Contrib Mineral Petrol (2005)
DOI 10.1007/s00410-005-0042-7
O R I GI N A L P A P E R
Frank McDermott Francisco G. Deln Jr.
Marc J. Defant Simon Turner Rene Maury
The petrogenesis of volcanics from Mt. Bulusan and Mt. Mayon
in the Bicol arc, the Philippines
Received: 20 March 2004 / Accepted: 12 October 2005

Springer-Verlag 2005
Abstract Pliocene to recent volcanic rocks from the
Bulusan volcanic complex in the southern part of the
Bicol arc (Philippines) exhibit a wide compositional
range (medium- to high-K basaltic-andesites, andesites
and a dacite/rhyolite suite), but are characterised by
large ion lithophile element enrichments and HFS ele-
ment depletions typical of subduction-related rocks.
Field, petrographic and geochemical data indicate that
the more silicic syn- and post-caldera magmas have been
inuenced by intracrustal processes such as magma
mixing and fractional crystallisation. However, the
available data indicate that the Bicol rocks as a group
exhibit relatively lower and less variable 87Sr/86Sr ratios
(0.70360.7039) compared with many of the other sub-
duction-related volcanics from the Philippine archipel-
ago. The Pb isotope ratios of the Bicol volcanics appear
to be unlike those of other Philippine arc segments. They
typically plot within and below the data eld for the
Philippine Sea Basin on 207Pb/204Pb versus 206Pb/204Pb
and 208Pb/204Pb versus 206Pb/204Pb diagrams, implying a
Editorial Responsibility: Ian Parsons
F. McDermott (&)
UCD School of Geological Sciences,
University College Dublin, Beleld, Dublin 4, Ireland
E-mail: frank.mcdermott@ucd.ie
F. G. D. Jr.
School of Policy, Planning, and Development,
University of Southern California,
Los Angeles, CA 90089, USA
M. J. Defant
Department of Geology, University of South Florida,
Tampa, FL 33620, USA
S. Turner
Department of Earth and Planetary Sciences,
Macquarie University, 2109 Sydney, NSW, Australia
R. Maury
CNRS-UMR 6538, IUEM, Universite Bretagne Occidentale,
29280 Plouzane, France
pre-subduction mantle wedge similar to that sampled by
the Palau Kyushu Ridge, east of the Philippine Trench.
143
Nd/144Nd ratios are moderately variable (0.51285
0.51300). Low silica (<55 wt%) samples that have
lower 143Nd/144Nd tend to have high Th/Nd, high Th/
Nb, and moderately low Ce/Ce* ratios. Unlike some
other arc segments in the Philippines (e.g. the Babuyan-
Taiwan segment), there is little evidence for the
involvement of subducted terrigenous sediment. Instead,
the moderately low 143Nd/144Nd ratios in some of the
Bicol volcanics may result from subduction of pelagic
sediment (low Ce/Ce*, high Th/Nd, and high Th/Nb)
and its incorporation into the mantle wedge via a slab-
derived partial melt.
Introduction
Late Cenozoic magmatism on the island of Luzon, the
Philippines, has produced two volcanic arcs: the Luzon
arc in the west and Bicol arc in the south-east (Fig. 1,
inset). The Luzon arc and its northern termination, i.e.
the Babuyan-Taiwan segment north of Luzon island,
has been the subject of numerous studies (de Boer et al.
1980; Hayes and Lewis 1984; Mukasa et al. 1987; Knittel
and Defant 1988; Knittel et al. 1988; Defant et al. 1988,
1989, 1990; Chen et al. 1990; McDermott et al. 1993). By
contrast, the Bicol arc, a chain of about a dozen volcanic
centres distributed along the length of the Bicol penin-
sula (Fig. 1) has received comparatively little attention.
The ca. 900 km2 Bulusan volcanic complex (BVC) at the
southern extremity of the arc (Fig. 1) is the main focus
of this study. It comprises the active cone of Mt. Bulu-
san, the 11 km wide Irosin caldera, and older dissected
volcanic centres that include the Gate Mountains at the
southern tip of the peninsula and Mt. Bintacan to the
west (Fig. 2). Here we present major element, trace ele-
ment, and isotope data for the BVC and for a small
number of historic lavas from Mt. Mayon in the
southern part of the Bicol peninsula (Fig. 1).
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Fig. 1 Map of the Bicol arc showing the major volcanic centres and the location of the Bintacan and Gate volcanics. Historic lavas
with historically active volcanoes denoted by a crater symbol (Mt. from the 1968 and 1984 eruptions from Mt. Mayon have also been
Mayon, Mt. Bulusan, Mt. Iriga). The study area outlined on the analysed. Inset map shows the location of the Bicol arc in a regional
southern tip of the peninsula shows the location of the Mt. BVC tectonic setting

An early petrological and tectonic study of the Bicol
arc ascribed its magmatism to partial melting of the
subducted Philippine Sea Plate (PSP) (Divis 1980). More
recent studies have emphasised the mantle wedge as a
source of the arc magmas (Knittel and Defant 1988;
Knittel-Weber and Knittel 1990; Deln et al. 1993;
Castillo and Newhall 2004). Previous work on the
isotope geochemistry of the Bicol arc volcanics has been
conned to a few studies in which the Bicol rocks were
analysed in a wider regional context. Divis (1980) re-
ported 87Sr/86Sr ratios in the range 0.70340.7047 for
Bicol arc andesites, although individual analyses were
not presented. Knittel and Defant (1988) noted that
rhyolite ows from Tiwi on the eastern ank of
 594,000m E 610,000m E 626,000m E

Ral
Ral

1,428,000m N
GUBAT

SORSOGON BAY
Ral QIg
Ral

Casiguran Ral
Ral
Ral
TGv
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QIg
Ral TGv
Magallanes Ral RQBh
TGv QIg
Ral
QIg
Ral RQBh
BANYO BACOLOD
Ral 842 QIg
TGv Mt. Bintacan QHb QSv
TGv QBtv RQBv Sharp Peak
QIg
1,412,000m N

Mt. Taripungso 1340

661 Ral
TGv QHb MT. BULUSAN
QTa
QJd 1565
724
QKd QSv Ral
QIg Mt.Jormajam Mt.Guho
PINIRINCIPE

Ral RQBh QAa RQBh Mt.Calunan

MAPASO SAN BENON 545
QIg Gabao Mag-Aso QCa
RQBh
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KILOMETERS

EXPLANATION: LEGEND:
Ral Recent slope wash & alluvial deposits POST CALDERA GROUP
RECENT

POST CALDERA GROUP QIg Irosin Ignimbrite

LATE
RQBh Flank lahars & Pyroclastics PLEISTOCENE 610
QMd Malobago Dome
BULUSAN VOLCANICS
PLEISTOCENE ?

PRECALDERA GROUP
RQBv Stratocone lavas & breccias
LATE PLEISTOCENE

QBtv Bintacan Volcanics

EARLY

QKd Talatak Dome

QHb Homahan Basalt
QJd Jormajam Dome
QCa Calunan Andesite
QAa Agoho Andesite
QTv Tabon-Tabon Volcanics
QTa Taripungso Andesite PRE BULUSAN
PLIOCENE
QSv Sharp Peak Volcanics TGv Gate Volcanics

Fig. 2 Detailed geological map of the BVC after Deln et al. (1993). The outline of the Irosin caldera is shown as the heavy dashed line in
the centre of the complex. Detailed descriptions of the units are given in the text
Mt. Malinao (Fig. 1) are characterised by relatively low
87
Sr/86Sr ratios (0.703770.70397), and they argued for a
depleted MORB-like mantle wedge prior to subduction-
related enrichments. In a regional study that included a
single andesite sample from Mt. Isarog (Fig. 1), Mukasa
et al. (1987) interpreted Pb isotope data to indicate a
MORB-type source characterised by a Dupal-type
(Dupre and Allegre 1983) anomaly. Subsequently, Ca-
stillo (1996) argued that the isotopic characteristics of
Philippine arc lavas do not reect a true Dupal anomaly,
but instead are intermediate between an Indian Ocean
MORB mantle-source and an enriched OIB-source
mantle end member. More recently, Castillo and New-
hall (2004) analysed a suite of samples from Mt. Mayon
volcano (Newhall 1979) and argued that the Bicol sub-
arc mantle is isotopically similar to Indian MORB, but
has been enriched by subducted pelagic sediments and
hydrous uids from the subducted basaltic crust of the
PSP.
In a study of the petrology, chronology, volcanology
and major and trace element geochemistry of a large
selection of volcanic rocks from the BVC, Deln (1991)
established a chronological framework for the pre-, syn-,
and post-caldera evolution of the complex. Deln et al.
(1993) published major and trace element data for rep-
resentative BVC samples, and focused on magma
chamber fractional crystallisation and mixing processes
that inuenced the composition of the more evolved
rocks (dacites and rhyolites). The present study builds
on these results and presents new trace element and
isotope data for a subset of the samples studied by
Deln (1991). By focusing on the more primitive sam-
ples, our primary objective is to constrain the nature of
the sub-crustal magma sources that may have contrib-
uted to the BVC rocks, and to oer insights into their
petrogenesis in the context of regional subduction-re-
lated magmatism on the Philippine archipelago.
Regional tectonic setting
In a region of considerable tectonic complexity (e.g.
Rangin et al. 1985; Stephan et al. 1986), the Bicol arc
oers relative simplicity. It forms part of the Quaternary
eastern Philippine arc, and is generated by westward
subduction of the PSP along the Philippine trench
(Fig. 1) that commenced in the Pliocene (Barrier et al.
1991; Cardwell et al. 1980). The oceanic crust of the
West Philippine Basin being subducted at the Philippine
Trench some 210280 km east of the arc is 4060 Ma
old, making it the oldest segment of the PSP (Hickey-
Vargas 1991). The subduction rate along the northern
segment of the trench, closest to the Bicol arc has been
estimated at 6.58.5 cm year 1 (Barrier et al. 1991), but
recent GPS measurements provide a somewhat lower
relative convergence value of 5.4 cm year 1 (Pubellier
et al. 2003). The Benio zone denes a fault plane that
dips 2410 and extends to depths of 100 km, but
apparently not directly beneath the Bicol arc (Cardwell
et al. 1980). Seismic tomography results show a region of
anomalously high seismic velocities close to 100 km
depth under the Bicol arc (Rangin et al. 1999). This
patch of seismically fast material may correspond to
cold parts of the newly subducted PSP slab. The absence
of deep earthquakes beneath the Bicol volcanoes sug-
gests that slip along the Benio zone in this part of the
Philippine Trench may be aseismic.
The three historically active volcanic centres in the
Bicol arc are Mt. Iriga, Mt. Mayon, and Mt. Bulusan
(Fig. 1). Volcanic deposits of the Bicol arc overlie
basement rocks that include Jurassic to Tertiary schists,
gneisses and ophiolites that have been intruded by mid-
Tertiary dioritic plutons, and are overlain by late Ter-
tiary to Quaternary sediments (Geary et al. 1988; Geise
et al. 1986). In the area around the BVC, the oldest non-
volcanic rocks consist of sediments of the Lower-Middle
Miocene Gatbo Formation (Travaglia and Baes 1979),
while Mesozoic schists outcrop on Rapu-Rapu island to
the north of the BVC (Geary et al. 1988).
Eruptive history and petrology of the BVC
Recent KAr age determinations (JICA-MMAJ 1999)
support and rene the eruptive history of the BVC de-
scribed previously by Deln et al. (1993). Eruptions of
high-K basaltic andesites and andesites dating from at
least 2.64 Ma to about 1.56 Ma form the Gate Moun-
tains, a northwest-trending eroded volcanic massif about
12 km wide and 46 km long at the southern end of the
BVC (Fig. 2). The high-K Gate volcanics are overlain by
a medium-K suite formed during successive pre-, syn-,
and post-caldera eruptions, and the possible reasons for
the change to medium-K volcanism are discussed below.
Medium-K pre-caldera volcanism had commenced by
1.10 Ma, forming several andesitic stratocones including
Mt. Bintacan, Mt. Tabon-Tabon, and Mt. Calunan to
the north of the Gate Mountains (Fig. 2). This cone-
building episode was followed by major eruptions of
dacitic to rhyolitic pyroclastic ows of the Irosin
Ignimbrite at approximately 3540 ka, resulting in the
formation of the 11 km wide Irosin caldera (Fig. 2).
Following caldera subsidence, a period of volcanic qui-
escence and lake sedimentation is indicated by peat
deposits beneath the Irosin plain (Travaglia and Baes
1979). Resurgent post-caldera magmatism in the BVC
started with the formation of the Sharp Peak volcano
(Fig. 2) and continues today through the active Bulusan
volcano which dates from at least 6 ka (Deln et al.
1993), with the last eruption in 1994. These post-caldera
vents developed not only inside the Irosin caldera, but
also northeast of the pre-caldera volcanic axis (Fig. 2),
continuing a northeasterly progression of eruptive
activity in the BVC.
The oldest pre-caldera lavas erupted in this part of
the southern Bicol arc were basaltic andesite and
andesite lavas of the high-K Gate suite containing phe-
nocrysts of plagioclase, clinopyroxene, amphibole and
magnetite in a pilotaxitic groundmass. Biotite is rare and
makes up a signicant (35%) proportion of the phe-
nocrysts in one sample only. Plagioclase phenocryts
range in composition from An5675 and are usually
normally zoned. The ubiquitous presence of 110%
amphibole phenocrysts is a distinctive feature of the
high-K lavas. These are up to 3.5 mm in diameter,
typically anhedral, and often surrounded by opaque
rims of pargasite to ferroan pargasite.
Lavas from the medium-K precaldera unit are pet-
rographically and mineralogically more diverse. Lavas
from Mt. Tabon-Tabon (QTv) and Mt. Calunan (QCa)
that form the prominent south-eastern wall of the Irosin
caldera (Fig. 2) are compositionally similar, with up to
20% subhedral plagioclase, 78% clinopyroxene, 3
4% orthopyroxene, and 37% magnetite phenocrysts in
a felty to pilotaxitic groundmass. The basalts and
basaltic andesites from Mt. Homahan (QHb, Fig. 2)
contain olivine (Fo6673) phenocrysts coexisting with
augite (Mg #=6073) and calcic plagioclase (An5576) in
an intergranular groundmass of plagioclase microlites,
glass, and clinopyroxene. The adjacent Bintacan volcano
(QBtv, Fig. 2) contains minor olivine-bearing, slightly
vesicular basaltic andesites, as well as more voluminous
porphyritic andesites. The latter is typically made up of
3040% phenocrysts of plagioclase (An6093), augite
(Mg #=65), and bronzite (Mg #=58) hosted by a hy-
alopilitic to intersertal matrix.
Dacite and rhyolite pumice from the Irosin Ignim-
brite (QIg) are the least porphyritic and most glass-rich
extrusives in the BVC. Phenocrysts typically comprise
about 5% of the pumice and usually consist of plagio-
clase (An3163), biotite (Mg #=51), and magne-
tite amphibole. Rare olivine and clinopyroxene
xenocrysts are found in a few samples. In thin section,
the pumice groundmass is a colourless to dirty-brown
vesicular glass showing pronounced owage texture.
Rounded mac inclusions range in size from several
millimetres to a few centimetres in diameter, and are
found in the pyroclastic ows. These inclusions are
characterised by vesicles (40%), andesitic composition,
and higher phenocryst content (2530%) compared
with their silicic host. Phenocrysts in these mac inclu-
sions include complexly zoned subhedral plagioclase,
pale green clinopyroxene and orthopyroxene, and dis-
seminated anhedral magnetite. The rhyolite dome of Mt.
Malobago (QMd), extruded east of the caldera (Fig. 2),
is chemically and petrographically similar to the pumice
of the Irosin Ignimbrite except that the former has
higher phenocryst content (15%) and contains rare
K-feldspar and quartz grains.
The Sharp Peak lavas (QSv, Fig. 2) are the earliest
post-caldera magmas erupted, and they exhibit three
distinguishing features relative to other post-caldera
BVC lavas. They are more basic in composition, are
highly vesiculated to scoriaceous, and often contain
rounded ne-grained inclusions. Phenocryst phases
typically include anhedral to subhedral plagioclase,
clinopyroxene, often forming glomerocrysts, subhedral
to euhedral orthopyroxene, magnetite, and rare (<1%)
olivine and amphibole. Phenocrysts are usually distrib-
uted in a hyalopilitic groundmass of dark brown glass
with some plagioclase microlites. Vesicles in the Sharp
Peak lavas constitute up to 50% of the total volume in
thin sections. Dioritic inclusions (>3 mm in diameter)
consisting of interlocking euhedral plagioclase, resorbed
amphibole, pyroxenes, and magnetite are common in
these lavas.
The younger post-caldera centres such as the Jor-
majam (QJd, Fig. 2) and Talatak Domes (QTd, Fig. 2)
are more dierentiated, less vesicular andesitic lavas. In
both domes, the lava has a felty matrix hosting a phe-
nocryst assemblage made up of plagioclase (An9360),
clinopyroxene (37%), orthopyroxene (35%), and
magnetite. A variety of textures are observed in Talatak
Dome plagioclase phenocrysts including corroded
inclusion-rich cores with inclusion-poor rims, discon-
tinuous zoning, inclusion-free cores with inclusion-rid-
dled rims, and oscillatory zoning. In the Jormajam
Dome, the coexistence of subhedral olivine grains (1%)
and 23% opaque-rimmed hornblende implies chemical
disequilibrium in the crystallising magma.
Porphyritic andesitic lavas from the active
Mt. Bulusan cone contain about 3545% phenocrysts of
plagioclase (An7040), augite (Mg #=65), hypersthene
(Mg #=56), and magnetite in a pilotaxitic to felty ma-
trix. Anhedral olivine (12%) and amphibole (<15%)
phenocrysts are also observed in some thin sections.
Analytical techniques
Major and trace elements were analysed by XRF at
X-RAL, Ontario, Canada and at the Open University,
UK. Typical detection limits were 0.01 wt% and 2 ppm
for the major and trace elements, respectively. REEs and
selected trace elements were determined by ICP-MS
following HClO4/HF digestion for selected samples.
REE contents in two samples from the historic eruptions
on Mt. Mayon were determined by INAA at the Open
University. Sr and Nd isotopes were analysed by thermal
ionisation mass spectrometry (TIMS) at the Open Uni-
versity and corrected for within-run mass bias to
86
Sr/88Sr=0.1194 and 144Nd/146Nd=0.7219. All Sr and
Nd data are reported relative to the following values for
NBS 987 (0.71025) and La Jolla (0.51184). Uncertainties
determined from the 2r reproducibility of the NBS 987
and J&M standards during the course of analysis were
28 ppm for Sr and 2125 ppm for Nd.
Pb was analysed in temperature controlled runs
(1,250C) in static multi-collector mode on a Finnigan
MAT 262 at the Open University, and the ratios were
corrected for 1& per atomic mass unit mass-
fractionation using the recommended values for NBS
981 (Todt et al. 1996). Blanks for Sr, Nd, and Pb were
typically <1 ng, 500 and 300 pg, respectively.
Th, U and 226Ra concentrations and 230Th/232Th
isotope ratios were determined on a subset of the
samples at the Open University by TIMS on a high
abundance sensitivity Finnigan MAT 262 equipped with
an RPQ-II energy lter. Samples were spiked with
229
Th-, 236U, and 228Ra tracers and dissolved using HF
HClHNO3 in Savillex beakers. Treatment with HCl
and H3BO3 was used to obtain completely clear solu-
tions and to ensure sample-spike equilibration. Details
of the UTh separation and analytical techniques can be
found in Turner et al. (1998), and the procedures for
228
Ra purication and analysis were identical to those
described in Turner et al. (2000). UTh mass spectro-
metric procedures were similar to those described in van
Calsteren and Schwieters (1995). U, Th, and 226Ra
concentrations were determined to a precision of better
than 1.0% (2r), and the U and Th isotope ratios have an
external reproducibility of 1.0% (2r) which was
monitored using the Open University standard solution
ThUStd. Reproducibility of (226Ra/230Th) is estimated
to be 1.3% (Turner et al. 2000). Total procedural blanks
were typically 100 and 50 pg, respectively, for U and Th
and <0.1 fg for 226Ra. All blanks are insignicant rel-
ative to the 30300 ng of U and Th and the 20200 fg of
Ra that were separated and analysed. Determinations of
the AThO and TML Th standards yielded
(230Th/232Th)=1.0170.005 (n=5) and (230Th/232Th)=
1.0790.005 (n=2) during this period. Repeat deter-
minations of the Mt. Lassen Ra standard yielded an
average of 226Ra=1,0659 fg g 1 which is within error
of the values quoted by Volpe et al. (1991). Decay
constants used in the calculation of activity ratios were
k238U=1.5511010 a 1; k234U=2.83510 6 a 1; k232
Th=4.94810 11 a 1; k230Th=9.19510 6 a 1;
226 4 1
k Ra=4.33210 a .
Major and trace element chemistry
Most of the Bicol arc samples analysed here are inter-
mediate in character and are largely basaltic andesites
Fig. 3 K2O versus SiO2 4.0
diagram for the BVC rocks and
the two historic Mayon
samples. The late-Pliocene to
early-Pleistocene Gate volcanics
form a high-K calc-alkaline 3.0
suite. The data eld enclosed by
the dashed line represents data
Wt % K2O
for volcanics from Mt. Mayon
(Castillo and Newhall 2004). 2.0
Data symbols arranged in the
stratigraphic order of the units
that they represent
1.0
0.0
48 52
and andesites (5362% SiO2). On a K2O versus SiO2
diagram (Fig. 3), the BVC rocks can be subdivided into a
Pliocene to early Pleistocene high-K suite comprised al-
most exclusively of the pre-caldera Gate volcanics, and a
younger Pleistocene to Holocene medium-K suite. The
oldest high-K Gate volcanics and the medium-K pre-
caldera Bintacan basaltic andesites and andesites are calc-
alkaline (sensu-stricto) using the original denition of
Peacock (1931), as discussed recently by Arculus (2003).
The syn-caldera eruptives, dominated by the Irosin
Ignimbrite and the Malobago Dome rocks, represent the
most dierentiated magma erupted in the BVC, with SiO2
contents in the range 6676% (Fig. 3). The mac inclu-
sions within the Irosin Ignimbrite are intermediate in
composition, with silica contents in the range 58
59 wt%. In contrast with the pre-caldera rocks, the post-
caldera Sharp Peak volcanics and the Agoho andesite
tend to be calcic (sensu-stricto), as are the late Pleistocene
to historic basaltic andesites and andesites from
Mt. Mayon. Both Jormajam Dome samples are andesitic
(c. 60 wt% SiO2), but as discussed below probably rep-
resent the product of magma mixing processes.
At a given SiO2 concentration, the high-K Gate vol-
canics contain greater Na2O and P2O5, but lower Fe2O3,
MgO, and CaO than the younger medium-K eruptives.
Although some scatter is noted for the syn-caldera
samples, most of the major elements from the medium-
K suite show good linear correlation with SiO2 (Deln
et al. 1993). Al2O3, CaO, Fe2O3, MgO, and TiO2 de-
crease with increasing SiO2 (not shown). There is greater
scatter for Na2O, MnO, and P2O5, but in general Na2O
increases while MnO and P2O5 decrease with increasing
dierentiation.
Both of the historic samples analysed from Mt. Ma-
yon are basaltic andesites. They plot within the medium-
K series on Fig. 3 and dene a narrow compositional
range relative to the larger suite of late Pleistocene to
historic Mt. Mayon suite analysed by Castillo and
Newhall (2004).
Pliocene to early
Pleistocene Gate Mayon
volcanics
Bulusan stratocone
Jormajam dome
Syn-caldera
eruptives
Agoho andesite
Sharp Peak
volcanics
Irosin Ignimbrite
Malobago Dome
Bintacan volcanics
Homahan Basalt
Calunan andesite
Gate volcanics
56 60 64 68 72 76
Wt % SiO2
 Chondrite normalised REE patterns are shown in
Fig. 4. All samples are LREE enriched (Lan/Ybn in the
range 412), and a high-K andesite from the Gate
volcanics (sample B220) exhibits the highest REE
concentrations. In detail, the Bicol arc rocks exhibit
higher Lan/Ybn at a given silica value compared with
those from the Macolod Corridor to the north-west
(Fig. 1, inset). The single sample analysed here from
the pre-caldera Homahan basalt is also LREE en-
riched, but that from the pre-caldera Calunan andesite
has a REE pattern similar to the post-caldera rocks.
There is a tendency for higher La/Yb ratios in the
silicic syn-caldera samples (Irosin Ignimbrite and
Malobago Dome samples), largely reecting their
lower HREE abundances. Thus, the Irosin Ignimbrite
and Malobago Dome samples have Lan/Ybn ratios of
1012 compared with <10 for the other BVC units.
Most of the basalts and basaltic andesites have mod-
erate negative Eu anomalies (Eu/Eu*=0.830.98), but
the dacitic and rhyolitic Irosin Ignimbrite samples
(B146A and B1B) have distinctly more negative Eu
anomalies (Eu/Eu*=0.50.65). In common with many
intra-oceanic subduction-related volcanics (e.g. Wood-
head 1989; Elliott et al. 1997; George et al. 2003), the
BVC samples exhibit small negative cerium anomalies,
with Ce/Ce* in the range 0.880.97.
N-MORB normalised (Sun and McDonough 1989)
trace element abundances for selected samples are
1000 Bulusan stratocone
Agoho andesite
Sharp Peak volcanics
Irosin Ignimbrite
Malobago Dome
Jormajam dome
Bintacan volcanics
100 Homahan basalt
Rock/Chondrite
Gate volcanics
10
1 Previously published Pb isotope data for the Babuyan
La Ce Pr Nd Sm Eu Gd Tb Dy Ho Er Tm Yb
Fig. 4 Chondrite normalised REE data for the BVC. Data symbols
as in Fig. 3
shown in Fig. 5. All samples show characteristic sub-
duction-related enrichments in the large ion lithophile
(LIL) elements and LREE, with relative depletions in
Nb and Ti. Unlike some arcs (e.g. parts of the Mari-
anas arc, Elliott et al. 1997) there is no evidence in any
of the Bicol rocks analysed for systematic depletion of
the HFS elements relative to N-MORB. However, the
absence of strong negative HFS anomalies in the Bicol
rocks may reect their higher overall incompatible
trace element contents, and there is no evidence, for
example, for unusually low LREE/HFS ratios (e.g. La/
Zr). The high-K Gate volcanics exhibit a distinctive
trace element pattern and are characterised by higher
concentrations of all of the trace elements in Fig. 5,
except for Nb which is signicantly lower than that of
the medium-K rocks. The medium-K (mostly basaltic
andesites and andesites) exhibits trace element patterns
that are typical of subduction-related magmas (Fig. 5a)
and are trace element enriched compared with similar
samples from the Marianas arc (Elliott et al. 1997). By
contrast, the dacites and rhyolites of the Irosin
Ignimbrite and syn-caldera Malobago Dome (Fig. 5b)
exhibit stronger LIL element enrichments relative to
the more mac samples, and are also characterised by
lower abundances of the middle to heavy REEs and the
HFS elements.
Isotope data
87
Sr/86Sr ratios in the Bicol arc volcanics are relatively
low (0.703730.70399) compared with those from many
of the other arc segments of the Philippine archipelago
for which data are available (e.g. the Babuyan-Taiwan
arc segment, the Luzon/Mindoro arcs, and the Macolod
Corridor; Fig. 6). 143Nd/144Nd ratios in the Bicol arc
rocks are relatively high (Fig. 6), but extend to lower
values than those of Central Mindanao (Sajona et al.
2000) and Camiguin Island in the southern Philippines
(Castillo et al. 1999). Data for basalts erupted in the
Macolod corridor, an extensional zone to the west of
Bicol (Defant et al. 1988, 1989, 1991; Forster et al. 1990)
exhibit distinctly higher 87Sr/86Sr and slightly lower
143
Nd/144Nd isotope ratios relative to data for the Bicol
arc (Miklius et al. 1991; Mukasa et al. 1994; Knittel et al.
1997). Similarly, basalts from the Bataan segment in the
south Luzon part of the western arc exhibit a more en-
riched character with higher 87Sr/86Sr and lower
143
Nd/144Nd than in the Bicol rocks. The low
143
Nd/144Nd ratios of the north Luzon and the Babu-
yan/Taiwan segments of the western Philippine arc sys-
tem (Fig. 6) have been well documented previously (e.g.
Defant et al. 1989; Chen et al. 1990; McDermott et al.
1993), and are in sharp contrast with the data presented
here for the Bicol volcanics.
and Taiwan arc segments (McDermott et al. 1993; Ca-
stillo 1996) are characterised by steep arrays displaced
away from the Northern Hemisphere reference line
Fig. 5 N-MORB normalised
trace element patterns for a the
basalts, basaltic andesites, and
andesites from the BVC and
Mt. Mayon and b the high-silica
Irosin Ignimbrite and
Malobago Dome samples. Data
symbols as in Fig. 3. The grey
shaded pattern (sample AGR2,
Agrigan, Marianas) is shown
for comparison (Elliott et al.
1997)

(NHRL) on 207Pb/204Pb versus 206Pb/204Pb and
208
Pb/204Pb versus 206Pb/204Pb diagrams, and were
interpreted to reect the inuence of subducted terrige-
nous sediment. Prior to this study Pb isotope data for
the Bicol arc volcanics consisted of a few samples from
Mt. Mayon only (Castillo 1996) and a single analysis
from a late Miocene andesite ow from near Mt. Isarog
(Mukasa et al. 1987). An important observation is that
the new data for the Bicol arc exhibit lower 207Pb/204Pb
and 208Pb/204Pb at a given value of 206Pb/204Pb com-
pared with almost all of the other arc segments in the
Philippine archipelago. The data plot within and slightly
below the eld for the Philippine Sea Basin MORB
(Hickey-Vargas 1991, 1998) on a 207Pb/204Pb versus
206
Pb/204Pb diagram (Fig. 7a), but are clearly below this
eld on a 208Pb/204Pb versus 206Pb/204Pb diagram
(Fig. 7b). Thus, the data extend towards and into the
data eld for the Palau Kyushu Ridge (PKR), a
spreading centre to the east of the Philippine Trench that
is characterised by systematically lower 207Pb/204Pb and
208
Pb/204Pb compared with other segments of the Phil-
ippine Sea Basin (site 448, Hickey-Vargas 1991). Data
for the Mt. Mayon 1968 and 1984 eruptions plot close to
or even slightly below the NHRL on the Pb isotope
diagrams, although when a larger group of late Pleis-
tocene to historic samples from Mt. Mayon are taken
into account (Castillo 1996; Castillo and Newhall 2004),
the Mayon data dene a steep array on both the
207
Pb/204Pb versus 206Pb/204Pb and 208Pb/204Pb versus
206
Pb/204Pb diagrams. There is no evidence for the Du-
pal-type Pb isotope anomaly inferred previously for this
arc segment (Mukasa et al. 1987).
The U-series data are presented in Fig. 8. All of the
Bicol samples exhibit a relatively narrow range in
 0.51320 tent with its Pliocene age and so no information about
Philippine
Sea
Basin
subduction-related UTh fractionation can be derived
0.51310 PKR from its Th isotope data.
Mindanao/Camiguin 226
0.51300 Luzon Arc
Ra data for the 1968 and 1984 basaltic andesites
(Bataan segment) from Mt. Mayon were included in a study of the
226
0.51290
Macolod Corridor Ra230Th systematics of subduction-related rocks
0.51280 worldwide (Turner et al. 2001). Both samples exhibit
Nd/144 Nd

moderate Ra excess relative to many subduction-related

Mindoro Arc
0.51270 magmas, with 226Ra/230Th ratios of 1.51 and 1.59 for the
samples erupted in 1968 and 1984 AD, respectively. Since
143

0.51260 226
Ra has a relatively short half-life (1,622 years), the
0.51250 data require that radium addition occurred recently
compared with the timescales required to achieve secular
0.51240
equilibrium with 230Th (approximately 8,000 years, or
0.51230 ve half-lives of 226Ra).
0.51220
0.703 0.704 0.705 0.706 0.707 15.70 a
87 86
Sr/ Sr
MC
15.65
Fig. 6 87Sr/86Sr versus 143Nd/144Nd diagram for the Bicol volca-
nics. Also shown are the data elds for basalts from the Philippine TS
15.60 BS

Pb/204Pb
Sea Basin (Hickey-Vargas 1991, 1998)). The data eld for the Palau asin
Kyushu Ridge basalts (PKR) is shown separately as a shaded eld. S ea B
SP ine
The data eld enclosed by the dashed line represents data for 15.55 lipp
volcanics from Mt. Mayon (Castillo and Newhall 2004). Data CM M Phi
sources for Philippine subduction-related rocks are as follows: RL
207

NH
Mindanao/Camiguin (Sajona et al. 2000; Castillo et al. 1999), 15.50
Bataan Arc (Knittel et al. 1988; Mukasa et al. 1994), Macolod PKR
Corridor (Knittel et al. 1997; Mukasa et al. 1994), Mindoro Arc 15.45
(Knittel et al. 1988), Taiwan/Babuyan segments (Vidal et al. 1989;
Chen et al. 1990; McDermott et al. 1993), North Luzon
(McDermott et al. 1993). Typical 2r measurement errors are 15.40
smaller than the data symbols 17.8 18.0 18.2 18.4 18.6 18.8 19.0 19.2
206 204
Pb/ Pb
(230Th/232Th) ratios (0.891.07), and the ratios are 39.30 b n
moderately low compared with subduction-related lavas asi
39.10 e aB
globally. Of the published Th isotope data for subduc- eS
pin
tion-related lavas worldwide, only those from the Luzon 38.90 ilip
MC
Ph
CG
arc (McDermott and Hawkesworth 1991) and Indonesia
Pb/204Pb

TS
38.70
(Rubin et al. 1989; Gill and Williams 1990) exhibit sys- BS

38.50
tematically lower (230Th/232Th) ratios (Fig. 8). Five of M
RL
the six samples analysed for Th isotopes plot close to, 38.30 SP NH
208

CM

but slightly to the right of the equiline on a (230Th/232Th) 38.10 PKR

versus (238U/232Th) diagram (Fig. 8, inset) indicating 37.90

relatively small but recent (<350,000 years) enrichments
(26%) in U relative to Th. U enrichments are com- 37.70
monly observed in subduction-related lavas (e.g. Gill 37.50
and Williams 1990; McDermott and Hawkesworth 1991; 17.8 18.0 18.2 18.4 18.6 18.8 19.0 19.2
Condomines and Sigmarsson 1993) and are usually 206
Pb/ 204
Pb
attributed to preferential release of uranium from the
subducted slab. The sixth sample (B-107B, a basaltic Fig. 7 a 207Pb/204Pb versus 206Pb/204Pb isotope ratios for the Bicol
andesite from the post-caldera Sharp Peak vent in the volcanics. b 208Pb/204Pb versus 206Pb/204Pb isotope ratios for the
Mt. BVC) is unusual because it exhibits relatively low Bicol volcanics. Also shown in both diagrams are elds for
published data for other arc segments of the Philippines archipel-
(238U/230Th), indicating recent Th enrichment (c. 20% ago. Data for terrigenous sediments from the South China Sea west
excess Th) relative to uranium. In common with many of the Manila Trench (McDermott et al. 1993) are shown for
low (230Th/232Th) lavas, the Mayon and Bulusan comparison (grey diamonds). Data elds: M Mayon (Castillo and
samples have relatively high Th contents (1.7 Newhall 2004), MC Macolod Corridor (Mukasa et al. 1994), BS
10.5 ppm), with the highest values occurring in the early Batan segment (McDermott et al. 1993), SP Southern Philippines
(Castillo et al. 1999), TS Taiwan segment, CM Central Mindanao
high-K suite (e.g. sample B-220; Fig. 5). The latter is in (Sajona et al. 2000). Typical (2r) measurement error ellipses are
UTh secular equilibrium (Table. 1, 2, 3, 4, 5), consis- shown in the upper left of each diagram
 3.0
Nicaragua
2.0
(230Th/ 232Th)
Pacific arcs
1.1
1.0
1.0
0.9
0.8 B220
Indonesia
0.7
0.7 0.8
0.0
0.0 1.0 2.0
(
238
U/
232
Th)
Fig. 8 (230Th/232Th) versus (238U/232Th) equiline diagram for the
Bicol volcanics (lled circles) in the context of subduction-related
suites worldwide. Also shown for comparison are U-series data for
the North Luzon lavas (open circles) after McDermott et al. (1993).
The data eld for Pacic arcs includes data from the Marianas
(McDermott and Hawkesworth 1991; Elliott et al. 1997), Tonga-
Kermadec (Turner and Hawkesworth 1997), Vanuatu and Indo-
nesia (Turner et al. 2003), and the Aleutians (George et al. 2003).
The data eld for Nicaragua is after McDermott and Hawkesworth
(1991) and Reagan et al. (1994) and that for Kamchatka is after
Turner et al. (1998). Inset diagram shows details of the Bicol data.
Typical 2r measurement error ellipses are shown in the upper left of
both diagrams
Discussion
Compositional variations within the Bicol rocks
Deln et al. (1993) showed that the steep decrease in
Al2O3, CaO, Fe2O3, MgO, and TiO2 with increasing
SiO2 in the dacites and rhyolites can be modelled as the
products of crystallisation and removal of plagioclase,
pyroxene, olivine, and magnetite, while a sharp change
in slope in the Harker diagrams at about 6668% SiO2
was interpreted to reect the onset of biotite K-
feldspar quartz fractionation. However, the results of
mass-balance calculations show that the high-K suite
(Gate volcanics, Fig. 3) is unlikely to be related, either as
parent or daughter magma, to the medium-K suite
through crystal fractionation (Deln et al. op. cit.).
Trace element systematics also indicate that the high-K
suite (Fig. 3) cannot be related to the medium-K lavas
through shallow-level magmatic processes such as
crystal fractionation or crustal assimilation, implying a
distinct parental magma (Deln et al. 1993). Since there
are no obvious dierences in Sr, Nd, or Pb isotopes
between the high- and medium-K suites, one explana-
tion is that the incompatible element enriched high-K
suite reects small degree melts of the mantle wedge that
were subsequently re-melted to form the parental mag-
mas of the medium-K rocks. We note that the high-K
Gate volcanics were erupted westsouth-west of the
medium-K volcanics, and hypothesise that trench-ward
(eastward) ow in the mantle wedge produced a source
for the medium-K suite that previously had small degree
melts extracted to generate the magmas of the high-K
Gate volcanics.
Magmatic dierentiation processes in the crust
clearly played a role in the petrogenesis of the syncaldera
and post-caldera stages of the BVC, given the wide range
B107B in rock types and the petrographic evidence for dis-
1968
B1B B148 equilibrium textures and magma mixing described
1984 above. Highly vesicular cognate mac inclusions in the
Irosin Ignimbrite provide evidence that basaltic magma
was entrained by the more siliceous melts prior to the
0.9 1.0
ignimbritic eruption at 3540 ka. Although no detailed
phase chemistry data are available for the inclusions,
3.0 their bulk chemistry is andesitic (average SiO2=58%),
and their petrography is dominated by acicular crystals
of orthopyroxene and plagioclase, with rare olivine
embedded in a highly vesiculated glassy groundmass.
These inclusions may have formed when hot basaltic
recharge, later erupted as Sharp Peak lavas (SiO2=51
54%), intruded a cooling reservoir of rhyolitic melt,
eectively forming a zoned magma chamber. Sub-
sequent degassing and rapid crystallisation of the
basaltic blobs at the magmatic interface may have
facilitated mixing that led to the catastrophic caldera-
forming eruption (Deln et al. 1993). Similarly, the
Jormajam Dome andesites exhibit petrographic evidence
for chemical disequilibrium, probably reecting magma
mixing (subhedral olivine grains and opaque-rimmed
hornblende). The REE and other trace element data for
the Jormajam Dome rocks (Figs. 4, 5) are consistent
with mixing between a basaltic magma (similar to the
pre-caldera Homahan basalt, for example) and a silicic
rock (e.g. Irosin Ignimbrite composition).
The most striking feature of the new Sr isotope data
for the Bicol arc is the narrow range in 87Sr/86Sr, and we
note that even the rhyolitic Irosin Ignimbrite sample
exhibits relatively low 87Sr/86Sr (0.70390). The range in
87
Sr/86Sr presented here is similar to that for the Putsan
rhyolite (0.703770.70387) analysed by Knittel and De-
fant (1988), and for volcanics from Mt. Malinao
(0.703740.70397) published by Knittel-Weber and
Knittel (1990). The Irosin Ignimbrite sample also
exhibits high 143Nd/144Nd (0.51291) relative to other
Philippine arc segments. Thus, despite the occurrence of
late Jurassic schists in the southern part of the Bicol
peninsula (Geary et al. 1988), the present indications are
that if crustal anatexis or crustal contamination was a
signicant process in generating the rhyolitic volcanics
in the BVC, it did not result in large shifts in their
radiogenic isotope ratios. Nonetheless, discussions on
the nature of the subduction-related processes respon-
sible for the petrogenesis of the Bicol arc rocks (below)
will be restricted to the basaltic and basaltic andesite
samples.
Table 1 New major element data for selected volcanics from the Bicol arc

Sample SiO2 TiO2 Al2O3 Fe2O3 MnO MgO CaO Na2O K2O P2O5

Post-caldera
Bulusan strata-cone (RQBv)
B34 59.1 0.53 17.7 6.49 0.15 2.99 7.16 3.53 1.80 0.18
B-125 59.6 0.53 17.8 6.45 0.15 2.92 6.9 3.63 1.76 0.20
B-128A 58.1 0.57 17.5 6.88 0.15 3.54 7.43 3.55 1.68 0.20
B-120A 59.4 0.51 17.8 6.27 0.14 3.06 6.89 3.64 1.72 0.15
Jormajam dome (QJd)
90-02 61.2 0.46 17.6 5.36 0.13 2.43 6.02 3.55 1.93 0.17
B-45 59.4 0.51 18.0 6.01 0.14 2.71 6.70 3.37 1.88 0.19
Agoho andesite (Qaa)
B-126A 59.8 0.54 17.6 6.51 0.14 3.07 6.84 3.62 1.80 0.17
B-116A 57.5 0.59 17.1 7.43 0.15 3.81 7.45 3.38 1.57 0.18
B-118A 59.1 0.48 17.9 6.16 0.14 3.07 6.98 3.53 1.73 0.19
B-119 59.5 0.54 17.7 6.37 0.14 3.10 6.69 3.59 1.77 0.17
Sharp peak volcanics (QSv)
90-18 54.3 0.50 19.7 7.14 0.15 4.00 8.59 3.18 1.06 0.17
90-04 50.9 0.58 20.7 8.49 0.20 3.86 6.75 2.57 0.15 0.18
B-107B 53.9 0.51 19.4 7.47 0.16 4.19 7.99 3.32 1.08 0.16
Caldera
Irosin Ignimbrite (Qlg)
B-1B 75.6 0.17 13.6 0.82 0.08 0.27 1.38 4.39 3.05 0.04
B93 65.7 0.28 16.4 2.97 0.12 1.25 3.21 4.02 2.25 0.11
Pre-caldera
Bintacan volcanics (QBtv)
B-140A 59.2 0.52 18.10 6.45 0.17 2.58 6.09 3.83 1.92 0.35
B-148 52.5 0.71 20.8 8.09 0.16 3.79 9.73 2.97 0.87 0.22
B-169 57.7 0.56 18.4 7.34 0.16 3.02 7.06 3.48 1.70 0.25
90-08 53.6 0.68 19.7 7.88 0.16 3.67 5.61 2.90 1.29 0.25
Calunan andesite (Qca)
B-184 55.1 0.76 18.0 8.54 0.17 4.02 8.09 3.42 1.20 0.20
90-05 56.1 0.66 18.7 7.21 0.15 3.35 8.14 2.96 1.40 0.17
Gate volcanics (TGv)
B-168 58.2 0.62 17.8 6.11 0.14 2.45 6.27 3.42 3.11 0.28
B-192 57.5 0.55 18.7 6.79 0.14 2.89 6.90 3.71 1.79 0.27
B-213A 53.5 0.81 17.9 8.94 0.17 3.49 7.51 2.75 2.06 0.23
B-216 60.9 0.56 17.6 5.51 0.13 1.61 4.96 4.57 2.76 0.36
B-220 58.3 0.94 18.6 5.56 0.12 2.17 6.12 4.21 2.47 0.31
90-10 53.3 0.67 18.7 7.59 0.17 3.75 8.36 3.07 1.90 0.26
Mt. Mayon
1968 54.7 0.72 18.6 8.44 0.17 4.33 8.46 3.38 1.12 0.30
1984 54.7 0.71 18.6 8.31 0.16 4.23 8.45 3.32 1.13 0.30

All values in wt%. Data for samples B34, B-107B, B-148, B93, B-220, B140A, and B-1B were presented previously by Deln et al. (1993),
but are included here because new isotope data and/or trace element data are provided for these samples in Table. 3 and 4. Map units refer
to those shown in Fig. 2

Evidence for the nature of the Bicol magma sources
On a 207Pb/204Pb versus 206Pb/204Pb diagram (Fig. 7a),
data for the BVC rocks analysed here plot entirely
within and below the eld of Philippine Sea MORB,
implying that, unlike the Taiwan, Babuyan and N. Lu-
zon segments of the Luzon arc (McDermott et al. 1993;
Castillo 1996), they do not require that a large propor-
tion of their Pb inventory be derived from subducted
terrigenous sediment. Data from DSDP Leg 59 site 448
on the PKR, the spreading centre to the east of the
Philippine Trench, exhibit unusually low 207Pb/204Pb
and 208Pb/204Pb ratios (Hickey-Vargas 1998) and plot
just below the Bicol arc data on the PbPb isotope
diagrams. Thus, the new Pb isotope data for the Bicol
volcanics permit the involvement of subducted sediment
in their petrogenesis if the pre-subduction mantle wedge
had unradiogenic 207Pb/204Pb and 208Pb/204Pb similar to
that sampled by the PKR to the east of the arc (Fig. 7).
The two historic Mt. Mayon basaltic andesites analysed
here (1968 and 1984) exhibit low 207Pb/204Pb and
208
Pb/204Pb ratios, and plot closest to the data eld for
the PKR, implying that their Pb inventory could have
been derived from a mantle wedge with this isotopic
composition. A possible alternative explanation, namely
that low 206Pb/204Pb and 207Pb/204Pb signature of the
Table 2 Trace element data for selected Bicol arc volcanics

Sample number Ba Cr Nb Ni Rb Sr Y Zr

Post-caldera
Bulusan strato-cone
B-128A 463 26 6 <2 28 511 24 113
B-120A 443 23 <2 <2 35 385 15 105
B34 437 24 <2 83 41 419 14 116
Jormajam dome
B-45 543 20 4 <2 41 452 15 116
90-02 556 19 2 2 44 435 11 117
Agoho andesite
B-125 474 23 4 <2 41 453 17 115
B-126A 496 27 2 <2 40 419 19 108
B-116A 437 15 3 7 36 427 11 96
B-118A 452 4 5 <2 39 437 18 108
B-119 465 23 7 2 37 427 16 111
Sharp peak volcanics
B-107B 225 22 42 <2 25 392 16 78
90-18 233 14 3 13 24 423 12 73
90-04 311 27 2 3 4 444 20 92
Caldera
Irosin Ignimbrite
B-1B 793 21 7 <2 88 175 15 100
B93 792 <2 7 <2 64 323 7 109
Pre-caldera
Bintacan volcanics
B-140A 799 25 <2 <2 35 675 16 131
B-148 284 20 3 4 17 519 15 72
B-169 652 25 3 <2 34 582 21 105
90-08 748 <2 4 4 18 530 46 104
Calunan andesite
B-184 262 30 <2 <2 25 423 22 92
90-05 334 8 3 <2 30 405 21 78
Gate volcanics
B-168 833 15 8 <2 85 726 28 231
B-192 669 11 <2 <2 50 654 21 123
B-213A 573 3 4 <2 48 513 15 112
B-216 986 7 4 <2 77 589 35 204
B-220 976 4 <2 <2 60 602 42 183
90-10 590 28 <2 7 46 752 16 134
Mt. Mayon
1968 353 8 4 6 21 713 23 98
1984 363 12 4 7 20 714 24 99

All values are in ppm. Data for samples B34, B-107B, B-148, B93, B-220, B140A, and B-1B were presented previously by Deln et al.
(1993), but are included here because new isotope data and/or trace element data are provided for these samples in Table. 3 and 4. Map
units (Fig. 2) for these samples are given in Table 1

Bicol volcanics reects Pb from subducted oceanic crust
formed at the PKR is considered less likely for mass-
balance reasons, because any sediment component
would dominate the Pb budget, and therefore the iso-
topic composition of slab-derived Pb.
However, other published data for Mt. Mayon lavas
(Castillo and Newhall 2004) with a wider compositional
range than the two samples analysed here, indicate that
volcanic products from Mayon exhibit a considerable
range in Sr, Nd, and Pb isotopes. This larger dataset
strongly suggests a role for subducted sediment in the
genesis of some Mt. Mayon lavas (Castillo 1996; Castillo
and Newhall 2004). Considering the Pb isotope dataset
for the Philippine archipelago as a whole, however
(Fig. 7), it is evident that there are distinct intersegment
variations in the dataset that probably reect processes
other than sediment subduction. For example, the sub-
parallel nature of the Pb isotope data arrays (Fig. 7)
implies a relatively large range in 206Pb/204Pb (18.218.5)
within those samples least likely to have been aected by
subducted sediment-derived Pb (i.e. lowest 207Pb/204Pb).
Thus, the clear evidence for coupled systematic latitu-
dinal variations in the isotopic character of the sub-
ducted sediment signature (McDermott et al. 1993) may
Table 3 INAA trace element data for selected Bicol arc lavas

Sample number U Th Hf La Ce Pr Nd Sm Eu Gd Dy Er Yb

Post-caldera
Bulusan stratacone
B-34 1.2 4.3 3.1 14.4 26.8 3.3 13.5 2.9 0.83 3.1 2.5 1.9 1.9
Jormajam dome
90-02 1.2 4.3 2.7 16.6 31.5 3.3 13.6 2.7 0.92 2.7 2.2 1.6 1.4
Agoho andesite
B-116A 1.0 2.9 2.7 14.3 26.2 3 13.3 2.8 0.79 3.1 2.8 1.9 1.9
Sharp peak
B-107B 0.6 1.5 2.1 9.4 18.1 2.1 9.9 2.5 0.66 2.3 2.4 1.5 1.6
Caldera
Irosin Ignimbrite
B-1B 2.2 7.4 2.4 21.1 35.2 3.3 11.8 2.3 0.31 1.6 1.3 1.0 1.2
B-93 1.6 6.2 1.7 18.7 32.9 3.3 12.0 2.1 0.74 1.9 1.7 1.2 1.2
Pre-caldera
Bintacan volcanics
B-140A 0.8 2.8 3.2 31.4 56.5 7.1 28.7 4.8 1.47 4.4 3.2 2.1 2.0
B-148 0.8 2.6 1.9 13.3 25.3 3 13.8 3.1 0.94 3.6 3.2 2.1 1.9
Gate volcanics
B-220 3.2 12.3 5.1 35.1 64 7.1 31.0 6.2 1.53 6.5 5.8 4.0 4.2
Mt. Mayon
1968 0.57 1.8 2.6 16.3 31.8 19.6 4.3 1.30 2.2
1984 0.60 2.0 2.7 15.8 31.7 19.5 4.3 1.30 2.2

Data for samples B-148, B-220, B-1B, and B-107B were presented previously by Deln et al. (1993), but are included here because new
isotope data are provided for these samples in Table 4

be superimposed on mantle domains with distinct iso-
topic characteristics along the archipelago (Castillo
1996).
Previously published U-series data for ve Holocene
basaltic andesites from the Taiwan segment of the Lu-
zon arc (McDermott and Hawkesworth 1991) were
characterised by very high Th contents (1424 ppm),
low (230Th/232Th) ratios (0.550.67), and high
208
Pb*/206Pb* ratios (0.981.02) that were ascribed to
mantle source modication by subducted sediment. By
contrast, the (230Th/232Th) ratios for the historic and
Holocene basaltic andesites from Mt. Mayon and the
BVC (post-caldera Sharp Peak vent) presented here
(Table 5) exhibit higher (230Th/232Th) ratios (0.891.07),

Table 4 New Sr, Nd and Pb isotope data for selected volcanics from the Mt. Bulusan volcanic complex and Mt. Mayon volcanics in the
Bicol arc
87
Sample Sr/86Sr 143
Nd/144Nd 206
Pb/204Pb 207
Pb/204Pb 208
Pb/204Pb

Post-caldera
Sharp peak volcanics
B-107B 0.70375 0.512892 18.453 15.516 38.220
Caldera
Irosin Ignimbrite
B-1B 0.70390 0.512908 18.460 15.513 38.263
Pre-caldera
Bintacan volcanics
B-148 0.70385 0.512870 18.455 15.504 38.227
Gate Mountain volcanics
90-10 0.70387 18.521 15.525 38.383
B-220 0.70399 0.512937 18.482 15.497 38.320
Mt. Mayon
1968 0.70373 0.512872 18.480 15.483 38.163
1984 0.70373 0.512909 18.484 15.493 38.175

Map units refer to those shown in Fig. 2

Table 5 U-series data for selected volcanics from the southern Bicol arc
226
Sample Age (years) Ra (fg g 1) Th (lg g 1) U (lg g 1) (238U/232Th) (230Th/232Th) (230Th/238U) (226Ra/230Th)
Bulusan volcanic complex
B107B 1020 kaa 2.049
B1-B 3540 kaa 7.153
B148 >40 <400 kaa 2.177
B220 2.14 Ma 10.54
Mt. Mayon
1968 32 years 306.06 1.726
1984 16 years 316.75 1.985
a
Denotes approximate ages based on radiocarbon dating of the Irosin ignimbrite, stratigraphic and geomorphic considerations, while
B220 has been dated using KAr (Deln et al. 1993). The Mt. Mayon samples 1968 and 1984 were erupted in the years 1968 and 1984 AD,
respectively. 226Ra measurements were completed in the year 2000 AD. All data are as measured, i.e. no age corrections have been applied
with Th contents lower by about an order of magnitude
(1.72.0 ppm). The Bicol rocks exhibit markedly lower
208
Pb*/206Pb* (0.950.96) compared with those from the
Luzon arc to the north (0.981.02), suggesting that their
sources had lower time-integrated Th/U ratios for geo-
logically long (>106 year) timescales. The absence of
large UTh disequilibria in these samples indicates either
uid-related enrichments of the mantle wedge were rel-
atively small and/or that uid-related enrichments oc-
curred, but they are relatively old compared with the
timescales required to preserve signicant disequilibria
(several hundred thousand years). A notable exception is
sample B107B, a basaltic andesite from the post-caldera
Sharp Peak volcano in the Mt. BVC that exhibits low
(238U/230Th), plotting to the left of the equiline on
Fig. 8. Paradoxically, this sample is also characterised
by higher Ba/La and Sr/Th ratios than any of the Bicol
rocks analysed here. These ratios are often interpreted to
reect a slab-derived hydrous uid signature, and so the
expectation would be that this sample should have high,
not low (238U/232Th). A possible explanation is that the
observed high Ba/La and Sr/Th ratios reect old
(>350,000 year old) modication of its mantle wedge
source by slab-derived uids, and that the source had
evolved back on to the (230Th/232Th)(238U/232Th) eq-
uiline prior to the late Pleistocene episode of partial
melting that gave rise to its magma. An alternative
explanation is that sample B107B represents a magma
generated by partial melting of a garnet-bearing source
with DU>DTh. It has been shown that depending on
garnet compositions, Sr can behave more incompatibly
than Th during melting in the presence of residual garnet
(van Westrenen et al. 2001). In those circumstances it is
possible that 230Th excess would be accompanied by
high Sr/Th ratios, as seen in sample B107B.
The 226Ra/230Th systematics for the two historic
Mayon samples analysed here appear to require recent
radium addition and rapid transport of melts to the
surface (e.g. Turner et al. 2001; Bourdon et al. 2003).
Several arcs for which 226Ra and 230Th data are avail-
able appear to dene broad positive correlations on Ba/
Th versus (226Ra/230Th) diagrams and an intriguing
possibility is that such arrays may dene the Ba/Th
ratios of the source prior to the recent addition of
0.598 0.885 1.070 1.209
2.296 0.974 0.960 0.986
0.713 0.993 0.962 0.968
2.766 0.796 0.793 0.996
0.572 1.005 1.003 0.998 1.512
0.603 0.921 0.887 0.963 1.589
(presumably slab-derived) radium (Turner et al. 2001).
Such enrichments would be expected to increase U/Th
ratios and therefore reduce any partial melting related
230
Th excesses. In the context of the available global
database for subduction-related rocks, the two samples
analysed here exhibit only moderate levels of radium
enrichment. They are characterised by Ba/Th ratios that
are intermediate between the low values of trace element
enriched arcs such as the Sunda arc and the Lesser
Antilles, and the high values that characterise the more
depleted arcs such as the Tonga-Kermadec and the
Mariana systems. Thus, the radium data for the two
historic Mayon samples require recent (<10,000 year
old) uid-related trace element enrichment.
At rst sight, the relatively high 143Nd/144Nd ratios
observed in the Bicol rocks analysed thus far (Castillo
and Newhall 2004; this study) appear to preclude sig-
nicant involvement of low 143Nd/144Nd subducted
terrigenous sediment in their mantle source. However, if
as implied by their Pb isotope systematics, the mantle
wedge beneath the southern Bicol arc is isotopically
similar to that sampled by the PKR, then it had high
143
Nd/144Nd (c. 0.51310) and low 87Sr/86Sr (c. 0.7034)
prior to the introduction of any subduction-related sig-
nature (Fig. 6). The observation that the Bicol samples
are displaced to higher 87Sr/86Sr and lower 143Nd/144Nd
relative to their putative Palau Kyushu-type mantle
wedge is important, because it permits the involvement
of some subducted sediment in their petrogenesis. Sim-
ple mass-balance mixing calculations suggest that the
involvement of a few % subducted sediment could ac-
count for the observed Pb, Sr, and Nd isotope ratios in
the Bicol volcanics, although such calculations are nec-
essarily rough because the elemental contents of the end
members are poorly constrained. Thus, we argue that
the low 87Sr/86Sr and high 143Nd/144Nd exhibited by the
Bicol samples (relative to other parts of the archipelago
such as the Macolod Corridor, for example) may in part
reect an isotopically depleted (relative to the mantle
sampled by the Philippine Sea Basin basalts) pre-sub-
duction mantle wedge, and not necessarily that an iso-
topically enriched subduction-component is negligible.
In Fig. 9a, 143Nd/144Nd ratios are plotted against
Th/Nb ratios for all of the subduction-related rocks
from the Philippines for which data are available. Also
included for comparison are the data elds for the
Marianas arc (Elliott et al. 1997). In the Mayon (Castillo
and Newhall 2004) and Macolod Corridor datasets
(Defant et al. 1988, 1989; Forster et al. 1990; Defant
et al. 1991; Miklius et al. 1991; Mukasa et al. 1994) high
Th/Nb ratios are associated with low 143Nd/144Nd ra-
tios. The rationale for this diagram is that because both
thorium and niobium are relatively insoluble in slab-
0.5131 a on Figs. 9 and 10. Moreover, in some suites (e.g. the
Marianas
0.5130 Mayon
Nd/ 144 Nd
derived hydrous uids, correlated variability such as that
observed here must reect either pre-existing melt-re-
lated enrichments in the mantle wedge or the inuence of
subducted sediment. Overall, in the Bicol arc data there
is a strong tendency for the highest Th/Nb ratios to be
developed in the most silicic samples, reecting the
tendency for Th to behave more incompatibly than Nb
during high-level (crustal) fractionation processes. For
this reason our interpretations of the causes of high Th/
Nb will be restricted to the lower (<55 wt%) silica
samples, and only these lower silica samples are plotted
Macolod Corridor data and the Mayon dataset of Ca-
stillo and Newhall (2004), the highest Th/Nb ratios are
clearly associated with the low silica (basaltic) samples.

Mayon (low
SiO2) Unlike some subduction-related volcanics (e.g. Elliott
et al. 1997) the Bicol rocks do not exhibit Nb contents
0.5129 lower than that of average N-MORB (Fig. 5a) and their
high Th/Nb ratios are largely a reection of their high
143

Macolod Th contents. One explanation is that high Th/Nb ratios

Corridor
0.5128 reect the inuence of subducted sediments, and an
AUC GLOSS objective of Fig. 9 (discussed below) is to test whether
the data can be explained by bulk addition of subducted
0.5127
0.0 0.5 1.0 1.5 2.0
N-MORB OIB

1.00
b 0.5131
Macolod
Corridor
Marianas
Mayon Mayon
Mayon (low 58.3
54.7
0.95 SiO2) 0.5129 53.9 75.6
Nd/144 Nd

52.5
Ce/Ce*

54.7

Marianas
0.5127
143

0.90

0.5125 Upper crust

Hole
0.85 801

0 0.5 1.0 1.5 2.0 0.5123

Th/Nb
143 144
Fig. 9 a Nd/ Nd versus Th/Nb ratios for samples from the
Bicol arc. Four of the ve Bicol samples have <55 wt% SiO2 (data
symbols as in Fig. 3). Also shown (dashed outlines) are the data for
Mayon volcano in the Bicol arc (Castillo and Newhall 2004). The
Mayon samples fall into two groups and it is the lower silica group
(<52.6 wt% SiO2) that exhibits highest Th/Nb ratios. Also shown
for comparison are published datasets for the Marianas (Elliott
et al. 1997) and the Macolod Corridor volcanics (Knittel et al.
1997). The black shaded area represents typical MORB composi-
tions. The vertical arrows on the abscissa mark the Th/Nb ratios of
average upper crust (AUC) after Taylor and McLennan (1985), and
an estimate of the global average subducting sediment (GLOSS)
after Plank and Langmuir (1998). Measurement errors are typically
smaller than data symbol size. b Ce/Ce* versus Th/Nb ratios for the
Bicol samples (data symbols as in Fig. 3). Also shown for reference
are the data elds for the Marianas and Macolod Corridor (data
sources as in Fig. 9a). Uncertainties in calculated Ce/Ce* are
estimated to be up to 0.02 at the 2r level, reecting the analytical
errors associated with the REE analyses and the choice of
chondrite values (error bar in upper left of diagram)
0.0 0.5 1.0
GLOSS
Th/Nd
Fig. 10 143Nd/144Nd versus Th/Nd ratios for samples from the
Bicol arc with data elds from Mt. Mayon (Castillo and Newhall
2004), the Marianas (Elliott et al. 1997), and the Macolod Corridor
(Knittell et al. 1997). Also plotted are the values for bulk pelagic
sediment from Hole 801 (ODP Leg 129) east of the Mariana
Trench (Elliott et al. 1997) and an estimate of the composition of
global subducting sediment (GLOSS) after Plank and Langmuir
(1998). The Th/Nd ratio of the average upper crust is taken from
Taylor and McLennan (1985) and should be indicative of those
terrigenous sediments. The two sloping dashed lines are mixing
trajectories between a depleted mantle composition similar to the
N-MORB source and pelagic sediment (Hole 801) and a terrige-
nous-dominated sediment (GLOSS). Most of the data plot to the
right of the mixing lines indicating that the low 143Nd/144Nd end
member must have had higher Th/Nd ratios than that of bulk
pelagic or pelagic-terrigenous mixed sediments. Typical 2r mea-
surement errors are smaller than the data symbols
sediment or if addition via a sedimentmelt component
is required.
An additional line of evidence for sediment involve-
ment in the source of the Bicol rocks is that in common
with a minority of arcs worldwide (e.g. the Marianas,
Vanuatu, Aleutians, Guatemala), the Bicol and Maco-
lod Corridor volcanics exhibit subtle negative cerium
anomalies. Negative Ce anomalies are often taken to be
a signature of subducted pelagic as opposed to terrige-
nous sediment, because of their association with bio-
genic phosphatic debris (e.g. sh teeth) that inherit REE
patterns from seawater (e.g. Hole et al. 1984; Plank and
Langmuir 1998; George et al. 2003). While analytical
errors on Ce/Ce* ratios are likely to be relatively large
(0.02), the tendency for low Ce/Ce* to be associated
with high Th/Nb is consistent with the notion that
subducted sediment, or a melt thereof, is responsible for
the low 143Nd/144Nd, high Th/Nb end member observed
in some of the low silica (<55 wt% SiO2) samples in
Fig. 9. A key question is whether negative Ce anomalies
are robust indicators of subducted pelagic sediment and
for this reason our interpretations remain tentative. We
note, for example, that in shoshonitic lavas from the
Tavau volcano, Fiji, negative cerium anomalies were
attributed to interactions between melt and highly oxi-
dising uids (Rogers and Settereld 1994). In the case of
the Tavau rocks, however, additional evidence for the
role of highly oxidising uids included the absence of Eu
anomalies, despite strong petrographic evidence for
plagioclase accumulation, and the early appearance of
titanomagnetite in the fractionating assemblage. In the
absence of such evidence for unusually oxidising con-
ditions in the Bicol magmas we tentatively interpret the
small negative Ce anomalies as reecting subducted
pelagic sediment or more likely, a partial melt thereof
involving a slab-melt component (e.g. Maury et al.
1999). As in the Marianas and Aleutians (Elliott et al.
1997; George et al. 2003), the Th/Nb ratios of the basalts
and basaltic andesites exceed those of typical pelagic
sediments suggesting that bulk sediment addition is
unlikely.
Samples with low 143Nd/144Nd ratios also exhibit
high Th/Nd ratios (Fig. 10), and in this diagram binary
mixing yields straight-line relationships. Also shown in
Fig. 10 are various estimates of the likely Th/Nd ratios
of subducted sediment. Shown for reference is a com-
monly used estimate of average bulk sediment, so
called Global Subducted Sediment (GLOSS; Plank and
Langmuir 1998) that has a Th/Nd ratio of 0.26, lower
than that of the upper continental crust (0.41, Taylor
and McLennan 1985). Pelagic sediments tend to have
lower Th/Nd ratios (e.g. 0.124 for bulk pelagic sedi-
ment from Hole 801, Elliott et al. 1997). Thus,
depending on the ratio of pelagic to terrigenous sedi-
ment being subducted, the Th/Nd ratio of the bulk
sediment is likely to be in the range 0.10.4.
Assuming that its 143Nd/144Nd ratio is lower than
about 0.5127, it seems unlikely that the low
143
Nd/144Nd component of many of the Bicol or
Macolod Corridor rocks could reect bulk sediment
addition to the mantle wedge. Instead it appears that
sediment addition occurred via a small degree partial
melt that fractionates the trace element ratios of the
bulk subducted sediment, and in particular raises the
Th/Nb and Th/Nd ratio of this end member. Samples
such as B148 (Bintacan volcanics), for example, are
true basalts (52.5 wt% SiO2) and exhibit Th/Nb ratios
in excess of 0.8, signicantly higher than that of any
likely subducted sedimentary end member. Similar
arguments apply to the two Mayon samples analysed
here and more particularly to the low-silica Mayon
group of Castillo and Newhall (2004), see Fig. 9a.
Similarly, many of the Bicol rocks exhibit Th/Nd ratios
that exceed those of average OIB and estimates of bulk
subducted sediment at several sites globally (Elliott
et al. 1997; Plank and Langmuir 1998; George et al.
2003).
A key remaining issue is whether the sediment com-
ponent was added via a slab-derived partial melt that
included a small melt contribution from the subducted
oceanic crust. Importantly, previous studies (Schiano
et al. 1995; Maury et al. 1999) have demonstrated that
mantle xenoliths from northern Luzon arc lavas exhibit
enrichments consistent with the presence of a slab-de-
rived partial melt that includes a contribution from a
very low degree melt of the subducted oceanic crust.
Similar processes have been reported in the Kamchatka
arc (e.g. Kepezhinskas et al. 1995, 1996; Kepezhinskas
and Defant 1996). In the absence of mantle xenolith data
for the Bicol arc there is at present no strong evidence
that the sediment-related component was added to the
mantle wedge via a melt that included a melt fraction
from the subducted oceanic crust. We note however that
thermal modelling (Peacock 1990; Peacock et al. 1994)
permits that small amounts of slab melting may occur
during the transient stage accompanying the initiation of
subduction, a situation that may pertain beneath this
part of the Philippine archipelago where subduction
along the Philippine Trench commenced within the past
34 Ma (Sajona et al. 1993).
Conclusions
Volcanic rocks from the BVC and from Mayon volcano
in the southern part of the Bicol arc exhibit a wide
compositional range. The earliest (Pliocene) eruptives
from the BVC (Gate volcanics) are a distinct high-K
suite characterised by strong incompatible trace element
enrichment. Field, petrographic and geochemical evi-
dence indicates that intracrustal processes such as
magma mixing and fractional crystallisation played an
important role in the petrogenesis of the more evolved
syn- and post-caldera magmas. Volcanics from Mayon
appear to be dominated by medium-K basaltic andesites
and andesites (Castillo and Newhall 2004; this study),
with LIL enrichments and HFS element depletions
typical of subduction-related rocks. None of the Bicol
rocks display depletions in the HFS elements relative to
N-MORB that are a feature of some other arcs. As a
group, the Bicol lavas exhibit lower and less variable
87
Sr/86Sr ratios (0.70360.7039) than those from the
Bataan arc, the Macolod Corridor, the Mindoro arc,
and the Taiwan/Babuyan segments of the Philippine
archipelago. Pb isotope ratios typically plot within and
below the data eld for the Philippine Sea Basin and the
NHRL on 207Pb/204Pb versus 206Pb/204Pb and
208
Pb/204Pb versus 206Pb/204Pb diagrams. We interpret
this to reect the presence of a pre-subduction mantle
wedge of Indian Ocean type, similar to that sampled by
the PKR, east of the Philippine Trench. Previous claims
for the presence of a Dupal-type Pb isotope signature
(Mukasa et al. 1987) are not supported by the new data.
Samples with lower 143Nd/144Nd tend to have high Th/
Nd, high Th/Nb, and low Ce/Ce* ratios, interpreted to
reect subduction of pelagic sediment. The low
143
Nd/144N rocks exhibit Th/Nb and Th/Nd ratios that
are higher than those of typical subducted pelagic sedi-
ment, indicating that the latter was incorporated into the
mantle wedge as a slab-derived partial melt rather than
as a bulk sediment mixture. Unlike the Luzon and the
Bayuban-Taiwan arc where eastward subduction along
the Manila trench of terrigenous sediments can account
for much of the isotopic variability, the Bicol arc vol-
canics appear to reect westerly directed subduction of
pelagic sediments along the Philippine Trench. The new
data extend the range of isotopic compositions previ-
ously published for the Philippine volcanics, and rein-
force suggestions that there are distinct mantle domains
beneath the Philippine archipelago (Castillo 1996), as
well as distinct regional isotopic signatures in the sedi-
ments being subducted along it (McDermott et al. 1993).
Acknowledgements The authors wish to thank Pat Castillo for a
pre-print of a manuscript on the Mt. Mayon volcanics and for
permission to refer to the data contained therein. FMcD gratefully
acknowledges support from a University College Dublin Newman
Scholarship during the early stages of this study. We acknowledge
the thorough and constructive reviews by John Maclennan and an
anonymous reviewer that greatly improved the manuscript.
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