ELSEVIER

Earth and Planetary Science Letters 169 (1999) 189205

Helium and lead isotope geochemistry of the Azores Archipelago

Manuel Moreira a,b, , Re gis Doucelance a , Mark D. Kurz b , Bernard Dupre a,c , Claude Jean Alle ` gre a
Laboratoire de Ge ochimie et Cosmochimie, URA CNRS 1758, Institut de Physique du Globe de Paris, Universite Denis Diderot Paris 7, 4 Place Jussieu, 75252, Paris Cedex 05, France b Department of Marine Chemistry and Geochemistry, Woods Hole Oceanographic Institution, 360 Woods Hole Road, MS25, Woods Hole, MA 02543, USA c Laboratoire de Geochimie, OMP, UMR-CNRS 5563, 38 rue des 36 ponts, 31400, Toulouse, France Received 21 April 1998; revised version received 10 March 1999; accepted 11 March 1999
a

Abstract New helium and lead isotopic data for basalts from the Azores archipelago (North Atlantic) show that the Azores have 4 He=3 He ratios both higher and lower than MORB values. Good covariations of helium and lead isotopes are observed at the scale of the archipelago, and suggest the coexistence of two mantle components in the Azores which are identied by data from Sa o Miguel and Terceira. The eastern part of Sa o Miguel island displays radiogenic helium (4 He=3 He > 140,000, R = Ra < 5:1) and lead (20.00, 15.75 and 40.33 for 206 Pb=204 Pb, 207 Pb=204 Pb and 208 Pb=204 Pb). The 207 Pb=204 Pb and 208 Pb=204 Pb ratios for Sa o Miguel are unusually radiogenic for oceanic basalts. Terceira basalts contain relatively unradiogenic=primitive 4 He=3 He ratios, with a minimum value of 64,000 ( R = Ra D 11:3), and relatively high lead isotopic ratios (206 Pb=204 Pb D 20.02, 207 Pb=204 Pb D 15.64 and 208 Pb=204 Pb D 39.35). We propose that the Terceira source has a composition produced by a mixing between recycled oceanic crust (high 206 Pb=204 Pb) and entrained lower mantle o Miguel island isotopic signature may be due to sampling of local (km-size) heterogeneity (high 3 He) material. The Sa located at relatively shallow depth. The preferred origin of this heterogeneity is the Jurassic delamination of subcontinental lithosphere, which occurred during rifting and opening of the North Atlantic. The primitive helium ratios were also observed on the Mid Atlantic ridge at 38.5N, reecting plumeridge interaction, whereas radiogenic ratios (>100,000) were observed at latitude higher than 40N and may reect the inuence of the Sa o Miguel component at the ridge. 1999 Elsevier Science B.V. All rights reserved. Keywords: helium; lead; isotope ratios; Azores; magmas; mixing

1. Introduction Helium isotopic ratios measured on Oceanic Island Basalts (OIB) display very large variations
Corresponding

author. Fax: C1 508 457 2193; E-mail: mmoreira@whoi.edu

compared to Mid Oceanic Ridge Basalts (MORB). The relatively homogeneous MORB source reservoir has a 4 He=3 He mean value of 88,000 5000 ( R = Ra D 8) [1] whereas the 4 He=3 He isotopic ratios observed in OIB range from 25,000 ( R = Ra D 30) for Loihi seamount samples [2] to values higher than 150,000 ( R = Ra D 4:8) for the GoughTristan da

0012-821X/99/$ see front matter 1999 Elsevier Science B.V. All rights reserved. PII: S 0 0 1 2 - 8 2 1 X ( 9 9 ) 0 0 0 7 1 - 0

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CunhaSt Helena island group [35]. A two-layered mantle best explains these results, where the upper mantle represents the MORB source, which is highly degassed and well mixed by convection [1], whereas the primordial signal observed in Loihi seamount basalts is attributed to the presence of a less degassed reservoir, which is probably located in the lower mantle [2,6]. The signicance of the radiogenic helium signatures observed in the GoughTristan da CunhaSt Helena island group remains controversial. These signatures have been attributed to the injection, through subduction, of oceanic crust and sediments into the upper mantle, which will present high (U C Th)=3 He ratios and be stored for some time at the 670 km boundary layer, prior to eruption [3,5,7]. An alternate view attributing the high 4 He=3 He ratios to shallow, magma chamber contamination processes (unrelated to the mantle), originally discussed by Condomines et al. [8] and Zindler and Hart [9,10], was more recently defended by Hilton et al. [11]. Based on results from Heard island (Indian Ocean), where both primitive and radiogenic helium isotopic ratios have been measured, Hilton and co-workers propose that most the hotspots are in fact low 4 He=3 He hotspots, and the observed radiogenic helium signature may reect shallow depth contamination, either by interaction of the plume with oceanic crust or radiogenic 4 He production in a degassed magma chamber. Lead isotopes also display different histograms for MORB and OIB. Ocean island samples usually present more radiogenic signatures and, again, exhibit more variability, than lavas from spreading centers [10,12,13]. Differences in lead isotopic compositions between oceanic islands are still debated. They could reect plume source heterogeneities [14,15], material entrainment during plume ascent [16,17] or interaction between plumes and lithospheric mantle [18]. Due to the different decay constants, lead isotopes are less sensitive to in situ production, and cannot be related to magma chamber outgassing. This study focusses on the Azores archipelago, which is considered to belong to the high 4 He=3 He hotspot category [1921], and presents new helium and lead isotopic results for six islands from the Azores archipelago: Faial, Graciosa, Pico, Sa o Miguel, Santa Maria and Terceira. Good covaria-

tions between helium and lead isotopes are observed at the scale of the archipelago, and suggest the coexistence of two components in the Azores; the two end members are best identied by data from Sa o Miguel and Terceira islands. The Eastern part of Sa o Miguel island displays radiogenic helium (4 He=3 He > 140,000) and lead (20.00, 15.75 and 40.33 for 206 Pb=204 Pb, 207 Pb=204 Pb and 208 Pb=204 Pb) signatures, whereas Terceira basalts present primitive 4 He=3 He ratios, with a minimum value around 64,000 ( R = Ra D 11:3), similar 206 Pb=204 Pb ratio (20.02), but signicantly lower 207 Pb=204 Pb (15.64) and 208 Pb=204 Pb (39.35). All other island results are interpreted in terms of binary mixing between the local MORB mantle source and these two plume components.

2. Geographical situation and sample locations The Azores archipelago is composed of nine islands (Corvo, Faial, Flores, Graciosa, Pico, Santa Maria, Sa o Jorge, Sa o Miguel and Terceira), which represent the emerged part of a large oceanic platform (Fig. 1). Located at the triple junction between the Eurasian, African and American plates, the plateau is crossed over by the Mid-Atlantic ridge; seven islands (Faial, Graciosa, Pico, Santa Maria, Sa o Jorge, Sa o Miguel and Terceira) stand at the East of the ridge, two (Corvo and Flores) are located to the west, on the American plate. The oldest rocks are observed on Santa Maria (8 Myr) and Sa o Miguel (4 Myr for the Eastern part) islands [2225]. Other volcanics, including the central part of Sa o Miguel, were erupted during the Pleistocene and Holocene. Historic lavas have been found in most areas of the archipelago (including Sa o Miguel island), and the most recent volcanism occurred on Faial in 1957=58 (Capelinhos site). The lava compositions range from basalts to trachy-andesites and some peridotitic nodules have been observed on Pico, Faial and Terceira islands [26,27]. Samples from the islands of Santa Maria, Sa o Miguel, Terceira, Pico, Graciosa and Faial, were analyzed. Sample locations are given on Fig. 2 and in Appendix A.

M. Moreira et al. / Earth and Planetary Science Letters 169 (1999) 189205

191

42 N

AZORES
M.A. R
m 00 20

40 o N
C Fl Triple junction F ? G

Te rc
T

ra ei t rif

38 N

P SMi

SMa

east Azores fracture zone

32 W

28 W

Fig. 1. Location map of the Azores archipelago (modied after Turner et al. [34]). Triple junction has been proposed to be located at 38.5N [41,57], rather than in the straight continuity of the Terceira rift. Abbreviations for the island names: Santa Maria ( SMa), Sa o Miguel (SMi), Terceira (T), Graciosa (G), Pico (P), Faial (F), Flores (Fl) and Corvo (C).

3. Analytical procedure Helium analyses were performed on millimeter sized olivine and pyroxene phenocrysts separated from fresh lavas. Samples from the Eastern side of Sa o Miguel island were ankaramites with large olivine and pyroxene crystals, up to 2 cm in size; most of the other lavas were alkali-basalts. Measurements were preferentially done by crushing, in order to avoid possible in-situ radioactive decay or production of 3 He cosmogenic and to obtain the inherited helium trapped in inclusions [3,28]. The powder of the crushed olivines and pyroxenes from sample ACO95-68 (ankaramite from Sa o Miguel) were also melted in vacuo to release the gases located in the matrix, which allows an evaluation of the contribution from radiogenic and cosmogenic helium. Most of the helium measurements were performed in Paris using a glass mass spectrometer and extraction line. Due to diffusion, prior measurements with two purications using hot titanium getters and trapping on a cold head in our KO-

VAR glass ARESIBO II mass spectrometer yielded signicant 4 He blanks for very low helium concentration samples such as phenocrysts (olivines, pyroxenes) from oceanic basalts [29,30]. Thus, we developed a shorter crushing procedure which now yields a 4 He blank of 5 10 10 0.5 cm3 STP, a signicant improvement to previous blank values of 1:5 0:5 10 8 cm3 STP. A charcoal trap was installed close to the crusher which retains all active gases, except He and Ne, during 30 minutes of cryo-pumping at liquid nitrogen temperature. 3 He is analysed on an electron multiplier and 4 He, depending of the absolute amount of gas, on a Faraday cup, or on the electron multiplier. Using only 30 minutes of purication in a very small volume, the helium introduced into the extraction line by diffusion is very small, leading to low blanks. This procedure makes possible the measurement on this mass spectrometer of very low level samples using 1 or 2 g of olivine or pyroxene. This new procedure was tested by repeated analysis of a oceanite sample from Re union island (Indian

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M. Moreira et al. / Earth and Planetary Science Letters 169 (1999) 189205

Faial Island
5km
ACO95-49 ACO95-47 ACO95-s
Capelinhos

FA12 FA10 ACO95-53 FA6 ACO95-52 FA44 FA2 FA1 FA3

FA7

ACO95-55

ACO95-20

Pico Island
1718-1720

5km
Pico

ACO95-26 -40 ACO95-33 ACO95-30

Santa Maria Island

S6

S9 S14

5km

So Miguel Island
ACO95-66 SM7 SM319
nordeste 1563

ocean), whose olivines are known to have a very homogeneous 4 He=3 He isotopic ratio of 56,000 1000 ( R = Ra D 12:9 0:2) [31,32]. Using different amounts of olivines (0.5, 0.8 and 1.3 g, respectively), we obtained reproducible 4 He=3 He results of 55,296 3254, 55,918 4152 and 55,591 2740. Some helium analyses were also performed in the Woods Hole Oceanographic Institution where the blank is typically 3 to 5 10 11 cm3 STP [33]; these data are italicized in Table 1. There is a good agreement between the data obtained in the two laboratories. Sample ACO95-3, which was collected at the 1563 lava ow from Queimado peak eruption, have given 4 He=3 He ratios of 149,600 and 133,830 similar to the ratio of 133,800 of one sample from the same lava ow analyzed by M.D. Kurz (sample #SM88-45, unpublished results) indicating good inter-laboratory agreement. Lead chemical separation was performed on 0.5 g of powdered samples using the procedure of Manhe ` s et al. [34], in a clean room under controlled atmosphere. This permits one to maintain the total Pb blank below 0.35 ng. Lead isotopic ratios were measured on a Thomson THN 206 mass spectrometer and calibrated against SRM981 NBS [35] standard measurements, with a statistical mass discrimination factor of 1 0:3 per amu. The total precision, tested by duplicate analysis, is better than 0.05% (2 ) per mass unit difference in the isotopic ratio.
ACO95-62 SM169 SM150

4. Results Results are given in Tables 1 and 2. Helium concentrations obtained by crushing range from

SM139 ACO95-56 ACO95-3 ACO95-68

5km

Terceira Island
1761

ACO95-12

ACO95-9 ACO95-10 ACO95-11 T28

ACO95-16 T2 ACO95-14 T7 T9

5km

Fig. 2. Faial, Pico, Santa Maria, Sa o Miguel and Terceira island sampling maps, modied after Forjaz et al. [67].

Footnote to Table 1: R = Ra is the 3 He=4 He ratio normalized to the AIR value of 1:384 10 6 . is the uncertainty. Uncertainty in the helium concentrations is approximately 5%. The last column gives the percentage of 4 He blank contribution (which was 4 He 5 10 10 cm3 STP in Paris and 3 to 5 10 11 at WHOI). Data in italics were analyzed in the Woods Hole Oceanographic Institution isotope facilities. Measurements were conducted on olivine (Ol.) and clinopyroxene (CPX). Re-crush means that samples were crushed a second time, sequentially, in an attempt to insure complete extraction, and also to resolve any contributions from radiogenic helium. The experiments conducted by melting of powder remaining after crushing are abbreviated mp.

M. Moreira et al. / Earth and Planetary Science Letters 169 (1999) 189205 Table 1 Helium concentration (in 10 Sample Faial ACO95-sand ACO95-47 ACO95-49 ACO95-52 ACO95-53 ACO95-55 FA10 FA12 Pico ACO95-20 ACO95-20 ACO95-26 ACO95-30 ACO95-30 b ACO95-30 b ACO95-33 ACO95-40 Santa Maria S6 Sa o Miguel ACO95-3 ACO95-56 ACO95-62 ACO95-62 ACO95-66 ACO95-68

193

cm3 STP=g) and isotopic ratios (corrected for blank) for Azores samples Weight (g) 1.04 1.33 1.79 1.58 1.08 0.38 1.01 1.13 0.19 0.35 1.84 1.32 0.96 1.01 1.08 1.17 0.97 0.17 1.19 1.46 1.02 1.97 1.07 1.42 0.33 Re-crush 0.31 1.61 2.82 3.02 0.32 Re-crush 0.18 1.08 1.88 1.02 0.34 1.74 0.30 0.10 0.20 1.60 0.27 0.99 0.14 0.19
4 He

Mineral

(10 4.9 6.8 0.53 43 4.5 1.2 0.54 2.0 1.2 1.7 3.6 1.4 36 13 7.6 3.2 1.0 0.19 1.4 1.8 0.50 0.23 0.60 0.33 0.20 0.06 0.37 3.3 3.4 3.3 2.4 0.02 0.48 0.41 0.59 1.5 1.4 0.23 0.13 1.6 0.93 2.2 0.14 1.2 0.50 0.26

8)

R = Ra

4 He=3 He

Blank (%) 1 14 4 3 1 1 11 3 2 2 1 2 0.2 1 1 1 3 17 2 3 29 12 9 16 7 25 4 1 1 1 82 6 11 8 3 1 9 13 3 3 2 13 5 7 10

Ol. Ol. Ol. Ol. Ol. Ol. Ol. Ol. Ol. Ol. CPX Ol. Ol. Ol. CPX Ol. Ol. Ol. Ol. Ol. Ol. Ol. CPX Ol. Ol. mp CPX CPX CPX CPX mp

7.5 0.5 8.0 0.2 8.3 1.2 8.7 0.1 7.2 0.4 8.4 0.1 5.6 1.7 7.8 0.5 8.0 0.1 10.0 0.1 10.0 0.2 10.0 0.3 8.8 0.1 10.3 0.1 9.7 .0.1 8.9 0.5 7.5 0.9 7.7 0.3 4.8 0.6 5.4 0.5 4.5 1.2 6.1 1.9 3.0 1.1 5.9 2.0 4.1 0.1 3.8 0.4 4.4 0.1 2.6 0.1 4.0 0.3 4.4 0.7 4.06 0.03 4.3 0.8 1.6 0.1 10.4 1.6 11.3 0.8 11.0 0.4 9.3 0.1 7.0 1.8 8.5 0.2 9.5 0.1 9.4 0.1 9.4 0.5 9.7 0.3 8.0 0.8 10.3 0.2 8.1 0.2

95960 6630 90890 1930 87160 12090 86320 1210 99940 5940 85970 700 129720 40520 92280 5780 89601 2378 72545 415 72110 1730 72550 2480 81820 870 70150 890 74320 1070 80910 4620 95960 10830 94376 3242 149600 133830 162070 118450 240850 121640 174317 189644 163180 276840 180550 163470 178200 170000 461980 17650 13490 43520 36900 88310 41160 5047 20408 4310 11670 11910 24600 1360 30520 18610

ACO95-68 ACO95-68 (melt) ACO95-68

Terceira T2 T7 T9 T28 T28 ACO95-9 ACO95-10 ACO95-11 ACO95-12 ACO95-14 ACO95-16 Graciosa G1

Ol. Ol. Ol. Ol. Ol. Ol. Ol. Ol. Ol. Ol. Ol. Ol. Ol.

69530 10570 63780 4620 65510 2140 77550 430 103070 26910 85165 2350 75858 709 76965 680 77200 3710 74604 2326 90420 8520 70437 1415 89600 2380

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M. Moreira et al. / Earth and Planetary Science Letters 169 (1999) 189205

Table 2 Lead isotopic compositions determined for some Azores samples Sample Faial FA1 FA2 FA3 FA6 FA7 FA10 FA12 a FA44 a Graciosa G1 Pico P1 a
206 Pb=204 Pb 207 Pb=204 Pb 208 Pb=204 Pb

19.332 19.318 19.607 19.137 19.130 19.471 19.607 19.707 19.20 19.60 19.80 19.96

15.555 15.541 15.574 15.601 15.605 15.619 15.642 15.635 15.60 15.59 15.60 15.61 15.56 15.56 15.58

38.796 38.746 38.943 38.814 38.816 39.123 39.314 39.296 38.89 39.10 39.18 39.37 39.07 39.01 39.30

Santa Maria S6 a 19.14 S9 a 19.01 S14 a 19.28 Sa o Miguel West SM7 a SM319 a Nordeste SM139 a SM150 a SM169 a
a Previously

19.47 19.48 20.00 19.96 19.96

15.59 15.62 15.78 15.75 15.74

39.32 39.37 40.33 40.19 40.31

published by Dupre (PhD thesis).

1:7 10 9 cm3 STP=g for olivines from sample S6 (Santa Maria) to 4:3 10 7 cm3 STP=g for olivines analysed in a xenolith from Faial island (ACO95-49). Helium isotopic ratio vary between 63,780 ( R = Ra D 11:3) and 276,840 ( R = Ra D 2:6) in T2 (Terceira) and ACO95-68 (Sa o Miguel) samples respectively. Helium concentrations obtained for melting after crushing of sample ACO95-68 were 3:7 10 9 cm3 STP=g for the olivines, with a 4 He=3 He ratio of 163,180 4310 ( R = Ra D 4:4 0:1) which is similar to the crushed ratio (4:1 0:1), and 4:8 10 9 cm3 STP=g for the pyroxenes with a helium ratio of 461,980 18,610 ( R = Ra D 1:6 0:1). This ratio is much more radiogenic than the crushed ratio (4:06 0:03). The agreement between 4 He=3 He ratios obtained by crushing in this sample, despite

the presence of radiogenic 4 He in the clinopyroxene strongly suggest, that the crushing data reects the magmatic helium. This point is illustrated in Fig. 3c, where good agreement in 4 He=3 He ratios is obtained for several different extractions and over a wide variation in 4 He concentrations. Three distinctive island groups have been distinguished on the basis of helium isotopic results (Fig. 3): (1) Sa o Miguel island, for which 4 samples have been analysed, has the most radiogenic 4 He=3 He ratios. One sample (ACO95-3) was from a historical lava ow (Queimado peak eruption, 1563) whereas the 3 others are Pliocene ankaramites [23]. They all display very radiogenic 4 He=3 He ratios, from 121,640 41,160 to 276,840 11,670, with a weighted mean value of 140,660 for the historical sample ACO95-3 (crushed samples). These data agree with previous measurements from Sa o Miguel by Kurz (g. 8.10 of [36]). (2) Faial, Graciosa and Santa Maria islands all exhibit a MORB-like helium signature, with 4 He=3 He ratios ranging from 85,970 1210 to 94,380 3240 (Faial ACO95-55 sample displays an higher but uncertain value of 129,720 40,520). (3) Pico and Terceira islands have a more dispersed helium signature and range from typical MORB ratios to relatively primitive values, such as 63,780 4620 for Terceira T2 basalt and 70,150 890 for Pico ACO95-30 sample. Lead isotopic results (Table 2) for the Azores islands are all relatively radiogenic in composition compared to local MORB. However, the respective positions of the ve islands in PbPb space suggests a similar grouping of Azores islands (Fig. 4), with good helium and lead covariations at the scale of the archipelago: (1) Eastern Sa o Miguel samples have relatively high 206 Pb=204 Pb ratios, around 20, and very radiogenic 207 Pb=204 Pb and 208 Pb=204 Pb values, up to 15.78 and 40.33 respectively, which are clearly different from those measured on other islands. (2) Faial and Santa Maria basalts represent the least radiogenic compositions of the archipelago, with a mean value of 19.50 for 206 Pb=204 Pb, 15.60 for 207 Pb=204 Pb and 39.00 for 208 Pb=204 Pb. (3) Pico and Terceira samples exhibit lead isotope ratios ranging from FaialSanta Maria values (19.50,

M. Moreira et al. / Earth and Planetary Science Letters 169 (1999) 189205
10 -9 10 -8 10 -7
Kurz (unpublish) Pico

195

4He/3He

150000

Sao Miguel Terceira

4.8

R/Ra

100000

MORB

7.2

14.5
Faial Santa Maria

4He/3He

150000

Graciosa

4.8

R/Ra

100000

MORB

7.2

14.5 ACO95-68 4He/3He 400000

rad iog

mp
c rc mp

Olivine CPX crush re-crush melt powder

1.8

R/Ra

300000 rc rc 10 -9 4He

2.4

eni c

200000

c mp 10 -8 c

inherited helium

3.6

10 -7

(ccSTP/g)

Fig. 3. 4 He=3 He ratios vs. 4 He concentrations (in cm3 STP=g) for Azores samples. Grey lines correspond to the MORB 4 He=3 He mean value of 90,000 [1,68]. Top gure represents the Pico, Terceira and Sa o Miguel islands. Some Sa o Miguel data from Kurz (unpublished) were added. Middle gure shows Faial, Santa Maria and Graciosa basalts. One can see the isotopic ratios are exactly the same as the mean MORB ratio. Bottom gure represents two experiments on the ankaramite ACO95-68 from the Nordeste area on Sa o Miguel. Step crushing and powder melting extractions were performed on olivines and clinopyroxene to constrain the post eruption radioactive production of 4 He. The results show that the 4 He=3 He ratios are always the same during crushing (olivine and CPX), but different for CPX melting due to the higher U content of CPX. This implies the 4 He=3 He ratios obtained by crushing are representative of the magmatic values, and have not been altered by post-eruptive radiogenic helium (see text).

15.60 and 39.00) to radiogenic compositions similar to Sa o Miguel basalts for 206 Pb=204 Pb (20.02), lower for 207 Pb=204 Pb (15.64) and 208 Pb=204 Pb (39.35) [37,38]. Moreover, similarly to helium,

PicoTerceira and FaialSanta Maria associated elds are not totally distinctive. These three groups were also proposed by Turner et al. [38] based on trace element-isotope systematics

196
17.5
a

M. Moreira et al. / Earth and Planetary Science Letters 169 (1999) 189205
18.5 19.5 20.5 21.5 17.5
c

18.5

19.5

20.5

21.5

15.8

SM
Tu

SM
Tu

M 15.8

Pb/204Pb

15.7

15.7

T
ENA 15.6

T
15.6

207

BE
Graciosa Faial Pico Santa Maria Sao Miguel
Previous studies

BE

15.5

MORB 36-40N
NHRL

MORB o 36-40 N
NHRL

15.5

Terceira

SM
M Tu

SM
M Tu 40.0 40.5

40.5

40.0

Pb/204Pb

39.5

T BE BE

39.5

39.0

39.0

208

38.5 MORB 36-40N

ENA MORB o 36-40 N

38.5

38.0

37.5
NHRL

Faial Pico Santa Maria Sao Miguel

Previous studies

38.0

37.5

Terceira 19.5 20.5 21.5 17.5 18.5 19.5 20.5 21.5

17.5

18.5

206

Pb/204Pb

206

Pb/204Pb

Fig. 4. Lead isotopic diagrams, showing end-member positions of Sa o Miguel and Terceira [37] islands. (a) 206 Pb=204 Pb vs. 207 Pb=204 Pb. (b) 206 Pb=204 Pb vs. 208 Pb=204 Pb. Also reported are previous Sa o Miguel [38,48] results, the Northern Hemisphere Reference Line (NHRL, as dened in [69]), Bulk Earth average value (BE) [58], and representative elds for local MORB [7073], Tubuaii and Mangaia islands [7476]. SM and T points are postulated to be representative of the Azores plume compositions. (c) 206 Pb=204 Pb vs. 207 Pb=204 Pb. (d) 206 Pb=204 Pb vs. 208 Pb=204 Pb. ENA elds (East North America tholeiitic samples [59]) can be interpreted as reecting binary mixing between a end-member with low lead isotopic ratios and Sa o Miguel end-member SM.

where for example, the Th=Nb is higher for Sa o Miguel island [38]. Fig. 5 shows the 4 He=3 He ratio against the 206 Pb= 204 Pb ratios for the different Azores archipelago islands. The three groups can be easily distinguished on this gure.

5. Discussion 5.1. The Eastern Sa o Miguel radiogenic helium signature Since Sa o Miguel island is one of the oldest islands in the archipelago (up to 4 Myr [23,25]), high

M. Moreira et al. / Earth and Planetary Science Letters 169 (1999) 189205

197

R/Ra
14.5 7.2 4.8 3.6

Graciosa Faial Santa Maria Terceira Sao Miguel (Kurz)

Recycled oceanic crust

21

St Helena

206Pb/204Pb

20
Terceira Sao Miguel

Faial - St Maria-Graciosa

19
Reunion Heard 1

MORB 35-40N Gough Heard 2

18

Loihi

n-MORBs

50,000

100,000

150,000

200,000

4He/3He
Fig. 5. 4 He=3 He ratios versus 206 Pb=204 Pb ratios for Azores Archipelago basalts and some other islands. Some Sa o Miguel data from Kurz (unpublished) were added. Other data are from the literature.

He=3 He ratios measured in some samples could be explained by post-eruptive decay of Th and U, particularly for samples with low helium and high U and Th contents. Sample crushing procedures are performed to liberate the inherited gases contained in uid and melt inclusions, but 4 He production could occur in the matrix with subsequent diffusion into the inclusions, or partial release by crushing. However, both the low concentration Pliocene ankaramites (2.3 to 6:0 10 9 cm3 STP=g for ACO95-62, 66 and 68) and historical lava ACO95-3 (434 yr), whose olivines contain around 1:6 10 8 cm3 STP=g 4 He, display
4

radiogenic helium isotope ratios, which strongly suggests that the unique radiogenic signature of Sa o Miguel cannot totally result from such a decay process. Only old samples could have been modied, starting from a minimum ACO95-3 olivines like radiogenic value (140,000, we will consider, in the following, as the Nordeste Sa o Miguel helium signature) to reach ratios as high as 276,840 (ACO95-68 CPX) as illustrated by the melting experiment (Fig. 3). The melt of the ACO95-68-CPX powder has given a 4 He=3 He ratio of 461,980 18,610, much

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more radiogenic than the crushed value of 178,200. This can easily be explained by post-eruptive 4 He production since this sample has an age between 2 and 4 Ma [23]. Using a U concentration of 0.012 ppm and a Th=U ratio of 2.9 for CPX [39] we can obtain a U=He age of 1.2 Ma for sample ACO95-68. This age is in good agreement with the K=Ar age [23] considering the uncertainty on the U content and the Th=U ratio. However, for olivines, crushing and melting have given the same helium isotopic ratios (Fig. 3), indicating that 4 He production from U and Th decay is negligible for olivines. This shows that the radiogenic helium isotopic ratios observed in the samples from the Nordeste area do not represent post-eruptive decay of Th and U. Zindler and Hart [9,10] and Hilton et al. [11] have proposed that high 4 He=3 He ratios measured in some OIB could reect shallow depth contamination at high levels in the crust. The presence of ankaramite samples with low pressure pyroxenes (high total Al o Miguel island is consistent and low AlVI ) on Sa with the existence of shallow magma chambers beneath the Azores archipelago [23]. Plume source contamination is modeled by a two-component mixing and the expression of the mass ratio between plume ( Mi ) and contaminant (oceanic crust) material ( Mc ) is then given by: 8 4 4 9 He He > > > > > > 3 < 3 3 He Mc He SM He i = 3 i 4 4 > Mi > He He He c > > > > : ; 3 He 3 He c SM where .4 He=3 He/SM , .4 He=3 He/i and .4 He=3 He/c refers to the Sa o Miguel island, Sa o Miguel plume and contaminant representative helium values, [3 He]i and [3 He]c to the plume and contaminant concentrations (cm3 STP=g). We used results obtained by Staudacher and Alle ` gre [40] on 22 My old oceanic crust (which corresponds to the approximate age of the nearby Azores crust [41]) as a contaminant material ([3 He]c D 5 10 14 cm3 STP=g and .4 He=3 He/c D 2 107 ), the value of 140,000 for Sa o Miguel island composition, o and Terceira-like 4 He=3 He ratio (60,000) for Sa Miguel plume. The 3 He concentration in the plume material is thought to be intermediate between lower (2:5 10 9 cm3 STP=g) [42] and upper mantle (1:1

10 10 cm3 STP=g) [43,44] values because the helium ratio we took is very different from the lower mantle ratio of 20,000. Let us take 5 10 10 cm3 STP=g for the 3 He content for the Terceira plume. The Mc = Mi result (4000%) suggests that important magma chamber outgassing, at least 99.9%, is required to be consistent with a plume contamination scenario. In the previous calculations, we do not consider the possibility of radiogenic decay in a degassed magma chamber. Using 3 He concentration estimated above (5 10 10 cm3 STP=g) in the following 4 He radioactive production equation (t in Ma, U in ppm and He in cm3 STP=g): 4 4 He He D 3 C 3 He He 0 t Th [U] 8 t 4:35 C 2:8 10 U [3 He] we can determine the time interval t necessary to increase the initial helium ratio ( 4 He=3 He)0 from 60,000 (Terceira less primitive value) to the presentday value .4 He=3 He/t of 140,000. Assuming a Th=U ratio of 2.75 [38] and a U concentration of 0.040 ppm (we postulate Terceira plume uranium to be intermediate between lower mantle material [6] and recycled altered oceanic crust [15] based on lead isotope systematics, cf. Section 5.2), we need to invoke very large outgassing (at least 99.999%) to obtain magma chamber interval time consistent with classical estimates of magma residence time (between 10 and 10,000 yr [45,46]). Similar calculations can be done with lead isotopes. However, using a Terceira-like isotopic com o Miguel position (207 Pb=204 Pb D 15.64) for the Sa plume and the most radiogenic value (207 Pb=204 Pb D 15.64) measured in old oceanic crust (1437 My) near the Azores archipelago [47] as a contaminant does not allow to obtain 207 Pb=204 Pb ratios that are as high as those determined on Sa o Miguel samples (207 Pb=204 Pb D 15.78). Contamination by recent Atlantic sediments is also unlikely, given the high 208 Pb=204 Pb ratios [48]. There is no evidence for such an extensive outgassing in the Sa o Miguel olivine samples, which show similar He content to olivines from other islands, in particular from Terceira. Kurz et al. [20] have observed a variation of the 4 He=3 He ratio with

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the longitude on Sa o Miguel island (with a decrease westward), similar to the 87 Sr=86 Sr and 206 Pb=204 Pb variations [20,48,49]. Because these variations and correlations are difcult to explain by shallow depth contamination, we propose a deeper origin for the o Miguel basalts. high 4 He=3 He ratios measured in Sa A source effect also appears to be consistent with the heliumlead covariations observed at the scale of the archipelago. Kurz et al. [3], Vance et al. [4], Graham et al. [5], Hanan and Graham [16] and Hanyu and Kaneoka [7] have postulated that the radiogenic helium measured in Gough, Tristan, St Helena and some Pacic islands can be explained by recycling into the mantle of oceanic crust or sediments, and reinjection of this material in plume sources. Subducted plates should have high (U C Th)=3 He ratios because helium is outgassed to the atmosphere during ridge magmatism and during subduction. After storage for some time in the mantle, this will give high 4 He=3 He ratios by U and Th -decay. Lead and strontium isotope signatures are consistent with such a scenario [38,49], especially the high 207 Pb=204 Pb ratios which imply old U=Pb fractionation. Recycling of subducted altered oceanic crust and sediments allows to increase the U=Pb ratio [15,50], and then give very radiogenic 207 Pb=204 Pb ratios with time. 5.2. The Terceira helium signature Kurz et al. [19] rst proposed the presence of a high 4 He=3 He plume beneath the Azores archipelago, based on helium isotopes measurements in MORB glasses near the Azores platform. However, it turns out that the Azores hotspot is also characterized by low 4 He=3 He, since primitive values (4 He=3 He 65,000) have been measured in this study in some Terceira and Pico samples. Production of cosmogenic helium [28] in Terceira or Pico samples remains very unlikely, as all the analysed basalts are relatively young (some are historical, see Table 1 and Appendix A) and were sampled at low altitude, generally in freshly exposed surfaces. Moreover, we have analyzed these samples by crushing which primarily releases the inherited helium trapped in inclusions; only a small fraction of the cosmogenic helium is released by crushing and should be negligible for these samples. Therefore, the primitive helium has to originate within

the source of the plume. It may come from the lower mantle, source of primitive helium for most of oceanic islands (Hawaii, Iceland, Galapagos or Re union islands). The [3 He]LM =[3 He]UM concentration ratio between the lower and upper mantle should be roughly 10 [6,51] so even a small amount of entrained lower mantle could transfer a primitive helium isotopic signal. A helium signature similar to Terceira was found on nearby Atlantic MORB glasses (Fig. 6, [52]) thereby conrming the plume ridge interaction already observed for REE, Sr, Nd and Th=U systematics [5356]. The somewhat different helium observations by Kurz et al. [19], could simply be due to the different sampling scale of this study. For example, most of the MORB samples from 39N are very degassed, and may have been dredged off the ridge axis since the ridge is not well dened in this area. In fact, the helium signature recorded by MORB glasses displays very localized primitive values (around 38.5N; Moreira and Alle `gre [52]) which seems to correspond to the location of the triple junction [41,57] (Fig. 6). Most primitive helium ratios measured on Terceira samples could be explained by mixing between primitive mantle having high 3 He (4 He=3 He D 20,000) and two other discrete mantle sources: MORB mantle (4 He=3 He D 90,000) and a low 3 He plume best represented by data from Sa o Miguel (4 He=3 He D 140,000). Helium alone cannot resolve between the two hypotheses. However, lead isotopic ratios (Fig. 4a,b) show that the Terceira signature cannot result from binary mixing between the Sa o Miguel plume and lower mantle material. The present-day composition of the lower mantle certainly corresponds to a binary mixing between Bulk Earth material and about 17% of depleted mantle [58], and then is few different from Bulk Earth composition. The Terceira signature probably reects mixing of high material, lower mantle material and entrained depleted asthenospheric material, whereas the observed trend for Terceira island may represent shallow interaction between this specic material and the local MORB mantle source. 5.3. TerceiraSa o Miguel: same hotspot? Since we excluded a shallow contamination origin for explaining the He data in Sa o Miguel island, the

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120,000

100 000

4He/3He

N MORB
80,000

60,000 36 38 40 42
o

44

46

LATITUDE ( N)
Fig. 6. 4 He=3 He ratios measured in MORB as a function of the latitude along mid Atlantic ridge between 35 and 40N, modied after Kurz et al. [19] (crosses) and Moreira and Alle ` gre [52] (diamonds). Note that the minimum of the 4 He=3 He ratio is close to 38.5N, which is the supposed triple junction between African, American and European plates [41,57].

Azores archipelago helium signature, with coexistence of both radiogenic and primitive ratios, seems to be paradoxical. Identication of recycled terrigenous sediments in the source of Sa o Miguel basalts does not give information about the depth of this specic material and there are two models for the generation of the Azores islands. The rst one proposes the Azores plume deep source may be isotopically heterogeneous, containing a mixture of recycled subducted terrigenous sediments, altered oceanic crust and lower mantle material. A low degree of melting has permitted to exhibit the sedimentary signature (radiogenic) of the source (the fertile part of the mixture, i.e. sediments melt preferentially) in Sa o Miguel basalts (Nordeste), whereas other islands result from higher extent of melting and reect mixing of recycled oceanic crust, lower mantle and upper mantle materials. The origin of this heterogeneous source may result of the entrainment by a plume coming from the lower mantle of material stored at the 670 km discontinuity or higher or reects the heterogeneity of the source itself. The second model proposes the Azores plume deep source is isotopically homogeneous, with a Terceira like signature (mixing of lower mantle material and himu material). Sa o Miguel island basalts sample a very localized upper mantle heterogene-

ity, melted by the rising of the Terceira plume or blob. This heterogeneity could correspond to subducted oceanic crust and sediments stored under the north america continent during the pre-Grenville subduction [59], recycled into the upper mantle by delamination occurring during the opening of the North Atlantic ocean (Fig. 4c,d and Fig. 7). Again, intermediate helium and lead compositions reect interaction with the local MORB mantle source (Faial, Graciosa, Pico : : : ). Such a model can be validated by the fact that East North American basalts (ENA), that correspond to the nearest subcontinental material from the Azores, show linear trend in PbPb diagrams (Fig. 4b) which could reect mixing between a source with low 206 Pb=204 Pb 207 Pb=204 Pb and 208 Pb=204 Pb ratios, which could be subcontinental mantle [60,61], and a component with Sa o Miguel-like signature which could be a mixing of sediments and recycled oceanic crust. We propose this component was stored below the North America before injection in the North Atlantic mantle by delamination during the opening of the North Atlantic. This model is similar to the proposal of Widom et al. [48], involving shallow interaction of the plume source with delaminated subcontinental lithosphere enriched by metasomatism. Radiogenic helium ratios measured in some continental xenoliths or continental basalts that sample the subcon-

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Pre-Grenville subduction

201

a
>1Ga

b
1Ga

Grenville continent - continent collision

Rifting

c
ENA / High Atlas

200 Ma

delamination

d
ENA America

Sea floor spreading

High Atlas MAR Africa

200 -10 Ma

e
America MAR T SMi Africa

10 Ma

"Terceira" plume or blob

Fig. 7. Schematic evolution of the North Atlantic to explain the Azores isotopic data (model 2). (a) Pre-Grenville subduction [59] brings some oceanic crust and sediments into the subcontinental lithospheric mantle. (b) End of the subduction with the Grenville collision. (c) and (d) Opening of the Atlantic ocean is accompanied by some delamination, which provides regional enrichment of the Azores mantle. (e) Sa o Miguel volcanism samples some localized km-size heterogeneity corresponding to old recycled material.

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tinental lithosphere can account for such a model [62,63]. In both model 1 and model 2, we postulate a regional enrichment of the asthenosphere beneath the Azores. The observed radiogenic helium signature is not restricted to Sa o Miguel island. Kurz et al. [19] have measured 4 He=3 He ratios higher than 100,000 in North Atlantic MORB glasses (for latitudes comprised between 40N and 50N; Fig. 6), which are consistent with contamination of the local MORB mantle source by delaminated subcontinental lithosphere (occurring during the opening of the Atlantic ocean). Such a hypothesis has been already proposed to explain specic Pb and Sr radiogenic signatures of the Oceanographer transform zone basalts [64] at 35N, and could also be proposed to explain similar isotopic anomalies identied on the Mid Atlantic Ridge at 14N [43,65], 43N and 46N [56]. Recent discovery of very old zircons in the Mid Atlantic Ridge are also consistent with such a model [66].

Acknowledgements M.M. would like to thank Pascale Louvat very much for his help during the mission in Azores and patience during rock sampling, and the team of the Earth Sciences department from Universidade dos Ac ores, in particular Pr. Victor Forjaz and J.C. Nunes for discussions and help during the Azores trip. B. Bourdon, J. Kunz and Th. Staudacher are thanked for discussion and improvement of the manuscript. D. Graham, I. Kaneoka and R. Poreda helped to improve the quality of the manuscript by their review comments. Josh Curtis is thanked for his help during analyses in the Woods Hole Oceanographic Institution. This is IPGP contribution 1574 and WHOI contribution 9893. [CL]

Appendix A. Sample locations

Sample locations are also given on Fig. 2. Some location are in [37].

6. Conclusions The Azores archipelago corresponds to the second hotspot where three distinctive helium isotopic signatures have been observed: MORB values found at Santa Maria, Graciosa and Faial islands, primitive values for some Terceira and Pico basalts, and radiogenic values in Eastern Sa o Miguel. The only other oceanic island where 4 He=3 He ratios both higher and lower than MORB are found is Heard Island [11]. The helium data are correlated with lead isotopic compositions observed on the same islands and are interpreted in terms of source variations. The existence of such a multiple isotopic signature can be explained by two scenarios. The rst model proposes that the heterogeneous Azores plume source has evolved from Sa o Miguel to Terceira composition, by various degrees of melting of heterogeneous mantle. The second hypothesis is that the Azores plume is homogeneous with a Terceira like composition. The origin of the Sa o Miguel signature would then correspond to sampling of very local km-size heterogeneities, resulting from the delamination of enriched subcontinental lithosphere, which occurred during the Jurassic opening of the North Atlantic.

Faial ACO95-sand Olivine rich sand from the Capelinho place. Results from projection of submarine eruption during the 1957 eruption. ACO95-47 Collected on the chimney in the rim that separates the historical eruption of the Capelinho (1957 =58) from the Complexe do Capelo (<800 yr). ACO95-49 Xenolith taken on the beach of the Baia da Ribeira das Cabras. Unknown age. ACO95-52 Sand with olivines and augites taken in the beach of Varadouro. ACO95-53 Collected on the road leading to the caldera near the CabeodosTrinta Pic. ACO95-55 Porto de Feiteira. Pico ACO95-20 Olivine and pyroxene rich basalts from the 1718-20 ow (Fase de Sta Luzia), collected near the airport. Basalt collected on the road between Sa o Roque do Pico and Lajes. Bottom of the Pic de Felipe (complexe da Madalena). Xenolith collected in the Misterio de Silveira (phase de Sta Luzia, 1718-20). Collected near Caelano (Ponta da Faca) (complexe da Madalena). Same location as 26.

ACO95-26

ACO95-30 ACO95-33 ACO95-40

Sa o Miguel ACO95-3 1563 Queimado Pic lava ow. ACO95-56 Collected on the road between Ribeira Grande and Ponta Delgada near the Dr Ferreira Pic.

M. Moreira et al. / Earth and Planetary Science Letters 169 (1999) 189205 Nordeste ACO95-62 ACO95-66 ACO95-68 Terceira ACO95-9 ACO95-10 ACO95-11 ACO95-12 ACO95-14 ACO95-16

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Ankaramite collected near the Guihermo ou dos Moinhos river. South of Lomba da Fazenda. Ankaramite collected near the Mulher river. South of Santana. Ankaramite collected near Faial da Terra.

1761 lava ow at the bottom of the Pico do Fogo. Collected near the road between Biscoitos and Angra Do Heroismo (near the Pico do Fogo). Collected in the Guiherme Moniz Caldeira (north). Collected near Faieis in a river (Rib. das Pedras). Collected near the road between Sa o Sebastiao and Feteira (near Boavista). Collected near the road near Rossio de Sant Ana.

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