Mineralium Deposita (2005) 40: 7699 DOI 10.

1007/s00126-005-0468-x

A RT I C L E

Philip M. Scotney Stephen Roberts Richard J. Herrington Adrian J. Boyce Ray Burgess

The development of volcanic hosted massive sulde and baritegold orebodies on Wetar Island, Indonesia

Received: 25 January 2005 / Accepted: 7 February 2005 / Published online: 12 April 2005 Springer-Verlag 2005

Abstract Wetar Island is composed of Neogene volcanic rocks and minor oceanic sediments and forms part of the Inner Banda Arc. The island preserves precious metalrich volcanogenic massive sulde and barite deposits, which produced approximately 17 metric tonnes of gold. The polymetallic massive suldes are dominantly pyrite (locally arsenian), with minor chalcopyrite which are cut by late fractures inlled with covellite, chalcocite, tennantitetetrahedrite, enargite, bornite and Fe-poor sphalerite. Barite orebodies are developed on the anks and locally overly the massive suldes. These orebodies comprise friable barite and minor suldes, cemented by a series of complex arsenates, oxides, hydroxides and sulfate, with gold present as <10 lm free grains. Linear and pipe-like structures comprising barite and ironoxides beneath the barite deposits are interpreted as feeder structures to the barite mineralization. Hydrothermal alteration around the orebodies is zoned and
P. M. Scotney (&) S. Roberts School of Ocean and Earth Science, Southampton Oceanography Centre, University of Southampton, Southampton, SO14 3ZH, UK E-mail: philip.scotney@wrg.co.uk Tel.: +44-1234-353996 R. J. Herrington Department of Mineralogy, Natural History Museum, Cromwell Road, London, SW7 5BD, UK A. J. Boyce Isotope Geosciences Unit, SUERC, East Kilbride, Glasgow, G75 0QF, UK R. Burgess Department of Earth Sciences, University of Manchester, Manchester, M13 9PL, UK Present address: P. M. Scotney WRG, 3 Sidings Court, White Rose Way, Dancaster, DN4 5NU, UK

dominated by illitekaolinitesmectite assemblages; however, local alunite and pyrophyllite are indicative of late acidic, oxidizing hydrothermal uids proximal to mineralization. Altered footwall volcanic rocks give an illite KAr age of 4.70.16 Ma and a 40Ar/39Ar age of 4.930.21 Ma. Fluid inclusion data suggest that hydrothermal uid temperatures were around 250 270C, showed no evidence of boiling, with a mean salinity of 3.2 wt% equivalent NaCl. The d34S composition of suldes ranges between +3.3& and +11.7& and suggests a signicant contribution of sulfur from the underlying volcanic edice. The d34S barite data vary between +22.4& and +31.0&, close to Miocene seawater sulfate. Whole rock 87Sr/86Sr analyses of unaltered volcanic rocks (0.707480.71106) reect contributions from subducted continental material in their source region. The 87Sr/86Sr barite data (0.70760.7088) indicate a dominant Miocene seawater component to the hydrothermal system. The mineral deposits formed on the anks of a volcanic edice at depths of $2 km. Spectacular sulde mounds showing talus textures are localized onto faults, which provided the main pathways for high-temperature hydrothermal uids and the development of associated stockworks. The orebodies were covered and preserved by post-mineralization chert, gypsum, Globigerina-bearing limestone, lahars, subaqueous debris ows and pyroclastics rocks. Keywords Gold Barite Massive sulde Banda Arc Submarine hydrothermal systems

Introduction
Spectacular examples of asymmetric massive sulde mounds, anked by barite deposits, are preserved on Wetar Island, Indonesia. The orebodies occur marginal to hydrothermally altered volcanic rocks, which overly ocean oor basalts, and are preserved beneath postmineralization Globigeriena-bearing limestones, lahars,

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subaqueous debris ows and pyroclastic rocks (Sewell and Wheatley 1994; Herrington and First 1996; Scotney et al. 1999). Associated hydrothermal alteration has argillic characteristics and the sulde mounds contain pyrite, chalcopyrite, tennantite, covellite and low-Fe sphalerite. Mineralization occurred at around 4.7 Ma (Herrington and First 1996) and, unusual for a volcanogenic massive sulde (VMS) system, only the precious metal-bearing barite resource was exploited. As a result, a subrecent VMS system is exceptionally preserved and exposed within open pits and associated drill core. Ore at Kali Kuning contained 1.9 Mt at 4.6 g/t gold, 151 g/t silver and 60% barite, with 2.2 Mt at 4.0 g/t gold, 146 g/t silver and 40% barite at Lerokis (Abadi 1996). Volcanogenic massive sulde systems are often signicant repositories of gold and silver (see Hannington et al. 1999 for review). Various factors are recognized to play an important role in the gold enrichment. These include the tectonic setting of the deposits, which in turn inuences the nature of the igneous basement, and the physical and chemical characteristics of the hydrothermal uids, in particular temperature, salinity and oxygen fugacity (Hannington et al. 1999). The gold bearing characteristics of the sulde assemblage and the argillic nature of the alteration at Wetar Island, has led to speculation that the hydrothermal uids responsible for the gold mineralization contained a signicant contribution of magmatic volatiles (Sillitoe et al. 1996). This paper describes the mineralization and alteration preserved on Wetar, and the results of uid inclusion and stable and radiogenic isotope studies. These new data provide a better understanding of the nature and origin of the hydrothermal mineralizing system. Furthermore, as a relatively young system of Miocene age, the Wetar deposits provide an ideal opportunity to link observations from active systems on the ocean oor with a system only recently incorporated into the geological record.

Geological setting Wetar Island forms part of the Inner Banda Arc, an array of active and inactive volcanic islands surrounding the Banda Sea, which are the result of the arc-continent collision of the NNE moving (75 mma1) IndianAustralian plate beneath the Eurasian plate (Audley-Charles 1986; Masson et al. 1991) (Fig. 1). This zone of plate contact lies along the Java Trench to the west and continues into the Timor Trough. Seismic refraction surveys indicate that the TimorTanimbar Trough (1,200 km in length, up to 70 km wide and 23 km deep) is presently underlain by continental lithosphere, varying between 31 km and 40 km in thickness from west to east (Audley-Charles 1986; Masson et al. 1991). The Outer Banda Arc is dominantly non-volcanic in origin, with Timor, to the south of Wetar preserving an accretionary prism and central collision complex, which was accreted onto the front of the Australian continental plate. Richardson and Blundell (1996) proposed that a substantial part of the collision complex consists of a micro-continental fragment that lay some considerable distance to the north of the Australian continental margin, and which collided with the subduction zone at approximately 8 Ma. Seismic velocity and gravity modelling suggests that the collision complex across the Timor prole is 3760 km thick and 135160 km wide (Woodside et al. 1989; Richardson and Blundell 1996). The frontal portion of this collision complex consists of a number of high-angle thrusts imbricated from the subducting Australian continental margin (Hughes et al. 1996) (Fig. 2). Uplift rates in both the accretionary zone and associated islands of the inner volcanic arc are high, with eastern parts of Timor presently situated 3 km above sea level (Snyder et al. 1996). Microfaunal and palaeobathymetry studies, on the islands of Timor, Buru, Seram and Kai, show that continent-arc collision has produced episodic uplift of the outer islands at rates

Fig. 1 Location map of Wetar Island, Indonesia showing principal tectonic and volcanic features of the Banda Arc. After Hamilton (1979), Varekamp et al. (1989), Breen and Silver (1989) and Masson et al. (1991). The Banda Arc is divided into an Outer nonvolcanic and Inner volcanic arc. The extent of the Australian continental crust is shown within the inset

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Fig. 2 Simplied cross-section of the Banda Orogen based on geophysical data from Masson et al. (1991), Richardson and Blundell (1996) and Snyder et al. (1996). Timor was formerly an outlier of Australian continental crust and is now trapped between the Inner Banda Arc and the Australian continental margin. The collision zone is dominated by shallow, southward dipping faults, which have accommodated crustal shortening and thickening within the zone of collision

of between 500 mm ka1 in a million years, to 5,000 mm ka1 in some hundreds of thousands of years (De Smet et al. 1989). These results indicate that uplift rates dier greatly along the arc, with some islands experiencing long episodes of submergence intermittent with rapid pulses of uplift during the PlioceneQuaternary. A complex zone of normal and strike-slip faulting osets the Inner Banda Arc between the islands of Alor and Wetar, to a distance of approximately 50 km (Fig. 1) (Masson et al. 1991). Recent GPS measurements, seismicity data and seismic reection proles suggest that the Wetar Thrust, located at the northern edge of the inactive segment of the Inner volcanic Banda Arc, accommodates the majority of the present day 75 mma1 convergence, between the Australian margin and the Banda Arc (Silver et al. 1983; McCarey 1988; Genrich et al. 1994). This thrust may represent the site of incipient arc reversal, due to the increased diculty in subducting the buoyant Australian continental plate post-arrival of the Australian continental margin with the collision zone at approximately 2.4 Ma (Richardson and Blundell 1996).

Materials and methods

Geological information was obtained from the open-pit mines, outcrops and exploration drill-core. Polished thin sections were examined in both reected and transmitted light. Standard XRD and FTIR methods were employed to characterize alteration mineralogical assemblages on 135 samples. Mineral chemistry was determined by electron microprobe analysis using a Cameca SX50 at the

Natural History Museum, London. Operating conditions were 15 kV (accelerating voltage), 20 nA (beam current) and count time of 20 s. Doubly polished uid inclusion chips were prepared to a thickness of 100 lm. Microthermometric analyses were completed on a Linkam TMS600 stage calibrated against a pure H2OCO2 inclusion at low temperatures, and checked daily against internal standards. Accuracy is estimated at 0.1C for low-temperature phase changes (100C to 0C) with a precision 0.1C and 2C, for homogenization measurements between 100C and 400C, respectively. Suldes were prepared for conventional isotopic analysis at SUERC by standard heavy liquid, magnetic, diamond micro-drilling and hand picking techniques. Barite was prepared by micro-drilling. In both cases, around 510 mg was used for isotopic analysis. Minor contamination by non-S-bearing phases was tolerated, and has no eect on the nal data. Suldes were analyzed by standard techniques (Robinson and Kusakabe, 1975) in which SO2 gas was liberated by combusting the suldes with excess Cu2O at 1,075C, in vacuo. Barite analyses were performed by the technique of Coleman and Moore (1978), in which SO2 gas is liberated by combustion with excess Cu2O and silica, at 1,125C. Liberated gases were analyzed on a VG Isotech SIRA II mass spectrometer, and standard corrections applied to raw d66SO2 values to produce true d34S. The standards employed were the international standards NBS-123 and IAEA-S-3, and the SUERC standard CP-1. These gave d34S values of +17.1, 31 and 4.6&, respectively, with 1r reproducibility better than 0.2&. Data are reported in d34S notation as per mil (&) variations from the Vienna Canon Diablo Troilite (V-CDT) standard. Selected barite concentrates for sulfate oxygen analyses were carefully cleaned by washing in Aqua Regia, and thorough rinsing in deionized water. Oxygen was then extracted following the method of Hall et al. (1991). The evolved CO2 was analyzed on a VG Sira 10 mass spectrometer, with all results reported in standard delta notation as & variations relative to the V-SMOW international standard. Replicate analyses of the NBS-

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Fig. 3 Simplied geological map of Wetar Island, after Nash and Snodin (1992) and Farmer and Cliord (1993). The map shows the principal mineralized areas, structural lineaments, and key geological units

127 BaSO4 standard during these analyses gave +9.60.3&. Sr isotopes were measured at Southampton Oceanography Center on a seven-collector VG Sector 54 mass spectrometer with a separable-lament source. Isotope ratios were determined as the average of >100 ratios by measuring ion intensities in multidynamic collection mode and fractionation corrected by normalization to 86 Sr/88Sr = 0.1194. Measured values for standard NBS SRM-987 were 87Sr/86Sr = 0.710242 13 (2 SD, n=42). Stepped heating Ar/Ar data for biotite grains and illite separates (<2 lm), were analyzed at the University of Manchester, UK with analytical techniques following that of Kendrick et al. (2001). Samples of the syenogranite and dacite were disaggregated by light crushing, and individual biotite grains (25 mm in length) were hand picked and cleaned in deionized water. Due to the ne-grained nature of the illite sample it was expected that there would be signicant recoil loss of 39Ar during irradiation, therefore, this sample was vacuum encapsulated in a quartz vial prior to irradiation. The recoil 39 Ar gas was extracted using an ultra-violet wavelength laser to drill into the tube. The recoil 39Ar amounted to only 5% of the total 39Ar released from the sample and was recombined in the total age calculation. Geology of Wetar Island Wetar Island measures approximately 110 km by 40 km and is composed entirely of Neogene volcanic rocks and minor oceanic sediments (Sewell and Wheatley 1994).

Submarine, basalticandesites, with local pillows, form the volcanic basement to the island (Fig. 3). The basalticandesites are intruded by rhyo-dacite domes (Ruxton 1989) and overlain by dacitic lavas, tus and breccias, debris ows and lahar deposits (Fig. 4). Reef limestones are evident around the perimeter of the island at varying heights. Radiometric dating, largely KAr, of the volcanic assemblages suggests that the basement volcanic rocks, to the south of the island, were extruded around 12 Ma with overlying dacites, diorites and basalticandesites deposited between 7.78 Ma and 3.03 Ma (Abbott and Chamalaun 1981). A Globigerina-bearing limestone outcrops on Wetar Island, which locally overlies basalticandesitic volcanism and mineralization hosted by calc-alkaline andesites to rhyodacitic ows. This limestone yields a biostratigraphic age of between 5.2 Ma and 3.9 Ma (Herrington 1993), and based on the ratio of planktonic:benthic assemblages (Table 1), is likely to have formed in up to 2,000 m of water and possibly deeper (J. Murray, personal communication). Uplift rates for Wetar based on these parameters are 420 570 mm ka1, which are consistent with the lower rates calculated for Timor in the outer arc (De Smet et al. 1989; Audley-Charles 1986b). Based on these uplift rates, the localized areas of mineralization on the Wetar Island edice would have emerged from the Banda Sea between 0.5 Ma and 0.4 Ma. However, the central spine of Wetar (1,500 m, present height) would have emerged around $3 Ma based on the current height dierentials, and likely uplift rates. Subaerial lahars generated along the central spine of Wetar developed into extensive subaqueous debris ows. These units, locally up to 250 m in thickness, covered mineralized areas and inlled topographic depressions. After collision of the Australian margin with the Outer Banda Arc, at approximately 2.4 Ma (Richardson and

80 Fig. 4 Stratigraphic column and summary of tectonic and geochronological data from the Kali Kuning, Lerokis and Meron areas of Wetar Island. Age constraints are: (1) Scotney 2002 (Ar/Ar); (2) Herrington 1993 (K/Ar); (3) Abbott and Chamalaun 1981 (K/Ar); (4) Herrington 1993, a biostratigraphic age for a postmineralization Globigerina bearing limestone from the Kali Kuning deposit. The Zanclian and Messinian aged strata are locally referred to as the mine sequence

Blundell 1996) uplift may have been substantially increased. In particular, the development of the Wetar thrust and subsequent back-arc thrusting may have aided in the rapid exhumation of the Wetar volcanic edice. Geology of the sulde deposits Volcanic and structural setting of the deposits The economic deposits of Kali Kuning and Lerokis zones 4 and 5 are located towards the central and northern part of the island (Fig. 3). These deposits, and the majority of other recognized mineralized zones, which lie within the central part of the island, are bound to the west and east by extensive NWSE and NESW
Table 1 Planktonic and Benthic foraminifera assemblages identied within post-mineralization limestones at Kali Kuning Planktonic assemblage includes Orbulia universa Globigerinoides conglobatus Globigerinoides sacculifer Globorotalia menardiform group Sphaeroidinella dehiscens Benthic assemblage includes Cibicidoides Globocassidulina Favocassidulina Fontbotia Pleurostomella Stilostomella Uvigerina

trending faults. The base of the volcanic stratigraphy comprises ne-grained basalticandesitic ows, which dip around 10 towards 028. Overlying the basal vesicular basalts and basalticandesites is a >450 m thick sequence of altered volcanic rocks, locally termed the mine sequence (Fig. 4). At the base of this sequence green, chloritic altered, vesicular pillow lavas are well preserved. Up section andesitic to rhyodacite ow units and local breccias are preserved, and these are the host rocks to the mineralization. Unconformably overlying this sequence are a series of post-mineralization lahars and debris ows, which appear geomorphologically controlled by the palaeotopography. Local hydrothermally altered dykes cross-cut the mine sequence, with clear evidence of post-mineralization dykes restricted to unaltered EW striking andesitic dykes, which cut lahars and debris ows within coastal exposures. The deposits are discordant to the local stratigraphy and are associated with faults. The Lerokis zone 5 mound developed at the intersection of a northwest and westerly trending structure and the Kali Kuning sulde mound is located along a northwesterly trending fault. Massive suldes Two well-preserved polymetallic sulde mounds at Kali Kuning and Lerokis zone 5 have exposed dimensions of $15010070 m and $1209030 m, respectively (Fig. 5ad). Pre-mining, no sulde mounds were exposed

Planktonic:Benthic ratio = 99:1

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Fig. 5 a View northnorthwest of the Kali Kuning (KK3) deposit. The irregular nature of the sulde mound is clear; pre-mining, the entire mound was covered by baritic ore. Hydrothermal alteration is evident around the deposit, post-mineralization lahars / debrisows are shown. b Exposed sulde mound at Kali Kuning. Height of the sulde mound is approximately 60 m. c Lerokis zone 5 situated at a topographic height of 550 m on a prominent ridge (view approximately north). The host depression for the barite ore deposit is evident. Conformable, post-mineralization volcaniclasticsediment overlies the massive sulphide mound. Pre-mined and remediated zones 1, 2 and 3 are also shown. d Exposed sulde mound at Lerokis zone 5, height of the sulde mound above the pit oor is approximately 15 m. Extensive gossanous material surrounds both deposits

at the surface. In plan, the mounds are broadly arcuate. The sulde mounds are blocky in appearance, with clasts of massive pyrite ranging in diameter from a few centimeter up to boulders some 30 cm across (Fig. 6). Talus and redeposited suldes occur marginal to the mounds where matrix supported angular fragments of massive sulde are held in a ne-grained sulde mud. Minor evidence for seaoor reworking is evident at Lerokis zone 5, where a 30 cm zone of interbedded sulde and volcaniclastic material overlies the mound. Chert, gypsum and globigerina-bearing limestone overlie the Kali Kuning sulde mound. At the margin of the sulde mounds, negrained poorly consolidated granular pyrite marks the contact zone (0.22.5 m) between the sulde mound and the associated barite deposits. The mineralogy of the massive sulde mounds is dominated by pyrite, accounting for >98% of all suldes present with minor amounts of chalcopyrite and sphalerite. Typical of seaoor suldes, the pyrite and chalcopyrite often show porous textures as well as collomorphic growth zones up to 3 mm across (Fig. 7a). The collomorphic pyrite tends to nucleate on and around euhedral pyrite grains (Fig. 7b). This texture appears most frequently at the margins and upper parts of the sulde mounds. Chal-

copyrite frequently rims and locally replaces pyrite (Fig. 7c) and is more apparent at the margins of the sulde mounds and particularly at the base of mounds and in the underlying footwall. Occasional banding of pyrite and chalcopyrite is evident on a centimeter scale. A later fracture network permeates the pyritic mounds, with a sulde assemblage dominated by covellite, Fe-poor sphalerite and lesser amounts of tennantite and tetrahedrite and tabular barite laths (Fig. 7d). Overall, typical sulde abundance within the mounds are pyrite >> chalcopyrite > sphalerite > covellite/marcasite/tennantite/tetrahedrite and bornite. No sulde mound is evident at the Lerokis zone 4 deposit despite drilling beneath the barite mineralization. All three deposits are surrounded by extensive gossanous material.

Fig. 6 Blocky sulde talus at the base of the Lerokis zone 5 sulde mound

82 Fig. 7 Photomicrographs of polished sulde sections: py pyrite; cpy chalcopyrite; sp sphalerite; ba barite; ten tennantite; cov covellite; si silica. ae eld of view = 5 mm, f eld of view = 2.5 mm. a Collomorphic pyrite (sample 097056, Lerokis zone 5) within the massive pyritic sulde mound. b Euhedral pyrite cores overgrown by collomorphic pyrite (sample 097009). c Chalcopyrite replacement of pyrite (sample 097059). d Fracture-ll sulde assemblage (sample 097016). e Disseminated pyrite within an altered volcanic clast in the Lerokis zone 5 footwall, rimmed by pyrite and a fracture-ll assemblage of sphalerite and covellite (sample 097122). f Detail of fracture-ll sulde assemblages in e, showing variation in tennantite composition

Stockwork zones The pyritic mounds at Kali Kuning and Lerokis zone 5 are underlain by stockwork zones which reach to a depth of >210 m below the Lerokis zone 5 deposit and >150 m below Kali Kuning. The stockwork zone is hosted by hydrothermally altered, locally vesicular, silicied volcanic rocks. Brecciated, angular volcanic footwall clasts are rimmed by suldes up to 4 mm in thickness and also contain disseminated suldes (Fig. 7e). The stockwork veins range from <1 mm up to 4 cm in width and contain pyrite, chalcopyrite and sphalerite. Intense vein and disseminated mineralization occurs within an extremely silicied zone immediately beneath the sulde mound at Lerokis zone 5 and appears to be related to a fault intersection. Disseminated pyrite is also abundant in this zone and is generally euhedral to subhedral (usually <1 mm). Gold was observed in association with a zone of intense clay (illite) alteration in the stockwork beneath the Lerokis zone 5 sulde mound (Herrington 1993). A late sphalerite, tennantite and covellite-rich fracture network (Fig. 7e, f) locally permeates the stockwork zone.

Barite deposits The mined gold-rich barite deposits have been termed barite sands by Sewell and Wheatley (1994) and Scotney et al. (1999) due to their unconsolidated friable nature. At Kali Kuning and Lerokis zones 4 and 5 the deposits contain on average $6070% barite, and up to 90% barite where more massive. The barite consists of a friable mass of barite crystals, which shows variable degrees of cementation and colour variation, such that chaotic bedding with evidence of slumping are locally dened. Individual barite crystals typically range in size between 2 mm and 4 mm, up to a maximum of approximately 7 mm in length. Barite crystals typically show euhedral, rectangular, rhombohedral and polyhedral forms (Fig. 8a). Cross-bedding within the barite is reported by Sewell and Wheatley (1994), suggesting the local reworking of barite on the seaoor; however, these features were largely evident pre-mining and within the upper parts of the deposits. At Kali Kuning, barite overlies and locally surrounds the sulde mound. The contact zone between the massive sulde and barite deposit is gradational, with a zone of granular pyrite, clay and barite up to 2 m thick.

83 Fig. 8 a SEM image of rectangular, rhombohedral and polyhedral interlocking barite crystals from the Kali Kuning ore zone (sample 096879). b Relationship of aresendescloizite (ad), arsenbrackebuscite (ab) and mimetite (m) as cementing phases within the Lerokis zone 4 barite ore zone. c Secondary nature of anglesite (an) pseudomorphing galena and cementing barite laths. d Barite lath rimmed by jarosite (ja) and subsequently rimmed / cemented by karibibite (k) and arsenbrackebuscite (ab)

The matrix of the poorly consolidated barite largely comprises collomorphic Fe-oxide, traces of clay material and arsenates (Table 2), with increased cementation towards the footwall contact. Arsendescloizite, arsenbrackebuscite and mimetite are all found intergrown, cementing tabular barite (Fig. 8b). Anglesite is observed pseudomorphing galena and as a cementing phase to tabular laths of barite and brecciated fragments (Fig. 8c). Arsenbrackebuscite occurs as rhombic crystals (<20 lm) showing compositional zoning (Fig. 8b,d), with cores depleted in As and Pb and enriched in Sb and S compared to the margins; this phase also occurs as amorphous cement. Euhedral barite laths are cemented by jarosite and a complex intergrowth of karibibite and arsenbrackebuscite (Fig. 8d). Gold occurs in the baritic ore unit as free grains and in one instance attached to a barite lath (Fig. 9). An association between gold and Feoxides is also noted by Herrington (1993). The Hg bearing phase moschellandsbergite occurs at the stratigraphically highest position of the Kali Kuning barite ore zone near to the overlying chert and limestone cover, whereas, the Ag-bearing mimetite phase along with the majority of the complex arsenates tend to occur at the base of the Lerokis zone 4 barite deposit; which coincides with the highest Au and Ag grades reported towards the base of other ore zones, e.g. Lerokis zone 1 and Kali Kuning (Sewell and Wheatley 1994). Variable amounts of sulde phases, predominantly pyrite and galena are included within the barite laths (see

Table 2 Barite ore cementing and inclusion phases identied at Wetar Island Minerals identied cementing barite Anglesite: PbSO4 Romerite: Fe2+ Fe3+ 2 (SO4)414H2O Silica/Jasper: SiO2 Mimetite: Pb5(AsO4)3Cl Moschellandsbergite: Ag2Hg3 Jarosite: KFe3+ (SO4)2(OH)6 3 Fe-oxides Arsendescloizite: PbZn(OH) (AsO4) Arsenbrackebuscite: Pb2(Fe,Zn) (AsO4)2H2O Karibibite: Fe3+ As3+ O9 2 4 Plumbojarosite: PbFe3+ 6 (SO4)4(OH)12 Perroudite: (Hg5Ag4S5Cl4) Clorargyrite: AgCl Cerussite: PbCO3 Dusserite: BaFe3(AsO4)2 (OH)5H20 Cinnabar: HgS Copiapite: Fe2+ Fe3+ 4 (SO4)6(OH)220H2O 2+ 3+ Romerite: Fe Fe2 (SO4)414H2O Minerals identied included within barite Sphalerite: ZnS Galena: PbS Chalcopyrite: CuFeS2 Argentite: Ag2S Acanthite: Ag2S Pyrite: FeS2 Bournonite: PbCuSbS3 Bornite: Cu5FeS4 Jordanite: Pb14(AsSb)6S23 Boulangerite: Pb5Sb4S11 Geochronite: Pb14(SbAs)6S23 Stibio-Luzonite: Cu3SbS4 Enargite: Cu3AsS4

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Fig. 10 Examples of Fe-oxide barite pipe structures, approximately 1.5 m in height, preserved at the base of the Lerokis zone 4 barite ore deposit

Fig. 9 Anhedral, <20 lm gold grains adhering to barite laths

major components of the systems: stockwork zone, sulde mounds and barite deposits (Fig. 11). Stage I Pyrite (+ chalcopyrite + sphalerite + marcasite). Forming the massive sulde mounds, and associated stockworks. Stage Ia Barite as poorly consolidated barite ore deposits, typically with inclusions of mound suldes, anking the massive sulde mounds. Gold is evidently associated with barite precipitation. Notably, sulde inclusions in the proposed feeder structures to the barite deposits only contain inclusions of suldes typically reported for the massive sulde event, e.g. pyrite, sphalerite, chalcopyrite, with no evidence of sulfosalts as inclusions. Stage II Multiple fracture events reactivate the stockwork zone and the sulde mounds. These veins show chalcopyrite/sphalerite intergrowth, Fe-poor sphalerite, Zn-poor tennantite, Zn-rich tennantite tetrahedrite, covellite, bornite, digenite and barite. Tabular barite laths up to 7 mm long are associated with this event. Stage III Late barite veins with individual crystals up to 5 cm developed both proximal and distal to mineralization and coating external faces of the sulde mounds. Stage IV Cementation of the barite deposit by oxides, arsenates and sulfates other than barite (see Table 2) and partly through the local oxidation of suldes. The relationship of this event to stage III is uncertain. Alteration Intense zones of alteration are present within the footwall to Kali Kuning, and Lerokis zones 4 and 5. At the Kali Kuning orebody, the immediate footwall to the sulde mound and barite mineralization exhibits intense silicication, including microcrystalline silica and cristobalite,

Table 2). Included phases range from euhedral to anhedral in form and the size of inclusions are generally <50 lm in diameter. Signicantly more suldes are included within barite laths from the barite orebodies compared to barite inclusions from within the sulde mound and stockwork structures. Barite also occurs as disseminated laths within stockwork zones (up to 1 cm), as vug ll within sulde mounds, associated with the fracture-ll sulde assemblage and as coatings on external sulde mound faces. Vein barite occurs both proximal and distal to mineralization with individual crystals up to 5 cm in long dimension. Iron oxidebarite pipe structures Distinct iron oxidebarite structures are preserved at Kali Kuning and Lerokis zones 4 and 5. These structures are pipe-like in appearance and, at Lerokis zone 4 (Fig. 10), are 11.5 m high and $1.5 m in diameter and are located towards the base and central part of the mined barite deposit. At Lerokis zone 5 two irregular structures (1 m 12 m) are present (Fig. 5d) and at Kali Kuning two iron oxidebarite pipe features are observed, one at the base of the mined barite ore zone, the other directly underlying the chert and limestone cover rocks. All these structures comprise abundant anastomosing layers of barite separated by layers of iron oxides, (goethite and limonite). Locally, incorporated clasts of vesicular and highly altered volcanic rocks are noted, which were probably derived from the volcanic footwall. Mineral paragenesis The mineralization on Wetar can be subdivided into paragenetic stages based on observations from the three

85 Fig. 11 Paragenetic sequence for the mineralization events at the Wetar Island ore deposits

and a clay alteration assemblage of illite, pyrophyllite, kaolinite and minor alunite. This alteration gives way laterally and vertically to an illitesmectite assemblage, which passes outwards to zones of chloritic alteration (Fig. 12a). At Lerokis zone 5, a similar zonation is observed, with the most intense alteration associated with the stockwork that underlies the sulde mound. Beneath the massive sulde mound is a $25 m thick zone of

Fig. 12 a Illitesmectite and chloritic alteration zonation around the Kali Kuning ore following removal of the barite. b Zoned alteration sequence around the Lerokis zone 4 orebody, major phases are shown determined by XRD, FTIR and initially by PIMA: qtz microcrystalline quartz; ill illite; ja jarosite; goe goetite; chl chlorite; sm smectite; kao kaolinite; al alunite. The rivers S. Koreng, S. Kelapa Tiga and the mine road are shown. Located at the centre of the ore zone are the Fe oxide/barite pipe structures. c

silicication, microcrystalline silica, and extensive argillic alteration, illite, pyrophyllite and kaolinite. Beneath this zone the predominant alteration is chloritic. At Lerokis zone 4 (Fig. 12b), which lacks an exposed sulde body, the immediate footwall to the barite deposit is a zone of quartzillite rich alteration and microcrystalline silica. Residual silica and local jarosite veins are observed (Fig. 12c, d). This alteration passes outwards into a zone of quartzillite, illitesmectite and nally chloritic alteration. Intense silicication is observed within the footwall adjacent to all the barite deposits. More peripheral footwall zones to the barite deposits show predominantly chloritic alteration, which is well exposed in road cuts away from the mineralization. The alteration around the Wetar mineralization is thus extensive, intensive and zoned. The dominant alteration assemblages comprise silicication proximal to mineralization, moving outwards and downwards to

86

illitesmectite and nally to distal chlorite. Although spatially restricted, the presence of pyrophyllite, kaolinite and local alunite suggest that low pH uids at moderate temperatures have contributed to the alteration in the immediate footwall to the sulde mounds and the barite ore deposits (Reyes 1990).

erite. Bournonite and jordanite are common as tiny inclusions in larger barite laths. Minor suldes Covellite and digenite are common in the stage II veins and bornite plus argentite are common inclusion phases in barite laths. The covellite from stage II cross-cutting veins in the sulde mound and stockworks contain between 0.2 wt% and 1.3 wt% arsenic. Barite Barite appears as a ubiquitous phase throughout the main sulde mound, sulde talus breccias, barite ores, stage II stockwork veins and stage III veins. The mineral chemistry of the barites is variable with both Sr-poor and Sr-enriched types present in samples from the stockwork and the ore. Barite cementing phases The phases cementing the barite ores are largely iron oxides, hydroxides, complex arsenates and sulfate phases, many of which are amorphous. Distinct phases analyzed include mimetite, arsenbrackebuscite, arsendescloizite, anglesite and moschellandsbergite. Mimetite contains signicant silver, along with the minor argentite as inclusions in barite, and was probably the source for the silver recovered in the vat-leach processing of the barite ore. Along with cinnabar, metacinnabarite, perroudite and tiemannite (De Roever 1991), moschellandsbergite is a major host for mercury in the barite ore, the presence of which was discovered during early gold production at Wetar and subsequently recovered during processing (Sewell and Wheatley 1994). Fluid inclusion studies A representative suite of barite samples, encompassing all stages of ore paragenesis, were analyzed using microthermometric techniques. These included samples from the stockwork zone, barite ore, late vein barite and iron oxidebarite feeder structures to the barite ore. The majority of analyzed samples (7 of 11) were collected from the Lerokis zone 5 deposit. Optical examination indicates that >95% of all barite hosted inclusions are associated with secondary and pseudo-secondary inclusion trails (Fig. 14a), approximately 5% appear primary. The solitary bi-phase primary inclusions are two phase (L + V) and range in size from 12 lm to 25 lm; these are described type 1A. Type 1B are also two-phase liquid plus small amounts of vapour inclusions (L + V), which occur as pseudo-secondary and secondary trails. Recognition of a few mono-phase (L) inclusions (by rst and nal ice-melt phase changes) are described as Type 2.

Mineral identication Pyrite Pyrite is ubiquitous in all associations except barite ores and the associated pipe structures where iron is generally present as oxides. Stage I pyrite, forms the bulk of the sulde mound contains a distinct arsenian pyrite. This pyrite often shows complex grains or collomorphic banded zones (Fig. 13a, b) and may contain up to 6.7 wt% As (Table 3). The arsenian cores to complex grains often contain idiomorphic inclusions of barite. Overgrowth pyrite is characteristic of the later part of stage I, immediately pre-dating or coincident with main stage chalcopyrite. This later pyrite (stage Ia) is characteristically arsenic-poor. Chalcopyrite Chalcopyrite is associated with the overgrowth pyrite and locally replaces the earlier stage I pyrite. Compositional variation in the chalcopyrite is negligible with respect to paragenetic association. Chalcopyrite often occurs intergrown with later stage II barite. Sphalerite Sphalerite is associated with the chalcopyrite and as a later phase with sulfosalts and late barite. Earlier chalcopyrite-associated sphalerite is generally opaque to translucent in thin section, reecting an elevated iron content of up to 6 wt% Fe. Later sulfosalt-associated sphalerite (stage II) is generally iron-poor, often less than 0.1 wt% Fe (Table 3). Sulfosalts Tennantite is a minor accessory of the chalcopyrite sphalerite stage of mineralization and is more abundant in stage II cross-cutting veins containing covellite, digenite, bornite and barite. In the earlier stage (chalcopyrite + sphalerite, Fig. 7d), the tennantite is generally zinc-poor with between 0 wt% Zn and 1 wt% Zn, $31 wt% S, $17 wt% As and 0.13.9 wt% Sb. In the later association (+covellite), both zinc-poor and zincian tennantite are found (Fig. 7f). Zn-rich tennantite contains up to 8.3 wt% Zn, $27 wt% S and $19 wt% As and between 0.4 wt% and 6.5 wt% Sb. Zincian tetrahedrite is often seen as inclusions in Fe-poor sphal-

87

Fig. 13 Back-scattered electron microphotographs of As zonation within massive pyrite samples from the Lerokis zone 5 sulde mound. Point locations correspond to the microprobe traverse, the graphs illustrate the variation of As along each sample, a sample 097009; b sample 099903

Inclusions are concentrated towards crystal margins particularly in stockwork associated samples (Fig. 14b). Microthermometry results For all Type 1 uid inclusions, the degree of ll (F) ranges from 0.6 to 0.95, typically around 0.90.95, no daughter phases are observed and many inclusions show evidence of decrepitation or leakage (Fig. 15a). Homogenization of inclusions (Th) is consistently L + V to L and occurs between 144C and 314C with a mode of 238C (n=206) (Table 4, Fig. 15b). First icemelt temperatures (Tfm) occur between 20C and 24.4C (n=35), with nal ice melting (TMice) between 0.9C and 3.1C (mode 1.6); corresponding to salinities of 1.65.1 wt% equivalent NaCl (Bodnar, 1993) (Fig. 15c and d). This suggests that salinities span the salinity of seawater ($3.2 wt% equivalent NaCl). Although the petrographic data allows the inclusions to be subdivided into Type 1A, 1B and Type 2 inclusions, they show similar Th and salinity ranges

throughout the paragenesis, which suggest no signicant evolution of the hydrothermal uid throughout the barite crystallization and that a single-phase uid was responsible for the precipitation of barite within the system. However, the variable salinities above and below that of seawater suggest that super-critical phase separation may have occurred deeper in the system (Delaney and Cosens 1982; Bischo and Pitzer 1985). The Globigerina-bearing limestone caps the mineralization at Kali Kuning and preserves fauna, including Favocassidulina, and benthic:planktonic foraminifera ratios, which suggest deposition occurred at least 2,000 m below sea-level and possibly considerably deeper (J. Murray, personal communication). These results contradict those of Sewell and Wheatley (1994), who suggested that the mineralization occurred in water depths of <600 m. Based on a minimum depth estimate of 2,250 m and a maximum estimate of 3,000 m, the conning pressure equates to a homogenization temperature correction of +23C and +40C (Bodnar and Vityk 1994). If the maximum correction is applied, the Wetar Island average trapping temperature will be 275C. The uid inclusion data suggest that the hydrothermal uids responsible for the barite deposition throughout the Wetar hydrothermal systems were similar in salinity and temperature to those currently venting as white smoker uids on active vent sites at mid-ocean ridges (Rona et al. 1993).

88 Table 3 Representative analysis of Wetar Island mineral phases from the Kali Kuning and Lerokis orebodies, Indonesia Stage py I py Ia ten Ia bor Ia sph Ia sph II tet II ten II bour ga Ia Ia cpy Ia arg Ia jor Ia py Ia Mim ars IV IV Cementing phases 2.09 0.20 0.65 0.46 0.25 14.02 0.13 0.07 22.60 30.67 0.03 0.02 0.79 0.15 73.05 50.65 0.09 0.04 0.04 0.00 0.15 0.33 99.85 96.60

Sulde phases S Ag As Ba Cd Cu Fe Hg Pb Sb Se Zn Total Wt% 48.01 6.71 0.03 44.37 0.04 0.04 99.20 52.60 0.19 0.19 0.20 46.48 0.38 100.04 31.23 0.05 15.91 0.07 45.80 0.04 3.95 0.13 0.16 97.34 30.46 0.10 0.46 62.21 7.15 0.03 0.03 100.43 32.61 0.12 0.23 6.12 0.06 0.03 0.03 58.28 97.48 32.29 0.07 0.48 1.56 0.10 0.19 0.04 64.98 99.71 25.16 0.01 7.02 38.56 2.20 19.87 0.05 5.22 98.07 26.56 17.79 41.24 0.11 3.10 0.06 8.30 97.16

Sulde inclusion phases within barite 19.36 0.06 1.83 0.16 12.78 0.05 41.08 22.57 0.03 97.92 13.74 0.26 0.07 0.79 0.02 84.37 1.31 0.01 0.16 100.73 34.32 0.10 0.87 34.62 29.07 0.14 0.12 0.07 99.30 12.00 80.34 0.06 2.63 0.06 1.26 0.65 1.20 0.01 98.21 17.94 11.12 0.42 0.03 69.48 0.64 0.05 99.68 51.64 0.02 1.42 0.67 0.23 44.86 0.04 0.04 0.18 99.08 Cl SO2 FeO ZnO As2O5 SeO2 Ag2O PbO Sb2O3 BaO HgO Bi2O3 Total compound%

Sulde phases (wt %): py pyrite; sph sphalerite; tet tetrahedrite; ten tennantite; bour bournonite; ga galena; cpy chalcopyrite; arg argentite; jor jordanite; bor bornite Cementing phases (compound %): mim mimetite; ars arsendescloizite

Stable isotopes d34S d34S analyses of 56 samples, comprising 29 suldes, 25 sulphates, 1 gypsum and 1 native sulfur from the deposits of Kali Kuning, and Lerokis zones 4 and 5, signicantly expand on earlier data and ranges reported by de Ronde (1995). Suldes were collected from all stages of mineral paragenesis and sulfates were recovered from barite bodies, within the mound suldes and from stockwork zones (Table 4).

Suldes The d34S values of pyrite within the massive suldes range from 6.2& to 11.7&, stockwork suldes range between 3.3& and 9.8& (Fig. 16 and Table 4). The poorly consolidated granular pyrite from the margins of the mounds, show a similar range of d34S to the massive suldes of between 8.5& and 11.7&. No signicant variations are observed for the dierent sulde phases, sphalerite, chalcopyrite and a mixture of sphalerite, tennantite and covellite. The similarity of the sulde data from both the underlying stockwork and sulde

Fig. 14 ab Photomicrographs of barite hosted uid inclusions from Wetar Island. a Pseudosecondary and secondary trails in samples 097084, decrepitated inclusions are also evident (d). b Abundant 2 phase inclusions in sample 097106, a pronounced reduction in number of inclusions is evident toward the crystal core

89

mounds suggests a common source of sulfur at each deposit. The mean value of d34S for this study is 8&, close to d34S values of +5 and +7& reported for Indonesian arc lavas by De Hoog et al. (2001). It is suggested that arc-related lavas are enriched in d34S as a result of the signicant incorporation of reduced seawater sulfate during petrogenesis. In general, disseminated sulde in the stockwork system has a similar range of d34S to the mineralization (mound and vein stockwork, Table 4). This consistency of d34S suggests a genetic correlation between the volcanic sulde and mineralization. Anomalously heavy d34S is a common occurrence in these settings (e.g. Arribas 1995). Sulfates The d34S of sulfates recovered from the Barite deposits of Wetar varies between 22.4& and 26.9&, with the heaviest d34S values, up to 31&, recorded from the stage III barite veins distal to the ore deposits (Fig. 16). Ohmoto et al. (1983) reported similar d34S barite values from Kuroko deposits, whereas, Goodfellow and Franklin (1993) report barite d34S values from the Bent Hill system, which are considerably less than seawater, by as much as 10&. The Wetar sulfate data reect or are heavier than the predicted Miocene seawater sulfate value of d34S 22& (Claypool et al. 1980). Ohmoto et al. (1983) suggested that mixtures of seawater sulfate and hydrothermal uid sulfate, with equilibrium d34S values of between 29& and 34& between 280C and 200C, could account for the values observed in Kuroko systems. However, only limited mixing of seawater and hydrothermal uid would return the d34S sulfate values to seawater, as modern vent uids contain extremely low levels of dissolved sulfate (Scott 1997). Chiba et al. (1998) suggested that increases in d34S observed for anhydrite in the TAG mound is due to the partial reduction of seawater sulfate by ferrous iron in the hydrothermal uid. Given that the formation of barite requires the mixing of seawater and hydrothermal uid a similar interpretation is favored. The heaviest d34S sulfate values are reported from the distal stage III barite veins and suggest that seawater and hydrothermal uid mixtures are subject to closed system reduction, highlighted by the peripheral vein at +31& (Table 4, sample 099938). Notably, coexisting pyrite and barite pairs commonly give unrealistic isotope equilibrium temperatures (usually higher), which corroborates our observations that the pyrite and barite is seldom co-precipitated. Goodfellow and Franklin (1993) account for the relatively light d34S data at Bent Hill, by the mixing of barium in vent uids with sulfate formed by the oxidation of pre-existing suldes, or H2S from the hydrothermal uid, either within chimney structures or in the underlying sulde mound. There is no evidence for this at Wetar. However, the gypsum and native sulfur d34S

Fig. 15 Fluid inclusion microthermometric data from Wetar Island barite samples

Table 4 Isotopic and microthermometric data obtained for the Wetar samples d18O (SMOW) 2 SE Range n 16 22.122.8 4 15 2.53.8 22.5 1.42.3 1.9 n n KK KK 0.70764 7 196262 235 Av Range Av Range Av Th (C) TFm (C) Tmice (C) NaCl (wt%) Description
87

90

Sample

Material analyzed

d34S (CDT)

Sr/86Sr

Location

111943

Barite

22.78

100134

Barite

24

096877 096878 096879 096889 100133 100103 10.9 13.3 0.70909 7 0.70773 7 209289 242 21 2122.5 4 17 21.9 11.9 1.6 1.73.2

Barite Barite Barite Barite Barite Gypsum

24.23 26.98 23.65 22.39 9.1 12.8

KK KK KK KK KK KK KK KK KK KK KK KK KK KK KK KK KK

096890 096858 096879 111943 111943 100134 096857 097228 111942 100144

Pyrite Pyrite Pyrite Pyrite Chalcopyrite Pyrite Pyrite Pyrite Pyrite Native sulfur

11.55 8.55 8.44 9.52 10.25 11.69 10.37 10.78 8.47 15.8

097333 6.5 7.7 8.7/9.4 8 8 7 8 8 8 8 8 217302 255 24 2021.8 199269 144212 233 194 18 15 183237 220 15 189267 197309 228 240 17 20 20.421.8 2224.4 8.4 6.8 11.3 10.5 7.8 7.7 0.70807 0.7083 0.7088 0.70836 0.70786 0.70829 0.70827 0.70774 0.70801

Pyrite

9.89 21.1 23 21.1 2.6 22.7 1 1 3 1 11 1.12.1 0.92.4 1.62.6 1.21.8 1.42.7 1.6 1.6 2.2 1.6 2.2 6 16 12 17 22 1.93.6 1.64.1 2.84.3 2.13 2.54.5

111979 111931 096948

Barite Barite Barite

25.18 26.3 24.6

L4 L4 L4 L5 L5 L5 L5 L5 20.7 5 1.83.1 2.1 17 2.55.1 L5 L5 L5

099917

Barite

24.2

099939 099938

Barite Barite

23.9 31

099933

Barite

27.8

099923

Barite

24.5

097106

Barite

27.5

097106

Pyrite

3.33

097104

Sphalerite

6.1

Barite asso. with suldes Barite asso. with suldes Barite ore Barite ore Barite ore Barite ore Barite ore Post-mineralization cover Granular pyrite Granular pyrite Sulde mound Sulde mound Sulde mound Sulde mound Sulde mound Sulde mound Sulde mound Vein from the footwall Vein/disseminated pyrite Barite ore Barite ore Baritic feeder structure Barite asso. with suldes Barite ore Barite vein, distal to sulde mound Barite vein, proximal to sulde mound Baritic feeder structure Disseminated stockwork barite Disseminated stockwork suldes Disseminated stockwork suldes

097098 L5 L5 L5 L5 L5 L5 L5 L5 L5 14 1.73.6 L5 L5 L5 L5 L5

Pyrite

6.7

L5

111997

Pyrite

7.25

099902 099917 097219 8.6 5.8 11.3 0.70873 210288 245 18 1.62.4 11 2.1 2.84.1 0.70809 8 0.70836 186314 269 20 22.122.5 4 16 3.24.1 22.4 1.92.8 2.2

Pyrite Pyrite Pyrite

6.92 6.26 8.4

097122

Barite

28.1

097059

Barite

22.7

097024

Barite

24.6

097023 8.9 8.6 0.70854 8 187286 230 22 21.4 1 12.1 1.8 0.70836

Barite

24.43

097098

Barite

25.04

097084

Barite

27.02

097084

Pyrite

9.03

097084

Sphalerite

4.26

097122 097122

Pyrite Cov-spha-ten

8.02 6.91

097041 097024 097059 097059 097023 097009 096920 0.70773 0.70773 0.70775 0.70834 21 17 18 17

Pyrite Pyrite Pyrite Chalcopyrite Pyrite Pyrite Whole-rock

6.56 8.57 8.01 7.44 7.52 7.4

L5 L5 L5 L5 L5 L5 KK

096921

Whole-rock

096922

Whole-rock

096884

Whole-rock

Disseminated stockwork suldes Pyrite vein, distal to sulde mound Sulde mound Sulde mound Vein/disseminated pyrite Barite asso. with cov-spha-ten Barite asso. with suldes Barite asso. with suldes Barite asso. with suldes Disseminated stockwork barite Disseminated stockwork barite Disseminated stockwork suldes Disseminated stockwork suldes Stockwork suldes Cov-spha-ten stockwork suldes Stockwork suldes Stockwork suldes Sulde Mound Sulde mound Sulde mound Sulde mound Coastal basalt sample Coastal basalt sample Coastal basalt sample Altered volcanic rock

91

92 Location Meron Meron L4 Meron KK

Altered post-mineralization dacite Post-mineralization dacite Altered volcanic rock Brecciated stockwork volcanic Altered, vesicular footwall volcanic Altered volcanic rock Syeno-granite Basalticandesite Basalticandesite

KK L5

KK

values, suggest oxidation of excess H2S in the hydrothermal uid and local oxidation of suldes may be important in their formation. d18O The sulfate oxygen data vary between d18O of 5.8& and 11.3& (Table 4), with a mode at 9&. As the barite d18O data are shifted to values both higher and lower than the composition of seawater, the sulfate oxygen data suggests isotopic exchange has occurred. Nevertheless, the d18O mode of 9& coincides with the d18O value of seawater sulfate and suggests that the bulk of barite precipitated in equilibrium with seawater. The d34S and d18O stable isotope data suggest the predominant source of sulfur in the suldes was derived from the volcanic rocks in the basement, with the sulfur in the sulfate largely derived from seawater and rearms the importance of hydrothermal uid and seawater mixing in the formation of VMS systems (Teagle et al. 1998a, 1998b; Roberts et al. 2003).
87

NaCl (wt%) Tmice (C) Av n

Description

KK Kali Kuning; L4 Lerokis Zone 4; L5 Lerokis Zone 5; cov-spha-ten covellite, sphalerite, tennantite composite sample

Range

Sr/86Sr

Whole-rock 87Sr/86Sr analyses were completed on variably altered host volcanic rocks, and barite separates from the massive barite bodies, fractures within the sulde mounds and iron oxide-barite pipe structures. The barite data range between 87Sr/86Sr 0.7076 and 0.7088 with no systematic variation according to setting (Fig. 17). The 87Sr/86Sr ratios of the barites are considered to reect mixtures between Miocene seawater (87Sr/86Sr 0.70849, Farrell et al. (1978)) and hydrothermal uid. However, the majority of the data plot close to the value of Miocene seawater suggesting a signicant contribution of seawater to the barite formation. Notably, one analysis shows a 87Sr/86Sr ratio of 0.70644 (Herrington 1996), from the stockwork of an undeveloped mineral prospect, Batu Kapal (Fig. 3). This value suggests that locally the hydothermal end member value may be less than 0.70644, and also indicates that less radiogenic basement may be involved in the source of Sr to this hydrothermal uid. The whole-rock data of variably altered basement show 87Sr/86Sr values between 0.7074 and 0.7116. These values are typically more radiogenic than MORB, and are consistent with data reported from surrounding islands (Whitford et al. 1977; Margaritz et al. 1978; Varekamp et al. 1989; Vroon et al. 1993, 2001). The more radiogenic values of 0.71165 and 0.71106, from dacitic ows, suggest a signicant contribution of continental crust and or sediment in the generation of these post-mineralization magmas (Vroon et al. 2001; Elburg et al. 2002). Values of up to 0.72227 are reported by McCulloch et al. (1982), however, the nature of these samples is uncertain. The unaltered volcanic samples tend to show 87Sr/86Sr ratios between 0.70748 and 0.70781 and Sr values

TFm (C) Th (C) 2 SE

Range 20

Av

Range

Av

12

17 7

Sr/86Sr

0.71166

0.71107

0.70747 0.70772

0.70789 Whole-rock 100129

d34S (CDT)

d18O (SMOW)

87

Whole-rock

Whole-rock

Whole-rock Whole-rock

Table 4 (Contd.)

Sample

Material analyzed

096168

096167

111914 097106

111935 111999 111994 096926

Whole-rock Whole-rock Whole-rock Whole-rock

0.70819 0.70803 0.70781 0.70748

23 21 7 9

93

Fig. 16 Comparison of sulfur isotope data from the Kali Kuning, Lerokis zone 4 and 5 sulde barite deposits

>160 ppm (160388); which are substantially changed during alteration. The progressively altered samples show a signicant decrease in whole-rock Sr concentration to <60 ppm with a concomitant increase in the 87 Sr/86Sr value from 0.70746 to 0.70833. The most highly altered samples show Sr concentrations and 87Sr/86Sr signatures that suggest that the samples have undergone complete isotopic exchange with seawater (Fig. 18). ArAr age determinations Three samples were chosen for ArAr age determination in order to better constrain the age of mineralization and
Fig. 17 Histogram summarizing the range in 87Sr/86Sr for Wetar Island sulfate and whole rock data. Data from Herrington (1996) is included. s syeno-granite; d dacite

volcanic events of the area. Samples of the following intrusive and volcanic rocks were analyzed: (1) a syeno grantite intrusion (sample no. 111999) collected from the Kali Lurang river in the Meron area; (2) a post-mineralization capping dacite ow (sample no. 097167) from Meron; and (3) a ne-grained illite (sample no. 056896, <2 lm size fraction) collected from the hydrothermally altered footwall volcanic rocks at Lerokis at a depth of 26 m below the mineralization. Herrington (1993) reported a K/Ar age of 4.70.16 Ma for the illite sample. ArAr data are given in Table 5 and shown as apparent age spectrum diagrams in Fig. 19. Errors are quoted at the one standard deviation level and include the uncertainty in monitor age (Hb3gr 107211 Ma). An isotope correlation diagram of 39Ar/40Ar versus 36 Ar/40Ar (not shown) reveals that the trapped 40 Ar/36Ar ratios are lower than the present day atmospheric ratio (295.5) constrained most precisely by the syenogranite sample to be 2843. Previously, Nagy et al. (1999) determined similar anomalously low

94 Fig. 18 87Sr/86Sr v ppm Sr from variably altered Wetar volcanic rocks. Increased alteration coincides with lower ppm Sr and more radiogenic 87 Sr/86Sr ratios, reecting increased interaction with Miocene seawater. The syenogranite and post-mineralization dacites are omitted from this gure

40

Ar/36Ar ratios from dacite ows and attributed them to either a minor contaminant at m/z 36 in the mass spectrometer, or fractionated atmospheric argon within the samples. The age obtained from the illite sample of 4.930.21 Ma is within error of the K/Ar age of the same sample (4.70.16 Ma) reported by Herrington (1993). The age of the syenogranite intrusion and dacite ow are 4.730.16 Ma and 2.390.14 Ma, respectively (Fig. 19). The age data indicates that the spatially related syenogranite intrusion (proximal to the Meron prospect) and the mineralization are the same age and therefore implies that this intrusive event supplied heat to the hydrothermal system. The ArAr age of the illite is within error of the previously published conventional KAr age (Herrington 1993) and indicates mineralization of the Lerokis deposit occurred between 4.7 Ma and 4.9 Ma. The age of the post-mineralization dacite ow indicates that volcanism continued at least as recently as 2.4 Ma, which is the proposed age for the collision and accretion of the Australian continental margin with the Outer Banda Arc in the region of Timor (Richardson and Blundell 1996). The sample may record a period of extension within the Inner Banda Arc as a direct result of compressional tectonics to the south in the Outer Arc. The age of the dacite ow also indicates that the debris ow that overlies the Meron deposit also occurred post2.4 Ma. This new age data coupled with the Sr data conrms an increasingly contaminated source region under Wetar Island, progressively modied by subducted continental material (SCM) related to tectonic events further to the south.

Evolution of the hydrothermal system The data collected suggest that the Wetar massive sulde and barite deposits were formed on the anks of a volcanic edice during the development of the Inner Banda Arc. Observations of the volcanic stratigraphy and tectonics suggest the Wetar edice initially formed around 12 Ma due to extensive rifting and associated volcanism within oceanic crust. The mineralization is associated with bimodal volcanism, on a basement of basalts and basalticandesite, which most likely formed around 5 Ma, given the dates of the overlying mine sequence. The major sulde mounds show talus textures and are localized on faults, which provide the main pathway for high temperature hydrothermal uids and the development of associated stockworks (Fig. 20a). Within the massive sulde mound much of the pyrite is arsenian (up to 6.7 wt%), and given the established relationship between arsenic and gold content of pyrite (Cook and Chryssoulis 1990; Cline 2001; Pals et al. 2003) may represent an initial reservoir for Au subsequently remobilized by later hydrothermal uids responsible for the baritegold ore. The pyrite d34S data suggest that the sulfur is sourced from basement arc volcanic rocks, modied by a subduction zone component, which is also suggested by the whole rock 87Sr/86Sr data. The slightly elevated d34S values, compared to arc values, indicates a component of reduced seawater sulfate during pyrite precipitation. The hydrothermal uids responsible for sulde precipitation produce a well zoned, intensive alteration sequence (Fig. 12b) with illitesmectite centered on the mineralization and chlorite alteration dee-

Table 5 Stepped heating Ar/Ar data for biotite grains and illite separates (<2 lm), Wetar Island, Indonesia. Amounts of Cl and K obtained from measured 38ArCl and 39ArK using the Hb3 gr monitor and the parameters of a = 0.5420.01, b = 4.370.03 and J = 0.0170930.000026 Sample No. 111999 097167 056896 Location Meron area Meron Lerokis Sample type Biotite Biotite Illite Weight (mg) 12 11 9.1 Cl (ppm) 2,2886 9,4047.1 13.880.90 K (Wt%) 7.350.01 8.730.01 7.900.01
40

Ar*106 cc/g

Age (Ma) 4.730.16 2.390.14 4.930.21

1.350.4 0.751.2 1.380.05

95

Fig. 19 Age versus cumulative 39Ar released during stepped heating for the Wetar Island samples

per and distal to the ore zones. The heat source driving the hydrothermal convection is most likely intrusive syenogranite bodies at depth, which from Ar/Ar dating are known to be coeval with mineralization. Following massive sulde development, barium rich uids are discharged as white smokers, from the hydrothermal system and in particular at the margins of the sulde mound (Fig. 20b). The distribution of barite suggests these uids exploit many of the fracture systems previously employed to develop the massive sulde mound. For example, barite inltrates the base of the sulde mound and lls any voids and fractures present. The d34S barite data suggest that the sulfate in the barite is predominantly seawater derived, whereas, the barium is most likely derived from the destruction of feldspars, within the andesites and felsic volcanic rocks of the basement. Fluid inclusion data show that the hydrothermal uids were at around 250270C, with no evidence of boiling. However, the salinities are greater and less than seawater, suggesting super-critical phase separation may have taken place, prior to egress on the seaoor. The form, location, isotope and uid inclusion data of the iron oxidebarite structures, strongly suggest

Fig. 20 Schematic evolution of the Wetar deposits: a T1, the Wetar deposits initiated as typical volcanogenic massive suldes with a zoned footwall alteration predominantly propylitic to argillic in character (Kuroko like). b T2, the barite deposits originate as a peripheral vent system, with uids circulating through the sulde mound and undergoing signicant mixing of seawater. As the system evolves conductively cooled hydrothermal uids circulate beneath the massive sulde mound generating the alteration and reecting the passage of more oxidized and acidic uids. This results in the argillic to advanced argillic alteration observed. This is also the major Au-precipitation phase. c T3, the sulde and barite system is preserved beneath limestones and lahars, prior to exhumation from the ocean oor, due to continued collision of the Australian continental margin and the Outer Banda Arc

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they are the palaeouid conduits for the barite deposits. Gold is signicantly enriched in the barite mineralization and is closely related to its formation and the most intense phases of alteration. The presence of high levels of arsenic in the barite ore matrix suggest that zone rening of the initial arsenian pyrite may be important. It is questionable whether black smoker mineralization was still occurring at this time. The limited nature of the covellite dominated assemblage, and accompanying d34S, d18O data, suggest that no signicant contribution of magmatic volatiles was involved in the formation of the Wetar orebodies. For example, no isotopically light d34S values were observed for suldes or sulfates compared to Hine Hina or Conical Sea-Mount (Herzig et al. 1998) at least no contribution that could be detected beyond the copious amounts of seawater that must have circulated in the system. There is no compelling evidence that the uids responsible for mineralization boiled at the sites of deposition, however, they may have been subject to supercritical phase separation, which is becoming an increasingly recognized phenomenon in modern vent systems. The sulde and barite orebodies are preserved on the seaoor by the subsequent precipitation of chert, gypsum and limestone and, perhaps most signicantly, by the accumulation of lahars and debris ows (Fig. 20c). A dacite ow, within the lahars and debris ows gives an age of 2.4 Ma and records continued volcanism on the Wetar edice post-3 Ma.

Gold is commonly associated with low-T uids in modern hydrothermal systems. High concentrations of gold are reported in low-T ZnBaSiO2 precipitates (Hannington et al. 1986; Hannington and Scott 1988; 1989). In the Zn-rich chimneys of Snake Pit, Cd, Pb, Sb, Ag and Au are considered to have directly precipitated in the Zn-suldes, with the highest Au contents (>500 ppb) observed in the Zn-rich chimneys and massive Zn-rich suldes at the surface of the deposit (Foquet et al. 1993). At the JADE hydrothermal eld, Au enrichment correlates well with the barite content of the samples, with minute rounded Au grains observed between barite crystals (Halbach et al. 1989, 1993). The Au-rich samples also showed higher concentrations of As, Ba, Sb, SiO2 and Ag, similar to Wetar. The similarity between the Wetar gold mineralization and observations from active white smoker systems is striking, suggesting there was a signicant role for such uids in the origin of the mineralization.

Au-rich volcanogenic massive suldes and Wetar The mineralogy of the ore deposits at Wetar is highly analogous to that reported from back-arc spreading centers, e.g, Lau Basin, where visible gold was rst documented in a white smoker chimney (Herzig et al.1993). In particular, the mineralogy and precious metal content of the Wetar deposits are strongly comparable to hydrothermal vent elds developed on island-arc or continental crust, e.g. Okinawa Trough (Halbach et al. 1989, 1993). The importance of the Aucomposition of the igneous basement in the generation of Au-rich VMS is debated. Herzig and Hannington (1993) suggest that back-arc lavas are not signicantly enriched in gold compared to MORB, and that a goldenriched source is not a prerequisite to the development of gold-rich VMS systems. However, Moss et al. (2001) investigating the Manus Basin, suggest that the Auenriched arc lavas, typically at 6 ppb compared to 1 ppb and below for MORB, may have an important inuence on the Au-forming potential of the system. Although not developed directly on continental crust, the isotopic data for Wetar provide strong evidence for a signicant component of continental crust and or sediments in the generation of the volcanic edice that hosts the VMS mineralization. Using simple mass balance equations, the amount of basement required to be stripped of gold to produce the Kali Kuning deposit signicantly increases from 0.5 km3 for a basement of 6 ppb Au to $3 km3 for a basement with only 1 ppb Au. These values climb to 0.8 and 5 km3, if extraction eciency rates more in keeping with experimental work are assigned (Moss et al. 2001). Such a dramatic reduction in the rock volumes required to generate the Au-mineralization suggests that the Au content of the volcanic basement may well play an important role in the generation of Au-rich VMS. Herzig and Hanning-

Discussion and comparisons

Wetar deposits in comparison with modern systems The uids responsible for barite precipitation with associated gold and sulfosalt assemblages show strong similarities to late stage hydrothermal uids reported elsewhere in modern seaoor deposits. For example, late stage hydrothermal uids rich in Pb, As, Sb, Ag, +Au were reported from Axial Seamount (Hannington and Scott 1988); with up to 6.7 ppm Au reported from an associated sulfosalt assemblage. Furthermore, galena, anglesite and sulfosalts of Pb, Ag, As, and Sb are frequently associated with low-T venting uids, and the mineralogy of white smokers are typically enriched in barite, sphalerite and consistently report elevated Au values (Koski et al. 1984). The Spire at Axial Seamount shows both high- and low-Fe sphalerite, with the higher values associated with the main stage ore formation (Hannington and Scott 1988). This is also the case for Wetar with low-Fe sphalerite restricted to the later fracture network. These data are consistent with a uid evolution that evolved from a reducing uid at low pH and high T (350C) to a relatively oxidizing uid at high pH and lower T due to cooling and mixing with seawater.

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ton (1993) note that gold appears most abundant in suldes associated with immature seaoor rifts in continental or island-arc crust, settings dominated by calc-alkaline volcanic rocks, including andesites, dacites and rhyolites. Notably, the Au-rich VMS system at Boliden is thought to have developed within calcalkaline to dacite rocks within an island-arc located on continental crust or a thin continental margin (Vivallo and Claesson 1987; Allen et al. 1996; Billstrom and Weihed 1996). Similarly, the Au-rich Eskay Creek deposit formed within a mid-Jurassic arc of calc-alkaline to dacitic rocks that developed on an earlier Triassic arc and Palaeozoic volcanic and sedimentary rocks (Macdonald et al. 1996).

Summary and conclusions

The massive sulde and baritegold mineralization of Wetar Island, Indonesia, provides a signicant perspective on the formation of Au-rich barite in arc situations. The mineralization at Wetar relates to arc volcanism triggered as the Banda Arc and Australian continental plate collide. Progressive stages of mineralization are recognized, dominated by the early arsenian pyrite with associated chalcopyrite and minor barite. Later sulfosalts, low-Fe sphalerite and further stages of barite and then oxide mineralization developed, leaving a complex mineralization over intensely altered footwall volcanic rocks showing argillic and local advanced argillic alteration close to mineralization. The presence of oxide-cemented barite ores and iron oxide-cemented barite pipes are evidence of the later, oxidized hydrothermal uid dominated by seawater sulfate. These oxidized uids released arsenic and gold from earlier arsenian pyrite precipitating free gold with barite and complex iron-bearing arsenates with signicant contained silver and mercury.
Acknowledgements PS acknowledges the generous nancial support of BHP-Billiton, The Natural History Museum and The University of Southampton. The logistical and nancial support of BHP-Billiton through Chris Farmer, David Hopgood, David First and James Macdonald is particularly acknowledged. Tony Fallick, John Murray, Andy Barker, Robin Armstrong, Ernie Rutter and Damon Teagle provided key insights throughout the project. The SUERC is funded through support of the Natural Environment Research Council (NERC) and the Scottish Universities. AJB is funded by NERC support of the Isotope Community Support Facility at SUERC. We acknowledge careful review of the manuscript by Donna Sewell and an anonymous referee.

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