supported by the National Science Foundation (grant EAR-0100881 to DRH). Additional funds for field
expenses came from UCSD (Earth Sciences Program to LJ)
15 of 17

Geochemistry
Geophysics
Geosystems

jaffe et al.: tracing magma sources

and UNM (Research Allocations Committee to TF). We thank

Justin Kulongoski and Pat Castillo for valuable support in the
field, Mark Erdmann for arranging accommodations in
Manado, and Purnama Hilton for help with LIPI in Jakarta.
Alison Shaw, Martin Walhen and Bruce Deck all helped
with laboratory analyses. Colin Macpherson, Robert Hall
and the SE Asia Research Group, London, kindly supplied
Figure 1. We thank J. Varekamp, J. Foden, G. Bebout
(Guest Editor) and one anonymous referee for useful comments. We also thank GRDC director Bambang Dwiyanto
(Bandung) for his support of the project.

References
Allard, P. (1992), Global emissions of helium-3 by subaerial
volcanism, Geophys. Res. Lett., 19, 1479 1481.
Apandi, T. (1977), Geologic map of the Kotamobagu quadrangle, North Sulawesi, Geol. Res. and Dev. Cent., Bandung,
Indonesia.
Dow, J. (1976), Porphyry copper exploration in Block II,
Sulawesi, Newsl. 8, p. 6, Geol. Res. and Dev. Cent.,
Bandung, Indonesia.
Effendi, A. C. (1976), Geologic map of the Manado quadrangle, North Sulawesi, Geol. Res. and Dev. Cent., Bandung,
Indonesia.
Elburg, M., and J. Foden (1998), Temporal changes in arc
magma geochemistry, northern Sulawesi, Indonesia, Earth
Planet. Sci. Lett., 163, 381 398.
Fischer, T. P., D. R. Hilton, M. M. Zimmer, A. M. Shaw, Z. D.
Sharp, and J. A. Walker (2002), Subduction and recycling of
nitrogen along the Central American margin, Science, 297,
1154 1157.
Gasparon, M., D. R. Hilton, and R. Varne (1994), Crustal
contamination processes traced by helium-isotopesExamples from the Sunda Arc, Indonesia, Earth Planet. Sci. Lett.,
126, 15 22.
Gerlach, T. M., and B. E. Taylor (1990), Carbon isotope
constraints on degassing of carbon dioxide from Kilauea
volcano, Geochim. Cosmochim. Acta, 54, 2051 2058.
Giggenbach, W. F., and R. L. Goguel (1989), Collection and
analysis of geothermal and volcanic water and gas samples,
Rep. CD2401, 81 pp., Chem. Div., New Zealand Dep. of Sci.
and Ind. Res., Wellington, New Zealand.
Hall, R. (1996), Reconstructing Cenozoic SE Asia, in Tectonic
Evolution of Southeast Asia, edited by R. Hall and D. J.
Blundell, Geol. Soc. Spec. Publ., 106, 153 184.
Hall, R., and G. J. Nichols (1990), Terrane amalgamation in
the Philippine Sea margin, Tectonophysics, 181, 207 222.
Hamilton, W. (1979), Tectonics of the Indonesian region, U.S.
Geol. Surv. Prof. Pap., 1078, 345 pp.
Hatherton, T., and W. R. Dickinson (1969), The relationship
between andesitic volcanism and seismicity in Indonesia, the
Lesser Antilles, and other island arcs, J. Geophys. Res., 74,
5301 5310.
Hilton, D. R., and H. Craig (1989), A helium isotope transect
along the Indonesian archipelago, Nature, 342, 906 908.
Hilton, D. R., J. A. Hoogewerff, M. J. van Bergen, and
K. Hammerschmidt (1992), Mapping magma sources in

10.1029/2003GC000660

the east Sunda-Banda arcs, Indonesia: Constraints from

helium isotopes, Geochim. Cosmochim. Acta, 56, 851 859.
Hilton, D. R., K. Hammerschmidt, S. Teufel, and H. Friedrichsen
(1993), Helium isotope characteristics of Andean geothermal fluids and lavas, Earth Planet. Sci. Lett., 120, 265
282.
Hilton, D. R., T. P. Fischer, and B. Marty (2002), Noble
gases and volatile recycling at subduction zones, in Noble
Gases in Cosmochemistry and Geochemistry, edited by
D. Porcelli, C. J. Ballentine, and R. Weiler, Rev. Mineral.,
47, 319 370.
Hiyagon, H. (1994), Retention of solar helium and neon in
IDPs in deep-sea sediment, Science, 263, 1257 1259.
Keeling, C. D. (1984), Seasonal, latitudinal, and secular variations in the abundance and isotopic ratios of atmospheric
CO2: Results from oceanographic cruises in the tropical Pacific Ocean, J. Geophys. Res., 89, 4615 4628.
Kerrick, D. M., and J. A. D. Connolly (2001), Metamorphic
devolatilization of subducted oceanic metabasalts: Implications for seismicity, arc magmatism and volatile recycling,
Earth Planet. Sci. Lett., 189, 19 29.
Kienast, M. (2000), Unchanged nitrogen isotopic composition
of organic matter in the South China Sea during the last
climatic cycle; global implications, Paleoceanography, 15,
244 253.
Kulongoski, J. T., and D. R. Hilton (2002), A quadrupolebased mass spectrometric system for the determination of
noble gas abundances in fluids, Geochem. Geophys. Geosyst., 3(6), 1032, doi:10.1029/2001GC000267.
Lallemand, S. E., M. Popoff, J. P. Cadet, A. G. Bader,
M. Pubellier, C. Rangin, and B. Deffontaines (1998),
Genetic relations between the central and southern Philippine trench and the Sangihe trench, J. Geophys. Res., 103,
933 950.
Macpherson, C. G., E. J. Forde, R. Hall, and M. F. Thirwall
(2003), Geochemical evolution of magmatism in an arc-arc
collision: The Halmahera and Sangihe arcs, eastern Indonesia, in Intra-oceanic Subduction Systems: Tectonic and
Magmatic Processes, edited by R. D. Larter and P. T. Leat,
Geol. Soc. Spec. Publ., 219, 207 220.
Marty, B., A. Jambon, and Y. Sano (1989), Helium-isotopes
and CO2 in volcanic gases of Japan, Chem. Geol., 76, 25
40.
Marty, B., T. Trull, P. Lussiez, I. Basile, and J. C. Tanguy
(1994), He, Ar, O, Sr and Nd isotope constraints on
the origin and evolution of Mount Etna magmatism, Earth
Planet. Sci. Lett., 126, 23 39.
McCaffrey, R. (1983), Seismic-wave propagation beneath the
Molucca Sea arc-arc collision zone, Indonesia, Tectonophysics, 96, 45 57.
McCaffrey, R., E. A. Silver, and R. W. Raitt (1980), Crustal
structure of the Molucca Sea collision zone, Indonesia, in
The Tectonic and Geologic Evolution of Southeast Asian
Seas and Islands, Geophys. Monogr. Ser., vol. 23, pp.
161 177, AGU, Washington, D. C.
Morrice, M. G., and J. B. Gill (1986), Spatial patterns in the
mineralogy of island-arc-magma seriesSangihe-Arc, Indonesia, J. Volcanol. Geotherm. Res., 29, 311 353.
16 of 17

Geochemistry
Geophysics
Geosystems

jaffe et al.: tracing magma sources

Morrice, M. G., P. A. Jezek, J. B. Gill, D. J. Whitford, and

M. Monoarfa (1983), An introduction to the Sangihe Arc
Volcanism accompanying arc arc collision in the Molucca
Sea, Indonesia, J. Volcanol. Geotherm. Res., 19, 135 165.
Peacock, S. M., T. Rushmer, and A. B. Thompson (1994),
Partial melting of subducting oceanic crust, Earth Planet.
Sci. Lett., 121, 227 244.
Peters, K. E., R. E. Sweeney, and I. R. Kaplan (1978), Correlation of carbon and nitrogen stable isotope ratios in sedimentary organic matter, Limnol. Oceanogr., 23, 598 604.
Poreda, R., and H. Craig (1989), Helium isotope ratios in
circum-Pacific volcanic arcs, Nature, 338, 473 478.
Priadi, B. (1993), Geochimie du magmatisme de louest et du
nord de Sulawesi, Indonesie: Trecage des sources et implications geodynamiques, Ph.D. thesis, Univ. of Toulouse, Toulouse, France.
Pubellier, M., R. Quebral, C. Rangin, B. Deffontaines,
C. Muller, J. Butterlin, and J. Manzano (1991), The Mindanao collision zone: A soft collision event with a continuous
Neogene strike-slip setting, J. Southeast Asian Earth Sci., 6,
239 248.
Pubellier, M., A. G. Bader, C. Rangin, B. Deffontaines, and
R. Quebral (1999), Upper plate deformation induced by subduction of a volcanic arc: The Snellius Plateau (Molucca
Sea, Indonesia and Mindanao, Philippines), Tectonophysics,
304, 345 368.
Sajona, F. G., R. C. Maury, M. Pubellier, J. Leterrier, H. Bellon,
and J. Cotton (2000), Magmatic source enrichment by
slab-derived melts in a young post-collision setting, central
Mindanao (Philippines), Lithos, 54, 173 206.
Sano, Y., and B. Marty (1995), Origin of carbon in fumarolic
gas from island arcs, Chem. Geol., 119, 265 274.
Sano, Y., and S. N. Williams (1996), Fluxes of mantle and
subducted carbon along convergent plate boundaries, Geophys. Res. Lett., 23, 2749 2752.
Scarsi, P. (2000), Fractional extraction of helium by crushing
of olivine and clinopyroxene phenocrysts: Effects on the
3
He/4He measured ratio, Geochim. Cosmochim. Acta, 64,
3751 3762.
Shaw, A. M., D. R. Hilton, T. P. Fischer, J. A. Walker, and
G. E. Alvarado (2003), Contrasting He-C relationships
in Nicaragua and Costa Rica: Insights into C cycling
through subduction zones, Earth Planet. Sci. Lett., 214,
499 513.
Silver, E. A., and J. C. Moore (1978), Molucca Sea collision
zone, Indonesia, J. Geophys. Res., 83, 1681 1691.

10.1029/2003GC000660

Snyder, G., R. Poreda, A. G. Hunt, and U. Fehn (2001),

Regional variations in volatile composition: Isotopic
evidence for carbonate recycling in the Central American
volcanic arc, Geochem. Geophys. Geosyst., 2, doi:10.1029/
2001GC000163.
Stephen, H., and T. Stephen (Eds.) (1963), Solubilities of
Inorganic and Organic Compounds, vol. 1, Introduction to
Binary Systems, Pergamon, New York.
Sukamto, R. (1979), Tectonic significance of melange on the
Talaud islands, Northeastern Indonesia, Bull. 2, pp. 7 19,
Geol. Res. and Dev. Cent., Bandung, Indonesia.
Tatsumi, Y., M. Murasaki, E. M. Arsadi, and S. Nohda (1991),
Geochemistry of Quaternary lavas from NE Sulawesi
Transfer of subduction components into the mantle wedge,
Contrib. Mineral. Petrol., 107, 137 149.
Torgersen, T. (1989), Terrestrial helium degassing fluxes and
the atmospheric helium budget: Implications with respect to
the degassing processes of continental crust, Chem. Geol.,
79, 1 14.
van der Meer, J. P. M., M. J. van Bergen, P. Z. Vroon, and
G. R. Davies (2002), Sr-Nd-Pb isotope constraints on magma genesis in the Sangihe Arc, North Indonesia (abstract), in
Goldschmidt 2002: The 2002 Geochemistry Conference,
A796, Cambridge, Cambridge, UK.
van Soest, M. C., D. R. Hilton, and R. Kreulen (1998), Tracing
crustal and slab contributions to arc magmatism in the Lesser
Antilles island arc using helium and carbon relationships in
geothermal fluids, Geochim. Cosmochim. Acta, 62, 3323
3335.
van Soest, M. C., D. R. Hilton, C. G. Macpherson, and D. P.
Mattey (2002), Resolving sediment subduction and crustal
contamination in the Lesser Antilles island Arc: A combined
He-O-Sr isotope approach, J. Petrol., 43, 143 170.
Varekamp, J. C., R. Kreulen, R. P. E. Poorter, and M. J.
Vanbergen (1992), Carbon sources in arc volcanism
with implications for the carbon cycle, Terra Nova, 4,
363 373.
von Huene, R., and D. W. Scholl (1991), Observations at
convergent margins concerning sediment subduction, subduction erosion, and the growth of continental crust, Rev.
Geophys., 29, 279 316.
Widiwijayanti, C., V. Mikhailov, M. Diament, C. Deplus,
R. Louat, S. Tikhotsky, and A. Gvishiani (2003), Structure
and evolution of the Molucca Sea area: Constraints based on
interpretation of a combined sea-surface and satellite gravity
dataset, Earth Planet. Sci. Lett., 215, 135 150.

17 of 17