Vol. S2, I•S?, pp.

914-92•

LEAD ISOTOPE COMPOSITION OF PERUVIAN GALENAS

J. LAURENCE KULP, G. C. AMSTUTZ, AND F. DONALD ECKELMANN

CONTENTS
PAGE

Abstract .............................................................. 914

Introduction ........................................................... 914
Geologicsetting ....................................................... 9! $
Results ............................................................... 918
Discussion ............................................................ 920
Acknowledgments...................................................... 921
References ............................................................ 922

ABSTRACT

Isotopic abundancemeasurementshave been made on the lead from

nineteengalena samplescovering a wide range of geographicaland geo-
logicalsettingsin the Tertiary hydrothermalmineralizationof the Central
Peruvian Andes. The results are strikingly similar, suggestingorigin
from a homogeneousmagmatic sourcederived from an average crustal en-
vironment with regard to its U/Pb and Th/Pb ratios. The consistency
of the lead isotopesthrough all zones of mineralization and over great
vertical and horizontal extent is further evidence against significant frac-
tionationof theseisotopesduring transportationand deposition.

I NTRODU CTIO N

A aECENTworldwidesurveyof the isotopiccompositionof lead ores by Bate,

Gast,Kulp, and Miller (3) has shownthat in someareasthere may be sig-
nificantdifferencesin the relative abundances
of lead isotopes. An intensive
studyof the leadisotopecomposition of the SoutheastMissouriLead Belt by
Eckelmann, Kulp andBrown (5) hasshownthat largevariationsexist,which
canbe systematically
relatedto the patternand relativeagesof ore in a single
district. The evidencein SoutheastMissourisuggestsinhomogeneous extrac-
tion of lead from moderatecrustaldepths. This pattern appearsto be the
samefor the entire MississippiValley wherethe lead orescannotbe conclu-
sivelyassociated
with major igneousintrusions. Other districtsrelatedto
igneousintrusives,
suchas alongthe easternborderof the BoulderBatholith,
do not show significantvariationsin the lead isotopeabundances
of galena
samples(Wright, personalcommunication).
The observed variationsin leadisotopes
are almostsurelydueto themixing
of leadswith differentradiogenic components.Variationsdueto fractionation
duringtransportation
anddeposition
havebeensuggested
(9) butthisremains
to be demonstrated.

• Lamont GeologicalObservatory,Palisades,New York, ContributionNo. 266.

914

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by Society of Economic Geologists, Mario Diaz
 LEAD ISOTOPE COMPOSITION OF PERUVIAN GALENAS 915
ß

SAMPLE SUMMARY

ph204 phz06
MOROCOCHA

SAN CRISTOBAL

18 93 833

CERRO BE PASCO

AM- 4 18 85 854
AM- 5 18 85 835
AM- 6 18 87 852
AM- 8 18 89 831
AM- 9 18 85 854
AM- I0 18 79 834
ß CERRO DE PASCO
AM- I I 18 92 837
18 86 834 Av

-IMA MOROCOCHA
, *
CASAPALCA.

•'• SANCRISTOBAL
• C'"SAPALC'" AM- 12 19 12 82õ
AM-14 1881 851
AM- 15 18 8:• 8:•9
AM-16 1892 853
AM-17 1889 830
AM- 18 18 97 829
AM- 19 18 96 85•

SCALE

• o
L ,ou
I •00
I ••0u•cES
I I I I
82' ?L' I 7L' '0' 66' 612"
•m. •.

The TertiaryPb-Zn-Cumineralization
of the PeruvianAndesrepresents
an areaof specialinterestwith regardto theisotopegeologyof leadfor several
reasons:(1) the strikingmineralogical zoningof the ore deposits,(2) the
greathorizontal
andverticalextentof theoreand'(3) thesynchroneity
of the
oresand major intrusivesin the area.
A representative
setof galenasamples wascollected
whichoriginates
from
a varietyof hydrothermal deposits
in CentralPeru (Fig. 1). The major
localities
areMorococha,SanCristobal, Cerrode PascoandCasapalca.The
leadisotope analysis
wasdoneusingthe leadtetramethyl procedure
andthe
massspectrometer described
by Bate,Miller andKulp (2).

GEOLOGIC SETTING

McLaughlin(7) has described the regionalgeologyof the Peruvian

Cordillera
fromwhichthe galenasampleswerecollectedandthisis briefly
summarized below. Thesampled
areaisunderlain
bya thickseries
of slightly

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by Society of Economic Geologists, Mario Diaz
 916 J. L. KULP, G. C. AMSTUTZ, AND F. D. ECKELMANN

metamorphosed argillites and sandstones

of possibleSilurian age (Excelsior
series). The overlying Permo-Carboniferousformations consist of sand-
stone, conglomeratesand a thick series of pyroclasticvolcanic material.
Mesozoicrocks from a sequenceof varying thickness,including mainly al-
ternating limestonesand sandstones,and Tertiary rocks comprise mostly
sandstonesand shales,plus various sequences of volcanicflows, tuffs, and
agglomerates.The sequenceis intruded by numerousstock-like igneous
massesvarying from quartz diorite to quartz monzoniteand granites,with
massiveor porphyritic textures. No intensivemassesof large batholithic
proportionsare exposed.
From a geneticstandpointthe Cerro quartz monzoniteporphyry is most ß
interesting. It is generallyregardedas the sourceof the ore depositsin the
Cerro de Pascodistrict but the "geneticassociationis a matter of inference
from other well known examplesrather than a direct deductionfrom local
observations"(7, p. 618). Pre-Mesozoicfolding and faulting produced
structuresof considerableintricacybut little is known except that theseare
widespread. Folding and faultingat the closeof the Mesozoic(north-north-
west trend) initiatedthe dominantstructuraltrend of the area. Folding and
faulting accompanied and followedthe period of igneousactivity. Tertiary
explosiveeruptionsbroke forth from many centersand blanketedthe country
with ash and agglomeratematerial which was involvedin the final phaseof
deformation.
Mineralizationis consideredto be definitelyassociated with the last period
of intrusiveactivity. Ore depositionbeganbeforethe final deformationand
continuedafter the last major movementshad ceased. The ore bodiesrange
in type from contactmetamorphic depositswith abundantmineralsindicative
of high temperatures to cinnabardepositsprobablyrelatedto the solutionsof
neighboringhot springs(Huancavelicaarea).
The samplelocalitiescover an area 80 miles long (trending north-south)
and representgeologicenvironments characterizedby (1) pronounced mineral
and metal zoningover considerable lateral and vertical distancesand (2) as-
sociationof vein and irregular "manto"-type ore occurrenceswith quartz
monzoniteintrusives. The Morocochasample(No. 1) comesfrom the fringe
of a mineralized area characterizedby pronouncedmineral zoning (hori-
zontallyand vertically) relatedto a groupof Tertiary quartz monzoniteintru-
sions. Ore in the Mesozoic limestones and sandstones occurs as veins and
irregular bodies(mantos), the latter type usuallyat or closeto igneouscon-
tacts. Mineralizationin the related intrusionsis dominantlycopper while
silver and lead appear in increasingamounts (relative to copper) with in-
creasingdistancefrom the intrusions. Zinc is abundantlyassociatedwith
copperin the intermediatezoneand dominantwith lead in the outer zone (8,
p. 517). The San Cristobalspecimensare similar in setting,occurring12
milessouthof Morocochaalongan anticlinalstructurecommonto both areas.
The depositis polymineralic,containingcopper-lead-zinc.The two samples
are from separatevein systemsin the outer zoneof mineralization. The ores
of the Cerro dePascodistrictoccurprincipallyalongthe easternand southern
marginsof a body of tuff and brecciafilling the deeplyerodedvent of an

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by Society of Economic Geologists, Mario Diaz
 LEAD ISOTOPE COMPOSITION OF PERUVIAN GALENAS 917

extinct volcano,and along a major zoneof faulting separatingMesozoiclime-

stone on the east from the altered Paleozoic sediments,Tertiary tuffs and
intrusiveson the west. Tabular replacementbodiesextend into the limestone
roughly parallel to the eastward dipping bedding. Subsequentto intrusion
of the Cerro monzonite,sulphidesolutionspassedupwardsalong the eastern
wall of the vent and producedone of the world'slargestpyrite deposits(over
one mile long and a maximumwidth of 1,000 feet). Galenaand sphalerite
occurin abundanceat variouspointsin the massivepyritic body. The true
controlling factors for lead-zinc mineralization are unknown. The overall
geneticrelationships betweenthe differentlead-zincdepositsin the Cerro mine
havenot beenestablished.The sevengalenasamplesfrom Cerro can there-
fore be classifiedonly in regard to their depthin the mine and occurrence
in
irregular shapedbodies. The Casapalcadepositis characterizedby the per-
sistenceof severalmain veins laterally (3,300 m) and vertically (1,400 m)

TABLE 1
ß

LEAD ISOTOPE ABUNDANCES OF GALENA SAMPLE

(Average standard error: 206/204 and 207/204 -- 0.1, 208/204 ----0.2,

207/206 = .002, 208/206 = .004)

Sample no. Locality Pb•4 PbZ0S Pb z07 Pb z0s 207/206 208/206

Am-1 Morococha 1.000 18.65 15.52 38.71

(La Estaca, Curia) 1.353 25.23 21.00 52.38 .832 2.076

Am-2 San Cristobal 1.000 18.98 15.81 39.45

1.329 25.23 21.01 52.43 .833 2.078

Am-3 San Cristobal 1.000 18.87 15.71 39.12

1.339 25.27 21.03 52.38 .832 2.073

Average 18.93 15.76 39.29 .833 2.076

Am-4A Cerro de Pasco 1.000 18.83 15.69 39.12

1.340 25.23 21.03 52.42 .834 2.078

Am-5 Cerro de Pasco 1.000 18.85 15.73 39.05

1.340 25.26 21.08 52.33 .835 2.072

Am-6 Cerro de Pasco 1.000 18.87 15.71 39,21

1.337 25.23 21.00 52.43 .832 2.078

Am-8 Cerro de Pasco 1.000 18.89 15.70 39.23

1.337 25.25 20.99 52.45 .831 2.077

Am-9 Cerro de Pasco 1.000 18.85 15.73 39.11

1.339 25.24 21.06 52.37 .834 2.075

Am-10 Cerro de Pasco 1.000 18.79 15.68 38.99

1.343 25.24 21.06 52.36 .834 2.074

Am-ll Cerro de Pasco 1.000 18.92 15.83 39.44

1.330 25.17 21•06 52.45 .837 2.084

Average 18.86 15.72 39.16 .834 2.077

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by Society of Economic Geologists, Mario Diaz
 918 ]. L. KULP, G. C. AMSTUTZ, AND F. D. ECKELMANN
TABLE 1---Continued

Sampleno. Locality pb2o• Pb•S Pb207 Pb=s 207/2015 208/2015

, ,

Am-12 Casapalca 1.000 19.12 15.78 39.43

Caprichosa 1.328 25.39 20.94 52.36 .825 2.062

Am-14 Casapalca Proper 1.000 18.81 15.64 39.16

1.340 25.21 20.96 52.47 .831 2.08I

Am-15 Casapalca Proper 1.000 18.82 15.61 39.03

1.343 25.28 20.96 52.42 .829 2.074

Am-16 Casapalca Proper 1.000 18.92 15.77 39.16

1.336 25.28 21.07 52.32 .833 2.070

Am-17 Casapalm Proper 1.000 18.89 15.68 39.11

1.339 25.30 21.00 52.37 .830 2.070

Am-18 Casapalca Proper 1.000 18.97 15.72 39.32

1.333 25.29 20.96 52.42 .829 2.073

Am-19 Casapalm Proper 1.000 18.96 15.76 39.27

1.334 25.26 21.02 52.39 .832 2.074

Am-20 Casapalm Proper 1.000 18.87 15.68 39.08

1.340 25.29 21.01 52.37 .831 2.071

Am-21 Casapalca Rosaura 1.000 18.84 15.72 39.01

1.341 25.27 21.08 52.31 .834 2.070

Average 18.92 15.71 39.20 .830 2.072

Average---Entireregion 18.88 15.71 39.18 .832 2.075
--.

togetherwith pronounced zoningand telescopingof zoneswithinindividual

veins. Mineral zonesgradefrom strongalterationand silverin the centerto
copper-lead-zincin the intermediatezone, and realgar-stibnite-carbonate
gangueat the extremities
of the vein system. Table2 indicates the samples
levelsin the mine togetherwith the isotopevalues.
RESULTS

The isotopicanalyses
of the galenasamples
are summarizedin Table 1.
The isotopic
abundances
aregivenon thebasisof 100percentandrelativeto
TABLE 2

VERTICAL DISTRIBUTION OF ISOTOPIC DATA IN THE CASAPALCA MINE

Sampleno. Mine level 206/204 207/204 208/204 207/206

14 1,200' 18.81 15.64 39.16 .831

20 1,200' 18.87 15.68 39.08 .831
15 1,400' 18.82 15.61 39.03 .829
16 1,400' 18.92 15.77 39.16 .833
19 2,100' 18.96 15.76 39.27 .832
17 2,300' 18.89 15.68 39.86 .830
18 2,700' 18.97 15.72 39.32 .829

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by Society of Economic Geologists, Mario Diaz
 LEAD ISOTOPE COMPOSITION OF PERUVIAN GALENAS 919

Pb•ø•'-1.000. The ratios 207/206 and 208/206 are also given along with
theaveragevaluefor eachdeposit. The averagestandarderror for eachratio
is given. This is equivalent
to the 66 percentconfidence
level. The standard
error is derivedfrom the standarddeviationobtainedfrom a standardsample
whichwasanalyzed73 timesduringthe periodin whichthesePeruviansam-
pleswere assayed. The Pb•ø• abundance
is mostuncertainand thus limits
the absolutevaluesof 206/204 etc.
The severalisotopicratiosare relatedto differentgeochemical effects. The
206/204 or 208/204 ratiosare mostsensitive to the additionof radiogeniclead.
The 207/206 and 208/206 ratios are independentof the Pb•ø• measurement.
The 207/206 ratio is indicativeof the time of extractionof the leadfrom the
sourcerocksand in somecasesmay indicatethe relativeage of mixedleads.
The 208/206 ratio is a sensitiveindicatorof the averageU/Th ratio of the
sourcerocksif the sourceis homogenized prior to transportationto the site
of deposition
higherin the crustand woulddetectmixingof the two leadsfrom
differentU/Th environments.
The vertical distributionof samplesin the Casapalcamine is given in
Table 2.

TABLE 3

LIST OF LOCATIONS AND DESCRIPTIONS OF SAMPLES

Sample no. Mine area Location inside this mining area and description of sample

Am-1 Morococha La Estaca---Cufia, outside mine in Anticona diorite.

Pockets and veins of galena, sphalerite, and barite.

Am-2 San Cristobal Manto-type ore body in uppermost portion of mine:

170 level, 015 stope, -t-3d floor, western ore body.
Large tabular "phenocrysts" of barite (3 inches long),
in a matrix of galena and sphalerite.

Am-3 San Cristobal San Antonio 470-425 stope. Galena in stringers and
pockets in limestone and vo]canics.

Am-4 Cerro de Pasco 596 No. 2 stope, 6th floor (500 level), Pb-Zn-ore body;
breccia.

Arno5 Cerro de Pasco 12175 No. 5 stope, 6th floor (1,200 level), Pb-Zn-ore
body; ?brecciated.

Am-6 Cerro de Pasco 12177 No. 5 stope, 13th floor (1,200 level), Pb-Zn-ore
body; ?brecciated.

Am-8 Cerro de Pasco 12278, arch back stope, 3d floor (1,200 level), Pb-Zn-ore
body; ?brecciated.

Am-9 Cerro de Pasco A-102 stope, 2nd floor (A level), Pb-Zn-ore body; dis-
seminated mineralization.

Am-10 Cerro de Pasco 6203 stope, 17th floor (600 level), veins and disseminations.

Am-ll Cerro de Pasco 6203 stope, 17th floor (600 level), veins and disseminations.

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 92O ]. L. KULP, G. C. •IMSTUTZ, •IND F. D. ECKELM•INN

TABLE 3--Continued

Sample no. Mine area Location inside this mining area and description of sample

Am-12 Casapalca Caprichosa; disseminated copper deposit in andesitic

lavas with a few stringers and fractures containing
galena, tetrahedrite, sphalerite, barite, etc.
Am-14 Casapalca C-vein North; 1,200 level. Silicified limestone with Pbs,
Zns, CuFeS2, quartz, clay, and carbonates as vein
minera.ls. Massive vein, meflium grained.
Am-15 Casapalca Face of C~vein South; 1,400 level; Galena in altered red
beds, with ZnS and pyrite in massive, medium grained
vein.

Am-16 Casapalca C-vein N; 1,400 level. Silicified limestone with Pbs, ZnS,
CuFeS2, pyrite, much carbonate, in massive, medium
grained vein.

Am-17 Casapalca 23 B 570 stope, 2,300 level. Large cubooctahedral galena

crystals with concave crystal surfaces produced by edge
growth. Crystals covered open lens-shape fissure,
about 3 m high and 10 m long. Little sphalerite and
quartz associated with galena.

Am-18 Casapalca L-25, 2,700 level. Massive coarse grained vein of quartz,
pyrite, Pbs and ZnS.

Am-19 Casapalca 21-N-East vein, 2,100 level. Massive, coarse grained ore
of ZnS, with PbS, quartz, and some pyrite.

Am-20 Casapalca 12-M-35 vein, 2,100 level. Massive, very coarse grained
ore with about equal amounts of ZnS, PbS, CuFeSx
and quartz.

Am-21 Casapalca Rosaura district (Casapalca outside mine); Medium to

fine grained massive galena with little pyrite.

DISCUSSION

The most striking thing about these data is the constancyof the lead
isotopeabundances.All of the samplesfrom San Cristobal,Cerro de Pasco
and Casapalcalie within the standarderror of the averagefor eachmine and
for the averageof the districtfor all isotoperatios. The Morocochasample
alsoagreesperfectlyin the 207/206 and 208/206 ratiosbut is slightlyoutside
the standarderror (lower) from the average206/204, 207/204 and 208/204
values. This suggests that the Pb•ø4analysismay be slightlyhigh in this ore.
It can be concludedthat the isotopiccomposition is constantto within
---+0.5%(the experimental uncertainty)for the entiredistrict. This should
becompared to variationsup to 13.4percentin the Southeast MissouriDistrict.
This constancy is particularlyremarkablewhenthe extremesof conditions
represented by the samplesare considered.The distancealongstrike is 80
miles; the verticaldistributioncoversat least400 m (Casapalca). From the
mineralassemblage and the iron contentof sphaleritein theseminesAmstutz
(1) suggests that Cerrorepresents highertemperatures of depositionthanthe
other three localities. The galenascancomefrom all zones(and presumably
all temperatures) from the highertemperature copperzonenearthe intrusive

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by Society of Economic Geologists, Mario Diaz
 LEAD ISOTOPE COMPOSITION OF PERUVIAN GALENAS 921

outwardto the lower temperatureleadrich zone. Silver increases alongwith

the lead. Zinc is strongestin the intermediatezone.
The Morocochasamplewas taken from an occurrenceoutsidethe mine
(La Estaca--Cufia). At 3'an Cristobalthe sampleswere far apart and taken
in pocketsof ore in limestonewhichis intimatelyassociated with barite. One
of these is from very coarse-grainedore. The Cerro ore occurs filling
breccia,disseminated in the countryrock and as distinctveins. At Casapalca
the samplescoverthe innerchalcopyrite zone,the main copper-lead-zinc zone
and the carbonate-realgar-stibnite periphery. Sample21 wascollectedin the
Rosauradistrict,an outlayerof the Casapalcavein system. SampleAm 12 is
from a peculiarsmallporphyrycopperdepositin lavaslocatedat Caprichosa.
It is not clearwhetherthis is of the sameage as the main Casapalcavein sys-
tem. At Casapalcaa wide range in crystalsize of the galenais also repre-
sented.
Althoughmore detailedstudy is required,the worldwidesurveyof the
leadisotopecomposition
of galenassuggestedthat leadoresdirectlyassociated
with Tertiary intrusivesare in generalnot significantlyradiogenic,and that
they will not showlargevariations. In the SantaRita districtof New Mexico,
wherecopper,zincandleadmineralizationare associated with quartzmonzonite
stocks,a studyof the sulfurisotopesin varioussulfidesalsoshowedsurprising
constancy. All of this suggeststhat where fracturesexist from the source
depthsdirectly,the hydrothermalphasecanleakout of a volumeelementof the
crustaboutasfastasit formsduringa heatingcycle. In thiscasevariationsin
leadisotope•ompositionof galenamaybe expected. Conversely, if the volume
elementis completelyhomogenized(molten) and somesilicatemelt is intruded
first, then followedby ore depositingsolutions,the lead isotopecomposition
shouldbe and is foundto be relativelyuniform.
The followingconclusions are suggested from this study:
1. The leadin theore deposits of the Cerrode Pasco-Casapalca-Morococha
district (80 milesin length) has almostconstantisotopiccompositionwithin
the limits of experimentalerror (i.e., about ---+.5%of the ratios 206/204,
207/204, 208/204). This stronglysuggests that the lead,and thereforethe
other economically importantmetals,camefrom a singlesource. The source
was mostlikely oneor severalcloselyrelatedmagmachambers.
2. The isotopiccompositionof the lead is consistentwith a Tertiary age
of mineralizationand a sourcerock composition similarto averagecontinent
crustwith regardto U/Pb andTh/Pb.
3. No measurable fractionationof the Iead isotopesoccurredin this com-
plex mineralization. It is becomingincreasinglyimprobablethat suchfrac-
rionationis ever importantin the caseof hydrothermallead mineralformation
associated with major intrusives. This is at leastfor an experimentaluncer-
tainty of ---+0.5%.
ACKNOWLEDGMENTS

The authorswish to acknowledgethe financialsupportof the Research

Division,Atomic Energy Commission,
whichmadepossiblethe investigation.

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by Society of Economic Geologists, Mario Diaz
 922 J. L. KULP, G. C. .4MSTUTZ, AND F. D. ECKELMANN

D. $. Miller was in chargeof the massspectrometerat the time thesemeasure-

ments were made, P. W. Cast, D. S. Miller and W. R. Eckelmann contributed
to the discussionof the data. The samplesand field descriptionswere pro-
vided by the secondauthor. The isotopicanalyseswere performedin the
Geochemistry Laboratoryof the Lamont Observatory.
LAMONT
GEOLOGICAL
OBSERVATORY,
•
COLUMBIA UNIVERSITY,
NEW YORK, N.Y.,
Aug. 12, 1957
REFERENCES

1. Amstutz, G. C., 1955, Temperature of deposition in central Peruvian mines on the basis of
the Fe: Zn ratio in sphalerites: Primer Congr. Geol. Peru, Lima (abstract).
2. Bate, G. L., Miller, D. S., and Kulp, J. L., 1957, Isotopic analysis of tetramethyllead:
Analytical Chemistry, v. 29, p. 84-88.
3. Bate, G. L., Cast, P. W., Kulp, J. L., and Miller, D. S., Isotopic compositionof lead in
lead minerals: in preparation.
4. Cerro de Pasco Corporation, Geological Staff, 1950, Lead and zinc deposits of the Cerro de
Pasco Copper Corporation in central Peru: Int. Geo. Congr., Rept. 18th Session, 1948,
Part VII, London, p. 154-186.
5. Eckelmann, F. D., Kulp, J. L., and Brown, J. S., 1958, Lead isotopes and the history of
mineralization in Southeast Missouri: Geol. Soc. America Bull., in preparation.
6. McKinstry, H. E., and Noble, J. A., 1932, The veins of Casapalca, Peru: Ecom Gzox.., v.
27, p. 501-522.
7. McLaughlin, D. H., 1924, Geology and physiography of the Peruvian cordillera, Depart-
ments of Junin and Lima: Geol. Soc. America Bull., v. 35, p. 591-632.
8. McLaughlin, D. H., and Moses, J. H., 1945, Geology of the mining region of central Peru:
Min. Met. Soc. Amer. Bull., November, p. 512-519.
9. Senftle, F. E., and Bracken, J. T., 1955, Theoretical effect of diffusion on isotope abundance
ratios in rocks and associatedfluids: Geochim. et Cosmochim.Acta, v. 7, p. 61-76.
10. Trefzger, E. F., 1937, Das Kupfererzvorkommen der Grube Morococha: Metall. u Erz, 34,
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11. Ward, H. J., 1954, Ore deposits of Cerro de Pasco: E1 Serrano, July, p. 1-3.

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by Society of Economic Geologists, Mario Diaz