18
SUPPLEMENTARY INFORMATION DOI: 10.1038/NGEO471 NATURE GEOSCIENCE | www.nature.com/naturegeoscience 1 Supplementary Material _____________________________________________________ Supplementary Figures Figure S1: Comparative systematics of Izu Bonin magmas and mid-oceanic ridge magmas. a. Pb/Yb vs Nb/Yb, b. Nd/Yb vs Nb/Yb. Note overlap between the trace element ratios of the basaltic-andesite to rhyolitic tephra with the more mafic magmas of the present-day arc. This shows that melt differentiation by crystallization of the principal phases olivine, pyroxene, plagioclase, and rare amphibole in medium-K, high-silica melts does not erase the source characteristics of the IB mantle melts 1,2 . The percentage of Pb added from slab to the IB arc is based on a mass balance calculation suggested by Pearce et al. 3 . The calculation assumes that IB arc magmas are a binary mixture of a ‘background mantle’ (that is, a mantle without subduction component) and a composite component from slab with contributions from the sedimentary and igneous oceanic crust. The melting in the background mantle is considered to be subjected to the same systematics as mid- ocean ridge magmas. Thus, elements not added from slab (e.g. Nb, Yb) must behave similarly as in MORB. By comparison to MORB, the percentage of an element added from slab can be estimated in the X/Nb vs Yb/Nb space, whereby X is the element to be investigated (e.g. Pb, Nd; Figure S1). Full equations are written out in Straub et al. 2 who showed that >90% of highly fluid mobile elements (e.g. Pb, Ba, Cs, Rb, U) at the Neogene Izu arc front are contributed from slab, but <30% of the light rare earth elements.

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Page 1: SUPPLEMENTARY INFORMATION - Nature Research · Asian dust is after Pettke et al.54, in Plank et al.52, and Jahn et al.55. Jurassic to Cretaceous igneous crust composition are from

SUPPLEMENTARY INFORMATIONdoi: 10.1038/ngeo471

nature geoscience | www.nature.com/naturegeoscience 1

# NGS-2008-12-01200 1

Supplementary Material _____________________________________________________

Supplementary Figures

Figure S1: Comparative systematics of Izu Bonin magmas and mid-oceanic ridge magmas. a.

Pb/Yb vs Nb/Yb, b. Nd/Yb vs Nb/Yb.

Note overlap between the trace element ratios of the basaltic-andesite to rhyolitic tephra with

the more mafic magmas of the present-day arc. This shows that melt differentiation by

crystallization of the principal phases olivine, pyroxene, plagioclase, and rare amphibole in

medium-K, high-silica melts does not erase the source characteristics of the IB mantle melts1,2.

The percentage of Pb added from slab to the IB arc is based on a mass balance calculation

suggested by Pearce et al.3. The calculation assumes that IB arc magmas are a binary mixture of a

‘background mantle’ (that is, a mantle without subduction component) and a composite

component from slab with contributions from the sedimentary and igneous oceanic crust. The

melting in the background mantle is considered to be subjected to the same systematics as mid-

ocean ridge magmas. Thus, elements not added from slab (e.g. Nb, Yb) must behave similarly as

in MORB. By comparison to MORB, the percentage of an element added from slab can be

estimated in the X/Nb vs Yb/Nb space, whereby X is the element to be investigated (e.g. Pb, Nd;

Figure S1). Full equations are written out in Straub et al.2 who showed that >90% of highly fluid

mobile elements (e.g. Pb, Ba, Cs, Rb, U) at the Neogene Izu arc front are contributed from slab, but

<30% of the light rare earth elements.

Page 2: SUPPLEMENTARY INFORMATION - Nature Research · Asian dust is after Pettke et al.54, in Plank et al.52, and Jahn et al.55. Jurassic to Cretaceous igneous crust composition are from

2 nature geoscience | www.nature.com/naturegeoscience

SUPPLEMENTARY INFORMATION doi: 10.1038/ngeo471

# NGS-2008-12-01200 2

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nature geoscience | www.nature.com/naturegeoscience 3

SUPPLEMENTARY INFORMATIONdoi: 10.1038/ngeo471

# NGS-2008-12-01200 2

# NGS-2008-12-01200 3

Figure S2. Age-area distribution of the ocean floor from Mueller et al.,4. Six intervals are shown

(A) 140 Ma, (B) 120 Ma, (C) 90 Ma, (D) 60 Ma, (E) 40 Ma and (F) 20 Ma. Mid-ocean ridges in white,

all other plate boundaries in black. Black triangles indicate subduction zone polarity. The

Mesozoic Pacific plate grew from three outward moving spreading centers: Izanaghi-Pacific Ridge

(NW), the Farallon-Pacific Ridge (NE) and the Phoenix-Pacific ridge (S). PAC – Pacific plate; IZA –

Izanaghi plate, FAR- Farallon plate, PHX – Phoenix plate, I-P rigde – Izanaghi-Pacific spreading

center, AUS – Australia, EUR – Eurasia. Brown filled circle estimated path of Site 581 (~124-127 Ma)

on the SE flank of the crust generated at the Izanaghi-Pacific Ridge.

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4 nature geoscience | www.nature.com/naturegeoscience

SUPPLEMENTARY INFORMATION doi: 10.1038/ngeo471

# NGS-2008-12-01200 4

SUPPLEMENTARY NOTES

The rock record of the Izu Bonin arc The rock record of the Izu Bonin arc has been summarized by Straub5,6. Lavas have been

recovered from the present-day arc (<1 Ma; between 27.7-34.7ºN) and the boninitic-tholeiitic

Eocene arc (~49-45 Ma). The Eocene arc has been sampled at the uplifted forearc islands

Chichijima and Hajajima, submarine Bonin Ridge (BR), and ODP sites 782 and 786. Except for

some late Eocene arc lavas (~37 Ma; ODP sites 793 and 792) and a Miocene sill (14 Ma, Site 793),

the remaining stratigraphic gaps can be bridged by time-precise fallout tephra with an average

temporal resolution ~1 Ma and precision6. The tephra was collected by SMS in 1992 and 1998 at

the ODP Gulf Coast Repository in College Station/TX from ODP Site 782A (30.8566ºN; 141.3085ºE,

ca. 120 km east of the present-day volcanic front, Figure 1). Two additional Quaternary tephra

samples from ODP Site 790C are included. The tephra is mostly dark-brown to grey ash-sized

fallout tephra. Pumice fallout is subordinate. All are tephra deposits were macroscopically visible

and display no or minimal signs of bioturbation or redeposition.

Absolute Ages of Samples

Except for the Miocene sill at ODP Site 793 (biostratigraphic age), the pre-Quaternary lavas are

were physically dated by various groups: ODP Sites 792 and 793 basementO. Ishizuka and R.

Taylor, pers. communication 2006,7), ODP Site 786, Chichijima and Bonin Ridge Escarpment8, and

Hahajima9. Tephra ages are based on the nannofossil biostratigraphy of Xu and Wise10 and Ar/Ar

dating of Schmidt11. Only age-corrected data were used, except for the Site 793 Miocene sill for

which no Th, U and Pb abundance data were available.

Data sources This study obtained new Pb isotope ratios that are presented together with selected new major

and trace element data in Tables 1 and 2. The new data are from samples from Site 782A fallout

tephra (n=63 samples), Site 790 fallout tephra (n=2), two clasts from the site 782A basement, two

Shikoku backarc basin basalts (glass from pillow rims of DSDP Sites 442 and 443) and two samples

from Sofugan Volcano (present-day arc, samples obtained from C. H. Langmuir). All other data

were collected from the literature, including the GeoROC12 and PetDB13data bases. Individual

publications for the Izu Bonin Mariana system are listed below.

Page 5: SUPPLEMENTARY INFORMATION - Nature Research · Asian dust is after Pettke et al.54, in Plank et al.52, and Jahn et al.55. Jurassic to Cretaceous igneous crust composition are from

nature geoscience | www.nature.com/naturegeoscience 5

SUPPLEMENTARY INFORMATIONdoi: 10.1038/ngeo471

# NGS-2008-12-01200 4

SUPPLEMENTARY NOTES

The rock record of the Izu Bonin arc The rock record of the Izu Bonin arc has been summarized by Straub5,6. Lavas have been

recovered from the present-day arc (<1 Ma; between 27.7-34.7ºN) and the boninitic-tholeiitic

Eocene arc (~49-45 Ma). The Eocene arc has been sampled at the uplifted forearc islands

Chichijima and Hajajima, submarine Bonin Ridge (BR), and ODP sites 782 and 786. Except for

some late Eocene arc lavas (~37 Ma; ODP sites 793 and 792) and a Miocene sill (14 Ma, Site 793),

the remaining stratigraphic gaps can be bridged by time-precise fallout tephra with an average

temporal resolution ~1 Ma and precision6. The tephra was collected by SMS in 1992 and 1998 at

the ODP Gulf Coast Repository in College Station/TX from ODP Site 782A (30.8566ºN; 141.3085ºE,

ca. 120 km east of the present-day volcanic front, Figure 1). Two additional Quaternary tephra

samples from ODP Site 790C are included. The tephra is mostly dark-brown to grey ash-sized

fallout tephra. Pumice fallout is subordinate. All are tephra deposits were macroscopically visible

and display no or minimal signs of bioturbation or redeposition.

Absolute Ages of Samples

Except for the Miocene sill at ODP Site 793 (biostratigraphic age), the pre-Quaternary lavas are

were physically dated by various groups: ODP Sites 792 and 793 basementO. Ishizuka and R.

Taylor, pers. communication 2006,7), ODP Site 786, Chichijima and Bonin Ridge Escarpment8, and

Hahajima9. Tephra ages are based on the nannofossil biostratigraphy of Xu and Wise10 and Ar/Ar

dating of Schmidt11. Only age-corrected data were used, except for the Site 793 Miocene sill for

which no Th, U and Pb abundance data were available.

Data sources This study obtained new Pb isotope ratios that are presented together with selected new major

and trace element data in Tables 1 and 2. The new data are from samples from Site 782A fallout

tephra (n=63 samples), Site 790 fallout tephra (n=2), two clasts from the site 782A basement, two

Shikoku backarc basin basalts (glass from pillow rims of DSDP Sites 442 and 443) and two samples

from Sofugan Volcano (present-day arc, samples obtained from C. H. Langmuir). All other data

were collected from the literature, including the GeoROC12 and PetDB13data bases. Individual

publications for the Izu Bonin Mariana system are listed below.

# NGS-2008-12-01200 5

Izu Bonin and Mariana Arcs

For the purpose of this study, the present-day Izu volcanic arc are all magmas erupted from arc

front volcanoes between 34º43’6”N and 27º42’N. The Neogene Izu rear-arc are all magmas behind

the Izu arc front between 34º38’N and 30º31’N. All arc front volcanoes of the Izu Bonin-Mariana

arc south of 27º42’N are considered part of the IBM transition and the Mariana arc. Data sources

are as follows: Amma-Miyasaka and Nakagawa14, Hochstaedter et al.15, Ikeda and Yuasa16,

Ishizuka et al.17,18, Langmuir et al.19, Shukuno et al.20, Tamura et al.21, Taylor & Nesbitt22, Yokoyama

et al.23, Elliott et al.24, Kohut et al.25, Lin et al.26, Bloomer et al.27, Pearce et al.28, Stern et al.29,

Woodhead30,31, Woodhead and Fraser32, Woodhead33, Woodhead et al.34, Wade et al.35, Sun et al.36,

Sun and Stern37, Stern et al.38, Peate and Pearce39,40, Taylor et al.41,42, Ishizuka et al.8, Hickey and

Frey43, Dobson44 and Taylor and Nesbitt9.

IBM Backarc Basins (Shikoku and Parece Vela Basin, Mariana Trough)

Hickey-Vargas45, Hickey-Vargas46, Gribble et al.47, Gribble et al.48, Stern et al.49 and Volpe et al.50.

Jurassic to Recent Pacific Crust outboard the Izu Bonin-Mariana arcs

Cretaceous to Recent pelagic sediment is from Plank and Langmuir51, Plank et al.52, Hauff et

al.53 and Hochstaedter et al.15. Asian dust is after Pettke et al.54, in Plank et al.52, and Jahn et al.55.

Jurassic to Cretaceous igneous crust composition are from Castillo et al.56, Castillo et al.57, Castillo

et al.58, Janney and Castillo59, Janney and Castillo60, Janney and Castillo61. Koppers et al.62, Koppers

et al.63, Koppers & Staudigel64,34 and Pearce et al.28.

Pb isotope data for other arcs

The Pb isotope data from NE Honshu, Kuriles, Kamchatka and Aleutians were collected from

GeoROC12 (‘precompiled’ mode’). The data were filtered to ensure that they represented arc front

volcanism with high slab contributions. Selection criteria varied according to data availability. NE

Honshu – only samples between 139º to 141.25ºE and 36.55º and 42.05ºN, and with Nb/La< 0.6,

Ce/Pb<5 and Nb <4.9 ppm; Kuriles – only samples with radiogenic Nd isotope ratios >0.513 and an

overall positive correlation of Sr and Nd isotopes as typical for fluid-dominated arc front magmas;

Kamchatka Nb/La<0.5, Ce/Pb <8 and Nb <11 ppm; Central and Western Aleutians with Nb/La

<0.5, Ce/Pb<10 and Nb <5.6 ppm. Tonga-Kermadec data are from Turner et al.65, Ewart et al.66 .

Lesser Antilles data are from Smith et al.67, Thirlwall et al.68 and Turner et al.69. Data on SW

Honshu, Ruykyu, Luzon and Sunda arcs are from GeoROC12 (‘pre-compiled’ mode).

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6 nature geoscience | www.nature.com/naturegeoscience

SUPPLEMENTARY INFORMATION doi: 10.1038/ngeo471

# NGS-2008-12-01200 6

SUPPLEMENTARY METHODS

Sample Preparation and Analytical Methods

Tephra sample preparation

A volume of ~5 to 10 cubic centimeters was freeze-dried and wet-sieved through a 32 µm or 63

µm polyester mesh using de-ionized water. Fresh tephra particles (pumice, scoria, glassy

fragments, juvenile lithics and scoria) were handpicked under a binocular microscope (typically

>200 mg to 1 g clean material). The hand-picked fraction was multiply washed with double-

distilled water and methanol in ultrasonic bath. Dried samples were split for the analyses of Sr-

Nd-Pb-Hf isotope analyses (particle separates) and bulk major and trace element analyses

(powders, were prepared in agate or alumina mortars).

Pb isotopes analyses

Analyses of Pb isotopes are either those of Schmidt11 (n=33 samples; see http://eldiss.uni-

kiel.de/macau/receive/dissertation _diss_00000465 for methods) or have been measured at Lamont

(n=13 samples, plus 2 replicates of Schmidt samples).

At the Geomar, sample chips were leached for one hour with hot 6N HCl and then digested in

hot HF +HNO3 solution prior to standard ion exchange procedures11. The total chemistry blanks

for Pb was <300 pg and is considered negligible. Pb isotope ratios were acquired on a Finnigan®

MAT 262 thermal ionization mass spectrometer in the static mode. External reproducibility of NBS

981 (n=20) gave 206Pb/204Pb= 16.898 (20,000 ppm, 2 sigma), 207Pb/204Pb= 15.439 (22,000 ppm),

208Pb/204Pb= 36.531 (35,000 ppm). Replicate analyses yielded an external reproducibility better than

0.05% per a.m.u. (atomic mass unit) for Pb.

At Lamont, sample chips for isotope analyses were leached twice with hot 6N HCl for 1 hour

and then digested in a 2:1 HF + HNO3 solution. Separation chemistry used Dowex AG1X-8 100-200

mesh resin using standard separation procedures published in the Lab Handbook of the Isotope

Geochemistry Lab at LDEO (http://www.ldeo.columbia.edu/res/fac/isotopelab/).

Pb isotope ratios were acquired on a VG Sector 54-30 thermal ionization mass spectrometer. Pb

was measured using a 207Pb/204Pb double spike. External reproducibility for Pb was established by

multiple analyses of double spiked NBS SRM 981 standard over the time of this project and gave

206Pb/204 Pb = 16.9298 (193 ppm 2 sigma), 207Pb/204Pb = 15.4898 (256 ppm), and 208Pb/204Pb = 36.7022

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nature geoscience | www.nature.com/naturegeoscience 7

SUPPLEMENTARY INFORMATIONdoi: 10.1038/ngeo471

# NGS-2008-12-01200 6

SUPPLEMENTARY METHODS

Sample Preparation and Analytical Methods

Tephra sample preparation

A volume of ~5 to 10 cubic centimeters was freeze-dried and wet-sieved through a 32 µm or 63

µm polyester mesh using de-ionized water. Fresh tephra particles (pumice, scoria, glassy

fragments, juvenile lithics and scoria) were handpicked under a binocular microscope (typically

>200 mg to 1 g clean material). The hand-picked fraction was multiply washed with double-

distilled water and methanol in ultrasonic bath. Dried samples were split for the analyses of Sr-

Nd-Pb-Hf isotope analyses (particle separates) and bulk major and trace element analyses

(powders, were prepared in agate or alumina mortars).

Pb isotopes analyses

Analyses of Pb isotopes are either those of Schmidt11 (n=33 samples; see http://eldiss.uni-

kiel.de/macau/receive/dissertation _diss_00000465 for methods) or have been measured at Lamont

(n=13 samples, plus 2 replicates of Schmidt samples).

At the Geomar, sample chips were leached for one hour with hot 6N HCl and then digested in

hot HF +HNO3 solution prior to standard ion exchange procedures11. The total chemistry blanks

for Pb was <300 pg and is considered negligible. Pb isotope ratios were acquired on a Finnigan®

MAT 262 thermal ionization mass spectrometer in the static mode. External reproducibility of NBS

981 (n=20) gave 206Pb/204Pb= 16.898 (20,000 ppm, 2 sigma), 207Pb/204Pb= 15.439 (22,000 ppm),

208Pb/204Pb= 36.531 (35,000 ppm). Replicate analyses yielded an external reproducibility better than

0.05% per a.m.u. (atomic mass unit) for Pb.

At Lamont, sample chips for isotope analyses were leached twice with hot 6N HCl for 1 hour

and then digested in a 2:1 HF + HNO3 solution. Separation chemistry used Dowex AG1X-8 100-200

mesh resin using standard separation procedures published in the Lab Handbook of the Isotope

Geochemistry Lab at LDEO (http://www.ldeo.columbia.edu/res/fac/isotopelab/).

Pb isotope ratios were acquired on a VG Sector 54-30 thermal ionization mass spectrometer. Pb

was measured using a 207Pb/204Pb double spike. External reproducibility for Pb was established by

multiple analyses of double spiked NBS SRM 981 standard over the time of this project and gave

206Pb/204 Pb = 16.9298 (193 ppm 2 sigma), 207Pb/204Pb = 15.4898 (256 ppm), and 208Pb/204Pb = 36.7022

# NGS-2008-12-01200 7

(247 ppm), respectively (n=52 for each). A blank for Pb was processed with each chemistry,

yielding an average of 160pg (n=4) and is considered negligible.

Pb isotope ratios measured at the Geomar and at Lamont were normalized to the values of

Todt et al.70 (206Pb/204Pb=16.9356, 207Pb/204Pb=15.4891 and 208Pb/204Pb=36.7006).

Trace element analyses

Bulk trace element analyses of sample powders were carried out either at the Centro de

Geociencias (CGEO), Juriquilla/Qro., UNAM, using a Thermo Series XII instrument (n=37), or at

the Institute of Geosciences (IfG) at Kiel University using a VG PlasmaQuad PQ 1 ICP mass

spectrometer with a multichannel analyser (n=21).

The data at the CGEO were obtained in three different runs between January and May 2007.

Powders were dissolved in HNO3 and diluted by a factor of 2000. Samples were blank-corrected

prior to correction for instrumental drift by internal standards (10 ppb Ge; 5 ppb of In, Tm and Bi)

and normalizing abundances to a highly enriched alkali basalt sample PS-99-25 from the Palma

Sola Massif71, that was repeatedly analyzed during each run. Standard calibration was done by

standard reference materials MAR (Lamont in-house standard; excluding W), BIR2 (excluding Ta,

Tl and P), JB2 and DNC (excluding Sb, Sn) and JA1 (for U and Th only). Calibrations were

strongly linear (R2 ≥0.999 for most elements). Average and relative standard deviation are based

on repeat analyses of a dacite sample from Izu volcanic front that was analyzed twice during each

run, as well as reference sample JA1, run as unknown excepting Th and U. Average and RSD% of

monitor samples are listed together with reference values in Table 3.

The IfG data were obtained in 1994. Analytical procedures are those of Garbe-Schönberg et al.72.

Powders were decomposed by a pressurized HF-HClO4-aqua regia attack. Accuracy and precision

of the mass spectrometer are considered better than 3% for the rare earth elements and better than

5% for most other trace elements72. The IFG analyses of the Site 782A as those used by Straub73

with the exception of one additional sample (782A-17X-1-56-58) reported by Schmidt11.

The values listed in Table 2 are reported corrected relative to concurrently analyzed standard

reference material BHVO-1 and BIR1 using the reference values from the Langmuir Laboratory at

Harvard University. After correction, the IfG data compare to the CGEO data within ≤10% for the

REE (except Ce, Nd), Ga, Cs, Pb, Sr, Ba, Zr, Y, Ba, within ≤20% for Sc, Tl, Rb, Th, U, Hf, Ce, Nd and

within ≤25% for Li, Nb and Ta. The agreement is considered satisfactory given that the sample

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8 nature geoscience | www.nature.com/naturegeoscience

SUPPLEMENTARY INFORMATION doi: 10.1038/ngeo471

# NGS-2008-12-01200 8

powders were prepared from different hand-picked fractions prepared in 1993 (for IfG) and 2006

(for CGEO).

For some tephra samples (n=4) and the two Shikoku Basin pillow basalts, trace element data

were obtained by laser ablation analyses. The analytical techniques are those of Straub et al.2 who

have already reported the tephra data and one of the Shikoku Basin pillow basalts. The laser-

ablation analyses were calibrated using a glass of BIR-1 standard material. No further correction

was applied with respect to the comparability of the glass data to the bulk data.

If multiple trace element data were available by two or three of the protocols described, highest

priority was given to the CGEO data, following the IfG data, and finally the laser ablation data.

The difference in material between bulk and microbeam methods (scoria vs glass) did not lead to

significant discrepancies as shown by the comparison of multiple trace element data on a single

sample obtained by various methods.

Major element analyses

Major element composition of bulk samples (n=64) were also obtained by different methods.

For the Shikoku basin pillow basalts, and for two thirds of the younger tephra samples of Site

782A (n=41), a bulk composition is the average of glass shard and melt inclusions compositions

that were obtained by electron microprobe analysis, see Straub5 for data and methods. Major

element compositions of the Eocene and Oligocene samples that either contain no glass shards or

no melt inclusion-bearing phenocrysts were obtained from powders of handpicked tephra

particles by ICP-ES (n=21).

ICP-ES analyses were performed following the procedures outlined by Kelley74. Sample

powders were ignited at 950ºC for 45 min to measure the loss on ignition (LOI), mixed with

lithium metaborate (1:4) and fused at 1050ºC for 15 min. Molten beads were dissolved in 5% nitric

acid, and diluted by mass to a final solution of 1:4000 in 2% HNO3. A procedural blank as well as

standard reference materials RGM1, JB2 and NBS688 were prepared in the same manner. Data

were reduced by blank subtraction, external drift correction and standard calibration using the

values of the Langmuir Laboratory at Harvard University (C. H. Langmuir, personal

communication, 2005). Calibrations were strongly linear (R2 ≥0.999) and sum of oxides were

within 1% on average. LOI of samples (between 0.3 and 6.6%) correlates with SiO2 content but not

with sample age (0-42 Ma) or the sum of oxides.

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nature geoscience | www.nature.com/naturegeoscience 9

SUPPLEMENTARY INFORMATIONdoi: 10.1038/ngeo471

# NGS-2008-12-01200 8

powders were prepared from different hand-picked fractions prepared in 1993 (for IfG) and 2006

(for CGEO).

For some tephra samples (n=4) and the two Shikoku Basin pillow basalts, trace element data

were obtained by laser ablation analyses. The analytical techniques are those of Straub et al.2 who

have already reported the tephra data and one of the Shikoku Basin pillow basalts. The laser-

ablation analyses were calibrated using a glass of BIR-1 standard material. No further correction

was applied with respect to the comparability of the glass data to the bulk data.

If multiple trace element data were available by two or three of the protocols described, highest

priority was given to the CGEO data, following the IfG data, and finally the laser ablation data.

The difference in material between bulk and microbeam methods (scoria vs glass) did not lead to

significant discrepancies as shown by the comparison of multiple trace element data on a single

sample obtained by various methods.

Major element analyses

Major element composition of bulk samples (n=64) were also obtained by different methods.

For the Shikoku basin pillow basalts, and for two thirds of the younger tephra samples of Site

782A (n=41), a bulk composition is the average of glass shard and melt inclusions compositions

that were obtained by electron microprobe analysis, see Straub5 for data and methods. Major

element compositions of the Eocene and Oligocene samples that either contain no glass shards or

no melt inclusion-bearing phenocrysts were obtained from powders of handpicked tephra

particles by ICP-ES (n=21).

ICP-ES analyses were performed following the procedures outlined by Kelley74. Sample

powders were ignited at 950ºC for 45 min to measure the loss on ignition (LOI), mixed with

lithium metaborate (1:4) and fused at 1050ºC for 15 min. Molten beads were dissolved in 5% nitric

acid, and diluted by mass to a final solution of 1:4000 in 2% HNO3. A procedural blank as well as

standard reference materials RGM1, JB2 and NBS688 were prepared in the same manner. Data

were reduced by blank subtraction, external drift correction and standard calibration using the

values of the Langmuir Laboratory at Harvard University (C. H. Langmuir, personal

communication, 2005). Calibrations were strongly linear (R2 ≥0.999) and sum of oxides were

within 1% on average. LOI of samples (between 0.3 and 6.6%) correlates with SiO2 content but not

with sample age (0-42 Ma) or the sum of oxides.

# NGS-2008-12-01200 9

SUPPLEMENTARY REFERENCES 1. Bryant, C. J., Arculus, R. J. & Eggins, S. M. The Geochemical Evolution of the Izu-Bonin Arc System: A

Perspective from Tephras Recovered by Deep-Sea Drilling. Geochem Geophys Geosys 4, 1094, doi:10.1029/2002GC000427 (2003).

2. Straub, S. M., Layne, G. D., Schmidt, A. & Langmuir, C. H. Volcanic glasses at the Izu arc volcanic front: new perspectives on fluid and sediment melt recycling in subduction zones. Geochem Geophys Geosys 5, Q01007, doi:10.1029/2002GC000408 (2004).

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# NGS-2008-12-01200 13

Supplementary Table 1: Pb isotope ratios of Izu Bonin arc volcanics and Shikoku Basin pillow basalts glasses. Sample_ID Age (Ma) 206Pb/204Pbm 207Pb/204Pbm 208Pb/204Pbm 238U/204Pb 235U/204Pb 232Th/204Pb 206Pb/204Pbi 207Pb/204Pbi 208Pb/204Pbi Analysta Sofugan Volcano Sof1A 0.0 18.491 15.527 38.281 5.23 0.038 7.68 18.491 15.527 38.281 as Sof-3 0.0 18.522 15.544 38.330 7.98 0.058 13.32 18.522 15.544 38.330 as Shikoku Backarc Basin 442B-19R2-59-63 19 17.767 15.413 37.485 7.25 0.053 18.57 17.746 15.412 37.468 as 443-62R3-71-74 17 17.806 15.416 37.550 6.42 0.047 18.27 17.789 15.415 37.535 as 444A-26R1-9-13 15 18.075 15.449 37.773 33.53 0.243 85.03 17.997 15.445 37.710 as Tephra fallout from ODP sites 782A and 790B/C 790C-7H-6-74-76 0.09 18.482 15.527 38.324 5.70 0.041 9.65 18.481 15.527 38.324 cc 782A-2H4-113-114 0.55 18.434 15.529 38.255 4.39 0.032 4.76 18.434 15.529 38.255 as 782A-2H5-136-138 0.63 18.447 15.535 38.286 4.39 0.032 5.68 18.447 15.535 38.285 cc

replicate b 0.63 18.450 15.540 38.294 4.39 0.032 5.68 18.450 15.540 38.294 as 782A-2H6-85-87 0.68 18.446 15.545 38.313 2.81 0.020 4.51 18.446 15.545 38.313 as

repeat b 0.68 18.428 15.538 38.280 2.81 0.020 4.51 18.428 15.538 38.280 as 782A-11X1-55-57 2.79 18.362 15.517 38.168 2.03 0.015 1.38 18.361 15.517 38.168 as 782A-11X-3-0-1 2.84 18.357 15.528 38.199 3.70 0.027 5.12 18.355 15.528 38.198 as 782A-15X3-9-10 3.78 18.412 15.533 38.240 2.38 0.017 3.41 18.411 15.533 38.239 as 782A-17X1-56-58 4.79 18.403 15.532 38.252 3.29 0.024 3.96 18.401 15.532 38.251 as 782A-17X4-0-2 4.79 18.385 15.516 38.204 2.95 0.021 3.32 18.383 15.516 38.203 as 782A-19X-2-24-26 6.03 18.448 15.539 38.337 2.06 0.015 2.75 18.446 15.539 38.336 as 782A-21X2-84-86 7.23 18.455 15.532 38.327 2.28 0.017 1.63 18.452 15.532 38.326 as 782A-21X3-0-2 7.27 18.418 15.538 38.348 3.01 0.022 4.65 18.415 15.538 38.346 as 782A-23X4-107-109 8.59 18.444 15.527 38.292 2.12 0.015 3.17 18.441 15.527 38.291 as 782A-26X4-52-54 10.30 18.398 15.503 38.160 3.86 0.028 5.66 18.392 15.503 38.157 as 782A-26X5-147-149 10.45 18.384 15.503 38.158 4.53 0.033 6.32 18.377 15.503 38.155 as 782A-29X6-124-126 12.27 18.371 15.506 38.166 2.31 0.017 3.45 18.367 15.506 38.164 as 782A-29X-CC-5-7 12.31 18.200 15.488 38.024 8.33 0.060 25.61 18.184 15.488 38.008 cc 782A-30X-CC-27-30 12.50 18.295 15.509 38.168 6.43 0.047 20.71 18.282 15.509 38.155 cc 782A-32X2-26-28 13.35 18.381 15.511 38.234 2.76 0.020 4.71 18.375 15.511 38.231 as

repeat b 13.35 18.392 15.519 38.266 2.77 0.020 4.71 18.386 15.519 38.263 as 782A-33X5-36-39 14.20 18.391 15.504 38.201 2.76 0.020 4.70 18.385 15.504 38.198 as 782A-36X3-57-59 26.22 18.367 15.515 38.287 1.89 0.014 3.39 18.359 15.515 38.283 as

repeat b 26.22 18.350 15.497 38.229 8.91 0.065 25.48 18.314 15.495 38.196 as 782A-37X-2-48-50 28.41 18.094 15.465 37.869 3.54 0.026 10.27 18.078 15.464 37.854 cc 782A-37X4-43-45 29.22 18.147 15.467 37.910 12.69 0.092 38.18 18.089 15.464 37.855 as 782A-37X6-105-107 30.22 18.312 15.487 38.135 3.51 0.025 8.78 18.296 15.486 38.122 as 782A-39X-1-21-23 33.26 18.431 15.544 38.338 0.70 0.005 1.20 18.428 15.544 38.336 cc

# NGS-2008-12-01200 14

replicate b 33.26 18.409 15.524 38.256 0.70 0.005 1.20 18.405 15.524 38.254 as 782A-39X-1-127-129 33.55 18.161 15.464 37.909 3.50 0.025 9.67 18.143 15.463 37.893 cc 782A-39X-2-16-18 33.66 18.165 15.463 37.910 4.44 0.032 11.93 18.142 15.462 37.890 cc 782A-39X2-42-44 33.73 18.171 15.467 37.931 3.90 0.028 9.69 18.151 15.466 37.915 as 782A-40X-1-93-96 36.11 18.242 15.472 37.992 5.38 0.039 11.59 18.212 15.471 37.972 cc 782A-41X-3-8-9 39.39 18.135 15.479 37.885 3.26 0.024 5.55 18.115 15.478 37.874 cc 782A-41X4-71-73 39.98 18.117 15.469 37.843 3.23 0.023 4.43 18.097 15.468 37.834 as 782A-41X-5-2-4 40.21 18.123 15.476 37.859 3.01 0.022 4.38 18.104 15.475 37.850 cc 782A-41X-5-58-60 40.36 18.112 15.470 37.836 2.97 0.022 3.97 18.093 15.469 37.828 as 782A-41X-5-99-100 40.47 18.128 15.476 37.865 2.66 0.019 3.68 18.112 15.475 37.858 cc 782A-42X-2-70-73 41.80 18.371 15.500 38.061 3.49 0.025 4.96 18.348 15.499 38.050 cc 782A-42X2-99-101 41.88 18.360 15.504 38.068 2.56 0.019 3.70 18.343 15.503 38.060 as Site 782A basement (volcanic pebbles) 782A-43X-CC-11-13 43.91 18.637 15.479 38.160 1.81 0.013 3.95 18.625 15.478 38.151 cc 782A-43X-CC-11-13 43.91 18.629 15.496 38.460 5.44 0.039 11.73 18.592 15.494 38.434 cc a: analyst: cc=Cornelia Class, as = Angelika Schmidt11 b: repeat: repeat of analysis in same lab; replicate: analyses in different labs

Page 14: SUPPLEMENTARY INFORMATION - Nature Research · Asian dust is after Pettke et al.54, in Plank et al.52, and Jahn et al.55. Jurassic to Cretaceous igneous crust composition are from

14 nature geoscience | www.nature.com/naturegeoscience

SUPPLEMENTARY INFORMATION doi: 10.1038/ngeo471

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nature geoscience | www.nature.com/naturegeoscience 15

SUPPLEMENTARY INFORMATIONdoi: 10.1038/ngeo471

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30.2

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ES

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21

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GEO

Page 16: SUPPLEMENTARY INFORMATION - Nature Research · Asian dust is after Pettke et al.54, in Plank et al.52, and Jahn et al.55. Jurassic to Cretaceous igneous crust composition are from

16 nature geoscience | www.nature.com/naturegeoscience

SUPPLEMENTARY INFORMATION doi: 10.1038/ngeo471

# N

GS-

2008

-12-

0120

0 17

a M

ajor

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men

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ents

: IC

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ake.

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) on

basa

lt sa

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om th

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site

"

Page 17: SUPPLEMENTARY INFORMATION - Nature Research · Asian dust is after Pettke et al.54, in Plank et al.52, and Jahn et al.55. Jurassic to Cretaceous igneous crust composition are from

nature geoscience | www.nature.com/naturegeoscience 17

SUPPLEMENTARY INFORMATIONdoi: 10.1038/ngeo471

# NGS-2008-12-01200 18

Supplementary Table 3: Primary standards and monitors for trace element analyses BIR-1 MAR DNC-1 JB-2 BHVO-1 JA1 abundances in ppm Nb 0.60 1.53 1.66 0.57 20.20 1.32 La 0.58 2.09 3.68 2.23 15.71 4.88 Ce 1.88 7.01 8.12 6.58 38.32 13.20 Nd 2.28 6.81 4.81 6.36 24.86 11.00 Yb 1.67 3.19 1.94 2.52 2.04 3.02 Pb 3.09 0.31 6.30 5.31 2.06 5.74 Th 0.046 0.11 0.26 0.28 1.25 0.76 U 0.007 0.06 0.05 0.15 0.42 0.35 Monitors at CGEO B140 RSD a JA1 b RSD %diff (n=6) 1s% (n=3) 1s% abundances in ppm Nb 3.15 1.8% 1.39 3.7% 4.7% La 8.37 0.8% 4.92 1.5% 0.8% Ce 21.8 0.5% 12.9 1.2% -2.0% Nd 16.7 0.6% 10.3 1.2% -7.2% Yb 4.76 0.3% 2.92 0.6% -3.5% Pb 3.61 0.4% 5.91 0.9% 2.9% Th 0.86 0.6% U 0.38 0.6% a RSD is based on one standard deviation of the average b JA1 was used as primary standard for U and Th Concurrent analysis of standards at IFG BIR-1 BHVO-1 abundances in ppm Nb 0.53 17.2 La 0.60 14.7 Ce 1.87 36.4 Nd 2.35 23.9 Yb 1.63 1.96 Pb 3.12 2.22 Th 0.033 1.23 U 0.014 0.418

Page 18: SUPPLEMENTARY INFORMATION - Nature Research · Asian dust is after Pettke et al.54, in Plank et al.52, and Jahn et al.55. Jurassic to Cretaceous igneous crust composition are from

18 nature geoscience | www.nature.com/naturegeoscience

SUPPLEMENTARY INFORMATION doi: 10.1038/ngeo471

# NGS-2008-12-01200 19

Supplementary Table 4: Primary standards and monitors for major element analyses JB2 NBS688 RMG1 abundances in wt% SiO2 52.81 47.85 74.23 TiO2 1.14 1.17 0.27 Al2O3 14.58 17.40 13.71 Fe2O3 14.27 10.35 1.86 MnO 0.21 0.16 0.04 MgO 4.53 8.48 0.21 CaO 9.91 12.10 1.25 Na2O 2.04 2.16 4.07 K2O 0.42 0.20 4.31 P2O5 0.10 0.14 0.05 LOI -0.37 1.02 3.40 Total 99.53 100.69 99.71 Monitors (in wt%) (data were collected in one run) B140 B140 JA1 –

acc a JA1 meas

% diff

SiO2 65.32 65.50 64.04 64.60 -0.9% TiO2 0.86 0.86 0.87 0.84 4.0% Al2O3 15.09 14.99 14.98 15.07 -0.6% Fe2O3* 5.99 5.95 6.95 7.00 -0.7% MnO 0.18 0.17 0.15 0.15 -0.2% MgO 1.64 1.63 1.61 1.47 8.5% CaO 4.92 4.88 5.68 5.97 -5.1% Na2O 5.07 5.10 3.86 3.95 -2.3% K2O 0.70 0.68 0.78 0.81 -3.3% P2O5 0.25 0.24 0.16 0.15 7.8% LOI 0.97 0.97 0.52 Total 100.12 98.97 99.08 102.32 a JA1 accepted value