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Geology,Geochemistry,andOrigin of High SulfidationCu-Au

Mineralizationin the NansatsuDistrict, Japan
Surveyof Japan,1-1-3Higashi,Tsuknba

of Mining,KyushuUniversity,

BHP Minerals, P.O. Box 619, Hawthorn, Victoria 3122, Australia

Instituteof Geological


Surveyof Japan,1-1-3Higashi,Tsukuba


The Nansatsu districtof southernKyushuhasbeenthe siteof calc-alkalinevolcanism for

thelast10m.y.,shiftingeastward withtime.Associated
hydrothermal activityfolloweddepo-
sitionof the volcanichostrocksby about0.5 m.y. andwascharacterized by interactionof
magmaticfluidswith meteoricwaterunderepithermalconditions, resultingin the formation
of highsulfidationCu-Audepositsat Kasuga,Iwato, andAkeshi.The orebodiesconsistof
>95 wt percentSiO2andresultfromleachingof the originalandesitclavaandpyroclastic
flowsby acidchloride-sulfate waters.Theseare inferredto haveformedwhenmagmatic
vaporscontainingHC1 and SO2condensed into meteoricwater. The residualsilica(now
quartz)orebodies arebestdeveloped wherethehostwasinitiallypermeable. Themargins of
the quartzbodiesare abrupt,with narrow(1-2 m) halosrepresenting the reactionfrontof
acid watersisochemicallydissolvingthe host rock. The halo comprisesalunite (strongly
zonedin Na andK, with P-richcores),dickitc,and/orkaolinitc_+pyrophyllite,gradingout
into illitc andinterlayeredillite-smectiteclays,andfinally,propyliticalteration.Thispattern
is characteristic of depositsof thistype throughoutthe world,for example,at Summitville,
Colorado,andLepanto, Philippines.
Mineralizationoccurredafterinitialleachingby the vaporcondensates, with metalstrans-
portedby a densemagmaticfluid.Mixingwith meteoricwaterandthe subsequent tempera-
ture decrease causedthe generaldecrease in gradetowardthe marginof the quartzbodies;
oregradesarerestrictedto thequartzbodies.Goldis mostcloselyassociated with enargite
and pyrite; later mineralsincludecovelliteand then sulfur.The laststageof activitywas
steam-heated, with descending watersoxidizingsulfidesto goethiteandlocallyremobilizing
Au intofractures(thisvariesin degreebetweendeposits). Erosionexposed the orebodiesto
supergene weathering,continuingthe sulfideoxidationandAu remobilization.
Stableisotoperesultsindicatethat hypogenealuniteformedfroma mixtureof magmatic
fluid(so = 7 + 2%0,D = -25 + 5%0,similarto nearbyactivevolcanicdischarges) withlocal
meteoricwater.In contrast,theclaysin themarginalhalohaveisotopiccompositions indicat-
inga bsoshiftof 6 to 8 permil fromlocalmeteoricwatervalues,probablydueto water-rock
interaction,and the/so valuesof residualsilicaquartzmay alsobe due to meteoricwater

0361-0128/94/1530/1-3054.00 1

domination.Fluid inclusionstudy of postmineralization quartz crystalsindicatesthat the

fluidshada salinityof aboutI wt percentNaCI equivduringlatequartzgrowth,thoughthere
is evidencein onesamplefor highersalinityfluidhavingbeenpresent,up to 30 wt percent
NaC1equiv(someinclusions containdaughtermineralsof haliteandsulfur).The Thvaluesof
over 1,000 measurements on late quartzfrom the ore zonesindicatethat the meantempera-
ture duringthatstagerangedfrom<200Cat Akeshito about200Cat Iwatoand230Cat
Kasuga.The presenceof vapor-richinclusions,somewith Thvsimilarto The,indicatethe
presenceat timesof a two-phasefluidin the centerof the orezones,with depthsof about150
to 300 m belowthe palcowatertable.The mineralizingfluidwasrelativelyoxidized(sulfide/
sulfateratioabout3:1), closeto pyrite-alunitecoexistence. Undertheseredoxconditions, a
pH of 3 andover a temperaturerangeof 200 to 300C, AuCI complexingmay dominate
over HAu(SH)2at salinitiesaboveabout2 wt percentNaCI.
Severalconditions areconducive for highsulfidationmineralizationto occur:(1) a crystal-
lizing magmaexsolves a fluid, with lower pressureconditionsfavoringmetalfractionation
frommeltto fluid,(2) the exsolvedfluidseparates intovaporandsalineliquidphasesdueto
immiscibility,with the latter beingmetalrich, (3) the gas-rich(HCI andSO2+ H2S)vapor
ascends to the surface,with at leasta portioncondensed into meteoricwater,forminganacid
fluid which leachesthe hostrock to createpermeablezonesfor later mixing,and (4) the
dense,metal-bearing fluidalsoascends intothisleachedzoneandprecipitates Cu sulfosalts,
sulfides,andAu uponmixingwithmeteoricwater.If thesalineliquidisnotreleased fromits
sourceadjacentto the magma,due to lack of fracturing,or if there is a stronghydraulic
gradientcausedby high relief, only the vapor-relatedstagemay occur.This will leave
leached,barrenrockwhichis characteristic of manyerodedvolcanicterranes.

Introduction volcanicrocks).Typicallow sulfidation veinmineral-

PLIOCENE epithermalCu-Au mineralizationoccursin ization is much better developed 50 to 80 km north
the Nansatsudistrict, locatedalong the southern in the Hokusatsudistrict(IzawaandUrashima,1989)
coastofKyushu(Fig.1a),andishostedby pyroclastic at Kushikino(Matsuhisa et al., 1985) and Hishikari
andlavaflowsof similarage.Hydrothermal activity (Izawa et al., 1990).
contemporaneous with volcanism resultedin strong The present-day activevolcanicfrontoccursabout
leachingof the volcanicrocksby acidfluids;the re- 25 kmeastof the Nansatsu deposits (Fig. 1). Studyof
suitingresidualsilica,nowquartz,providedthe host hydrothermalfluidsassociated with the activevolca-
for Cu andAu mineralization. The intimatespatial noesof southernKyushu,particularlyat nearbyKiri-
andtemporalrelationbetweenvolcanismandminer- shima (Hedenquist and Aoki, 1991) and Satsuma
alization,andthe evidencefor the presence of acid Iwojima (Shinoharaet al., 1993), providesinsight
fluids,raisesthe questionof the role of a magmatic into the originsof components in the acidfluidsand
their interaction with host rocks. Here we use our
input duringhydrothermalactivityand mineraliza-
tion. geologicandgeochemical studiesof the Nansatsu de-
The acid fluidsresponsiblefor leaching(Bethke, positsin conjunction with supporting informationon
1984) here and elsewhereare relativelyoxidized. activevolcanicfluidsto refinethe existingmodelsfor
The highsulfidation-stateminerals(BartonandSkin- the formationof highsulfidationmineralization.
ner, 1979) associatedwith mineralizationincludeen-
studiesof highsulfidationdeposits
argite, tennantite, and covellite, hence the term
"highsulfidation" (Hedenquist, 1987) for thistype High sulfidationmineralizationis increasinglybe-
of deposit,alsocalledthe "acidsulfate"type(Heald ing recognizedthroughoutthe world (Sillitoe,1989;
et al., 1987).Thestyleof alterationisadvanced argil- White and Hedenquist,1990), with somedeposits
lic, thoughthe residualsilicaquartzisnotincludedin containing in excessof 100 tonsof Au associated
thisterminology(MeyerandHemley,1967).In con- Cu sulfosalts and sulfides(e.g., Goldfield,Nevada;
trast,epithermalgoldmineralizationrelatedto near- Lepanto,Philippines;Chinkuashih, Taiwan;E1Indio,
neutralpH and relativelyreducedfluids(the deep Chile;PuebloViejo, DominicanRepublic).Ransome
fluidstypicalof manygeothermalsystems) is asso- (1907) firstproposed a deephypogeneoriginfor the
ciatedwithlowsulfidation-state mineralssuchaspy- acid fluids responsiblefor alterationat Goldfield.
rite andpyrrhotite.Thistype of epithermalmineral- Stevenand Ratte (1960) conducteddetailedstudies
ization is called "low sulfidation"(Hedenquist, on similar alteration related to the Summitville Au
1987), or "adularia-sericite"(Heald et al., 1987). depositin the SanJuanMountains,Colorado,andrec-
Minor veinsof thistype of mineralizationalsooccur ognizedthepatternof alterationcharacteristic ofthis
in the Nansatsudistrict at Kago (Fig. l a; hosted styleof mineralization.Recentstudieshavefocused
mainlyin basement rocksbut alsocuttingoverlying on mineralogicand stableisotopicstudiesin an at-

/. ,
Kyushu htkari
l(Hts X:. Kakutov . Ktrishma

o ] .."Sakurajim


0 km50
..: go ,
%/Iffl: oo/''g.y-o"? , ,. .

I %; u -'w.o x deposit
.,,,r.. , Probable


F- Pleistocene
flows . 0.
' Calderas
rE-q Nansatsu
E Upper
[J Nansatsu
IX-X-]LowerFormation Group(lateMiocene)
Kagoshima graben

F'/7 KawanabeGroup(midto lateCretaceous)

5.5-3.2 1.5-1.0 ~0 Ma Hydrothermal
9.9 (?) 8.0-6.4 6.2-3.7 4.1-1.1 1.5-0Ma Magmatic
1 Koshikilima Noma Makurazaki Kaimon Ata C.

+ ! v v +

-1 + v v +"
+ +

-2 [-+---

14 '++.F.
-3 [Magnetlte
limenit vi
[?, i':F//':
e series
'r- + +



km I 30

FIC. 1. a. Geologicmapof the Makurazaki(western)areaof the Nansatsu

Ministryof International
TradeandIndustry,1985).Insetshows the southern portionof Kyushu and
activevolcanoeswithintheKagoshima graben(hatchured) associated
withthepresentvolcanic front.
Thelocation ofgolddeposits
inboththeNansatsu(south) andHokusatsu (north)mineraldistrictarealso
shown.b. Northwestandwesttoeastcrosssection
(inset,a)throughthecomplete Nansatsu district,
oldestmagmatism in thewestto thepresent
front.Hydrothermal activity
hasalsoshifted east-
wardwithmagmatism (rangeofagesofmagmatism andmineralizationforeachareaareshown).

temptto clarifythe environmentandevolutionof the contactoutwardwith a zone of acid minerals(typi-

hydrothermal system(Stoffregen,1987;Hedenquist cally 1-10 m wide, thoughit canbe in excessof 100
et al., 1988;Arribas,1992;Ryeet al., 1992). m in somedeposits).This zone can includealunite,
This styleof mineralization
is typicallyhostedby kaolinitcand/ordickitc,pyrophylliteand/ordiaspore
calc-alkalinevolcanicrocks (and associatedsedi- _ zunyite(_ pyrite, _ barite), progressingoutward
ments)whicharestrongly leached,typicallyleavinga throughillitc or smectiteto extensive
vuggysilicaresidue,subsequently recrystallizedto ation and eventuallyfresh rock (Stevenand Ratte,
quartz.The residualsilicaquartzbodyhasan abrupt 1960). Sulfideandsulfosaltmineralizationgenerally

includesenargite(_ luzonite),pyrite, tetrahedrite haveformedasfar backasthe Early Proterozoicin

and/ortennantite,covellite,etc.,with Au commonly centralSweden(Enfsen). The oldexamples arecom-
closelyintergrownwith or includedin the sulfides monlyhighly metamorphosed (Chetwynd,Temora,
andsulfosalts, or sometimes in crosscutting veinlets. Enfsen)and may be stronglysheared(Chetwynd,
Quartzwhichfillsopenspaces, althoughcommon,is EnS, sen),resultingin a stratiformappearence.Some
mostlylate stage(in contrastto the residualsilicaof deposits(e.g.,Julcani)are similarin alterationstyle
the leachedhostrock,whichsubsequently recrystal- but havea distinctAg-Pbmetalassociation. Intrigu-
lizesto fine-grained quartz).The late quartzdeposi- ing similaritiesto thisstyleof alterationare foundin
tionresultsin portionsof the depositappearingmas- advancedargilliczonesof severalporphyryCu de-
sive. The sulfides and sulfosalts of the central zone posits,suchas Butte (Brimhalland Ghiorso,1983)
are commonlyoxidizedto a variableextentasthe re- andE1Salvador(Gustarson andHunt, 1975). Sillitoe
suitof late circulationof surfacewatersthroughthe (1989, 1991) and Vila and Sillitoe (1991), among
highlyfracturedorebody,causingsomeAu to be re- others,have noted a spatialrelationshipbetween
mobilizedlocally and concentratedwith goethite porphyryCu andhighsulfidation deposits.
(Urashimaet al., 1981; Stoffregen,1987; Sillitoeet Tokunaga(1954, 1955) first reportedthe zoned
al., 1990). natureof the acidalterationat Kasuga,andUrashima
The form of the depositsis variable,from strong (1975) usedthe term Nansatsu-type depositsfor the
fracturecontrolresultingin dominantveinsor lodes three main deposits,Kasuga,Iwato, and Akeshi.
(e.g.,LepantoandNalesbitan,Philippines;E1Indio, Other previousstudiesof the depositsin the Nan-
Chile) to lithologiccontrolresultingin the typical satsudistrictincludegeologyandexploration(Taka-
mushroomshapeof the Nansatsudeposits.Interme- shimaand Maruyama,1954; Saito and Sato, 1978;
diatesituations alsooccur,with permeabilityin some Urashimaet al., 1981, 1987;IzawaandCunningham,
casesenhancedby verticalzonesof hydraulicfrac- 1989; Ministryof InternationalTrade andIndustry,
turing, suchas at Summitville,Colorado;Lepanto 1985, 1988, 1989, 1990, 1991); ore mineralogy
and Nalesbitan,Philippines;and the Nansatsude- (Matsukuma,1960; Kawasakiet al., 1982; Imai et al.,
posits. 1983); and geochemistry (Takenouchi,1983; He-
In additionto the Nansatsu district,otherdeposits denquistet al., 1988). Gold wasfirst discoveredat
characteristic of the high sulfidationstyleof alter- Akeshi in 1890, and >18 metric tons of Au hasbeen
ationandmineralization includeLepanto(Gonzales, producedfrom the three deposits,at an average
1956; HedenquistandGarcia,1990; Garcia,1991) gradebetween3 and 6 g/t Au (Kasuga,6.7 metric
and Nalesbitan(Sillitoeet al., 1990), Philippines;tons;Iwato, 6.6 metric tons;Akeshi, 4.7 metric tons;
Chinkuashih, Taiwan(Huang,1955;Folinsbee et al., to early 1987); similaramountsremain in reserves.
1972; Huangand Meyer, 1982); Zhijinshan,China Minorproductionisalsorecordedfromthe Kurigano
(Renet al., 1992);FriedaRiver(Whalenet al., 1982) silicabody and the Kago and Misomequartz veins,
andWaftRiver(LeachandErceg,1990),PapuaNew the latter cuttinga residualsilicaquartzbody.The
Guinea;Motomboto,Indonesia(Carlileet al., 1990; best describedexamplesin the literature that are
Perello,1994);MountKasi,Fiji (Turner,1986);Te- mostsimilarto the NansatsudepositsincludeSum-
mora, Australia(Thompsonet al., 1986); E1 Indio mitville, Colorado(see Stoffregen,1987, for refer-
andAranada,1986;Jannas et al., 1990),La ences),Nalesbitan,Philippines(Sillitoeet al., 1990),
Coipa(Camus, 1990;Oviedoet al., 1991),andmany andRodalquilar,Spain(seeCunningham et al., 1990,
otherdeposits in Chile (Sillitoe,1991);Julcani(Pe- for references).
tersenet al., 1977;Deen, 1990;Ryeet al., 1992) and RegionalGeology
occurrences in southernPeru (Vidal et al., 1989);
PuebloViejo, DominicanRepublic(Kesleret al., Tectonicsettingand volcanichistory
1981;Russellet al., 1986;Munteanet al., 1990);the Major epithermalmineralizationin southernKyu-
Goldfielddistrict(Ransome, 1907; Ashleyand Sil- shu is associated with late Cenozoic volcanism re-
berman,1976;Vikre,1989)andParadise Peak(John latedto northwestsubduction of the PhilippineSea
et al., 1991), Nevada and Summitville,Colorado plate. This is closeto the northernlimit of the Ryu-
(Stoffregen,1987;Rye et al., 1992), UnitedStates; kyu arc (HibbardandKarig,1990). Presentvolcanic
Chetwynd,Canada(McKenzie,1986);Ensen,Swe- and geothermalactivity occursalong the north-
den(Hallberg,1994);Rodalquilar, Spain(Arribaset northeast-trendingKirishima volcanicbelt over a
al., 1989; Cunningham et al., 1990;Rytubaet al., steeply dipping (about 70 west) Wadati-Benioff
1990; Arribas,199'2);Bor, Yugoslavia (Jankovicet zone (Shionoet al., 1980). The major tectonicfea-
al., 1980);Recsk,Hungary(Baska et al., 1980);and ture associatedwith this volcanicbelt is the Kago-
Spahievo, Bulgaria(Velinovet al., 1972, 1990). shimagraben(Fig. la, inset),extendingover 130 km
Thisstyleof mineralizationismostcommonly pre- alongthe easternmarginof the HokusatsuandNan-
servedin Tertiaryrocks,thoughit is recognized to satsumineral districts(Izawa and Urashima,1989).

' ' ' i ' ' ' i ' . i ' ' i ' i , ,

This20-km-widedepression isassociated
with a large
[] Eruptionage
anomalously low gravityfeature(New EnergyDevel- 12
Mineralization age
opmentOrganization,1987) and containsthe Ka-
kuto,Aira,andAtacalderas, formedbyrhyoliticpyro- 0
clasticeruptions.Active andesiticto daciticvolcan- Koshikijima
._o 8
ismoccursat KirishimaandSakurajima,with recent 4--'

volcanismat Kaimondake, and 50 km to the south- E6 Noma0

west, at SatsumaIwojima.
Middle Mioceneilmeniteseriesgraniticintrusions 4

(15-12 Ma) arepresentthroughoutthe district(Fig.

lb) andin southernKyushu,with associated Snminer-
alizationbut only minorAu occurrences (Izawa and W , , , i , , xi-11
i , , , i , ,x, , Kaimo
, ,
1 O0 80 60 40 20 0
Urashima,1989; Izawa, 1992). All subsequent intru-
Distance km
sive and volcanicactivityis of the magnetiteseries
(Izawa,1992), with all majorAu depositsof Kyushu FIG. 2. Radiometricage (K-Ar) versusdistancefrom the vol-
relatedto thisstyleof magmatism. canicfrontfor freshvolcanicrocksandhydrothermalmineralsas-
Calc-alkaline subaerial volcanism has shifted to the sociatedwith Nansatsu
mineralization(aluniteandillite). Hydro-
thermalactivityoccurredon an averageof about0.5 to 0.7 m.y.
eastoverthe past10 m.y. or more,bothin the Nan- afterthe emplacementof the volcanichostrocks.Modifiedfrom
satsudistrict(Fig. 2; Izawa, 1992) andin the Hoku- Izawa (1992).
satsudistrict to the north (Izawa and Urashima,
1989). This pattern begins with magnetite series
granites westofKyushu( onKoshikijima (pre-
sumablythe subvolcanicequivalentof eroded vol- the Nansatsudistrict by the Lower Formationand
canicrocks)and continueseastwardto recentlyac- Upper Formationof the NansatsuGroup (Fig. 1).
tive Kaimondake. Thisshiftmaybe dueto a progres- Theseare comprisedof pyroxenehornblendeande-
sivesteepening of the west-dippingsubduction zone siteflows(7.6 Ma), pyroxeneandesiteflows(6.4-5.9
(Izawa, 1992). Hydrothermalactivity, both in the Ma) and their pyroclastics(Izawa, 1992), and tuf-
Nansatsu(Fig. 2) and Hokusatsu(Izawa and Ura- faceousmudstone andconglomerate, with the Upper
shima,1989) districts,hasalsofollowedvolcanicac- Formationcharacterizedby intercalationsof pyro-
tivity asthe underlyingmagmaticheatsourceshifted, clastics and mudstones within lava flows. Each forma-
with the peakof hydrothermal activityoccurringon tion has a maximum thickness of about 300 m. The
averageabout0.5 to 0.7 m.y. after depositionof the Lower Formationlies unconformably on the base-
host volcanic rocks. ment rocks,strikesnorthwestand dips 10 to 20
Basement rocks and structure
NE. The easternpart of the districtis characterized
by hornblendeandesiteflowsand pyroclastics, and
The Nansatsu districtis underlainby sedimentary tuffaceous siltstone of the Nansatsu Middle Volcanics
rocks of the CretaceousShimanto Supergroup (4.6-3.4 Ma), with a maximumthicknessof 300 m.
terrane(primarilyof the KawanabeGroup).Carbon- Theserocksoverliethe UpperFormationof the Nan-
aceous shale and sandstone with minor submarine ba- satsuGroupor rest directlyon the ShimantoSuper-
saltandchertarelocallymetamorphosed (Imaiet al., groupsedimentaryrocks.The Upper Formationof
1971) andhavebeeninterpretedasan accretionary the NansatsuGroup and, at Akeshi, the Nansatsu
prismof oceanicandtrench-fillsediments,and over- MiddleVolcanics are the principalhostsof mineral-
lyingfore-arcbasinandslopesediments (Sakaiand ization;the orebodiesexpandinto permeablepyro-
Kanmera,1981).The westernmarginof the Nansatsu clasticunitssandwiched by lesspermeablelavaflows.
districtisboundedby the Butsuzotectonicline (Fig. Young, postmineralizationrhyolitic pyroclastic
lb), separatingShimantobelt sedimentaryrocks rockscoverlow-lyingareasof the district.Theywere
fromthe Chichibuterrane.Major structures cutting eruptedfromthe Ata caldera(0.09 Ma) andthe Aira
basementrocksof the Nansatsudistrict,if present, caldera(0.02 Ma) andare up to 130 m thick.
are obscuredby the youngvolcaniccover,though
some north-northeast-trending lineaments were
mappedat sedimentarydisconformities in the out- The movementof magmaticandassociated hydro-
cropsof Shimantorocks,parallel to the regional thermal activity across the districtled to widespread
strikeof the basementsedimentary rocks. propyliticalteration(Fig. lb). Many quartz veinlet
systemsare locatedradial to a basementdepression
Volcanicstratigraphy in the vicinity of Kasuga(seebelow) and are asso-
The ShimantoSupergroup basementsedimentary ciatedwith analterationassemblage of zeolites(cha-
rocksare overlainin the westernandcentralpart of bazite, stilbite, laumontite,and wairakite),calcite,

andpyrite. The low sulfidationquartzveinsat Kago, suhisaet al. (1991) havesuggested that thisdepres-
5 km northeastof Kasugaandoutsidethe depression, sionmayrepresenta calderacollapse structure,from
have wairakite alteration in the wall rocks;the veins 3 to 5 km in diameter.The majorquartzbodiesof the
produced0.6 t of Au. About 2 km north of Iwato, Kasugaarealie on the innermarginof thisdepres-
thereisanextensivefiat-lyingareaup to 100 m thick sion,whereasthe Kagolow sulfidationvein system
of smectiteand cristobalitealteration(locallywith liesoutside,to the northeast(Fig. 3).
kaoliniteandillite) in pyroclastics(Ministryof Inter- Gravitydataforthisarea(MinistryofInternational
nationalTrade andIndustry,1990). Thisalterationis TradeandIndustry,1985) showa clearresidualBou-
underlainby freshand propyliticallyalteredlavas. guerlow anomalyof 3 mGalcenteredjustwestof
The alterationheremaybe dueto relativelycooland Makurazakicity(Fig. 3b), largelycoincidentwith the
dilute fluid outflowalongpermeablehorizonsfrom observedbasementdepression.An elongatehigh
the Iwato hydrothermalsystem. anomalyextendsfromthe westto Sonomi,consistent
withthelarge,high-density quartzbodynearthe sur-
The KasugaDeposit face.
Geology Figure4 shows a north-southcrosssection through
The Kasugadepositis associated with oneof sev- the Kasugadeposit,with geologybasedon surface
eral quartzbodieswhichcaphillsfrom Kuriganoon outcropandthe resultsfromsevendrill holes(Min-
the coastto Sonomi,about5 km northnortheast(Fig. istry of InternationalTrade and Industry, 1988,
3). ShimantoSupergroup basementrocksarepresent 1989, 1990; KasugaMining
nearby,to the west of the seriesof quartz bodies suits),all of whichreachedbasement. The somewhat
whichare hostedby volcanicrocksof the Nansatsu schematic alteration zonation is based on over 200
Formation.Basedon surfaceoutcropsand informa- samples examined by X-raydiffractometry. Detailsof
tion from 13 drill holes(Izawa, 1991), the elevation the mineralogy are discussed
of the top of the basementhasbeen determined.A
semicirculardepressionis apparent, open to the Hydrothermalalterationzoning
southeast, with up to 350 m of relief overa distance The alterationmineralzoningaroundthe quartz
of i km onitswesternmargin.Izawa(1991) andMat- bodyis easilyvisiblein the openpit of the Kasuga



v v v

v v v vVVvV
vv v v vvv

v v
.3 v


o 1

FIG.3. a. Geologic mapof theKasuga area,showingthedistribution

of silicabodiesandtheelevation
(relativeto sealevel)of the Shimanto
Supergroupbasement (determined fromsurface outcropanddrill
holedata).Locations ofdrillholesshownasdots,withthosereferredtointhispaperlabeled. b. Samearea
of a, showing the residualBouguergravityanomaly(in mGal),whichreflectsthe basement depression
underKasuga.ModifiedfromIzawa (1991).

Kasuga N
1-3 63-2 62-3 1-1 DD 5 DD 128 63-1

.... ' ' I Qz-vein

' ;[] Quaternarypyroclasticflows
[--] AlteredNansatsuGroupvolcanics

FIc. 4. North-south crosssection

of theKasugaarea(Fig.38),showing thegeology andslightly
schematic alteration
ofover200 samples from
surfaceoutcropanddrill holecore.ModifiedfromIzawa(1991).AI = alunite,Cal = calcite,Ch =
chlorite, Dt = dickitc,Gn= galena,PR= propylitic
Py= pyrite,Qz = quartz,Se= sericite
(illitc),Se/Sm= interlayeredsericite-smectite,
Sp= sphalerite.
LegendasforFigurela, though the
of the Nansatsu

mine, where it was first describedby Tokunaga The central massof the orebodytypicallycom-
(1954, 1955).It is essentially
the sameasthe typical prisesin excessof 92 wt percentSiO2asquartz,with
pattern at Iwato (Saitoand Sato, 1978; Urashimaet onlya traceof alkalisandlessthan1 wt percentA12Oa
al., 1981), aswell asthatobservedin similardeposits (Table1), indicatingextensiveleaching.Thisisappar-
(e.g., Summitville, Colorado; Steven and Ratte, ent texturally,with the rockhavinga vuggyappear-
1960; Lepanto,Philippines;Gonzales,1956; Garcia, ancein handsamples dueto the preferentialremoval
1991). of phenocrysts andpumicefragments; we callthisal-

TI_ 1. RockCompositions
of Ore Samplesfromthe Nansatsu

Kasuga Iwato Akeshi
No. of samples 10 8 11
AI 390-1,400 (902) 1,000-4,500 (2,362) 870-2,900 (1,786)
Ti 730-2,100 (1,202) 300-4,100 (1,746) 190-820 (539)
Fe 5,400-130,000 (42,840) 3,000-20,000 (8,475) 8,100-77,000 (33,700)
S 320-130,000 (39,835) 200-3,700 (1,337) 180-84,000 (29,320)
K 5-30 (7.5) 60-220 (134) 5-70 (30)
Na 5-20 (11) 5-60 (39) 5-20 (6.4)
Ca 40-110 (87) 60-180 (110) 30-190 (119)
Mg 20-80 (45) 5-70 (43) 5-90 (54)
Ba 4-16 (8.9) 13-47 (31) 6-45 (15)
Ag 0.1-6.4 (1.5) 1.8-6.8 (3.3) 1-9 (3.0)
Au 0.39-10.5 (3.2) 0.16-6.7 (2.8) 0.37-37.9 (6.2)2
As 68-4,800 (892) 1-16 (5.6) 8-1,200 (723)
Sb 15-910 (170) 5.4-37 (16) 11-1,600 (216)
Bi 1-27 (9.1) 1.2-14 (4.4) 4-140 (25)
Cu 47-26,000 (4,296) 7-27 (12) 48-2,500 (801)
Pb 10-90 (33) 20-40 (23) 5-70 (21)
Te 1.4-34 (8.1) 0.1-2.4 (1.0) 2.2-210 (32)
Se 4-34 (10) 1-8 (3.3) 2-14 (6.2)
Sn 1-74 (14) 1-8 (3.8) 1-68 (13)
Hg 0.005-0.4 (0.08) 0.27-7.4 (2.6) 0.005-0.58 (0.15)
Zn 0.5-36 (9.1) 0.5-11 (4.6) 0.5-10 (4.2)
Mo 1.8-5 (3.1) 1.8-5 (3.2) 1.4-3.4 (2.6)
W 0.25-5 (1.6) 0.25-1.5 (0.63) 0.25-3 (1.2)

Analyticalmethods includeinduction-coupled
plasma(ICP) emission
ICP massspectrometry
with Au analyzedby fire assay
all in mg/kg,asminimum-maximum
'Onevalueof 11,800mg/kgwascutto thenexthighest

teration"residualsilica,"thoughthe residualamor- with depth and is alsofoundin the quartzbody at

toquartz.Second- greaterdepthswheretherehasbeenlessquartzdepo-
ary depositionof silicaas quartz crystalsin open sition.Within the openpit, the diekite _+kaolinitc
spacesandin thematrixcanresultinamassively silici- andalunitezoneis generallylessthan2 to 3 m wide
fled rock. The residual silica zone contains remnant (Fig. 5) andcanlocallycontaina white Mg-rich(or
titaniaasrutileor anatase, plushydrothermal sulfides Al-rieh) ehlorite (Hashizumeand Izawa, 1983).
andsulfosalts,primarilypyriteandenargite-luzoniteAwayfromthe contactwith the quartzbody,minor
fillingvugs,followedby lateeovellite,with rarena- illitc occurs with the diekite and kaolinitc, here
tivesulfurthe latestvug-filling phase.Aluniteis also termedthe "argillic"zone.Thiszonationgradeslat-
presentlocallyfillingvugs,andminorbaritehasbeen erally at high levelsto interstratifiedillite-smeetite
noted. Up to 5 wt percentiron oxideatteststo the awayfrom the quartzbody.With increasing depth,
commonoccurrenceof goethiteandscoroditein the the kaolinitcanddiekitegiveway to a zoneof illitc
rust-coloredorebodyand indicatesthat the sulfide and chlorite.
contentof thequartzbody,in places< I wt percent, Beneaththe residualsilica-hosted orebodythe py-
wasoriginallymuchhigher.Althoughmuchof the rite content increases;this is to some extent related
ironoxidemaybe relatedto weathering,the occur- to a decreasein postdepositional oxidationwith
reneeofcoarsely crystalline scorodite(sometimes in- depth.Beneaththe argilliczonenarrowveinsoccur
tergrownwithfinequartzcrystals) overgoethiteand in propylitieallyalteredvolcanicrocksandbasement
the isotopic composition of latealunitesuggest that sedimentaryrocks.The geneticrelation of these
someoftheoxidation of sulfides beganwhilethehy- veinsto the overlyingquartzbodyis notwell under-
drothermalsystemwasstillactive. stood,thoughfluidinclusionresultsonthe veinsindi-
The residualsilicaquartzbodyhasanabruptcon- catehighertemperatures thanexpected,basedonre-
tactat itsmargins with anadvanced argilliczonecon- suitsfrom the quartzbodies(seebelow).The veins
tainingdiekite,aluniteof variablecomposition (see comprisequartz,calcite,andsulfides(pyrite,sphaler-
below),and kaolinite,with variableoccurrences of itc, andgalena),withwall-rockalterationdominantly
pyrophylliteand/or diaspore_+pyrite. Diekite is illitie. Based on available drill hole and old under-
morecommonthankaolinitcadjacentto the quartz grounddata, the Kasugaquartz body and its ad-
body,andincreases withdepth;alunitealsoincreases vancedargillichalo of aluniteand diekite-kaolinite

FIc. 5. Photographtakenin the Kasugaopenpit, 110-melevation,showingmushrooming of the

quartzbody(mainbody,or "stalk,"to left,andalongtopof photograph).
Ontheundersideof thequartz
bodymushroom thereis a 1-m-widehalo(lightcolored)of alunite-kaolinite-pyrophyllite,
ward (downin thiscase)to smectitealteration.

narrowfrom about500 by 100 m at an elevationof highestgradesaregenerallyassociated withlateiron

100 m to only severaltensof metersacrossnearsea oxide.A majorbrecciatedfracturezone cuttingthe
level (Tokunaga,1954, 1955; Urashimaet al., 1987); southeast marginof the orebody(Fig.6), however,is
theydisappear completelyat greaterdepths(Fig.4; weaklymineralized.
Izawa, 1991). The argillicalterationalsopinchesto The paragenicsequence, asobservedin vugs,ispy-
narrowhalosaroundthedeeperveinswithinpropyli- rite followedby enargite(_+luzonite) and quartz
tizedwallrock.Fluidinclusion Thvaluesfromquartz (crystalsup to 5 mm in length),with late covellite,
veinsbeneaththe Kasugaorebody(seebelow)are nativesulfur,scorodite,andgoethite.Althoughpri-
higherthanthosefor late,vug-fillingquartzcrystals maryAu appearsto be associated with enargiteand
withinthequartzorebody.In the planmapof the pit pyrite, someof the highestgradesof Au are asso-
(Fig. 6), the argilliczone is visiblewhere footwall ciatedwith clayandgoethitein fractures,indicating
portionsof the orebody(Fig.5) areexposed by min- thatAu mayhavebeenremobilized,at leastona local
ing.Drill hole128 (Fig.4) intersected the outerpor- scale.
tionof onelimbof the mushroom of thequartzbody. The Iwato Deposit
Mineralization Geology
The principalore mineralsin the depositareenar- The orebodiesat Iwato are hos..... , the Upper
giteandAu (electrum);luzoniteisrarelyfoundin the Formation of the NansatsuGrot. '-,lcanics,asat Ka-
upperportionoftheorebody, whereas pyriteisubiqi- suga(Fig. 1). The upper,erodedsurfaceof the ore-
tousthroughoutthe orebody.As is typicalfor this bodiesliesat anelevationof about200 m anddrilling
styleof mineralization;
Au ore iswhollycontainedin to 20 m below sea level has not reached basement
the quartzbodyanddoesnotextendintothe argillic sediments
(SaitoandSato,1978). However,the Shi-
halo.Goldgradesareroughlyconcentric in pattern, mantoSupergroup cropsout westof MountKunimi,
decreasing towardthe marginsof the quartzbody. 2.5 km north of the mine, at an elevationof about 200
The mainhigh-grade zone(above5 g/t Au)islocated m; basedon this and gravity surveying(Saitoand
in the westernpartof the openpit (Fig.6) wherethe Sato,1978), the basementis thoughtto be closeto
fracture densityis greatest(fracturezonestrend the limit of drilling beneathIwato. The Nansatsu
northeast).Ore-relatedsulfideandsulfosaltminerals Middle Volcanicscrop out at Mount Kunimi, 2 km
are commonlyconcentrated in fissures
whichcut the north of Iwato, and showno evidenceof alteration.
quartzbodyandin vugsafter leachedphenocrysts StronglyleachedNansatsuGroup rocksare vari-
and lithic-pumicefragments.These fracture zones ably siliceousover a length of nearly 2 kin, with
containfromten to severalhundredg/t Au, andthe widthsvaryingfrom200 to 400 m (Fig. 7). The east-

_. , ? 50l?0m

flow Widebreccia
zone "-' Footwall
Clayeymaterial Fracture
zone [ Quartzbody
FIc. 6. SketchmapoftheKasuga openpit,showing alteration
zones,thelatterassociatedwiththehighestgoldgrades in thecentralto westernportionof theopenpit.
Patches ofclayapparentlywithinthequartzbodyareduetothefootwall oftheorebody beingpenetrated
(Fig.5) in places,accentuated
by the severallevels(elev= 80-150 m) shownhere.

I higashi
orebodies,they are not necessarily
thehighestgrades ofore,andinsome cases,
ciasare belowore grade(IzawaandCunningham,
?/ formingore-grademineralization.
,.' Mr.Iwato
,' 244 m J U
.,'. /'" Orebody Thequartzbodyat Iwatoiselongate
over2 kmat
-'- r' L' Quartz body the surface.The texture of the residualsilicarock is
' ' O, , , 500m generally massive, thoughin placesa vuggyappear-
anceispreserved. Thesimple mineralogyconsists
FIG. 7. Map showingthe lateralextentof the Iwato quartz fine-grained quartz,minorrutile, and secondary
2 g/t Au cutoffgrade)completely
contained withinthe quartz quartzcrystals (from10or20/mtoseveral mmlong)
body. fillingvoids(IzawaandCunningham, 1989).Finely
disseminated pyriteis alsopresentwherethe rock
has not been oxidized. The siliceousrock contains95
ern zone strikes east-west and contains all the orebod- to 98 wt percentSiO2andonly0.2 to 1.1 wt percent
ies, whereasthe western half strikesnortheast.The A1203,indicating
of theoriginalan-
ridge-forming quartzrockattainsa maximumeleva- desite(56wt %SiOn,18wt %AlO3;IzawaandCun-
tion of 244 m. Gold mineralizationis ubiquitousin ningham, 1989, andTable1). The Fe contentof
the siliceous
rock,with a minimumof about0.2 g/t much of the quartz is low (0.1-0.5 wt % Fe as
Au within the outer boundaryagainstthe argillic FelOn),thoughpyrite-richrockcancontainup to 5
zone.An economiccutoffgradeof about2 g/t Au wt percentFe expressed asFelOn.Red,oxidized
definesthe individualorebodies(Fig. 7), with the quartzorecancontain 3 wt percentFe20,whereas
largestbodiesbeing Iwashita,Arabira, and Maru- marginal partlysilicifiedrockwith clayscontains
yama.The diameterof individualorebodiesis 100 to to 10 wt percentFelOn.Thetotalcontentof Na,K,
200 m, with a vertical extent of about 100 m. The Ca, and Mg is usually<0.1 wt percent(Table1;
quartz-richzone,nearlycontinuous at anelevationof IzawaandCunningham,
200 m, pinchesdownwardinto severalindividual The contact between the residual silica quartz
zones;in sectionthe bodieslook like upward-coal- zoneandtheadvancedargilliczoneistypically
lescedmushrooms(detailed crosssectionsin Saito sharp(Fig.8), though therecanbe a gradation
and Sato, 1978; Urashimaet al., 1981; and Izawa and partlysilicified
rockuptoa fewmeters
Cunningham,1989). commonlyoccursnear the contact,accompanying
The intensityof leachingandsubsequent silicifica- kaolinitein the partly silicifiedrock.The kaolinite
tionisstrongly controlled
bythelithologyofthevol- zoneisgenerally1 to 2 m wide,contains somequartz
canicsequence (SaitoandSato,1978; Urashimaet andfinelydisseminated pyrite,andgrades intosmec-
al., 1981). The Maruyamaorebody,hostedby tuff tite andillite-smectite argillicalteration.Lessthan
and tuff breccia,narrowsdownwardin pyroxenean- 10 to 15 m outwardfromthe quartzbodygreenish
desiteflows,andthenexpands againintoa lapillituff propyliticalteration is encountered, consistingof
sandwiched by lavaflows. smectite,chlorite,epidote,calcite,andpyrite,with
Gravitysurveys (MetalMiningAgencyof Japan, the primaryrocktexturepreserved. Latealteration
1969)indicatethatthe siliceousbodieshavea con- includes patches of hematiteandgoethiteaftersul-
trast of about 0.5 mGal abovethat of their argillic fidesandsulfosalts,
lessabundantthanat Kasuga(Ta-
halos. Resistivity measurements(Metal Mining ble 1).Lateveinlets ofalunitelocallyextendintothe
Agencyof Japan,1971)showthatthesilicified rock argillichalo.
hasa strongcontrast(500-3,000 ft m) compared Mineralization
with the surrounding argillizedrock (30-50 ft m).
Thesegeophysical features,combined withlithologic Sulfide and sulfosalt minerals at Iwato are fine
mapping, areimportant exploration guidesin thedis- grainedanddisseminated, and are lessabundant
trict. priortooxidation
thanatKasuga. Pyriteistheprinci-
Postsilicificationbrecciation is present at Iwato palsulfide;otherminerals, somewithalimitedoccur-
andisinterpreted to haveformedduringhydrother- rence(Urashima et al., 1981;Kawasaki et al., 1982),
malactivity(IzawaandCunningham, 1989).A well- includenativegold,electrum,argentite,pyrargyrite,
exposedbrecciapipe in the Iwashitaorebodywas canfieldite,chalcopyrite, bornite,chalcocite,enar-
mapped in detail,witha shapein cross section likea gite,native
copper, sphalerite,galena,molybdenite,
molartooth,withseveralrootsnarrowingdownward. stannite,cassiterite, andnativesulfur.Hematiteand
Athoughbrecciapipesat Iwatoarecontained by the goethitearecommon lateminerals,though scorodite

quartzbody, and gradesalsotend to decreasewith

ies, from 1:2 to 2:1 (SaitoandSato,1978).
The AkeshiDeposit
The orebodiesat Akeshiare hostedby the Nan-
satsuMiddle Volcanics,with mineralizationappar-
ently morestronglycontrolledby structuresthanat
Iwato. This feature reflects the dominance of fracture
permeabilityin the host pyroxeneandesitclavas
compared withthehigherbulkpermeability of older
pyroelasticunitswhichhostmineralizationat Kasuga
andIwato.Theageofmineralization hereistheyoun-
gestof the threedeposits(Fig. 2); Iwato andKasuga
orebodiesformedbeforedepositionof the Nansatsu
Middle Volcanicswhichhostthe Akeshideposit.
Most of the alteration visible at Akeshi consists of
the quartzbody(Fig. 10), varyingfromvuggyresid-
ual silica(with vugsfilled by sulfidesandsulfur)to

Plan155m B 0
i i i rn
i , 50

'7.;__..t3'.3,< ......'- ,
' '.'.'.'.'.
-' -- -'.'/ x',-
'' ~ V

FI. 8. Photograph showing the sharpcontactof the quartz

body(massive outcrop,to right)with the alunite-kaolinite
Thislatterzonegrades intothesmectite andinterlayered sericite-
smectite zone,whichgrades a further10 mto theleftintopropyli-
tic alteration.
Maruyama orebody2, westwallof the 160-meleva-
tion level, Iwato.

is not present,possiblydue to the lack of arsenical

PrimaryAu mineralization ishighlyvariableandin
generaldecreases towardthe margin(Fig.9), though
at depth and perhapsin plan there appearsto be
somestructural controlto theoreshoots (Fig.9, cross
section).The primaryAu isveryfinegrainedandhas
notbeenobservedunderthe microscope; however,
sincemostof the Au is recoveredby cyanidetreat-
mentafterfinegrinding,it is assumed thatthe Au is
not largely occludedby sulfidesor sulfosalts.Al-
thoughAu gradesarelocallyhigh(100-1,000 g/t) in
association with fracturescuttingthe quartzbody,
this is largelydue to secondary remobilizationas
heretheAu occurswithyellowclaysandgoethite,is
crystallineand coarsegrained(to 200 m), and is
highin fineness(940 -- 990; Urashimaet al., 1981).
Lowergradescommonly occuronthe marginsof the

L Plan(0 mL) A Section (m)lB

/: ::::::.:.::::',.L

.:. 2501

/ ::::' 5OO N auartz

No.3 :::':: .'
,.,:'rtal ': Ore
'/ /' ' ' Alteredandesile
(Nansalsu Middle

FIG. 10. Sketchmap(elev-- about180 m) andeast-west crosssectionof the Akeshideposit,showing

the distributionof the orebodies(labeled)in the zoneof residualsilica.Alterationincludesthe quartz
body,whichhasa sharpcontactoutwardwith the argillichalothat in turn gradesinto propyliticalter-
ation;youngAta pyroclastic rockslie unconformably overthe northeastern portionof the quartzbody.

massively silicifiedrock.Young(<0.1 Ma) pyroclas- Goldin primaryoreismostcloselyassociated with

tic rockslie directlyovermuchof the quartzbody, luzoniteand pyrite, whichit is commonlyincluded
whereasthe contactwith weaklysilicifiedandargil- by, basedonobservation of 1,000 Au particlesin pol-
lizedrockis presenton the northeast marginof the ishedsections(Tokunaga,1954). The Au rangesin
silicazoneat theaditlevel(elev-- 185m).Kaolin- observedsizefrom I to 100/am, averaging15/am in
itc and dickitcgradeoutwardinto smectiteonly, diameter.Gold is alsodirectlyassociated with fine
ratherthanillitcoraninterlayered clay,suggesting
a veinletquartzwithoutsulfides(Matsukuma,1960).
lowertemperature of formation
itc is alsolesscommonthan at Kasugaand Iwato, Geochemistry
thoughit waspresentat shallowlevels,nowmined.
One of the mostinformativehydrothermalmin-
There are three orebodies within the residual silica eralsthatcommonly formsin the highsulfidation
zone (Fig. 10), all steeplydippingpipelikestruc- vironmentis aluniteand relatedisomorphs. Alunite
tures.Body I (100 m northeast-southwest
and 40 m (KA13(SO4)2(OH)6) hasNa andCa analogues, natro-
wide)plungessouthwest at an angleof 60, froman aluniteand minamiite,respectively.The P-bearing
elevation of 250 mdownto 100m.Body2 hasa diam- analogueis crandallite(CaA13(PO4)(POaOH)(OH)6),
eter of about50 m anda verticalplungefroma 175- with a rare earth elementsubstitutingfor Ca and
to 125-melevation,then changes plungeto 40 to forming fiorencite (CeAla(PO4)2(OH)o); interme-
the west.The thirdbodyissmallerandisolatedfrom diatecompositions alsooccur,suchaswoodhouseite
the first two. (Cx13(PO4)(SO4)(OH)6), whichcommonlycontains
Miningat Akeshihasprogressed frombothunder- Sr, Ba, andPb. Mineralogicalandchemicalzonation
groundandopenpit, thelatterpresentlyat aboutan is usualfor hypogenealunite,providinginforma-
elevationof 250 m. Undergound exposures arecom- tion on changingfluid compositions (Aoki, 1991),
monlyrichin sulfides andsulfosalts (upto 10 vol%), whereasits isotopiccompositionprovidesthe best
more than in the openpits of Kasugaand Iwato, constrainton source(s)of the early, mostreactive
thoughthisislargelyrelatedto the degreeof oxida- fluids.Rye et al. (1992), in the first comprehensive
tion at the latter two deposits.Pyrite is mostabun- paperon the interpretationof aluniteisotopiccom-
dant,followedby luzonitedominant overenargite. position,discuss the S andO isotopesof the sulfate
Covellite,andin particular,nativesulfurarecommon site,andthe O and H isotopesof the OH site.K/Ar
aslatevugfillings.Scorodite is intergrown with lu- datingis alsopossibleon K-bearingalunite.
zonite(Matsukuma, 1960)andisthoughttobehypo- Hypogenealunitemineralsin the Nansatsu district
gene,whereasgoethiteis later and associated with includeearly formedwoodhouseite, which is com-
clay-filledfracturesthat canbe very rich in Au (to monly partially dissolved(Fig. 11a) or even com-
1,000 g/t). pletely replacedby later aluniteand natroalunite

c ""- I " d
1c. 11. Backscattered
electronimages of aluniteminerals.
a. Fromthepeakof Komatsugiyama
(quartzbodyabout1.5kmnorthof Kasuga), withleached (Sr,Ba)-woodhouseite
rimmed by
(darkgray)andalunite(lightgray);widthis 0.2 mm.b. FromKomatsugiyamaroadcut,
showingcompletelyleachedhexagonal woodhouseite
is0.2 mm.c. Zoned,fine-grained
alunitefromaditnorthof Iwato(5Feb87-21);widthis0.04 mm.d.
Unzoned finealunite
between cristobalite,
the Maruyama
argiiliczone,Iwato(5Feb87-16);widthis0.2 mm.

(Fig. 1lb). The alunitemineralsassociated

with Ka- natroaluniteandalunite,with texturescommonly in-
suga(Fig.11aandb)arerelatively coarse grained(up dicatingdissolutiondue to fluctuations
in fluidcom-
to 100m) in comparisonwiththefinergrained(sev- position.Crandalliteformswhenthe earlyacidfluids
eral m) aluniteat Iwato(Fig. 1l c). Althoughthe dissolveprimary apatite (Stoffregenand Alpers,
Iwatoalunitedoesnotshowanyremnantcrandallite, 1987), releasingP and REE, whereasSr and Ba are
it is stronglyzoned between K- and Na-rich end likely derivedfrom plagioclase and alkalifeldspar.
members.In contrast,the late K-rich alunite in veins Onceall apatiteisdissolved (noneis observedin the
cuttingthe Maruyamaargillic halo is very fine Nansatsu quartzbodies),thesealunitemineralsstop
grained(Fig.11d) andfillsopenspacesbetweencris- forming,andevendissolvepriorto precipitation
tobalite,supportinga coolerorigin(Stoffregen
and aluniteandnatroalunite.
Natroalunite is favoredby
Alpers,1992). highertemperatures,whereasaluniteis more com-
Aoki (1991) notesthat P-rich alunite minerals, mon at shallow levels.
commonly containingSr, Ba,Pb, andREE, are char- Kaolinireand its highertemperaturepolymorph,
acteristicof magmaticenvironments. Theseearly diekite,are commonin the Nansatsu deposits,with
formedminerals areovergrown byfineoscillations
of diekiteincreasing with depth.Diekite is alsomore

commonat Kasuga,wherethe inferredtemperatures clusionsfrom Takenouchi(1983), Hedenquistet al.

were hotter than at Iwato andAkeshi(seebelow).In (1988), andIzawa andCunningham(1989) are inte-
acid zonesof activePhilippinegeothermalsystems, gratedwith data from deep drill core (this study).
kaolinitchasa maximumoccurrencetemperatureof The majority of inclusionsstudiedare two phase,
about 200C, whereas dickitc is stable from 120C with both liquid-richand vapor-richinclusions com-
to ashigh as 280C (Reyes,1990, 1991; Reyesand mon.Where distinctionbetweenprimaryandsecond-
Giggenbach, 1992).Reyesalsonotesthatthe lowest aryinclusions ispossible(Roedder,1984), secondary
temperature for pyrophyllite formation is about inclusionshave similar to lower Th values.Quartz
200C;thisallowspyrophylliteto be usedto identify crystalsfrom one samplefrom the Kasugaore zone
the low-temperaturelimit of a dickite-pyrophyllite havefluidinclusions with cubichaliteandyellowsul-
assemblage,whereas the dicl<ite-kaoliniteassem- fur daughterminerals.
blageis stableat lower temperatures. Experimental The occurrenceof vapor-richinclusions iscommon
studies(Hemley et al., 1980) indicatethat kaolinitc at all three deposits,with someirregularlyshaped
and pyrophyllitecoexistover a wide temperature inclusions amenableto Th measurement. Thesehave
range, depending on the silica concentration.At Thvwhichare similarto or higherthancoexisting liq-
quartzsolubility,the temperatureof coexistence is uid-rich inclusionThe.This fact, and the skewed,
about 260C, whereasif cristobalitecontrolsthe sil- high-temperature tailson histogramplotsof Th(Fig.
ica solubility,the temperaturecan be as low as 12; likely due to two-phaseentrapment),indicate
160C (even lower for amorphoussilicaconcentra- that fluidsin thesesystems were sometimes boiling.
tions).Giventhe highlyacidfluidsin the earlystages The mean Th valuesfor Akeshi samples(elev =
of Nansatsu alteration and the isochemical dissolu- 185-250 m) rangefrom 160 to 200C, for Iwato
tion (exceptingsilica)of the rocks,the silicain solu- (elev -- 120-194 m) meanvaluesare largely180 to
tion likely exceededquartz solubility. Therefore, 220C, andfor Kasuga(elev = 90-130 m) the mean
pyrophylliteand kaolinitcmostlikely coexistedat Th valuesrangefrom 200 to 240C (Fig. 13). The
temperaturesbelow 260C, probablynear 200C wide rangesin Th for somesamplesfrom the same
wherethe two mineralsoverlapin thermalstability level of onedepositmaydue either to two-phaseen-
(Reyes,1990). Experimental results(Hemleyet al., trapmentor to actualtemperaturevariation.Tmdata
1980) suggestpyrophylliteand diasporeshouldnot for 26 inclusions from Iwato andKasugarangefrom
coexistat temperaturesless than 280C; however, 0.0 to -1.0C, with a -0.4C mean,indicatingthat
Reyes(1990, 1991) observedthe pair in texturalin- the fluidsformingthe late quartzare dilute (avg< 1
tergrowthandapparentequilibriumatmeasured tem- wt % NaC1equiv).
peraturesaslow as240Cin Philippinegeothermal Rangesand meanof Th data from thesethree de-
systems.This is consistentwith the occurrenceof positsare plotted individuallyversussampleeleva-
thesetwo minerals,commonlywith dickitc, at Ka- tion (Fig. 12). Hydrostaticboilingpoint curvesfor a
suga;they havenotbeenfoundin the otherNansatsu dilute, gas-poorfluid are constructedto envelop
deposits. mostof the lower and higher meanTh values,and
The claysin thesedepositshave basalspacings indicatethat the level of the palcowatertablewasat
slightlyshiftedfromwhite mica,due to a smallcom- about an elevation of 250 to 400 m. However, the
ponentof smectite,henceourusageofthetermillitc. watertablemayhavebeenlowerthanthe palcosur-
increasesawayfromthe facein areasof highrelief.Akeshiinclusions formed
argillichalo, and upward.Smectiteis particularly at <200C and less than 150 m below the water ta-
common withitslowertempera- ble, Iwato inclusionsformed at about 200C and 150
ture of formation. m or morebelowthe water table,andKasugainclu-
sionsformed at an averageof about 230C and as
Fluid inclusions much as 300 m below the water table.
Basedon resultsof Hashizume(1983), Th data of
Fluid inclusion data are available for vein and late
quartz crystalsin silicifiedbodiesfrom Sonomidake
quartzfromtheKasuga, Iwato,andAkeshi (2.5 km northeastof Kasuga;Fig. 3) havea meanof
quartzbodies,and alsofrom quartzveinsbeneath 235C (with 30 inclusions havinga normalhistogram
andadjacentto the Kasugaorebody,the lattersam- distribution, rangingfrom190-275C).Similarsam-
pledfromdrill core.All of the quartzsampled from ples from Kurigano(1.5 km southwestof Kasuga)
the quartz bodieswas depositedafter the initial have a mean of 200C; the 24 inclusionshave a nor-
leachingevent,with mostsamples beingpostsulfide mal histogramdistribution,ranging from 180 to
(andAu)deposition. Enargitewasexamined by infra- 230C. Quartz veinscutting ShimantoSupergroup
red microscopy,but fluid inclusionswere not found basementrocksbeneaththe Kuriganolocalityhavea
(A.R. CampbellandD.P. Mancano,pers.commun., slightlywider rangebut the samemeanTh, whereas
1992). Homogenization(Th) data of over 1,000 in- quartz veins cutting basementrocks beneath the

ation,andthepresence of calciteindicates
8''.s 25'
/ ' " 8
neutralpH fluids.Thesamplesarefrom140to 300 m
belowsealevel,withinabout200 m of thebottomof
lool _ the orebody.The averagehomogenization tempera-
tures of fluid inclusionsfrom these veins fall above
*-._.. I . %. 99 50
downward projectionsof the boilingcurveswhich
2oo originateat elevations
of 250 and400 m (Fig. 12),
I 55 " N thoughtheminimum Thvalueslie nearthecurves.
the veinsare relatedto the samesystemwhichwas
400 responsiblefortheoverlying deposit,theneitherthe
widerangesaredueto trappingoftwo-phase fluidor
the pressureswereabovehydrostatic at thisdepth.
theveinsarenotrelatedtoKasuga and
formedfrom highertemperaturefluids,either at
o pressuresabovehydrostatic or at greaterdepths be-
low thewatertable.A boilingcurveoriginating at an
-200 #s elevationof 500 m closelyapproximatesthemeanTh
Onesamplefromthe southeastmarginof the Ka-
Meters sugaorebody
(elev-- 100m)iscontained
by a major
breccia zone which cuts residual silica and contains a

a.s.,. .... L'..... Ivv

v .vvv
.,, .v .v,-
v vv 10
.. fewg/tAu.Quartzcrystals (5-10 mmlong)coated
goethiteandhematitecementthe brecciaandcon-

A ...[JJl.J..
. 66 taina varietyof fluidinclusion
in one crystal(A, Fig. 12) containtwo or
90 mL
B. ....,,,.
I.,, v,
moredaughter minerals,including halite,nativesul-
I ! fur (meltsat about120C),andpossibly
I hematite
-i o (Fig. 13a).Primaryvapor-richinclusions (withcrys-
Th* C TinC tal faceterminations;
Fig. 13b, c) are common,and
FIG. 12. Summary of fluidinclusiondataforAkeshi,Iwato,and somehomogenizeto vapor. T mmeasurements were
Kasuga(takenfrom Takenouchi,1983; Hedenquistet al., 1988; madeonover20 inclusions, includingthe condensate
Izawa and Cunningham,1989; this study).The rangeand mean in some particularlylargevapor-rich inclusions(Fig.
(up- or down-pointing triangle)of Th measurements are plotted 13b,c).TheT results foronecrystal(crystalA, 100-
versuselevationof samples (numberof measurements at eachele- m elev;Fig. 12) indicatea meanof about275C,
vationis shownby the numberin italicsat the end pointof the
range).Boilingcurves(for a dilute salinity,low gasfluid) were whereasfewermeasurements for anothercrystal(C)
fittedto thedatato envelopmostof themeanvalues.Thesecurves havemostT valuesnear225C,consistent with re-
projectto a 100Cwatertableat anelevationof about250 to 400 sultsfor othersamples nearthislevel.Valuesof Tv,
m for the threedeposits. However,the meanvaluesof Thfor inclu- largelyfor a third crystal,fall betweenthesetwo
sionsfromquartzveinsapproximately beneaththe Kasugaquartz
body(collected fromdrillcoreofDDH 2, 4, and5) arebetterfitby
a curveprojecting to a watertableat anelevation of about500 m. Theseobservations indicatethe presenceof a two-
All Tmdatafor the typicalinclusions fromIwatoandKasugaare phase fluid,onephasebeinga salineliquidandthe
plottedalongthe rightmargin(avgabout0.7 wt % NaCIequiv). othera relatively lowsalinityvapor.Onefluidinclu-
Samplehistograms of T datafromtwoKasuga samples, eachcom- sionin crystal A contains daughter crystals
prisingthreevug-fillingquartzcrystals(crytalsA, B, andC), are
alsoshown;Tvvaluesareplottedwiththe symbol"V." The 90-m with halite dissol'tion at 165C, whereas T is
elevationsampledataareconsistent withthe boilingcurves;data 274C,closeto theaverage forthelesssalineliquid-
from one crystalare skewedto highertemperatures,forminga richinclusions of thesamecrystal.Apparenthomoge-
"tail," possiblydueto someinclusions trappinga smallamountof nizationof a yellowish, roundeddaughtercrystal
vaporfroma boilingfluid.Thesamplefromthe 100-melevationis
fromthe marginalbrecciazoneandis uniquein that someinclu- coexistingwith haliteoccurs at about110to 120C,
sionsin crystalA containdaughterminerals(haliteandsulfur),and closetothemeltingtemperature ofnativesulfur.The
othershaverelativelyhighsalinities indicatedfromTmmeasure- halitedisappearance temperature indicatesa salinity
ments(twoTmvaluesof-6.4 and-7. IC are not plotted). of closeto 30 wt percentNaC1(Roedder,1984).The
Thvvaluesof vapor-rich inclusions in thiscrystalare
Kago depositcontaininclusionswith a mean of <250C, thoughthe other crystalshavehigher
205C(14 inclusionsrangingfrom 190-250C). values(Fig. 12). The condensate in someof the va-
Coresamples of quartzveinswerecollectedfrom por-richinclusions in crystalA freezesat -0.6 to
holesdrilledbeneaththe Kasugaorebody(Fig. 4). -2.4C, lower (moresaline)thanthe -0.7C mean
The veinsdonothavehalosof advancedargillicalter- for the liquid-richinclusions
in thiscrystal.

Dilute fluids(lessthan 2-4 wt % NaCI equiv)are

commonlyassociated with late, barrenquartz crys-
talsin high sulfidationdeposits.However,salinein-
clusionfluidsare sometimes noted,includingoccur-
rencesin Peru (Bruhaand Noble, 1983; Vidal et al.,
1989) and China (Ren et al., 1992). In particular,
Deen (1990) hasfoundhigh-salinityfluidsin enar-
gite-hostedinclusions from the Julcanideposit,and
preliminaryfluidinclusion dataonenargitefromLe-
pantoindicatesalinities of 12 to 20 wt percentNaCI
equiv(A.R.CampbellandD.P. Mancano,
mun., 1993), in contrastto <1 to 2 wt percentNaCI
equivin inclusions hostedby late quartz(JWH, un-
pub. results).The occurrence of salineinclusionsat
Kasuga issimilarto thatdescribed fortheRodalquilar
deposit(Sanger-von Oepenet al., 1990), whereliq-
uid-rich (2-5 wt % NaCI equiv), vapor-rich,and
daughtercrystal-bearing inclusions occur(the latter
30+ wt % NaCI equiv),with the salinityof inclusions
increasing with depth(Arribas,1992).

To examine the concentration and covariation of a
suiteof 45 elements,samples
were collectedfrom
Kasuga(10 samples),Iwato (8 samples),and Akeshi
(11 samples),coveringa rangeof Au grades(Table
1). Samplingwas restrictedto the quartz bodies,
withinandadjacentto ore zones.Samples fromKa-
plesfrom Akeshiare from underground, with sam-
plesvariablyoxidized(in particularaffectingAg,Cu,
Zn, andS).
Althoughthe numberof samplesanalyzedfrom
eachdepositissmall,theresultsarereasonably coher-
ent. Iwato is readily distinguishedfrom Kasuga,
whereasAkeshiis intermediate,thoughwith results
oftenshowinga degreeof overlapwith thosefrom
Kasuga.The dataare illlustratedby spiderplotsfor
11 elements of the ore suite which show variation
betweendeposits(Fig. 14). In particular,variationis
notedin the concentrations
of As, Sb, Bi, Cu, Pb, and
Hg, and in the ratiosof As/Sb,Sb/Bi,and Cu/Pb.
Theseareelementswhichcommonly exhibitmarked
variationwith depth in the high-levelportion of

Fc. 13. a. Photomicrograph of primaryfluid inclusions con-

tainingdaughterminerals,halite (H), andyellowish-tinted native
sulfur(S)in crystalA of thesamplefromtheKasuga breccia,100-
m elevation For the inclusionnear the ton
r, TmI11te is 165C
whereas theThl,
largerinclusionto thelowerrighthasa Tm,,,of 334C,though
thevaporbubblewasnotdosetohomogenizing. Widthofallpho-
tographsis 0.4 min.b. andc. Primaryvapor-rich
inclusions(V =
vapor,L = liquid),nearthe daughtermineral-bearinginclusions.
Th valuesof theseinclusions rangefrom 235 to 250C (with

10000- becausethis will tend to control both the minerals

and the distribution of the more volatile elements.
Fluid inclusionresults indicate that Iwato formed
about 100 m shallower and at a 20 to 30C lower
temperature thanKasuga, consistentwith the pres-
enceof dickiteat Kasuga. Thismayaccount for the
distinctionin geochemical (andmineralogical) pat-
ternsbetweenthetwodeposits, withAsandTe being
fixedat highertemperatures (atKasuga)andHg and
K depositing at lowertemperatures(theK likelyre-
flectsthepresence ofaluniteand/oraclay).Thegeo-
chemical signaturesareconsistent
withAkeshi form-
lOO ing at temperatures intermediateto IwatoandKa-
suga,thoughfluidinclusion resultsindicateAkeshi
formedat thelowesttemperature. Thismayreflecta
host-rockcontrolto traceelementenrichments(Nan-
satsu Middle Volcanics at Akeshi versus Nansatsu
Lower Formationat Kasugaand Iwato). Alterna-
mayhavebeenbiasedto marginal
zonesat Iwato where formationtemperatureswere
10000- relatively
Akeshi beenmined.Samples containinghighAu atIwatoare
alsorich in Sn,Bi, andSb (IzawaandCunningham,

K Cu Kasuga/;



Ag Au As Sb Bi Cu Pb Te Se Sn Hg

FIC. 14. Chemicaldata (Table 1) for orebodysamplesfrom 1'

Kasuga,Iwato,andAkeshi;concentrations in logmg/kg.Thereis a
markeddifferencein the chemicalpatternbetweenIwato (rela-
tively fiat), andKasugaand Akeshi(bothshapedlike an inverted 100Q- 10

W). Thisis unlikelyto be dueto weathering,asKasugais the most

in contrast
to Akeshi,whereunderground
sam- lOO.

epithermalsystems (relatedto theirvolatilityandthe

rapidly changingtemperatureof deposition;see

lb 100 1000 10000

Berger and Silberman,1985, and Silbermanand
Berger,1985, for the resultsof similarstudiesof low
sulfidationepithermaldeposits).Someof the differ-
encesbetweenthe three depositsare moreapparent
when plotted againstAs (Fig. 15). For example,
Iwato showsdistinctlylower amountsof Cu andTe
than Kasuga,with Akeshi intermediate,whereas
Iwato hasmore Hg andK. For elementssuchasCu
andK, thisreflectsthe abundanceof mineralssuchas
enargiteand claysor alunite,respectively,in the
The variationin the geochemical
signatureof the FIe. 15. Plotsof K, Cu,Te, Sn,Hg, andPbversus
Nansatsuquartzbodies(secondary oxidationaside) kg),showing thedistinction
between Iwatoandthebroadly
mayprimarilyreflectthe temperatureof formation, resultsfor KasugaandAkeshi.

1989). These geochemicalpatternscontrastwith of the originalfluidwasabout3:1. High-temperature

thoserelatedto Ag-richhighsulfidation
ore at Para- (800C)SO2-dominant gasfromthe SatsumaIwojima
disePeak,Nevada(Johnet al., 1991),whereHg, Ba, volcano,an islandsouthof the Nansatsudistrict, hasa
Bi, Pb, Sb,andSnhavehigherconcentrations thanin
ba4Svalue of about 12 per mil (Matsubayaet al.,
the Nansatsu deposits. 1975), thoughthisis affectedby the precipitationof
Stableisotopes largeamounts of nativesulfurwhichhasan isotopic
compositionof 0 to 2 per mil (Ueda et al., 1979);
weremeasuredtherefore,the totalS isotopecompositionwill lie be-
on pyrite, enargite,covellite,alunite,andnativesul- tween these two values,consistentwith the intrusive
fur withinandadjacentto the quartzbodiesof Ka- valueof 5 per mil.
suga,Iwato,andAkeshi(Table2). The pyriteanden- blSOandbDrelationships:To assess theorigin(s)of
argiteare generallyin intimatecontactin vugsand thewaterresponsible
for alterationin variouspartsof
are associatedwith Au mineralization.In contrast, the district, samplesof mineralsand whole rocks
with thesemineralswasnot found, were analyzed(Table2). One setof sampleswascol-
sothe nearestsulfides
or sulfosalts
weresampled. lected along a traverse from the center of the
The 34Svaluesof sulfides,sulfosalts,and native Maruyamaorebody2 at Iwato throughthe argillic
sulfurrangefrom0 to -5 per mil, averaging -2 per halo and into the propyliticmargin(Fig. 17). Also
mil (Fig.16).Anexception isslightlyheavyvaluesfor collectedwere samplesof residualsilicarecrystal-
twosamples offinelydisseminated pyritefromIwato; lized to quartzandquartzcrystalsat Kasuga,quartz
analysisof the bulk rock may have been contami- veinsin the Kasugaarea(fromdrill core),andquartz
natedby disseminated sulfatethat wasisotopically fromveinsonthe peripheryof the basementdepres-
heavy.In contrastto theseminerals,all hypogene sion(Fig. 3), aswell asone sampleof a quartzvein
alunitesampleshavevaluesrangingfrom 24.5 to 34 fromthe KagoAu deposit.Mineralseparates of kao-
per mil, whereasfine-grained alunitesamples in late linite, pyrophyllite,and A1 chloritefrom advanced
veinletscuttingthe argillichalohave 34Svaluesof argillichalosat KasugaandIwato were analyzed,as
about-2 per mil, similarto theaveragesulfidevalue. well asalunitefrom localitiesin and adjacentto the
These resultsare consistentwith the sulfides,sulfo- KasugaandIwato quartzbodies.
salts,andhypogenealuniteformingfromthe same The isotopicvaluesof quartz,clays,andaluniteare
acidfluidat 200 to 240C(thetemperature range shownin Figure18, plusthe compositions of coexist-
for an equilibriumfractionationof 28-25%0in 34S ing water, the latter calculatedfrom fractionation
betweensulfideandsulfatein the fluid;Ohmotoand factorsandan assessment of temperature(basedon
Rye, 1979). In contrast, the late veinlet alunite fluidinclusionandS isotoperesults,andmineralogi-
formedfromthe low-temperature (nonequilibrium)cal assemblage; Table 2). The residualsilicaquartz
oxidation of sulfidesimilarin isotopiccomposition to samplesfrom Kasugaand Iwato have relativelyuni-
the sulfide minerals. formb80values,indicatinga rangeof watercompo-
Althoughtextural evidencefor equilibriumbe- sitionfrom -2 to +2 per mil (basedon fractionation
tween the sulfideand sulfatemineralsis lacking, factorsof Matsuhisa et al., 1979, anda temperature
theseresultsare similarto thosefor hypogenesul- rangeof 200-230C estimatedfrom the S isotope
fides and sulfatesfrom high sulfidationsystems results).Quartz crystalsin vugsof the quartzbodies
wheretexuralrelationships suggest equilibriumwas andlater veinletshavethe samecomposition asthe
established (e.g., Marysvale,Utah, Cunninghamet residual silica quartz. The deep veins at Kasuga
al., 1984; Lepanto,Hedenquistand Garcia, 1990; (270C) and the peripheral veins (150-180C)
Summitville,Rye et al., 1992; Rodalquilar,Arribas, have80 compositions indicatinglighterisotopic val-
1992). The equilibriumtemperaturescalculatedare ues for their waters,lessthan 0 per mil. The Kago
consistentwith the temperaturesestimatedfrom vein sample (180-200C) has the lightest (O
fluid inclusionsin quartz that formedafter the sul- value,consistent with equilibrationwith present-day
fidesandsulfosalts;bothfluidinclusion andSisotope local meteoric waters (/1O -- -7.3%0 and /D --
datafromIwatoindicateslightlycoolertemperatures -48%0; Matsubayaet al., 1975).
of formationthanfor Kasuga. The kaoliniteandpyrophyllitesampleswere puri-
The totalSisotopecomposition of the originalfluid fied by sedimentationandcheckedby X-ray diffrac-
is not known.However,freshmagnetiteseriesintru- tometry to ensure that they were nearly free of
sionsofJapanhaveanaverage(34S valueof 5 permil quartzand other minerals.Their bsOvalueshavea
(Sasakiand Ishihara,1979). Assuming the freshin- rangeof about5 per mil, whereasthe bDvaluesfallin
trusivevalue of 5 per mil for the total ba4Sof the a narrowrangeof-69 to -72 per mil. Usingthe frac-
Nansatsufluids,an isotopicmassbalanceusingan tionationfactorsof Marumoet al. (1980), basedon
averageof-2 per mil for the sulfideand+26 per mil claysandwatersfrom geothermalsystems,the calcu-
for the sulfateindicatesthat the sulfide/sulfateratio latedfluidshavea bD valueof about-50 to -55 per

2. IsotopicCompositions
of Nansatsu

sS sO D
Sample Location Mineral (%0) (%0) (%0) T (C) T basis

6Feb87-5 90 mL Pyrite, diss. 5.5
6Feb87-6 100 mL Pyrite, diss. 3.2
6Feb87-12 100 mL Pyrite -0.2
6Feb87-12 100 mL Enargite -0.1
6Feb87-12 100 mL Covellite -2.2
6Feb87-12 100 mL Sulfur -2.3
Tokunaga 30 mL (?) Alunite 30.7
901012-4 Komatsugiyama, Alunite 24.2 6.6 -52 240 AI-Py= 24.4
1.5 km NE of Kasuga
833014 Uppermostlevel Alunite 25.6
6Feb87-1 80 mL Resid. silica 9.3 230 FI + SI
6Feb87-7 100 mL Resid. silica 11.2 230 FI + SI
6Feb87-12 100 mL Resid. silica 11.1 230 FI + SI
6Feb87-13 100 mL vug Quartzcrystal 11.9 230 FI + SI
DD5-230.4m 0 mL Resid. silica 8.4 230 FI + SI
DD2-285.5m -140 mL vein Quartzv. 2.7 270 FI
DD4-618.m -300 mL vein Quartzv. 5.1 290 FI
880307-3 100 mL vein Quartzv. 5.8 230 FI
6Feb87-8 100 mL Kaol+ pyroph<1 m 4.8 -69 230 FI + SI + Min
6Feb87-8 100 mL Clay whole rock 10.2
6Feb87-9 100 mL Kaol+ pyroph<1 m 6.7 -71 230 FI + SI + Min
6Feb87-25 110 mL Pyrophtriclinic 6.0 -72 230 FI + SI + Min
6Feb87-27 110 mL Pyrophmonoclinic 7.9 -71 230 FI + SI + Min
6Feb87-28 110 mL A1 chlorite 7.9 -72 230 FI + SI + Min
5Feb87-2 Iwashita191 mL Pyrite -0.5
5Feb87-4 Iwashita 170 mL Sulfur -0.8
5Feb87-15 Maruyama2 160 mL Pyrite -3.7
5Feb87-20 N. outcrop,sediment Pyrite -5.4
85062108 Iwashita177 mL Alunite 27.5 13.0 lost 200 AI-Py = 28
2708E Maruyama2 160 mL Alunitev. -1.8
5Feb87-16 Maruyama2 160 mL Alunitev. -2.0 7.6 -15 100-180 Assumed
5Feb87-21 1 km N, vein Alunitev, 28.7 15.5 -38 200 AI-Py = 28
Sakai-1 Arabira 90 mL Alunite 32.4 10.4
Sakai-2 Arabira 90 mL Alunite 32.0 11.8
Sakai-3 Arabira 90 mL Alunite 34.0 9.2
833006 Iwashita Alunite 30.5
5Feb87-10 Maruyama2 160 mL Resid.silica 10.3 200 FI + SI
5Feb87-11 Maruyama2 160 mL Resid.silica 11.0 200 FI + SI
5Feb87-12 Maruyama2 160 mL Resid.silica 11.0 200 FI + SI
5Feb87-13 Maruyama2 160 mL Resid.silica 11.0 200 FI + SI
5Feb87-14 Maruyama2 160 mL Resid.silica 10.1 200 FI + SI
5Feb87-14 Maruyama2 160 mL Quartzv. 10.3 200 FI + SI
83040601 Maruyama Resid.silica 10.3 200 FI + SI
83040601 Maruyamavein Quartzv. 9.9 200 FI + SI
5Feb87-18 Maruyama2 160 mL Kaol + mont + qtz 7.7
5Feb87-19 Maruyama2 160 mL Kaol< 1 m 10.1 -67 200 FI + SI + Min
5Feb87-19 Maruyama2 160 mL Claywholerock 13.8
5Feb87-5 Maruyama2 160 mL Propandesitc 7.4
7Feb87-2 N of Iwato Fresh andesitc 7.9
6Feb87-17 -50 mL Pyrite -2.8
6Feb87-17 -50 mL Sulfur -1.5
880309-1 2.8 km N of Kasuga,
v. Quartzv. 13.1 150 Smectite/illite
DD62MANU2 170.4 m, v. Quartzv. 11.5 (280) FI
880308-2 1 km NW of Kasuga,v. Quartzv. 12.5 180 Wair., laumon.
880308-1 Coast,0.5 kmSEof Quartzv. 11.7 150 Chabaz.,stilb.
880307-13 Kagov. Quartzv. 5.6 1800-200 FI
DD62MANU3 212.8 m, Pb-Znv. Quartz v. 7.9 2700-280 FI

Formation temperatures (TC)usedtocalculate fluidcompositions

plottedin Figure19havebeenestimated basedonmeanfluidinclusion Thn,sulfur
(SI),andmineralassemblage (Min);thepermildifference betweenaluniteandpyrite(AI-Py)islistedfor
somesamples of alunite,whereasthemineralassemblage (claysandzeolites)
aregivenforsamples awayfromthedeposits; lsOaunite
Abbreviations: diamonddrill hole = DD, disseminated= diss.,mL = sampleelevationin m, v = vein, chabazite= chabaz.,laumontite= laumon.,
montmorillonite = mont,propylitic= prop,pyrophyllite= pyroph,quartz= qtz, residualsilica= resid.silica,stilbite= stilb.

[] Py [] En [] Cv [] S AI

d i

Akeshi Steam-heate O Alunite

fluid/. SMOW
CI CI Kasuga m

IwatoI IBl

volcamc flutds

0 0
6 a4S%0 -5O

FIG. 16. Summaryof sulfurisotopedatafor the Nansatsu


per mil (Sasakiand Ishihara,1979), whereassulfidesin the low

5 / O-shifrClayduid
*e 0
sulfidationepithermalgoldveindepositat nearbyHishikariaver-
age0.3 per mil (Ishiharaet al., 1986).Datatbr pyrite(Py),enar-
gite (En), covellite(Cv), nativesulfur(S),and alunite(A1)are
-lOO I I / I
shown;someKasuga pyritesamples weredisseminated (diss)and
mayhavebeencontaminated by sulfateminerals. Residual
Quartz veins
mil at 200C, similarto the present-daylocal me- Deepatveins
teoric water; however, the 680 value is shifted
(enriched)by over8 per mil. Useof alternativefrac- 000 Peripheral
tionationfactorssuggested by O'Neil (1986) results 0 Kago veins
in a 6D valueof-70 per mil for the fluids,toolightto
explainby anyknownwateror process.
Residual silica and vein quartz
The three hypogenealuniteswhich were pure
enoughfor isotopicanalysis indicatea differenttrend Kasuga 0 Other localities
for their associatedwaters (Fig. 18). Based on O Iwato Calculated fluids

and i I i
givenby Stoffregen
(1991),andtempera- -10 0 +10 +20
tures of 200 and 240C (for Iwato and Kasuga, 80 %0
FIG. 18. Diagramshowingthe resultsof isotopicanalysis of
residualsilica(nowrecrystallized to quartz)andquartzcrystalsor
veins(sO only,plottedonthebottom),andclaysandalunite(D
Pyroxeneandesite vs.sO, plottedon the top).The calculatedcomposition of the
fluidsin equilibriumwiththeseminerals,plusthe compositions of
Tuffbrecc,a local meteoricwater (smallopen square)and high-temperature
volcanicfluids(largeopensquare)are alsoshown(Matsuoet al.,
1974; Matsubaya et al., 1975). A least-squaresfit line (dashed)
Sample point throughthehypogene alunitefluidsandthehigh-temperature vol-
canicfluid end memberextendsto an isotopiccomposition similar
to presentlocalmeteoricwaterandidenticalin D valuesto the
clayfluid.Thustheisotopic compositionof alunites recordmixing
of magmatic andmeteoricwaters,whereas the marginalclays(and
13 e12 possibly the veinquartzandresidualsilicaquartz)indicatethat
1 ;'o0 a meteoricwater dominatedon the marginsof the quartzbodies,
variablyshiftedin oxygenisotopecomposition due to exchange
Quartz vein with wall rocks.Someof the deepfluidsresponsible for veinfor-
ArGdkzed mationare identicalin isotopiccomposition to the SO-enriched
7r Propyitic,zone fluid that equilibratedwith the residualsilicaquartz, whereas
6 zone Quartz body
othersamples indicatea greaterproportionof unshiftedmeteoric
0 10 20 30 40 50 6b 70 water. One vein alunite from Iwato hasan isotopiccomposition
Distance m
which indicates that it formed in a steam-heated environment after
FIG.] 7. Plansketchof the Maruyamaopenpit '2,Iwato,show- a steam-heated temperaturerangeof 100-180C).K andI de-
ingthe rocktypes(pyroxene andesitclavaandtuffbreccia),alter- noteKasugaandIwato, respectively.
ationzoning,andsampling pointsfor a traversefromthe quartz
bodythroughthe argillichaloto propyliticalterationalongthe
west wall of the 160-m elevation. The results of sO values of
(allresidualsilicaquartzexceptfor onequartzvein, respectively,
thesesamples basedon S isotoperesults),the compo-
andthe propylitizedwholerock)are shown.Thereis noisotopic sitionof fluidsresponsiblefor formingthe alunites
zoningapparentacrossthe quartzbody. wascalculated.The Iwato fluid is relativelyheavyin

both80 andD, andissimilarto the composition of (Fig. 19). This informationmay be usedalongwith
high-temperature volcanicgasnowdischarging from fluid inclusionand stableisotopedatato determine
nearbySatsuma Iwojima(Matsuoet al., 1974; Mat- the evolution of the fluid composition.Effective
subayaet al., 1975;Shinohara
et al., 1993) andother leachingof components from the hostrocksduring
island-arcvolcanoes (Giggenbach, 1992a). The Ka- the initialstagesof activityrequiresa pH of lessthan
sugasamplefallson a mixingtrend betweenhigh- about 2 for aluminumto be soluble(Stoffregen,
temperaturevolcanicfluidsandlocalmeteoricwater. 1987). Thisextremeacidityisdueto the presenceof
Thistrendof mixingbetweenvolcaniccondensates HC1andH2SO4,bothof volcanicorigin.The narrow
and meteoric water is similar to that noted for fumar- alunite-kaolinite zone(generally1-2 m wide at Nan-
olicvapor(containing HC1)andrelatedacidfluidsat satsu;Figs.5 and8) maybe attributedto the narrow
the KirishimaandEsanvolcanoes in Japan(Heden- rangeof pH overwhichkaolinitcis stable,between
quistandAoki, 1991) andelsewherearoundthe cir- alunite and K mica (illitc or mixed layered illite-
cumPacific(Giggenbach, 1992a).A component of smectiteclays).Thisprogressive neutralizationby re-
magmaticwater containingacid volatilesmusthave actionwith the wall rock was noted by Stevenand
beenpresentin theNansatsu hydrothermal systems,Ratte (1960) in their studyof Summitville,andwas
atleastduringtheearlystages ofleaching andforma- confirmedby experimentalstudiesby Hemleyet al.
tionofalunite. However, thismagmatic watercompo- (1969).
nent clearlymixedwith meteoricwaters,evenin the Basedonthe mineralassemblage of pyrophyllite_
early (alunite)stage,whereasmeteoricwater domi- dickitc_ kaolinitcandalunite+ pyrite,the tempera-
nated in the marginalzone of argillicalteration. ture andredoxpotentialof the earlyfluidresponsible
Withoutinformation onthe deuteriumcompositionfor leachingis constrained (Fig. 20). The sulfide-sul-
of fluidsrelatedto the residualsilicaquartzand fate S isotopebalanceindicatesthat the fluidswere
quartz crystal samples,we cannot assesswhether slightlysulfidedominatedduringdeposition of alun-
thesefluidslie on a volcanic(magmatic)-meteoric itc andpyrite. This is consistentwith the fluid com-
mixingtrendor are simplyoxygen-shifted fromme- position deduced from the mineral assemblage.
teoric water values. It is also difficult to assessthe Basedon the data presentedand later discussion of
originof the fluidsresponsible for the lowsulfidation
quartzveinsin the district.The veinsperipheralto
Kasuga(alongthe marginof the basement depres- Time '

sion)were formedby waterslighterin O isotope

Highly reactive Mineralization Supergene
compositionthanthosewhichequilibratedwith the
alarger Magmatic fluid
meteoric water componentin the former, whereas Liquid
the fluidof the Kagoveinquartzwassimilarto the Meteoric water
localmeteoricwatercomposition (Fig.18).
The late-stagevein alunitefrom Iwato hasa 34S Permeability
development Leaching Brecciation
valuesimilarto that of sulfides,indicatingit has
Marginal halo
formedfromoxidation ofsulfideatatemperature too
low for fractionation to occur. The calculated 180 Quartz

valuefor its parentwaterliesnearbut to the left of Aiunite

atempera- Pyrite
ture rangeof 100 to 180C(i.e., steam-heated con-
ditions).If this formedfrom oxidationof sulfidesat Enargite
the calcu-
latedvaluewouldplot evenfartherto the left of the Gold (electrum)
meteoricwaterline.The largeD shiftfromlocalme- Coveilite
teoricwaterof thisparentalunitewaterisconsistent Sulfur
witha steam-heated origin,withisotopic enrichment
alonga nonequilibrium trendsimilarto thatnotedfor Goethite etc.
someactivegeothermalsystems(Henleyand Stew- FIG.19. Approximate paragenetic
sequenceof mineraldeposi-
art, 1983).Therefore,a portionofthe sulfidemineral tionandotherfeaturesin theNansatsudeposits.
In theinitialstage
oxidationin theseorebodies maybe dueto latesteam of thehydrothermalsystems, condensation
of magmaticvaporinto
ratherthanallbeingrelatedto weathering. meteoricwaterwasresponsible
heating, fordeveloping
that led to extensiverock leaching.The systemthen evolved
andmineral-fluidequilibria throughto the stagewheremeteoricdilutionof a metal-bearing
magmatic liquidcaused mineralization.
Latesupergene processes,
TheredoxstateandpH ofthefluidmaybeassessedsteam-heated activity,andweathering,resultedin oxidationof sul-
onthebasisof mineralassemblages
andparagenesisfideminerals,causinglocalremobilizationof gold.

The mineralizationwaslikely associated

with a saline
liquid,basedon sparsefluid inclusionevidenceand
Rock buffer the analogywith othersimilardepositswherethereis
more conclusiveevidence. However, the redox state
Low sulfidation of the salineliquid was likely similarto that of the
Au-Ag deposits early vapor, given the constancyof sulfideba4S
I 10 values.
Au (/zg/kg) 0.001 The mineralizationstagewasfollowedby deposi-
2 I tion of covelliteandthen nativesulfur(Fig. 19). This
I sequenceof mineralsis constantin all locationsob-
H2S servedat the threedeposits. Relativelyoxidizedcon-
ditionsprevailedduringwaningof hydrothermalac-
tivity andlater, asindicatedby the oxidationof sul-
fides to goethite, hematite, and scorodite; the
occurrence of late alunite indicates acid conditions,
andits lSOandD isotopecomposition suggeststhat
thiswasa periodof steam-heated activity.Duringox-
High sulfidation idationof sulfides(causedby steam-heating and/or
Cu-Au deposits weathering),someprimaryAu wasremobilizedinto
high-gradestructures,acquiringa high finenessin
the process(Urashimaet al., 1981).

-7 / '" /
H2SO3 A Model for the Formation of High Sulfidation
Mineral Deposits
The spatial,andpossiblygenetic,relationship be-
/// /
tween deep-seatedporphyryCu depositsand shal-
Crater lakes /' HSO4- low, high sulfidationCu-Au depositshasbeen dis-
10 ' 20 300 400 cussedby several authors (Sillitoe, 1973, 1983,
1989, 1991; Knight, 1977; Brimhall and Ghiorso,
Temperature(C) 1983). Salineliquidsare commonin the porphyryen-
FIG.20. Diagramofredoxpotential
(R}= 1ogf,/f,o)versus vironment,ubiquitouslyassociated with a low-den-
temperature(modifiedfromGiggenbach, 1991, 1992b,in press). sity vaporphase(Roedder,1984). The behaviorof
The mineralstabilityfieldsallowanestimateof the composition of these deep magmaticfluidshas been modeledby
the Nansatsu fluids.The high-temperature redoxstateis initially Henley and McNabb (1978), who suggestthat the
governedby the volcanicSO2/H2Sgasbuffer.As the condensed
vaporbeginsto reactwith the rock at temperatures< 400C, S- low-densityvaporcommonlyseparates fromthe par-
containingmineralsstartto formandredoxpotentialsmaybe gov- ent fluidanddischarges to the surfaceasvolcanicfu-
ernedby thecoexistence of alunite+ pyrite(arrows).Furthercool- maroles,leavinga high-density liquidat depth.Based
ingcauses increaseddissociationof acidsandincreasedleachingof on recent studiesof active volcanoes,Giggenbach
the hostrock.Subsequent ascentof a saline,metal-bearing liquid (1987), Hedenquistand Aoki (1991), Hedenquistet
followsa similarchemicalpath.The line of isomolarcoexistence of
HAu(SH)2andAuCI (lineof shortheavydashes) iscalculatedfora al. (1993), andShinoharaet al. (1993) observedthat
pH of 3 and a CI concentration of 1 wt percent(Giggenbach, in high-temperature fumarolesandrelatedacidwaters
press).The sameline appliesto a liquidwith a pH of 1 or 2 andC1 on the flanks of some volcanoes are derived from the
of 0.1 or 0.3 wt percent,or a pH of 4 or 5 and C1of 3 or 10 wt low-salinity magmaticvaporphase,formingchemical
percent,respectively.Parallellinescanbe drawnat the sameC1
concentration, with pH decreasing one unit for every2 log unit environments similarto thosein highsulfidationsys-
increasein Ra. Thesecalculations suggestthatC1complexing may tems.
Christenson andWood(1993) providegoodev-
dominateAu transportunderacid(pH < 3) andsaline(C1> 1 wt idence in the compositional variation of Ruapehu
%) conditionsat pyrite-alunitestability. Solubilitiesof Au as craterlake, New Zealand,for the existenceof a high
HAu(SH)a(in #g/kg)are plottedasverticaldashedlines(Giggen- sulfidation environment beneath the lake, with the
bach,1992b).The environment of low sulfidationAu mineraliza-
tion is also shown. lake'scomposition
affectedby magmaticvapordis-
charges.These are amongthe studiesthat have in-
fluencedthe modelwe presenthere for the forma-
tion of the Nansatsuand similardeposits.
the model,the earlyleachingwascausedby conden- The geologicand geochemicalconstraintson the
sationof a low-salinitybut gas-richvolcanicvapor nature of the hydrothermalsystemresponsiblefor
into meteoricwater.The depositionof enargiteand formingthe Nansatsu depositsare listedin Table 3.
Au occurredafter the initial leaching,formationof Clearlywe mustinvokethe involvementof high-tem-
the argillichalo,anddeposition of aluniteandpyrite. peraturefluidsrelatedto volcanicactivity,not only

TaBa3. GeologicandGeochemicalConstraintson the Nansatsu by the magmaticfluidandinvolvesS in two oxidation

Systems states,essentially SO (+4) and HS (-2), whereas
the other involvesthe FeIm and FeImin the rock;
Constraint Implications
these are the gasand rock redoxbuffers,respec-
Geologic Shallowdepth(epithermal);proximityto tively.
reconstruction volcanic vents and inferred relation to In the modelpresentedhere,the startingpointis a
underlyingmagmabodies magmatichydrothermal systemat a depthof a few
Radiometric Hydrothermalsystembroadly
dating contemporaneous with volcanism(related
kilometers,associated with a recent magmaticintru-
to late-stagemagmatism0.5 m.y. after sion(Burnham, 1979).Thedeepfluidwill separate at
eruptionof hostvolcanics) pressures < 1 kbarinto low-densityvaporandhigh-
Orebodyshape Relatedto permeabilitywith lithologic densityliquid (Pitzer and Pabalan,1986), asnoted
controlof fluidflowwherepermeableunits fromthe studyof fluidinclusions associatedwithpor-
control phyry Cu deposits.Fluid inclusions with daughter
Alteration Initial leachingof hostrockby veryacid(pH crystals (commonly includingchalcopyrite)areubiq-
mineralogy < 2) fluids,neutralizedby wall-rock uitousin the porphyryenvironment andindicatesa-
linities of 40 to 60 wt percent NaCI equiv. They
Ore gradescontained onlyby residualsilica
distribution quartz; lack of ore association with usuallycoexistwith gas-richvapor-dominant inclu-
and marginalclay halo indicateswall-rock sions(Roedder,1984). The volatilecomponents in-
association interactionnot important;goldclosely clude CO, SO, HzS, HC1, and HF, the dominant
associated with enargiteandpyrite; gasestypicalof volcanicdischarges (Giggenbach et
variablefracturecontrol,particularlyto al., 1986). The low-densityphase will containrela-
late remobilization
Fluid inclusions Temperatureaftersulfidedeposition200 to tively low concentrations of metalssuchasCu and
240Cin silicabodies,diluteboilingfluids; Au, since metals tend to fractionateinto the saline
depthbelowpalcowatertable100 to 300 liquid, alongwith NaC1,KCI, and other chlorides
m; evidencefor early salineliquid, (LagacheandWeisbrod,1977; Pitzer andPabalan,
probablysourceof metals
Stableisotopes Aluniteindicatesmagmaticwatercomponent 1986; Williamset al., 1991); unlikethe other chlo-
in mostacidpartof system,progressively rides, HCI partitionsto the vapor (H. Shinohara,
diluted with meteoric water, which pers. commun.,1993). This experimentally
dominatedin argillichalooutward; mined difference in metal content between vapor
entrainment of meteoric water also in silica
body responsiblefor mineralization;
andliquidis alsoconsistent with the observationof
magmaticsourceof SO (andHC1) for relatively metal-richfluids releasedfrom magmas
acidityandsulfur duringvolcaniceruptions(Hedenquistet al., 1993),
in contrastto the low metal concentrations
in high-
temperaturebut low-pressure
to generatethe extremeaciditynecessary for the ex- passively
degassing volcanoes
(Hedenquist andLo-
tensiveleachingbut alsoto accountfor the isotopic wenstern, is unlikelythatvol-
signatures of the hypogenealunite.However,there canicvaporsaresolelyresponsible
for mineralization
is alsoisotopicevidencefor the involvementof me- in this environment,as suggestedby Vennemannet
al. (1993) andothers,giventhe low metalfluxasso-
teoricwater,particularlyon the marginsof the resid-
ualsilicaquartzbodyduringformation of argillical- ciated with the low-pressurevapors.At pressures
teration,andafterleachingwithinthe quartzbody. higherthan thosepresentin the high sulfidation
The intimate associationof Au and Cu at Nansatsu epithermalenvironment,however,vaporscan con-
andin similarhighsulfidation deposits
with tain significantmetalconcentrations
(Hemleyet al.,
that of the low sulfidationenvironment,where Cu is 1992),dueto the largepressureeffectonthe distri-
notassociated withAumineralization,implyingbasic butionof components betweenvaporandsalineliq-
differences in the chemistryof metaltransportbe- uid (H. ShinoharaandK. Fujimoto,pers.commun.,
tweenthesetwo ore depositenvironments.
Here we 1993).
deposits, The vaporphaseis moremobilethanthe high-sa-
stressing the intimate associationof Au and Cu linity liquid,andbecauseof its relatively]owviscos-
(White,1991),withtherecentunderstanding of the ity anddensitycanpassfromthe environmentoflith-
factorscontrollingthe evolutionof volcanicfluids ostaticpressurethroughrockwhichis otherwiseim-
(Giggenbach,1991, 1992b).Thetwomajorcontrol- permeableto the dense,sa]ineliquid. When the
variablesinthehighsulfidation environ- gas-richvapor condensesinto groundwater (Fig.
mentare redoxpotentialand acidity(Giggenbach,g1a),SOwill disproportionate according to thereac-
1991, 1992b), with two end-memberbuffers in- tion 4SO + 4H20 = 3HSO4 + H2S (cf. Sakaiand
theredoxpotential ofmagmatic hydrother- Matsubaya,1977; Kiyosuand Kurahashi,1983). As
malfluids(Giggenbach, 1987).The firstis imposed temperaturedecreases to below300to 350C,both

a. Initial stage promotingthe influxof groundwater.An outward-

and upward-expanding alterationzone results,with
its rootscoincidingwith the zone where ascending
vaporscondenseinto groundwater and the acids
startto dissociate,hencethe characteristic upward
flaringof acidalteration(Fig. 2lb). An advancedar-
Vapor phase gilliczoneof aluniteanddickiteor kaolinite_+pyro-
Liquid phase
phylliteformson the marginof the reactionzone,
andasleachingprogresses, the zoneof residualsilica
Meteoric water
The dense,high-salinity, andmetal-bearing liquid
b. Highlyreactivestage will initially tend to remain at depth, adjacentto its
parent intrusion. However, if the lithostatic-pres-
suredsystemfracturesdueto tectonismor continued
..--{ Margin
L,[. I fluid
crystallizationof the intrusion(Burnham,1979), the
high-density liquidmaybe drivenupwardalongfrac-
tureswhichhavepreviouslybeen alteredby the va-
por condensate. During ascentthe liquid continues
to form a vaporphaseasthe pressuredecreases. A
/' ' IMixed
__ pH __Meteodc
portionof the components in thisfluidmayoriginate
from the wall rock once leachingbegins (Reed,
1992). The redoxstateof thisfluidmayalsobe traced
C. Mineralization stage in Figure 20, asboth it and the earlier vaporphase
will tendto be constrained by the SO2/HSgasbuffer
(Giggenbach, 1991) at high temperatures and high
fluid to rock ratios. As the fluid cools below 300C
reactionwith the wall rockgivesriseto the formation
of sulfate and sulfide minerals, with the redox state
beinggovernedby a pyrite-aluniteassemblage. This
suggestionis consistent
with the S isotopemassbal-
ancenotedfor deposits of thistype(onlyslightlysul-
fidedominated; Rye et al., 1992).Alternatively,the
coolingpathmaybe morereducingwithpyriteasthe
FIc. 21. Modelingof the differentstagesof evolutionof the predominantS-containingmineral (Giggenbach,
a Nansatsu-type
ore 1992b).
deposit(f?omWhite, 1991). a. Magmaticgases(HCI, SO2,H2S, Whenthe metal-bearing salineliquidascendsinto
etc.)initiallyrisealonga fracturein a low-density
vaporandcon- the porousleachedzone (Fig. 21c), mineralization
denseinto meteoricwater,heatingandacidifyingthe water.b.
Thisleadsto the leachingof the hostrockanddevelopment of a mayoccur.Giggenbach (1991, 1992b) modeledthe
neutralization halo(inset),with increasedpermeability
favoring transportof goldasHAu(SH)in anacidsolution(Se-
moremeteoricwater involvement. c. Subsequently
a magmatic, ward, 1973; Shenberger andBarnes,1989; Hayashi
metal-bearing salineliquidreaches theleachedzone.Mixingwith andOhmoto,1991).Othershavesuggested Au trans-
meteoricwater causesmineraldepositionandmineralization.
tivityin thesystem
wanes,leadingto supergene
pro- port asa chloridecomplexunderacidandoxidizing
cesses becoming dominant,
metals. conditions,thoughthere are yet few experimental
data for the appropriateconditions(Helgeson,
1969). Usingthe availabledata,the isomolarcoexis-
tenceof HAu(SH)andAuCI hasbeencalculatedfor
HC1 and H2SO4 in the condensate will increasingly a pH of 3 anda C1concentration of 1 wt percent(Fig.
dissociate(RuayaandSeward,1987). The resulting 20; Giggenbach, in press).HAu(SH)dominates over
acid watersisochemically leach most components AuCIcomplexing athigherpH andRi(logfx-i/fI-io,
fromthe hostrockat <300C (Fig.2lb), leavingan i.e., morereducingconditions)andlower C1concen-
amorphous silicaresidue.For example,acidconden- tration. However, new fluid inclusionevidence indi-
satesthatdischarge fromhot springsonWhite Island catesthathighersalinityliquids(in excess of 10 wt %
havea pH of <1 andcontainup to 2,000 mg/kgFe+3 NaC1equiv)are associated with Cu andAu mineral-
and similarconcentrations of A1 (Giggenbach and ization in the the high sulfidationenvironment.
Glasby,1977; Giggenbachand Sheppard,1989). Therefore,AuCI (or a similarcomplex)maydomi-
Thisdissolution ofthehostrockenhances permeabil- nateat the pH andredoxconditions of pyrite-alunite
ity (BrimhallandGhiorso,1983; Stoffregen, 1987), stabilityin the temperature rangeof 200 to 300C

and at a C1concentration > 1 wt percent(Fig. 20). be explainedby ourmodelif the metal-bearing saline
Nevertheless,the confirmationof this suggestion liquid neverreachesthe level of the quartz-alunite
awaitsmore reliable experimentaldata on chloride body,formedby the vaporcondensates (thoughthe
complexes of Au underacidandsalineconditionsat leached rocks can be enriched in volatile elements
temperaturesup to 300C. Cooling,possiblydue to suchasHg, As, and Sb).This situationmay occurif
mixingwith groundwater,maybe largelyresponsi- the lithostatic-pressured saline liquid (Burnham,
ble for Au deposition. For example,withinthepyrite 1979) is not releasedby fracturing,or if the highre-
stabilityfield, Au solubilityas HAu(SH).decreases lief of somestratovolcanoes causesa hydraulicgra-
by overtwoordersof magnitudefrom300to 220C dientthatpreventsthe densephasefromrisingto the
(Fig. 20; Giggenbach, 1992b);a similarsolubilityde- level of leaching.
creasewill alsooccurupon coolingif Au is trans- The modelpresentedhere requiresearly leaching
portedasa chloridecomplex. by a vaporcondensed intogroundwater,followedby
Eventuallythe magmatiesystemwill no longer ascentof a metal-bearingsalineliquid, and is sup-
supplythe densemetal-richliquid, due to resealing portedby the emergingfluid inclusionevidencefor
at depth and/or solidificationof the intrusion.The the presenceof a salineliquid in this environment.
finalstageof activity(subsequent to Fig. 21c) occurs The low concentrations and fluxes of metals in low-
oncethe systemis invadedby groundwater.During salinityvaporsof high-temperature volcanicfumar-
thiswaningstage,progressively moreoxidizedassem- oles(Hedenquist andLowenstern,
blageswill becomestableat lower temperature,in- suggest that a salineliquid is responsible for metal
eludingcorellite and native sulfur (Fig. 19); early transportat lowpressures. Infraredstudyofenargite-
formedsulfidesandsulfosalts mayalsobe oxidized. hostedfluidinclusions, nowin progress onsimilarde-
Subsequentweathering also contributesto over- posits,will helpfurtherto characterize the salinityof
printingof the primarymineralassemblage. fluidsresponsible for highsulfidation mineralization.
This model agreeswith observations of alteration
and mineralizationat Nansatsu(Table 3) and else- Summaryand Conclusions
where and is supportedby isotopicand fluid inclu- High sulfidationCu-Aumineralizationin the Nan-
sion data. Gold is relatively concentratednear the satsudistrictformedabout0.5 m.y. afterthe volcanic
center of the quartz bodies, closestto fracture hostrockswere erupted,probablywithin a few kilo-
(feeder)zones,with a decreasein gradetowardthe metersof volcanicvents.The surfaceexpression of
margins.Thisisconsistent with a decreasein the tem- thesesystems, while active,likely consistedof high-
peraturetowardthe marginsof the quartzbody as temperaturefumarolesand acidsprings.Early stage
the amount of meteoric water entrainment increases. alterationresultedfrom condensation of thesemag-
If the degreeof reactionwith thehostrock(affecting maticvaporsinto meteoricwaters.This formedacid
pH) were a majorcontrolon goldmineralization, the watersthat leachedthe hostandesite,mushrooming
highestgradeswould be expectedto occur on the where permeable pyroclasticunits were encoun-
marginsof the quartzbodies,associated with theclay tered.The centralupfiowregionwasleachedof most
halos;this is not so. The introduction of the Cu and rock components, leavingan amorphoussilicaresi-
Au by the salineliquid(bothpossiblytransported as due (subsequently recrystallized to quartz),whereas
chloridecomplexes) accounts for the intimateCu-Au the reactionzonehaloof alunite,pyrite, dickite,and
associationin these deposits.This association,and pyrophylliteexpandedwith continuedleachingof
the generaldecreasein Au gradestowardthe mar- the hostrock andpreviouslyformedalterationmin-
ginsof the quartzbodies,indicatesthat early high erals.The vaporseparatedfrom a salineliquid adja-
sulfidation Cu mineralization is not overprintedby a cent to the magma,and subsequentfracturingal-
later episodeof low sulfidationAu mineralization,as lowed the denseliquid to rise, transportingmetals
suggested by Berger and Henley (1989). The inti- underrelativelyoxidizingconditionsandpossiblyas
mate association of acid minerals and Au at Pueblo chloridecomplexes. Becausethis metal-bearingliq-
Viejo (Munteanet al., 1990) alsodoesnot support uid mixedwith meteoricwateroccupyingthe highly
the late introduction of low sulfidation fluids. permeablequartz body, enargite and Au precipi-
At Ugusu,on the Izu peninsulaof Japan(Iwao, tated, the latter largely due to decreasingtempera-
1962, 1963), the silicabodyandits argilliehaloap- ture causedby dilution;covelliteand sulfurdeposi-
pearidenticalto theNansatsu deposits, including iso- tion followed.Once the magmaticliquid no longer
topic characteristics (our unpublished results),but ascended,groundwater collapsedinto the system.
lackenargiteandAu mineralization
(Au < 0.2 g/t). This caused oxidization of the sulfides and sulfosalts
Similarly,extensiveareasof quartz-alunitealteration andformationof late vein alunite;it mayhavebeen
are commonalong the California-Nevadaborder, accompanied by someremobilization of Au intofrac-
thoughonly a few are mineralizedwith Au (H.F. tures.Erosionof 150 to 250 m of overlyingargillic
Bonham,Jr.,pers.commun.,1993).Theseareascan alterationduring the last 3 to 5 m.y. exposedthe

ridge-formingquartzbodiesto weatheringandcon-
tinued oxidation.
Aoki,M., 1991, Mineralogical featuresandgenesisof alunitesolid
for highsulfi- solutionin hightemperaturemagmatichydrothermalsystems:
dation mineralization to occur: GeologicalSurveyof JapanReport277, p. 35-38.
ArribasR.A., Jr., 1992, Geologyandgeochemistry of the Rodal-
1. A crystallizingmagmamust saturateand ex- quilargold-alunitedeposit;relationship to otherhydrothermal
solvean aqueousfluid. Lower pressureconditions, oredepositsin southeastern Spain:Unpublished Ph.D.disserta-
prevailingat shallowdepths(1.5-3 km),favormetal tion, AnnArbor,Michigan,Universityof Michigan,340 p.
fractionationfrom melt to fluid (Urabe, 1985; Hem- Arribas, A., Jr., Rytuba,J.J.,Rye, R.O., Cunningham, C.G., Pod-
wysocky,M.H., Kelly, W.C., Arribas,A., McKee, E.H., and
ley et al., 1992) andalsoexerta strongcontrolonthe Smith,J.G., 1989, Preliminarystudyof the ore depositsand
volatilecomposition of the fluid (ShinoharaandFuji- hydrothermalalterationin the Rodalquilarcalderacomplex,
moto, 1989). southeastern Spain:U.S. GeologicalSurveyOpen-FileReport
2. The exsolvedfluid mustseparateinto a gas-rich 89-327, 21 p.
Ashley,R.P.,andSilberman,M.L., 1976, Directdatingof mineral-
vaporand salineliquid (Pitzer and Pabalan,1986), izationat Goldfield,Nevada,by K-Ar andfissiontrackmethods:
with metalssuchasCu (Williamset al., 1991) andAu ECONOMIC GEOLOGY, v. 71, p. 904-924.
into the salineliquid. Barton,P.B.,Jr., andSkinner,B.J.,1979, Sulfidemineralstabill-
3. The gas-rich(HC1andSO + HS) vaporphase ties, in Barnes,H.L., ed., Geochemistryof hydrothermalore
must ascend to the surface and condense into me- deposits: New York,Wiley Interscience, p. 278-403.
Baska,C., Cseh-Nemeth,J., Csillag,J., Foldessy,J., andZelanka,
teoric water. This will form an acid chloride-sulfate T., 1980,The Resckporphyryandskarndeposit,Hungary:Soci-
fluid which reactswith the hostrock; the leaching ety of GeologyAppliedto MineralDepositsSpecialPublication
that resultswill createa permeablezoneof mixing. 1, p. 73-76.
4. The dense,metal-richliquidmustthenascend Berger, B.R., and Henley,R.W., 1989, Advances
standing of epithermalgold-silverdeposits,
in the under-
with specialrefer-
into the leachedzone and precipitateCu sulfosalts, enceto deposits of the westernUnitedStates: ECONOMIC GEOL-
sulfides,and Au. This probablyoccursbecauseof OGYMONOGO, PH6, p. 405-423.
coolingcausedby mixingof the relativelyoxidized Berger,B.R., and Silberman,M.L., 1985, Relationshipof trace-
andsalineliquidwithmeteoricwater.A highhydrau- elementpatternsto geologyin hot-spring-type precious-metal
deposits: Reviewsin Economic Geology,v. 2, p. 233-247.
lic gradientdueto steepreliefmaypreventthedense Bethke,P.M., 1984, Controlsonbaseandpreciousmetalmineral-
liquid from risingto the leachedzone, asnotedin izationin deeperepithermalenvironments: U.S.Geological Sur-
some active stratovolcanoes (Giggenbachet al., vey Open-FileReport84-890, 40 p.
1990). Alternatively,the salineliquid mayneverbe Brimhall,G.H, Jr., andGhiorso,M.S., 1983,Originandore-form-
releasedfrom its lithostaticallypressuredsite adja- ing consequences of the advancedargillicalterationprocessin
hypogene environments by magmatic gascontamination of me-
centto the crystallizingmagma.In thesecases,only teoricfluids:ECONOMIC GEOLOGY, v. 78, p. 73-90.
leached,barren rock may result, characteristicof Bruha,D.J.,andNoble,D.C, 1983, Hypogenequartz-alunite-pyr-
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mal solutionslabs.]:GeologicalSocietyof AmericaAbstracts
Acknowledgments with Programs,v. 15, p. 325.
Burnham,C.W., 1979, Magmasand hydrothermalfluids, in
We thank Minoru Kusakabefor oxygenisotope Barnes,H.L., ed., Geochemistry of hydrothermalore deposits:
analyses of alunite,KatsumiMarumofor D/H analy- New York,Wiley Interscience,p. 71-136.
sesof clayminerals,andOsamuMatsubayafor useof Camus,F., 1990, The geologyof hydrothermalgolddepositsin
hislaboratory,BobRye for useof hislaboratoryand Chile:Journalof Geochemical Exploration,v. 36, p. 197-232.
Carlile,J.C.,Digowirogo,S.,andDarius,K., 1990, Geological set-
guidancein the analysisof the isotopiccomposition ting,characteristicsandregionalexploration for goldin thevol-
of alunite,HitoshiSakaiandAkira Sasakifor permis- canicarcsof NorthSulawesi, Indonesia:Journalof Geochemical
sion to use their unpublishedisotopicanalysesof Exploration,v. 35, p. 105-140.
alunite, and Akira Sasakifor use of and assistancein Christenson,B.W., and Wood, C.P., 1993, Evolution of a vent-
his sulfurisotopelaboratory.We acknowledge the Zealand:Bulletinof Volcanology,
v. 55, p. 547-565.
KasugaMiningCompanyfor access to samples
of drill Cunningham, C.G, Rye, R.O., Steven,T.A., and Mehnert,H.H.,
core, Mr. Yamashitafor his assistance,
and the Metal 1984, Originsandexploration significance of replacementand
MiningAgencyof Japanfor access to their informa- vein-typealunitedeposits in the Marysvale volcanicfield,west
tion. Discussions in the Nansatsu district with An- centralUtah: ECONOMIC GEOLOGY, v. 79, p. 50-71.
Cunningham, C.G., Arribas,A., Jr., Rytuba,J.J.,andArribas,A.,
tonio Arribas,Dick Beane,Phil Bethke, Skip Cun- 1990, Mineralizedand unmineralizedcalderasin Spain;Part I,
ningham,JimRytuba,Dick Sillitoe,SachihiroTagu- evolutionof the LosFrailescaldera:MineraliumDeposita,v. 25
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amongall parties.We alsothankDick Sillitoeand leveligneous activity:A stable-isotope
Stuart Simmons for their constructive reviews of the ingdistrict,Peru:Unpublished Ph.D.dissertation,
Boulder, Col-
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