Journal of Volcanology and Geothermal Research 287 (2014) 12–21

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Journal of Volcanology and Geothermal Research

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Initial sub-aerial volcanic activity along the central Lesser Antillesinner arc: New K–Ar ages from Les Saintes volcanoes

Fabienne Zami a, Xavier Quidelleur b,c,⁎, Julia Ricci b,c, Jean-Frédéric Lebrun a, Agnès Samper b,c,1

a EA 4098 LaRGE, Université des Antilles et de la Guyane, Guadeloupe (FWI), Franceb Univ Paris-Sud, Laboratoire GEOPS, UMR8148, Orsay, F-91405, Francec CNRS, Orsay, F-91405, France

⁎ Corresponding author at: Univ Paris-Sud, LaboratF-91405, France.

E-mail address: xavier.quidelleur@u-psud.fr (X. Quide1 Now at: Institut de Physique du Globe (IPGP), Paris; F

http://dx.doi.org/10.1016/j.jvolgeores.2014.09.0110377-0273/© 2014 Elsevier B.V. All rights reserved.

a b s t r a c t

a r t i c l e i n f o

Article history:Received 7 April 2014Accepted 21 September 2014Available online 28 September 2014

Keywords:Les SaintesLesser AntillesK–Ar datingGeochemistryRecent arc activity

Wepresent newgroundmass K–Ar ages obtained using the Cassignol–Gillot technique, togetherwithwhole-rockmajor and trace elements, from Les Saintes islands (Terre-de-Haut and Terre-de-Bas). They are located along thenorthern Lesser Antilles inner arc, between Basse-Terre Island (western Guadeloupe) to the North and DominicaIsland to the South. Ages reveal that themain volcanic phase in Terre-de-Haut occurred between 2.98±0.04 and2.00 ± 0.03 Ma, and show that the onset of sub-aerial volcanism in Terre-de-Haut is slightly older (~0.2 Myr)than that of northern Basse-Terre. Volcanism in Les Saintes resumed to the west, with the rapid constructionof Terre-de-Bas Island at 0.888 ± 0.009 Ma. Major elements analyses show that most lavas from Les Saintes be-long to a sub-alkalinemedium-Kmagmatic series and aremainly andesites, with relatively rare basaltic andesitesand dacites. Rare earth elements spectra reveal a strong enrichment in light elements, as observed for Dominicalavas, and significantly higher than observed for Basse-Terre lavas. Noticeably, Terre-de-Bas spectra displaymoreenriched patterns relative to those from Terre-de-Haut lavas, suggesting a lower degree of partial melting or astronger sedimentary component incorporated to the subducting slab. Overall, geochemical signatures of LesSaintes and Dominica magmas display common characteristics, which we interpret as reflecting strong petroge-netic affinities, while both are significantly different from that of Basse-Terre lavas. Finally, this study provides aprecise timing of subaerial volcanism of Les Saintes Islands, which can be used to better constrain through timethe development of the tectonic half-graben where these islands lie, which is part of the arc-parallel en-echelonfaults system accommodating the oblique convergence of the North American plate from Montserrat toDominica. In addition, these results reveal that the initiation of Terre-de-Haut volcanism is presently the oldestdated volcanism from the northern part of the Lesser Antilles active arc.

© 2014 Elsevier B.V. All rights reserved.

1. Introduction

The Lesser Antilles magmatism results from the subduction ofthe North and South American plates beneath the Caribbean plate at arelatively low velocity of about 2 cm/yr (e.g., Hawkesworth andPowell, 1980). Two main volcanic arcs, which merge southward ofMartinique, were successively produced since Late-Oligocene, with atemporal westward displacement from the outer to the inner arc(e.g., Briden et al., 1979; Westercamp, 1979; Germa et al., 2011a). Theinner arc is presently active, with about 20 active volcanoes and morethan 34 historical eruptions. Within the Pliocene to Quaternary innerarc (e.g., Briden et al., 1979), Les Saintes Islands (Fig. 1) represent a

oire GEOPS, UMR8148, Orsay,

lleur).rance.

key target to study the onset of the inner-arc sub-aerial volcanismbecause only a rather small volume of magma erupted, and hence wasnot covered by younger activity, and it displays a prolonged activitythrough the Pliocene to early Pleistocene (Jacques et al., 1984). It is lo-cated to the South of Basse-Terre, thewestern part of Guadeloupe Islandwhere lies the active volcano of La Soufrière, and to the North ofDominica, with its northernmost active volcano of Morne aux Diables.Whole rock K–Ar ages obtained previously for Les Saintes (Jacqueset al., 1984) have been used to establish the most recent geological map(Jacques andMaury, 1988), but they can be considered as poorly reliable.Recent studies focusing on Lesser Antilles lavas demonstrated that signif-icant bias can affect whole-rock K–Ar ages, with overestimated ages inmany cases (e.g., Samper et al., 2007, 2008; Germa et al., 2011b). There-fore, it appears important to obtain new accurate ages in Les Saintes inorder to constraint the timing of the earliest inner arc activity. Moreoverour new petrology and geochemistry data lead us to investigate the rela-tionship between Les Saintes volcanism and that of the still active neigh-bor volcanic islands of Dominica and Basse-Terre.

Grenada

St Vincent

Ste Lucia

Martinique

Dominica

Guadeloupe

Montserrat

St Kitts and Newis NAM

2cm/yr

SAM

Accretionnary prism

Fore arc Bassin

64°W 62°W 60°W 58°W

18°N

16°N

14°N

12°N

Les Saintes

0.5 km03SA01

2.00 ± 0.03

Les Saintes

5 km

Terre-de-Bas Terre-de-Haut

03SA022.08 ± 0.03

03SA032.40 ± 0.04

12SA13b2.08 ± 0.03

12SA112.07 ± 0.03

12SA122.98 ± 0.04

04SA070.916 ± 0.03204SA04

0.889 ± 0.014

04SA060.882 ± 0.013

0.5 km

Chameau

Ilet à CabritDôme Napoléon

Pointe Morel

Morne Morel

Morne à Craie

Pain de sucre04SA0512SA14

Gros Cap

Pointeà l'Eau

Basse-Terre Island

(Guadeloupe)

Terre-de-BasTerre-de-Haut

NN

N

Fig. 1.Geodynamic setting of the Lesser Antilles arc. Thewhite arrows show the subduction of theAtlantic plate under the Caribbeanplate at a rate of 2 cm/yr (e.g., Macdonald et al., 2000).Bathymetry image is fromGeoMapApp using bathymetry data of Smith andSandwell (1997). The dashed andplain line shows the location of the outer older arc and the inner recent activearc, respectively. The right-side insert shows the location of Les Saintes Islands with respect to southern Basse-Terre (Guadeloupe Islands). The open circle shows the location of the activeSoufrière volcano. Normal faults locations are from Feuillet et al. (2011). Left and right lower frames show the location of samples analyzed here from Terre-de-Bas and Terre-de-Haut,respectively. Ages from this study, when available, are given in Ma.

13F. Zami et al. / Journal of Volcanology and Geothermal Research 287 (2014) 12–21

2. Geological background

Distribution of volcanism within the inner arc divides in a northern,a central and a southern arc segment, which differ by their magma pro-duction rates and their dominant composition of erupted magmas(e.g., Macdonald et al., 2000). Islands from the central arc segment,which includes Basse-Terre (Guadeloupe), Dominica and Martiniquefrom North to South, are themost active islands and present the largestemitted volumes of the inner arc (Wadge, 1984). Magma compositionsvary from tholeiitic (low-K) in the northern segment, through calc-alcaline (medium-K) in the central segment, to highly magnesianmagmas approximating primary magma compositions in the southernsegment (Brown et al., 1977). The dip of the Benioff zone varies fromabout 50° in the northern segment of the arc, to vertical in the southernsegment (Wadge and Shepherd, 1984). Based on Sr, Nd, Pb isotopes sig-natureswith continental crust similarities (e.g.,White and Dupré, 1986;Carpentier et al., 2008), it has been proposed that sediments are in-volved in magma genesis with varying degree, depending on the islandlatitude. Such variation has been related to the northward decreasingterrigenous sediments thickness present onto the subducting slab,away from their source located within the Archean South-American

craton (White et al., 1985), while conversely, pelagic sediment propor-tion increases northward. However, the origin of the sediment contam-ination remains debated, with either an assimilation process combinedwith fractional crystallization (e.g., Davidson and Harmon, 1989), or adeeper contamination of the source in the mantle wedge through sedi-mentmelting, with time varying proportion (e.g., Labanieh et al., 2010),or through enrichment in fluid-mobile elements (such as Ba, U, Sr, Pb).

The 9 km2 Les Saintes Islands are located between Basse-Terre andDominica, about 10 and 30 km away, respectively, within a 15 kmwide tectonic basin striking N135°E parallel to the arc (Fig. 1). This ac-tive Les Saintes graben belongs to the en echelon left lateral transtensivefault system that runs along the arc (Bouysse and Westercamp, 1990;Feuillet et al., 2001, 2002; Bazin et al., 2010), and accommodates theoblique component of the subducting plate. This fault system wasreactivated in 2004 during the Mw = 6.3 Les Saintes earthquake(Feuillet et al., 2011). Les Saintes archipelago consists of two mainvolcanic islands, Terre-de-Haut and Terre-de-Bas, which have a ratherlimited eruption rate compared to other islands from the central seg-ment of the inner arc. Based on whole-rock K–Ar ages, Jacques et al.(1984) and Jacques and Maury (1988) documented five distinct con-struction phases and proposed that magmatic activity was continuous

14 F. Zami et al. / Journal of Volcanology and Geothermal Research 287 (2014) 12–21

through the Pliocene–early Pleistocene for Les Saintes volcanoes. Theyproposed that the first phase, referred as the basal complex and charac-terized by emission of dark andesitic lavaflowswith twopyroxenes, ini-tiated ca. 5 Ma in the central part of Terre-de-Haut. They note that thisarea of the island appears deeply altered by intense hydrothermalism.They proposed that the second phase, which represents the mainbuild up phase of Les Saintes, occurred between 3.6 to 3 Ma. The thirdphase ranged from 2.8 to 2.4 Ma and ended with several intrusions inTerre-de-Haut, Ilet Coche (to the southeast of Terre-de-Bas) and Ilet àCabrit. Jacques et al. (1984) proposed that the activity of Terre-de-Haut ended at about 2 Ma with the emplacement during the fourthphase of a single quartz rich andesite neck, while Terre-de-Bas builtup at that time. Finally, the last phase took place only in Terre-de-Basbetween 1.3 and 0.6 Ma and consisted in few blocks-and-ash flowsmade of hornblende andesites.

Geochemical data from samples collected all over the archipelago(Westercamp and Mervoyer, 1976; Jacques et al., 1984; Jacques andMaury, 1988) show that most samples are acid andesites. Major ele-ments suggest that lavas evolved from calc-alkaline basalts to dacites.These studies showed that major elements variations are identical foreach proposed phase except for the last erupted lavas in Terre-de-Haut that are only represented by quartz-bearing acid andesites. Lavasdisplay a very porphyric texture, with phenocrysts of basic plagioclase,orthopyroxene, clinopyroxene and titanomagnetite, in a decreasingorder of abundance. These phenocrysts can be associated with amphi-boles, quartz, ilmenites and rare olivines. These authors concludedthat magmatism did not evolved significantly through time, and thatmajor elements from Les Saintes lavas result from a simple magmaticdifferentiation. Unfortunately, no trace elements were available.

In this study, we have sampled seven lavas flows in Terre-de-Hautand four in Terre-de-Bas islands (Fig. 1) in order to obtain new geochro-nological and geochemical data (major and trace elements).We carefullyselected the outcrops to ensure that the main lava flows associatedwith the main volcanic phases were sampled. Moreover, among these11 new sites, we revisited five units from Terre-de-Haut (03SA01,03SA02, 03SA03, 12SA12 and 12SA13) and one (04SA06) from Terre-de-Bas, previously analyzed by Jacques et al. (1984). At each location,large hand-size blocks of massive lavas void of macroscopic secondaryminerals or weathering were taken.

3. Analytical methods

3.1. K–Ar dating

Samples for dating were selected on the basis of a careful thin-section examination. Two samples (12SA14 and 04SA05) showingalteration were discarded. Depending of the rock texture, we have se-lected the 125–250 and 80–125 μm size-fractions in order to obtain ahomogeneous preparation. The groundmass was then obtained in anarrow density range using heavy liquids in order to eliminate possibleundetected traces of weathering. Finally, magnetic separation was ap-plied to remove possible residual phenocrysts.

Duplicated potassium (K) and argon (Ar) measurements wereperformed at the Laboratoire GEOPS (Orsay, France) using the unspikedCassignol–Gillot technique (e.g., Gillot et al., 2006). A detailed descrip-tion of the procedure followed here and uncertainties calculation canbe found in Germa et al. (2010). Potassium (K) contentwas determinedby flame spectroscopy and compared to reference standards MDO-G(K = 3.51%; Gillot et al., 1992) and BCR-2 (K = 1.486%; USGSStandard). Argon (Ar)wasmeasured using amulti-collector 180° sectormass spectrometer similar to the one described in Gillot and Cornette(1986), or using a VG quadrupole mass spectrometer describedin Rouchon et al. (2008). Argon analyses performed on both massspectrometers yielded identical argon results, as shown by duplicateanalyses of groundmass separates and/or plagioclase separates fromMar-tinique (Germa et al., 2010), as well as by age standards measurements

(Rouchon et al., 2008). The unspiked Cassignol–Gillot technique isbased on comparison of argon isotopes 36 and 40 from atmosphericand sample aliquots. The air pipette is calibrated by routine measure-ments of GL-O (Odin et al., 1982) and HD-B1 (Fuhrmann et al., 1987)standards. The former is characterized by a value of 6.679 × 1014 atomsof radiogenic 40Ar per gram content, while the age of 24.2 Ma (withK = 7.995%) is used for the latter (Hess and Lippolt, 1994; Schwarz andTrieloff, 2007). K isotopic ratios and 40K decay constants of Steiger andJäger (1977) have been used. All uncertainties reported in this studyare quoted at the 1σ level (Table 1).

3.2. Geochemistry

Following powder grinding, samples have been analyzed by Serviced'Analyse des Roches et Minéraux (SARM) at Centre de RecherchesPétrographiques et Géochimiques (CRPG), Nancy, France. For eachsamples, 200 mg of rock were melted with LiBO2 in Pt-Au crucible,and then dissolvedwith HNO3. The solution obtained has been analyzedby ICP-AES (Thermo Electron IRIS Advantage) for major and minor ele-ments, and/or by ICP-MS (Thermo Elemental X7) for 43 trace elements(Table 2). Calibration has been made with international standards(AN-G, BR, UB-N, DR-N, GH), which underwent the same processing(Govindaraju and Mevelle, 1987; Govindaraju et al., 1994; Carignanet al., 2001).

4. Results

4.1. K–Ar ages

We have obtained nine new K–Ar ages ranging from 2.98 ± 0.04 to0.882 ± 0.013 Ma (Table 1). K content of the groundmass analyzedrange between 0.749% and 1.695% and radiogenic 40Ar content between3.1% and 66.3%. Three groups of ages can be distinguished for Terre-de-Haut whereas we found only one in Terre-de-Bas (Fig. 1).

In Terre-de-Haut, sample 12SA12 from Napoléon dacitic domeprovides the oldest age of this study at 2.98 ± 0.04 Ma. The secondgroup represented by the Morne Morel sample 03SA03 has an inter-mediate age of 2.40 ± 0.04 Ma. Finally, the third group of foursamples, 03SA02, 12SA13b, 12SA11 and 03SA01 (Fig. 1) presentsclustered ages between 2.08 ± 0.03 and 2.00 ± 0.03 Ma (Table 1).These four latter samples are from the basal complex (Jacques et al.,1984), the Pointe Morel, the Pointe à L'Eau and Le Chameau dome,respectively.

The three lavas from Terre-de-Bas dated here display undistin-guishable ages, despite K content varying from 1.098% and 1.680% and40Ar radiogenic yield ranging from 3.1% to 24.5%, attesting that differentunits have been analyzed. At Petite Anse, the two samples 04SA06and 04SA04 yield ages of 0.882 ± 0.013 Ma and 0.889 ± 0.014 Ma,respectively, and at Anse des Muriers, sample 04SA07 is dated here at0.916 ± 0.032 Ma (Fig. 1). Such coherency suggests that Terre-de-Baswas constructed rapidly around 0.888 ± 0.009 Ma, as calculated usingthe inverse-variance weighted-mean of 04SA04, 04SA06 and 04SA07ages (Table 1).

4.2. Geochemistry

New major and trace elements analyses have been obtained for11 rocks from Les Saintes Islands (Table 2). We have completed our da-tabase with major elements analyses from 39 out of the 43 samplesfrom Jacques et al. (1984), excluding the basic enclaves. In addition,major and trace elements analyses from Basse-Terre (Samper et al.,2007, 2009) and Dominica (Brown et al., 1977; Lindsay et al., 2005)have also been considered for sake of comparison.

The total alkali versus Silica (TAS) diagram (Fig. 2) shows that all oursamples are andesites except sample 12SA12, which plots in the dacitefield. Their alkali content ranges from 4.1% to 6.2% and their silica

Table 1New K–Ar ages performed on groundmass separates. Column headings indicate sample and location names (T.H.: Terre-de-Haut; T.B.: Terre-de-Bas); geographic coordinates; potassium(K) concentration in percent; concentration of radiogenic 40Ar (40Ar*) in percent; concentration of radiogenic 40Ar (40Ar*) × 1012 in number of atoms per gram; age ± 1-sigma uncertain-ty of each measurement (in Ma); weighted mean ages ± 1-sigma weighted uncertainty (in Ma); mass spectrometer (M.S.) used (S: 180° sector mass spectrometer, Q: VG quadrupolemass spectrometer (Rouchon et al., 2008).

Sample (Island–Site) Coordinates(°N/°W)

K(%)

40Ar*(%)

40Ar*(×1012 at./g)

Age ± 1σ(Ma)

Mean age(Ma)

M.S.

12SA12 15°52'38.18″/ 1.695 26.9 5.3113 3.00 ± 0.04 S(T.H.–Morne Napoléon) 61°34'55.25″ 19.8 5.2421 2.96 ± 0.04 2.98 ± 0.04 S03SA03 15°52′29.0″/ 1.022 13.9 2.5600 2.40 ± 0.04 S(T.H.–Morne Morel) 61°34′24.5″ 15.1 2.5598 2.40 ± 0.04 2.40 ± 0.04 S03SA02 15°51′51.1″/ 0.749 13.6 1.6180 2.07 ± 0.03 Q(T.H.–Basal Formation) 61°35′14.4″ 13.0 1.63132 2.08 ± 0.03 2.08 ± 0.03 S12SA13b 15°52'44.75″/ 1.352 24.7 2.9772 2.11 ± 0.03 S(T.H.–Pointe Morel) 61°34'20.92″ 29.0 2.9020 2.05 ± 0.03 2.08 ± 0.03 S12SA11 15°52'40.34″/ 1.232 24.3 2.6922 2.09 ± 0.03 S(T.H.–Pointe à l'eau) 61°34'52.21″ 23.9 2.6439 2.05 ± 0.03 2.07 ± 0.03 S03SA01 15°51′27.9″/ 1.592 66.3 3.3023 1.98 ± 0.03 S(T.H.–Chameau Dome) 61°35′31.2″ 43.4 3.3570 2.02 ± 0.03 2.00 ± 0.03 S04SA07 15°51′11.5″/ 1.098 3.1 1.0636 0.927 ± 0.032 S(T.B.–Anse Murier) 61°37′34.1″ 3.2 1.0391 0.906 ± 0.031 0.916 ± 0.032 S04SA04 15°51′04.2″/ 1.680 12.8 1.5750 0.897 ± 0.015 Q(T.B.–Petite Anse) 61°38′51.3″ 14.5 1.5458 0.881 ± 0.014 0.889 ± 0.014 S04SA06 15°51′09.1″/ 1.307 23.3 1.1990 0.878 ± 0.013 Q(T.B.–Petite Anse) 61°38′45.1″ 24.5 1.2094 0.886 ± 0.013 0.882 ± 0.013 S

15F. Zami et al. / Journal of Volcanology and Geothermal Research 287 (2014) 12–21

content extends between 58.6% and 63.4%. Overall, they fall within therange of samples analyzed by Jacques et al. (1984) and the range depictedby Basse-Terre and Dominica lavas, although samples 12SA12 and

Table 2Newmajor and trace elements composition of whole-rock samples analyzed here (*: not date

Terre-de-Haut

03-SA01 03-SA02 03-SA03 12-SA11 12-SA12 1

wt.%SiO2 62.05 61.03 59.90 61.40 63.38Al2O3 13.43 17.14 17.31 17.20 16.17Fe2O3 10.05 7.28 7.25 6.73 6.18MnO 0.24 0.20 0.18 0.14 0.13MgO 3.34 2.04 2.11 2.27 1.43CaO 4.66 6.76 6.65 6.62 4.68Na2O 2.94 3.30 3.33 3.33 4.25K2O 1.33 0.79 0.79 1.03 1.53TiO2 0.81 0.48 0.51 0.56 0.68P2O5 0.19 0.21 0.20 0.15 0.23L.O.I. 1.41 0.92 1.60 1.42 1.48Total 100.44 100.13 99.83 100.85 100.12 1

ppmRb 37.28 22.63 28.99 24.61 30.06Ba 246.9 172.3 209.8 237.3 344.9 1Th 4.331 3.099 3.199 3.945 5.155U 1.140 0.846 0.825 1.010 1.299Nb 5.595 3.880 4.109 3.882 9.928Ta 0.435 0.307 0.316 0.327 0.683La 14.81 13.18 17.43 13.67 23.74Ce 30.23 28.80 36.05 27.31 52.66Pb 5.0848 2.9704 4.2886 7.062 5.4597Pr 3.741 3.484 5.111 3.334 6.625Sr 198.4 305.9 305.9 273.5 298.0 3Nd 16.66 15.98 21.58 14.91 30.45Zr 115.2 103.7 103.6 102 213.3 1Hf 3.172 2.827 2.853 2.872 5.528Sm 3.841 3.712 4.873 3.465 7.124Eu 0.974 1.145 1.333 1.011 1.839Gd 3.718 3.453 4.441 3.308 6.617Tb 0.617 0.563 0.711 0.550 1.071Dy 3.897 3.575 4.434 3.534 6.726Y 25.49 22.42 25.90 24.30 38.69Ho 0.838 0.761 0.881 0.742 1.358Er 2.561 2.288 2.602 2.288 3.971Tm 0.404 0.362 0.402 0.361 0.636Yb 2.851 2.596 2.814 2.580 4.363Lu 0.481 0.429 0.451 0.430 0.698

04SA05 are slightly above the general trend. K2O versus SiO2 diagram(Fig. 3) reveals that Les Saintes lavas mostly belong to the medium K,calc-alkaline arc series, although three samples from Terre-de-Haut

d sample).

Terre-de-Bas

2-SA13a 12-SA14* 04-SA04 04-SA05* 04-SA06 04-SA07

59.45 61.32 59.76 61.18 60.39 58.6117.54 16.31 17.63 17.77 17.37 17.607.42 6.44 7.21 7.05 6.50 7.530.17 0.13 0.15 0.11 0.17 0.192.09 1.96 1.62 0.28 1.63 3.256.80 5.50 6.53 5.71 6.43 7.833.46 3.27 3.69 4.39 3.56 3.420.72 1.13 1.21 1.83 1.22 1.000.55 0.51 0.61 0.87 0.55 0.700.23 0.17 0.16 0.27 0.17 0.172.10 3.33 1.06 0.72 2.29 0.15

00.53 100.06 99.62 100.17 100.26 100.45

7.483 29.28 30.07 31.69 28.58 22.9496.4 229.0 253.4 417.6 282.3 230.63.250 3.476 5.132 4.641 4.790 4.1470.662 0.873 1.316 1.110 1.269 1.2394.118 4.082 7.308 6.940 6.546 5.8530.326 0.346 0.610 0.520 0.603 0.511

15.34 19.45 17.45 18.95 36.68 17.8430.43 37.16 32.43 41.67 46.87 30.284.367 4.278 5.224 2.822 4.6251 4.3134.025 5.134 3.607 5.314 7.798 4.393

32.6 281.8 402.7 302.4 352.3 397.918.66 22.84 15.03 25.39 31.74 17.5503.5 111.4 94.97 161.6 102.9 100.62.854 3.009 2.466 4.297 2.731 2.6804.325 5.085 3.054 6.164 6.348 3.6651.304 1.212 1.066 1.587 1.712 1.1874.150 4.878 2.666 6.342 6.753 3.3650.680 0.787 0.420 1.020 1.010 0.5384.236 4.866 2.534 6.500 6.104 3.328

26.90 30.07 15.58 43.99 39.68 19.750.881 0.981 0.521 1.396 1.254 0.6692.600 2.822 1.522 4.155 3.548 1.9590.407 0.451 0.235 0.633 0.539 0.3112.872 3.131 1.621 4.293 3.565 2.1790.463 0.494 0.270 0.712 0.586 0.356

BT

DQ

45 50 55 60 65 700

2

4

6

8

10

Na 2

O+

K2O

SiO2

Basalt Basalticandesite

Andesite

Dacite

TrachydaciteTrachy-andesite

Basaltictrachy-andesite

Trachy-basalt

Phono-Tephrite

03SA0103SA0203SA0312SA1112SA1212SA13b12SA14

Terre-de-Haut

04SA0404SA0504SA0604SA07

Previous data

Terre-de-Bas

Fig. 2. TAS diagram of Les Saintes lavas. Small symbols are fromprevious analyses (Jacques et al., 1984),while larger symbols are from this study. The location of each new sample is shownusing the same symbols as in Fig. 1. The blue and green fields show the range of values displayed by lavas fromDominica (DQ; Brown et al., 1977; Lindsay et al., 2005) and Basse-Terre (BT;Samper et al., 2007, 2009), respectively.

16 F. Zami et al. / Journal of Volcanology and Geothermal Research 287 (2014) 12–21

(03SA03, 12SA13b and 03SA02) lie along the upper limit of the low K,Tholeiite arc series.

All samples have porphyric texture with plagioclase phenocrystsassociated with a variable amount of clinopyroxene, orthopyroxene,titanomagnetite, ilmenite, amphibole, and/or quartz phenocrysts. Thepresence of these minerals is compatible with the observed MgO,Fe2O3, CaO and TiO2 negative correlation relative to SiO2 (Fig. 3). Overall,values displayed by these Harker diagrams for Les Saintes are compara-ble with lavas from the northern islands of the Lesser Antilles arc(Macdonald et al., 2000). Sample 03SA01, from the Chameau dome inTerre-de-Haut, presents an anomalously low value in Al2O3 and highvalues in Fe2O3 and MgO, which can be related to its high contentin basic xenoliths. Finally, Fig. 3 shows that sample 04SA05 displays alow content in MgO, high TiO2 and Na2O values, and is slightly enrichedin Al2O3 and K2O relative to the general trends observed for majorelements of Les Saintes lavas. Such behavior could be explained by theassimilation of Na-rich plagioclases during magma ascent through anevolved reservoir.

Rare earth elements (REE; Table 2), when normalized to chondritevalues (Sun and McDonough, 1989), show an important enrichmentin light REE (LREE) relative to heavy REE (HREE; Fig. 4a). Similar enrich-ment is observed for Dominca lavas, while flatter spectra are observedfor Basse-Terre samples. Note that, for sake of comparison with LesSaintes samples, only samples with SiO2 content ranging between48% and 64% have been considered for the two latter islands. It can benoted that most samples from Les Saintes present a negative Eu anom-aly, suggesting strong plagioclase fractionation. Only sample 04SA04displays a positive anomaly, while sample 04SA07, also from Terre-de-Bas, do not show any Eu anomaly. Spider diagrams of incompatible ele-ments normalized to primitive mantle (Sun and McDonough, 1989)show typical patterns of subduction related magmas with Nb, Ta andTi depletions, and K and Pb enrichment (Fig. 4b). Overall, large-ionlithophile elements (LILE) abundance for Les Saintes is slightly higherthan for Basse-Terre volcanic rocks.

5. Discussion

5.1. Comparison with previously published ages

Previous K–Ar ages (herein referred using their original site number,e.g. S.33, in Jacques et al., 1984) obtained from Les Saintes islandsranged from 4.7 to 1.9 Ma and from 2 to 0.6 Ma for Terre-de-Haut and

Terre-de-Bas, respectively, suggesting a continuous volcanic activitythroughout this period (Jacques et al., 1984). Because, these resultsshow strong discrepancies with our new ages (Fig. 1 and Table 1), suchconclusion is not supported further.

In Terre-de-Haut Island, the oldest age previously published of4.71 ± 0.35 Ma was obtained on a dark andesitic lava flows with twopyroxenes (S.33) located to the North East of Morne à Craie, in the cen-tral part of Terre-de-Haut. Our new age of 2.08 ± 0.03 Ma obtained atthe same location (03SA02; Fig. 1) is much younger. Such strong differ-ence between previous whole-rock K–Ar and new K–Ar ages obtainedon groundmass using the Cassignol–Gillot technique has been observedfor lavas from different islands of the Lesser Antilles, such as Guade-loupe (e.g., Carlut et al., 2000), Dominica and St. Lucia (Samper et al.,2008) or Martinique (e.g., Germa et al., 2010). It has been attributedeither to slight weathering inducing K loss in the whole rock, or to theincorporation of xenocrysts, such as plagioclase feldspars, carryinginherited argon 40. Furthermore, our new age is statistically identicalto two other new ages from Terre-de-Haut of 2.07 ± 0.03 and 2.08 ±0.03Ma (12SA11 and 12SA13, respectively) suggesting a strong activityon Terre-de-Haut at that time. Note that a much older age of 3.07 ±0.15Ma (S.4)was also previously obtained for the latter sample. Locatedslightly to the South, MorneMorel (sample 03SA03 in Fig. 1) was datedat 2.69± 0.14Ma (S.1), while we obtained amore precise age of 2.40±0.04 Ma, which is again younger, albeit here compatible at the 2 sigmalevel with the previous age (Jacques et al., 1984). Field observation ofthe north-dipping Pointe Morel flows (12SA13) dated at 2.08 ±0.03 Ma supports our result that these lavas postdate the MorneMorel blocks and ash flow deposits (2.40 ± 0.04 Ma; 03SA03), as theyoverlap them. Two samples (S.75 and S.85) taken on Napoléon domehave been previously dated at 3.41 ± 0.17 and 3.10 ± 0.16 Ma. Ournew age of 2.98 ± 0.04 Ma (12SA12; Fig. 1) agrees with one of them.Finally, the two discordant ages of 3.47 ± 0.017 (S.38) and 2.77 ±0.14 Ma (S.81) obtained for the same unit of Le Chameau further high-light the poor reliability of the previous whole-rock K–Ar ages. Our newage of 2.00± 0.03Ma (03SA01; Fig. 1) for the same unit is younger andrepresents the youngest age obtained for Terre-de-Haut in this study(Table 1).

Regarding Terre-de-Bas, the three new ages ranging from0.882 ± 0.013 to 0.916 ± 0.032 Ma (Table 1 and Fig. 1) are undistin-guishable, while previous data ranged between 1.98 ± 0.30 (S.73) and0.64± 0.10Ma (S.70). However, it can be noted that sample S.68 datedat 0.85 ± 0.06 Ma (Jacques et al., 1984) is compatible with our new

03SA0103SA0203SA0312SA1112SA1212SA13b12SA14

04SA0404SA0504SA0604SA07

Previous data

Terre-de-Haut Terre-de-Bas

50 55 60 65 700.0

0.2

0.4

0.6

0.8

1.0

1.2

1.4

1.6

1.8

2.0

K2O

(w

t%)

B BA DA

High K

Low K

SiO2 (wt%)

Na 2

O (

wt%

)

50 55 60 65 702

3

4

5

SiO2 (wt%)

50 55 60 65 702

4

6

8

10

Fe 2

O3

(wt%

)

SiO2 (wt%)

50 55 60 65 700

1

2

3

4

MgO

(w

t%)

SiO2 (wt%)

50 55 60 65 7013

14

15

16

17

18

19

Al 2

O3

(wt%

)

SiO2 (wt%)

50 55 60 65 704

5

6

7

8

9

CaO

(w

t%)

SiO2 (wt%)

50 55 60 65 700.4

0.5

0.6

0.7

0.8

0.9

1.0

1.1

SiO2 (wt%)

TiO

2 (w

t%)

Calc-Alkaline Series

Arc Tholeiite Series

Medium K

Fig. 3. Harker diagrams showing the evolution of the major elements as a function of the SiO2 content. Symbols are the same as in Fig. 2.

17F. Zami et al. / Journal of Volcanology and Geothermal Research 287 (2014) 12–21

determination of 0.882 ± 0.013 Ma, obtained for 04SA06 sampled atthe same location, although our age is better constrained with a smalleruncertainty. Nevertheless, the youngest age from Jacques et al. (1984)(0.64 ± 0.10 Ma; S.70, Gros Cap) appears inconsistent with a secondage they obtained for the same formation (1.29 ± 0.10 Ma; S.71, GrosCap).

Overall, the new ages display lower uncertainties with a narrowerrange than previous whole-rock K–Ar data, as often observed in the Less-er Antilles, either with the Cassignol–Gillot technique (e.g., Samper et al.,

2007) or using the 40Ar/39Ar technique (Harford et al., 2002), bothapplied to the groundmass mineralogical phase.

5.2. Temporal evolution of Les Saintes volcanism

Our new K–Ar ages and geochemical correlations together with re-interpretation of Jacques et al. (1984) geological mapping, leads us todistinguish four successive phases for Les Saintes subaerial volca-nism. The first phase occurred around 2.98 ± 0.04 Ma and consists of

1

10

100

Cs Rb Ba Th U Nb Ta K La Ce Pb Pr Sr P Nd Zr Sm Eu Ti Dy Y Yb Lu

Roc

k/P

rimiti

ve M

antle

1

10

100

La Ce Pr Nd Pm Sm Eu Gd Tb Dy Ho Er Tm Yb Lu

Roc

k/C

hond

rites

a)

b)

BT

BT

DQ

DQ

Fig. 4. a) Rare earth elements spectra, normalized to the chondrite composition (Sun andMcDonough, 1989), for samples from this study, and b) Spider diagrams of incompatibleelements, normalized to the primitive mantle composition (Sun and McDonough, 1989).Symbols are the same as in Fig. 2.

18 F. Zami et al. / Journal of Volcanology and Geothermal Research 287 (2014) 12–21

dacitic lava flows and explosive breccia from Napoléon dome (Fig. 1).This phase seems to be associated to the Pointe Bombarde, the eastern-most part of Ilet à Cabrit, as suggested by the geological map (Jacques etal., 1984). Thus, the onset of Les Saintes aerial volcanism appears to berestricted to the northern part of the archipelago and is characterizedwith both extrusive and explosive volcanic activities. It is followed bythe second phase, which occurred slightly to the east and built up theMorne Morel at 2.40 ± 0.04 Ma (Fig. 1). It started with explosivephreato-magmatic activity and continued with the emplacementof pyroclastic flows. The third phase took place close to 2 Ma andwas apparently extended to the whole Terre-de-Haut Island. Itachieved the buildup of the island with the development of the PointeMorel basic andesitic flows to the North (2.08 ± 0.03 Ma; 12SA13)associated with the phreato-magmatic deposit from Pointe à L'eau(2.07 ± 0.03 Ma; 12SA11) and the dark andesite lava flow with twopyroxenes from the central part of Terre-de-Haut (2.08 ± 0.03 Ma;03SA02). This third phase ended with the emplacement of the volumi-nous Chameau dome dated at 2.00± 0.03Ma (03SA01) and, as inferredfrom the geologic map (Jacques et al., 1984), with several other intru-sions such as the Morne à Craie dike, an acid intrusion with quartz phe-nocrysts, and speculatively the Pain de Sucre intrusion (Fig. 1), whichdid not pass our selection criteria for dating. Whereas formations inthe central part of the island are deeply affected by hydrothermalalteration, all the intrusions (including the Chameau dome) that arewithin or close to the hydrothermal field do not appear to be affectedby this alteration. Therefore, it suggests that the hydrothermal activitylocated within the central part of Terre-de-Haut, took place between

2.08 ± 0.03 and 2.00 ± 0.03 Ma. The fourth phase was restricted toTerre-de-Bas where only ages younger than 1 Ma have been obtained(Fig. 1 and Table 1). As our three ages obtained from Terre-de-Bas areconsistent between 0.916 ± 0.032 and 0.882 ± 0.013, it appears thatTerre-de-Bas was built in a short time span as a composite volcanomade of andesitic lavaflows emitted from the central part,with a termi-nal activity located to the Southwest with production of Saint-Vincenttype nuées ardentes (Jacques et al., 1984).

Our new ages show that the subaerial construction of Terre-de-Hautlasted about 1Myr, between 2.98±0.04 and 2.00±0.03Ma. Volcanismin Les Saintes resumed about 1 Myr later, with the rapid construction ofthe ~1 km3 subaerial part of Terre-de-Bas around 0.888 ± 0.009 Ma(see paragraph 4.1), about 4 km west of Terre-de-Haut. A westwardmigration of volcanism occurred in the Lesser Antilles from the old tothe recent arc since Miocene. It is attributed to flattening of thesubducting slab due to the presence of low-density aseismic ridges(e.g., Bouysse andWestercamp, 1990). However, because thewestwardmigration observed from Terre-de-Haut to Terre-de-Bas between 2 and1 Ma remains within the recent arc, a more local explanation should beinvoked. We rather suggest that volcanism in Terre-de-Bas developedthanks to favorable conditions for magma to rise along the westernandmajor N140° trending fault of the Les Saintes half-graben. Similarly,it can be noted that offshore between Dominica and Les Saintes severalundated underwater volcanoes are present along this fault, as shown inFig. 2 of Feuillet et al. (2011) and may attest for tectonic control onmagma ascent.

The comparison of our new ages from Les Saintes (Table 1) withthose obtained for Basse-Terre acquired with the same technique(Samper et al., 2007), demonstrates that volcanic activities fromTerre-de-Haut and from the Basal Complex of northern Basse-Terre(from2.8 to 2.7Ma), located 50 kmnorthward,were coeval.When volca-nic activity resumed in Basse-Terre at 1.8 Ma, the volcanic activity inTerre-de-Haut already ended. Finally, while Terre-de-Bas was rapidlyconstructed around 0.888 ± 0.009 Ma, the Axial Chain massif of Basse-Terre, emplaced from about 1 Ma (Blanc, 1983), was also experiencinga relatively high magmatic extrusion rate of 5.4 ± 0.9 × 10−4 km3/yr,which is the highest rate calculated for southern Basse-Terre massifs(Lahitte et al., 2012).

Based on the available whole-rock K–Ar ages, the existence ofcoeval volcanic activities in Les Saintes and northern Dominica hasbeen previously proposed (Bellon, 1988). Unfortunately, besides adetailed stratigraphy recently published (Smith et al., 2013), no reliableages are available in Dominica to support such hypothesis.

5.3. Magmatic evolution of Les Saintes volcanoes

The geochemical data provide evidences that Les Saintes andDominica magmatism share common features, and are different fromthat of Basse-Terre. Indeed, Les Saintes and Dominica REE spectrapresent a marked enrichment in LREE (Fig. 4), while Basse-Terre lavasdisplay relatively flat patterns throughout its volcanic history (Samperet al., 2007). In addition, Terre-de-Haut and Dominica lavas have similarLa/SmCN ratio, which are significantly higher than observed for Basse-Terre (Fig. 5a), but three out of four samples from Terre-de-Bas displayeven higher La/SmCN ratios, close to the field of terrigenous sediments(Defant et al., 2001). We suggest that a magma mixing occurredbetween a typical Les Saintes magma, as revealed by the only uncon-taminated Terre-de-Bas samples, and sediment-contaminated magma,as revealed by the three samples with high La/SmCN ratio. Because allof Terre-de-Bas samples, provided a common age, we can speculatethat the arrival of a contaminated magma within an old magmaticchamber could have triggered the construction of Terre-de-Bas, simul-taneously with a westward migration of volcanism.

The diagram of Ba/LaCN versus La/SmCN, normalized to chondrite(Sun andMcDonough, 1989) shown in Fig. 5a, can be used to investigatethe role of fluids, melting rates and source contamination for arc

La / Sm

a) b)

c) d)

variable degrees of partial melting

depleted MORB mantle

hydr

ous

fluid

/mel

tm

etas

omat

ism

Terrigenoussediments

Lesser Antilles

Ba

/ La C

N

1

2

3

4

5

6

7

8

1 2 3 40

S. ANT

N. ANT

03SA0103SA0203SA0312SA1112SA1212SA13

04SA04

04SA0604SA07

04SA05

Terre-de-Haut Terre-de-Bas

90%IAB field

CN

0.5 1 1.5 2 2.5 3 3.5 40

0.2

0.4

0.6

0.8

1.0

1.2

1.4

1.6

1.8

Ba/

Th

CN La / Sm CN

0 1 2 3 4 5 6

2

4

6

8

10

12

Nb

Th0 1 2 3 4 5 6

100

200

300

400

500

Sr

Th

BT

DQ

BT DQ

BT

DQ

BT DQ

Fig. 5. a) Ba/La vs. La/Sm ratios (Defant et al., 2001). N. Ant and S. Ant. are deep-sea sediments values obtained for northern and southern Lesser Antilles, respectively (Plank and Langmuir,1998); Terrigenous sediments (gray field) are from White et al. (1985); IAB (island arc basalts) are from Kay (1980). b) Ba/th vs. La/Sm ratios. c) Nb vs. Th, and d) Sr vs. Th elements.Note that each element has been normalized to the chondrite composition (Sun and McDonough, 1989). Symbols are the same as in Fig. 2.

19F. Zami et al. / Journal of Volcanology and Geothermal Research 287 (2014) 12–21

magmas (Kay, 1980). Les Saintes samples present a relatively low Ba/LaCN ratio, also observed for Basse-Terre and Dominica, suggesting amoderate slab-fluid input. However, Terre-de-Haut lavas show a medi-um La/SmCN ratio, within the range of values observed for Dominicalavas, whereas the youngest Terre-de-Bas lavas have a much higherLa/SmCN ratio, except sample 04SA05, which displays the lowest ratioof all Les Saintes lavas. As the portion of slab sediments incorporatedinto the mantle wedge has been proposed as the main control ofthe La/Sm ratio for subduction related lavas such as in Martinique(Labanieh et al., 2012), we interpret the La/Sm values observed forLes Saintes as reflecting higher incorporation of sediments than forBasse-Terre lavas. The stronger metasomatism of Basse-Terre lavas isfurther evidenced by increasing Ba/Th ratios for lowering La/Sm ratios(Fig. 5b), while Dominica and Les Saintes lavas display similar low Ba/Th values. When scrutinized the evolution of either Nb or Sr as a func-tion of Th (Fig. 5c and d), lavas from Basse-Terre, Dominica andLes Saintes display strikingly different behaviors, with Dominica lavasbeing the most homogenous with less evidence for crustal contamina-tion. On the other hand, Les Saintes lavas display higher Nb and Srvalues than neighbor islands, which can further reflect a stronger sedi-mentary input.

Whenplotted as a function of time (Fig. 6), the SiO2 values display anoverall decreasing trend, but the scatteredMgO contents indicate that itshould not be related to any long-term crystal fractionation process. Onthe other hand, the La/Sm ratio displays a marked increasing trend,which could be related to higher sedimentary inputs (Labanieh et al.,2012), or alternatively, a decreasing rate of partial melting. Note thatsample 04SA05, which display anomalous contents in major elements

(Fig. 3) and a very low La/Sm ratio (Fig. 5a), has not been dated so can-not be plotted in Fig. 6.

Finally, Les Saintes geochemical characteristics are typical of evolvedmagmas in the Lesser Antilles central islands. They share commonfeatures with Dominica lavas, but differ noticeably from Basse-Terrelavas. More particularly, they display unique features that can beinterpreted as a pronounced signature of a sedimentary component.Evidently, isotopic analyses are needed to better constrain the detailednature of the source and the magmatic processes involved in magmageneration.

5.4. Insights regarding the onset of volcanism in the Lesser Antilles northernarc

Subaerial activity in Basse-Terre started at 2.79 ± 0.04 Ma (Samperet al., 2007), while inMontserrat an age of 2.58± 0.06Mawas obtainedusing 40Ar/39Ar (Harford et al., 2002). Northward to Montserrat, noreliable ages have been obtained so far. In Dominica, only the recentsouthern part has been investigated (e.g., Samper et al., 2008) and thenorthern and/or oldest subaerial activity remains devoid of reliableages. Southward, in Martinique, where the inner active arc and theouter arc merge, an intermediate arc has been active between 17 and7 Ma (Germa et al., 2010). It was followed by a westward drift of theactivity with the emplacement of the oldest phase of the Morne Jacobvolcano between 5.5 and 2.2Ma, whichmarks the onset of the subearialactivity of the recent arc in the central islands of the inner arc. Theage of 2.98 ± 0.04 Ma obtained here for Terre-de-Bas (Fig. 1; Table 1)is therefore the oldest age obtained for lavas from the northern part of

0

1

2

3

4

Time (Ma) 0 1 2 3

1

2

3

4

(La/

Sm

) chM

gO

58

59

60

61

62

63

64

SiO

2

Fig. 6. Evolution through time of SiO2, MgO, and La/Sm ratio normalized to the chondritecomposition (Sun and McDonough, 1989). Symbols are the same as in Fig. 2.

20 F. Zami et al. / Journal of Volcanology and Geothermal Research 287 (2014) 12–21

the recent arc and shows that there is an apparent latitudinal decreaseof the onset of subaerial volcanism in the recent arc, from5.5Ma inMar-tinique to 2.6 Ma in Montserrat. Taking into account the timing ofmagma ascent, the onset of volcanism in Les Saintes at 2.98 ± 0.04 Macould thus be used as a strong constraint to reconstruct thewestwardmi-gration of the arc and the shallowing of the North America subductingplate since Miocene.

6. Conclusions

Wehave shown that Terre-de-Haut was constructed in about 1Myr,between 2.98 ± 0.04 and 2.00 ± 0.03 Ma, while Terre-de-Bas was rap-idly emplaced at 0.888 ± 0.009 Ma. This demonstrates that volcanismin Les Saintes was not continuous, as previously inferred, but rather

presents a hiatus of volcanic activity of about 1 Myr. Lavas from LesSaintes have petrographic, mineralogical and geochemical characteris-tics of typical medium-K calc-alkaline lava from the central part of therecent active arc. Terre-de-Bas lavas present evidence for a strong com-ponent of terrigenous sediment contamination andpossible influence oftectonic structures on magma ascent. Our new ages reveal that theonset of the expression of subaerial volcanism along the northern LesserAntilles inner arc occurred in the late Pliocene at 2.98 ± 0.04 Ma in LesSaintes, slightly earlier (0.2 Myr) than in northern Basse-Terre. Howev-er, geochemical data do not support any strong relationship betweenBasse-Terre and Les Saintes volcanism, despite their geographical prox-imity. On the other hand, geochemical signatures of Les Saintes andDominica magmas display common characteristics, which we interpretas reflecting strong petrogenetic affinities. Moreover, Terre-de-Bas,the youngest island of Les Saintes, displays evidence for a strongcontinental-crust sedimentary contamination, which was not observedin neighboring islands. Finally, this study provides new reliable agesthat further extend the Lesser Antilles radiometric ages database,which, however, still needs to be completed for the sourthernmostand northernmost parts of the active inner arc.

Acknowledgments

We would like to thank P. Lahitte and D. Mollex for help withsampling, and C. Verati, J.M. Lardeau and M. Corsini for discussions.We have also appreciated arguing with colleagues from the geology de-partment of the Université des Antilles et de la Guyane. We thank thereferee and editor for their evaluation of the manuscript. This studywas funded by the Institut National des Sciences de l'Univers (CentreNational de la Recherche Scientifique) programs, and the EuropeanCommission EXPLORIS project (EVCR1-CT-2002-40026). This is LGMTcontribution no. 118.

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