ORIGINAL PAPER

Rune B. Larsen Æ Iain Henderson Æ Peter M. Ihlen

Francois Jacamon

Distribution and petrogenetic behaviour of trace elements in graniticpegmatite quartz from South Norway

Received: 9 February 2004 / Accepted: 13 April 2004 / Published online: 20 May 2004� Springer-Verlag 2004

Abstract The present study documents that the trace-element distribution in granitic quartz is highly sensitiveto CAFC processes in granitic melts. Igneous quartzefficiently records both the origin and the evolution ofthe granitic pegmatites. Aluminium, P, Li, Ti, Ge andNa in that order of abundance, comprises >95% of thetrace elements. Most samples feature >1 ppm of any ofthese elements. The remnant 5% includes K, Fe, Be, B,Ba and Sr whereas the other elements are present atconcentrations lower than the detection limit. Potas-sium, Fe, Be and Ti are relatively compatible henceobtain the highest concentrations in early formedquartz. Phosphorous, Ge, Li and Al are relativelyincompatible and generally obtain the highest concen-trations in quartz that formed at lower temperaturesfrom more evolved granitic melts. The Ge/Ti, the Ge/Be,the P/Ge and the P/Be ratios of quartz are stronglysensitive to the origin and evolution of the granitic meltsand similarly the Rb/Sr and the Rb/K ratios of K-feld-spars may be utilised in petrogenetic interpretations.However, the quartz trace element ratios are better atdistinguishing similarities and differences in the originand evolution of granitic melts. After evaluating thedifferent trace element ratios, the Ge/Ti ratio appears tobe most robust during subsolidus processes in the igne-ous systems, hence probably should be the preferredratio for analysing and understanding petrogeneticprocesses in granitic igneous rocks.

Introduction

The origin and evolution of silica-over-saturated igneousrocks are normally approached through the studies ofmajor and minor element chemistries of whole-rocksamples or individual minerals. However, quartz israrely considered a viable source of genetic informationbecause the trace-element concentration is very lowhence difficult to constrain with conventional analyticalmethods.

However, developments of the laser ablation induc-tively coupled plasma mass spectrometry (LA-ICP-MS)technique has overcome many of the analytical obstacles(Larsen and Lahaye 1999; Flem et al. 2002) and the traceelement composition of quartz may now be quantifiedby direct laser ablation sampling of quartz in thicksections. The great advantage with this in situ techniqueis that fluid, and solid inclusions can be avoided and thatdifferent generations of quartz may be sampled andanalysed separately (Fig. 1).

The scope of the present communication is to docu-ment the trace element evolution of granitic pegmatitequartz during the evolution from primitive to evolvedgranitic compositions and during subsolidus recrystalli-zation of quartz. It will be discussed how the trace ele-ment distribution in quartz compares to K-feldspar forwhich the chemical changes during the igneous evolutionof granitic rocks is well known.

Chemistry of quartz

Several studies are devoted to the setting and speciationof trace elements in quartz. However, very few works areconcerned with the chemistry of quartz as a function ofgeological processes. The following review of the traceelement chemistry of quartz is summarised from Frondel(1962); Dennen (1964, 1967); Dennen et al. (1970);Lehmann and Bambauer (1973); Fanderlik (1991); Per-ny et al. (1992); Gotze and Lewis (1994); Gotze and

Editorial responsibility: J. Hoefs

R. B. Larsen (&) Æ I. Henderson Æ P. M. IhlenGeological Survey of Norway,7491 Trondheim, NorwayE-mail: rune.larsen@ngu.no

R. B. Larsen Æ F. JacamonDepartment of Geology and Mining Engineering,Norwegian University of Science and Technology,7491 Trondheim, Norway

Contrib Mineral Petrol (2004) 147: 615–628DOI 10.1007/s00410-004-0580-4

Plotze (1997); Deer et al. (1997); Monecke et al. (2002);Muller et al. (2002a, b, 2003). Other sources are cited inthe text.

Quartz comprises a strong configuration of Si–Obonds that allows only a minimum of other elementsinto its structure. Accordingly, more than 50% of thebonds are covalent (Fig. 2a). Trace elements that may fitin to the atomic lattice structure of quartz includes Al, B,Ba, Be, Ca, Cr, Cu, Fe, Ge, H, K, Li, Mg, Mn, Na, P,Pb, Rb, Sr, Ti and U.

Quartz that at first glance appears clear and inclu-sion-free may contain >1,000 ppm of structurallybound trace elements. On the contrary, dark smokyquartz with many solid and liquid inclusions may benearly free of trace elements in the atomic lattice. Thesmoky colour is due to ionising radiation from neigh-bouring minerals (e.g. 40K in K-feldspar) (Larsen et al.

1998) and minute concentrations of structurally boundelements in colour centres of the quartz atomic lattice.However, other colour variations are signs of a highabundance of trace elements. Amethyst, for example,owes its colour to structurally bound Fe (e.g. Hassanand Cohen 1974; Lehmann 1975; Cohen and Makar1985; Aines and Rossmann 1986). Rose quartz owe itscolour to high concentrations of structurally bound Feand Ti (e.g. Hassan and Cohen 1974; Cohen and Makar1984, 1985) to Al–P substitutions (Maschmeyer andLehmann 1983) or, according to recent studies, may becaused by inclusions of sub-microscopic dumortierite[Al7(BO3)(SiO4)O3] fibres (Ma et al. 2002).

In the current study of quartz from Evje and Frolandwe are mostly concerned with Al, B, Be, Fe, Ge, K, Li,Na, P and Ti because these elements comprise >99% ofthe trace elements. Ti4+ and Ge4+, both being tetrava-

Fig. 1 Geological setting of theEvje and Froland pegmatitefields in South Norway

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lent ions, occur in the quartz lattice as simple substitu-tion for Si4+ (Fig. 2b). Phosphorous, which is a penta-valent ion, is integrated as coupled substitutionstogether with Al3+, or another trivalent ion (Fe3+ orB3+), in two neighbouring silicon-tetrahedron (Fig. 2c).Monovalent ions (Li+, K+ and Na+) either areaccommodated in atomic channels running parallel tothe c-axis or where lattice defects are prevalent (e.g.dislocations). Divalent ions mostly occupy vacancies(Be2+) or atomic cavities (Fig. 2d). They are chargebalanced by trivalent ions, mostly Al3+, which issubstituting for Si4+.

The granitic pegmatites

The Evje and Froland areas feature the two most studiedpegmatite fields in South Norway. They formed in theMezoproterozoic period from mantle or lower crustderived granitic melts (Sylvester 1964; Baadsgaard et al.1984; Pedersen et al. 2001; Larsen 2002). The precise ageis uncertain, but Rb/Sr dating on several pegmatitesyield ages between 852±12 Ma and 896±27 Ma (Syl-vester 1964; Pedersen and Konnerup-Madsen 2000). Arecent gadolinite U/Pb date from an unspecified peg-matite from the Evje field yielded an age of 910±14 Ma(Scherer et al. 2001) and several pegmatites from thecentral portions of the Evje area yielded Rb/Sr singlemineral isochron ages of 909±5 Ma (Andersen 2001)(Table 1). Accordingly, ages are overlapping and thechemistry as well as the mineralogy is nearly indistin-guishable for the pegmatite fields. However, subtlevariations in the accessory minerals together withstrongly contrasting REE patterns for K-feldspars implythat the pegmatites were derived from different parentmelts (Larsen 2002).

The pegmatites were emplaced in mafic host rockscomprising amphibolite, norite and mafic gneisses. Theyare extremely coarse-grained with individual crystalsvarying in size from decimetres to metres. The Evjepegmatites are modally zoned, typically comprising awall zone (WZ), one or several intermediate zones (IZ)and one or several core zones (CZ). WZ comprisesplagioclase, quartz, minor K-feldspar, biotite andmuscovite. IZ features decimetres to metre size amal-gamations of single biotite crystals growing towards theinterior of the pegmatite. Macro-perthitic K-feldspar,plagioclase and quartz are interspersed in near equalproportions between biotite and muscovite. Biotite is thedominant mica. CZ comprises large quantities of quartzthat normally contain rafts of euhedral K-feldspar andaccessory plagioclase. In Froland, modal zonation ispoorly developed or absent, but a distinctive modalgradation is common. Here, the proportion of plagio-clase and biotite is falling towards the interior of thepegmatites, whereas the proportions of K-feldspar andquartz are increasing.

Other than K-feldspar, plagioclase, quartz, biotiteand white mica, the typical primary igneous phases inthe Evje and Froland pegmatites includes magnetite,spessartite garnet, monazite, allanite-(Ce), xenotime,euxenite-(Y), fergusonite, gadolinite-group mineralsand beryl (Andersen 1926, 1931; Bjørlykke 1935, 1937,1939; Amli 1975, 1977). Garnet dominates the outerparts of IZ and monazite, xenotime, fergusonite andeuxenite-(Y) are nearly always associated with flakes ofbiotite at the transition between WZ and IZ. Together,these observations indicate that they formed duringearly and intermediate stages of crystallisation, whereasallanite-(Ce), gadolinite-group minerals and berylformed in the core zone from the last fractions ofpegmatitic melt (e.g. Bjørlykke 1935). Hydrothermal

Fig. 2a–d Structuralconfiguration of trace elementsin the ‘‘Low-quartz’’ atomiclattice. a Low quartz atomiclattice structure.b Configuration of tetravalentions (Ge and Ti) as singlesubstitutions for Si.c Configuration of coupledsubstitutions where apentavalent ion (P) and atrivalent ion (i.e. Al) substitutefor two Si-ions in neighbouringSi–O tetrahedrons hencefacilitate charge equilibrium.d Substitution of trivalent ions(Al, Fe, B) for Si generates acharge inequality of 1+.Charge balance is facilitated bya monovalent ion (Li, Na, K)that either is accommodated inchannels running parallel to thec-axis (Fig. 2a) or where latticedefects provides room for therelatively large ions

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replacement features are uncommon in both Evje andFroland (Bjørlykke 1935; Fought 1993; Stockmarr1994). Recent studies document that igneous volatilesin the Evje field comprises medium salinity H2O-CO2-NaCl fluids with 10–15 vol.% CO2 during formation ofthe IZ and low salinity H2O-CO2-NaCl-MgCl2-FeCl2fluids with 5–10 vol.% CO2 during formation of CZ(Larsen et al. 1998, 1999).

The Evje pegmatite field may be distinguished fromthe Froland field by the presence of monazite-(Ce)throughout crystallization of the pegmatites. Monazite-(Ce) is more rare in Froland whereas allanite is thedominating LREE-mineral (Bjørlykke 1935; Larsen2002). Another important difference is relative enrich-ment of the HREE in Froland K-feldspar, whereas theEvje K-feldspar demonstrates a relative enrichment inLREE (Larsen 2002). Accordingly, it is documented thatthe granitic pegmatites formed from two distinctivelydifferent parent melts (Larsen 2002).

Table 1 summarises the distinguishing features forgranitic pegmatites in the two areas.

Methodology

The analyses of quartz were accomplished with a stan-dard, double focusing sector field, ICP-MS (FinniganMAT, ELEMENT1) instrument with a CD-1 optionfrom Finnigan MAT and with an UV-laser from Finn-igan MAT/Spectrum, Berlin, Germany.

The following elements are included in the analyticalpackage: Al, B, Ba, Be, Cr, Fe, Ge, K, Li, Mg, Mn, Na,P, Pb, Rb, Sr, Th, Ti, U. Where 7Li, 9Be, 11B, 27Al,55Mn, 74Ge, 85Rb, 88Sr, 137Ba, 208Pb, 232Th, and 238Uwere analysed at low resolution (m/Dm=300); 23Na, 31P,25Mg, 47Ti, 52Cr, and 56Fe at medium resolution (m/Dm�3,500) and 39K at high resolution (m/Dm>8,000).The isotope, 29Si, was used as internal standard at lowresolution and 30Si was used at medium and high reso-lution. External calibration was done by using the

international standards: NIST612, NIST614, NIST616,RGM-1(USGS), Blank SiO2 and BAM no.1 SiO2

(Federal Institute for Material Research and Testing,Berlin, Germany). Blank SiO2 was used to constrain thedetection limits (LOD). LOD for most of the elementsare between 0.2 and 0.01 ppm. To improve the lowerlimit of quantification and the analytical uncertainty atlow concentrations, it is important to have calibrationcurves with well-defined intercepts rather than the two-point calibration (Typically Ar-blank and NIST612)that is the normal approach utilised by the LA-ICP-MScommunity. Laser ablation was accomplished in rastermeasuring 200·200 lm or less on 500 lm thick quartzwafers.

Each measurement consists of 15 scans of each iso-tope with a measurement time varying from 1 s per scanof K in high resolution to 0.02 s per scan of e.g. Mn inlow resolution. The choice of measurement time dependson the expected element concentration, the number ofchannels comprising the mass range and the requiredmass window.

To avoid problems associated with possible outliers(i.e. ‘‘spikes’’) caused by unstable ablation conditions, arobust statistical method was used to handle the rawdata (Wilcox 1997). The advantage with this method is ahigh break down point of 0.5 that makes it particularlyapplicable for the identification of outliers (Staudte andSheather 1990). An Ar-blank was run before eachstandard and sample. The background signal was sub-tracted from the response of the standard before nor-malisation against the internal standard. This was doneto avoid memory effects prevailing from the previoussamples. Finally, outliers were identified and removedfrom the background signal by the method describedabove.

Daily control of the precision and the accuracy of thecalibration curve are accomplished with control stan-dards that are not a part of the calibration curve or wererun as an unknown, for example NIST612. The uncer-tainty remained within ±10%.

Table 1 Determining features of the Evje and the Froland pegmatite fields

Evje Froland

Classification REE-Nb-Ti REE-Nb-TiAge Rb/Sr: 909±5 Ma, Andersen (2001) Rb/Sr: 893±50 Ma, Baadsgaard et al. (1984)

U/Pb: 910±14 Ma, Scherer et al. (2001) Rb/Sr: 896±27 Ma, Sylvester (1964)87Sr/86Sr 0.7063±0.061, Stockmarr (1994) 0.7023±0.0002, Baadsgard (1984)K/Rb, K-feldspar 363–79 321–79Morphology Sub-vertical and sub-horizontal dykes,

undeformedDykes, mostly vertical or horizontal in places stronglydeformed and sheared

Zonation Well developed modal zonation Poorly developed modal zonation but well developedmodally graded zonation

P and T 2–4 kb, 400–750�C, Larsen et al. (1998),Andersen (2001)

Not available

Major phases,most common

Plagioclase, K-feldspar (perthite), quartz,biotite, muscovite, garnet, magnetite

Plagioclase, K-feldspar (perthite), quartz, biotite,muscovite, magnetite

Common exotic phases,descending order

Monazite-(Ce), euxinite-(Y), xenotime-(Yb),gadolinite-(Y), fergusonite, allanite,

Allanite, euxinite-(Y), monazite-(Ce), fergusonite,xenotime-(Yb), gadolinite-(Y)

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More methodological information may be found inFlem et al. (2002).

Granitic pegmatite quartz

The proportion of quartz is increasing from the contact-and wall-zones towards the core of the pegmatite.During initial crystallization and the formation of thewall zone the proportion of quartz is typically around20% or less. IZ comprises 30–50% quartz graduallyincreasing to >80% in CZ.

For tectonically undisturbed pegmatite bodies, thequartz is sub- to euhedral and either glass clear or smokyin appearance. Smoky quartz is always present at the

vicinity of K-feldspar and gradually taper into clearquartz as the distance to the nearest K-feldspar crystalincreases to 20 cm or more (Larsen 2002). Accordingly,the smoky colour of quartz originates from decayingradiogenic elements in K-feldspar rather than being aresult of radiogenic elements in the quartz itself (Larsen1998).

Selected samples of quartz were studied with theSEM-CL technique in order to unveil primary and sec-ondary growth features (Fig. 3a–d). Most of the quartzis homogeneous and composed of only one generation ofprimary igneous quartz. In rare examples the igneousorigin of quartz is supported by lm scale oscillatoryzonation (Fig. 3a).

However, secondary replacement features do occur,particularly in the Froland pegmatites where tectonicoverprinting is more common (Henderson and Ihlen, inreview). Secondary quartz predominantly formed alongfractures and grain edges (Fig. 3d). However, the pres-ervation of primary igneous quartz imply that therecrystallization was not pervasive and LA-HR-ICP-MSanalysis (see later section) confirm that the overall traceelement distribution, with some notable exceptions, waspreserved during several episodes of recrystallization.

Fig. 3a–d SEM-CL uptakes of igneous quartz from the Evje andFroland pegmatite fields. a Oscillatory zonation of primary igneousquartz from the Evje field. b Homogenous primary igneous quartzfrom the Evje field. Bright luminescent quartz shows the outline ofa single crystal of quartz. c Laser ablation crater in the centre of theimage after laser ablation sampling of quartz along a predefinedraster. d Partial replacement of primary igneous quartz byinfiltrating aqueous fluid. Replacement is most pervasive alonggrain boundaries and is tapering towards fresh brightly luminescentigneous quartz in centre of grains

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Altogether, 93 granitic pegmatites were sampled forthe present study. At some localities more than tensamples would be collected. Normally we gathered twoquartz samples and two samples of K-feldspar in closeproximity to the quartz samples. The sample batcheswere gathered far apart both physically and in terms ofthe igneous evolution of the pegmatite. Accordingly, atleast one sample batch represents the pegmatite afterroughly 30–40% of the pegmatite had crystallized (cor-responding to the intermediate zone) in a setting wherequartz co-existed with an assemblage of K-feldspar,plagioclase and biotite±white mica. The other samplebatch comprised the pegmatite after >80% of the peg-matite had crystallized (corresponding to the core zone)in a setting where quartz co-existed with K-feldspar andaccessory plagioclase. By sampling these two ‘‘end-members’’, the quartz samples comprise a large part ofthe igneous history of the crystallization of a singlebatch of pegmatitic melt.

Structural bound trace elements in quartz

By weight, the dominant trace elements in quartz are Al,P, Li, Ti, Ge and Na in that order of abundance(Table 2). In most samples there are >1 ppm of any ofthese elements and together they comprises >95 wt.%of the trace elements. The remnant 5% comprises K, Fe,Be, B, Ba and Sr whereas other elements normally arepresent at concentrations lower than the detection limit.

To understand the distribution and type of traceelements in quartz, the trace elements may be classifiedaccording to their dominant structural setting in thequartz atomic lattice.

Accordingly, Ti and Ge are present in simple substi-tution after Si whereas P and an equivalent mol fractionof Al comprise coupled substitutions. Finally, Li+ Na + K + Be + Fe + B + Sr + Rb + Ba andexcess Al (i.e. excess after coupling with P), comprisesstuffed derivatives. Al, B and Fe may all be present astrivalent ions and may therefore be present in dualstructural settings, either as coupled substitutions or asstuffed derivatives. However, the mol proportions of Band Fe are insignificant, and, in the present case, may beignored (Table 2).

In assigning the trace elements to structural sites, Alis first allocated to sites where it is coupled with P (i.e.coupled substitutions) that, being a pentavalent ion,cannot otherwise be charge balanced in the atomiclattice.

From assigning the trace elements to the most logicalsites in the atomic lattice, it is demonstrated that quartzfrom the Evje pegmatite field incorporates a higherproportion of trace elements in simple substitutionsthan the Froland pegmatite field (Fig. 4a). It is alsoimplied that the Froland and the Evje pegmatite liquids,in this type of plot, follows distinctively different tra-jectories.

Trace elements in quartz compared to K-feldspar

The Sr/Rb and the Rb/Ba ratios of K-feldspar areexceptionally sensitive to the composition of the graniticmelt. These ratios will decrease and increase, respec-tively, as the granitic system develops from primitivecompositions at high temperatures to evolved composi-tions at lower temperatures (e.g. Shearer et al. 1985;Kontak and Martin 1997; Larsen 2002).

When the proportions of trace elements in quartz areplotted against the Sr/Rb and the Rb/Ba ratios in ternarydiagrams, the relative proportions of trace elements fol-lows an increasing trajectory during the early stages ofigneous differentiation (Fig. 4b–d). However, during thelater parts of the igneous differentiation the relativeproportion of trace elements decline along a steep tra-jectory towards the Rb/Ba apex of the ternary diagrams.When the K-feldspar ratios are plotted against the totalconcentration of simple substitutions in quartz, theFroland and Evje pegmatites follows distinctively dif-ferent paths during the igneous evolution (Fig. 4b).Accordingly, it is implied that the Evje pegmatites obtainhigher relative proportions of simple substitutions whencompared to the igneous evolution of the Froland quartz.

Being ternary diagrams, Fig. 4a–d does not documentthe trace element evolution in absolute concentrationsbut rather demonstrate relative similarities and differ-ences between the pegmatite fields.

To fully understand the partitioning of trace elementsbetween quartz and the co-existing granitic melts, thedistribution of key trace elements in quartz are com-pared to the distribution of Rb, Pb and Ga in K-feld-spar. In particular Rb, but also Pb and Ga are stronglyincompatible elements in granitic melts hence theirconcentration in K-feldspar will increase as the graniticmelt develops from primitive to progressively moreevolved compositions (e.g. Shearer et al. 1985; Kontakand Martin 1997; Larsen 2002).

In a first approach, only pegmatite localities fromEvje are evaluated given that they are less deformed andrecrystallized than the Froland pegmatites. Also, inEvje, it was possible in most pegmatites to samplepristine K-feldspar in direct contact with quartz.

The concentrations of Geqz and Pqz in quartz areincreasing proportionallywith the concentration ofRbkfs,Pbkfs and Gakfs in K-feldspar (Fig. 5a,b). The concen-tration of Tiqz, Beqz, Feqz andKqz in quartz is falling as theconcentration of Rbkfs, and in most cases also Pbkfs isincreasing in K-feldspar (Fig. 5c–f). The trends for Beqzare well constrained, whereas the trends for Feqz and Kqz

are more erratic. Titaniumqz is negatively correlated withRbkfs. The concentration of Alqz and Liqz is inconsistentwhen compared to Rbkfs and Pbkfs. Apparently theconcentrations of bothAlqz andLiqz are increasing up to acertain point after which they follow a path of constantRb-values or, in the case of Liqz, the path becomes neg-ative with the highest concentrations of Liqz coincidingwith lowest concentrations of Rbkfs (Fig. 5g,h).

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Table 2 Trace elements in quartz

Location Area UTM-East UTM-North n Li Be Al P K Ti Fe Ge Sr

81 Evje 434300 6475200 3 14.2 0.249 47.1 18.4 – 16.87 11.57 2.96 0. 08482 Evje 434475 6475550 3 10.6 0.297 48.8 21.3 1.01 11.85 1.71 1.32 0. 01583 Evje 434650 6476725 6 6.0 0.338 52.3 15.6 5.49 22.15 2.37 1.25 0. 06384 Evje 436150 6477500 6 11.9 0.348 217.7 18.5 21.10 16.66 4.20 2.87 0. 48985 Evje 435750 6478050 6 11.7 0.265 42.9 16.2 1.59 20.37 1.86 1.62 0. 00186 Evje 435675 6478700 6 12.2 0.241 98.1 14.0 13.61 22.12 2.27 1.40 0. 00387 Evje 435400 6481750 6 8.2 0.244 68.2 15.7 34.22 28.74 2.01 1.14 0. 03088 Evje 433350 6483750 6 4.9 0.225 72.1 12.7 2.66 16.70 1.56 2.22 0. 32889 Evje 433600 6483800 3 3.5 0.150 30.4 14.0 2.61 31.42 5.10 1.18 0. 01690 Evje 435350 6485500 6 3.9 0.172 78.9 16.3 8.45 24.47 1.81 2.14 0. 56591 Evje 436575 6486150 6 9.4 0.122 140.3 18.8 16.24 28.08 3.68 1.69 0. 09292 Evje 437175 6488600 6 7.2 0.100 93.8 20.7 9.95 30.06 1.88 1.81 0. 01893 Evje 436500 6489800 6 10.6 0.147 171.7 18.4 25.49 31.00 1.59 2.02 0. 6061 Froland 469400 6495320 1 11.4 0.088 46.2 11.1 1.92 7.02 0.58 1.29 0. 0942 Froland 469550 6495170 1 16.0 0.074 35.8 12.0 2.76 7.24 0.12 0.95 0. 2693 Froland 469630 6494860 2 13.8 0.065 36.5 11.9 0.90 5.23 0.21 1.23 0. 0634 Froland 466760 6494840 3 13.2 0.036 34.3 10.8 1.32 7.87 0.85 1.84 0. 0785 Froland 467330 6494900 2 10.9 0.071 32.6 13.1 1.08 6.37 0.69 1.04 0. 0496 Froland 465090 6485700 1 8.8 0.141 35.4 10.8 2.34 8.28 0.45 2.96 0. 0737 Froland 465490 6485910 1 7.7 0.170 50.9 12.1 3.01 7.73 0.20 3.61 0. 0248 Froland 465970 6485750 2 7.5 0.131 44.1 12.1 6.99 13.32 0.91 0.82 0. 0759 Froland 464600 6488210 1 11.8 0.053 30.9 12.5 1.06 7.99 0.28 1.43 0. 04010 Froland 463920 6487680 1 16.7 0.158 96.9 9.4 24.05 12.38 1.08 2.46 0. 82211 Froland 463320 6487190 1 11.2 0.102 65.2 10.8 6.85 10.78 0.34 0.98 0. 19112 Froland 462900 6486800 1 5.4 0.049 60.7 10.7 5.53 14.72 0.71 1.53 0. 11913 Froland 467760 6496180 1 10.0 0.008 35.4 9.4 4.50 6.08 0.49 1.22 0. 04414 Froland 467640 6495980 1 4.2 0.008 23.7 15.1 1.44 6.69 0.50 0.94 0. 05215 Froland 466900 6491300 2 7.0 0.056 24.2 13.3 0.85 8.87 0.27 1.77 0. 03416 Froland 466830 6490950 1 8.9 0.065 22.6 15.3 1.59 8.36 0.60 1.16 0. 01917 Froland 467570 6490930 1 9.3 0.084 57.8 11.0 1.37 7.07 0.27 1.31 0. 22318 Froland 467620 6490570 1 11.5 0.071 32.9 9.6 1.36 6.15 0.43 2.52 0. 07119 Froland 467500 6490450 1 9.6 0.134 28.9 11.9 0.79 6.13 0.57 1.60 0. 03520 Froland 467470 6490330 1 8.2 0.050 19.9 9.7 0.54 5.76 0.38 2.42 0. 00421 Froland 467180 6488530 1 6.4 0.008 14.0 10.1 0.70 9.81 0.24 1.48 0. 02823 Froland 467560 6491190 1 11.0 0.064 36.2 11.0 2.69 8.21 0.15 2.23 0. 04224 Froland 466930 6495660 1 9.1 0.027 24.1 10.9 0.79 9.31 0.22 1.30 0. 02025 Froland 467280 6495520 1 9.9 0.096 40.7 9.5 1.54 16.60 0.62 1.19 0. 02326 Froland 467330 6495550 1 10.0 0.039 18.0 10.2 0.99 11.22 0.20 0.56 0. 02327 Froland 462940 6486490 1 6.3 0.030 32.2 11.3 2.76 17.43 0.60 1.09 0. 14928 Froland 468630 6495470 1 10.6 0.073 35.4 10.8 1.06 8.61 1.69 1.14 0. 02029 Froland 468880 6495320 1 9.0 0.090 8.5 14.6 3.88 6.56 3.11 1.07 0. 07230 Froland 470400 6495730 1 5.4 0.040 26.6 10.7 1.57 5.27 0.50 1.58 0. 02631 Froland 470350 6495480 1 10.0 0.020 20.3 9.9 0.74 6.07 0.28 1.34 0. 03632 Froland 469880 6495790 1 8.2 0.072 20.7 11.0 1.59 5.01 0.37 1.07 0. 01633 Froland 467410 6487690 1 8.1 0.118 30.4 11.2 3.45 9.53 0.63 2.21 0. 07434 Froland 467120 6488120 1 11.0 0.091 34.3 10.2 1.12 3.06 0.31 2.21 0. 02235 Froland 466560 6489740 1 15.4 0.120 40.4 11.2 0.52 5.95 0.60 1.85 0. 01736 Froland 466790 6490080 1 16.7 0.081 37.2 10.4 0.74 8.90 0.30 0.87 0. 02637 Froland 466670 6490050 1 9.7 0.040 67.9 10.9 10.91 7.49 0.57 1.33 0. 53638 Froland 466630 6489810 1 14.9 0.165 33.8 11.0 1.15 9.36 0.27 3.06 0. 01439 Froland 466460 6489670 1 11.1 0.105 28.7 10.9 0.45 5.85 0.49 1.98 0. 01940 Froland 466260 6488050 1 11.4 0.048 19.1 11.6 0.63 9.59 0.59 1.02 0. 02741 Froland 465630 6487720 1 13.3 0.018 24.5 9.8 4.97 8.33 1.08 1.01 0. 00842 Froland 466500 6488290 1 14.0 0.029 24.8 10.1 4.15 8.51 1.14 1.20 0. 01843 Froland 466330 6487770 1 8.8 0.011 16.7 10.0 0.48 13.32 0.25 0.84 0. 02644 Froland 466260 6489620 1 7.5 0.157 56.3 17.1 0.96 4.98 0.28 1.38 0. 03645 Froland 466690 6487320 1 11.9 0.061 36.8 10.8 0.42 5.29 0.14 2.77 –46 Froland 466470 6486880 1 8.6 0.034 33.5 10.6 0.47 5.98 0.23 1.12 0. 03347 Froland 468730 6494860 1 12.7 0.047 62.8 10.1 2.11 4.25 0.84 1.90 0. 03748 Froland 468280 6494470 1 9.7 0.038 43.6 9.7 1.16 10.15 0.12 0.99 0. 03149 Froland 467150 6493200 1 8.4 0.035 22.8 15.1 0.75 7.47 0.38 0.70 0. 06750 Froland 468020 6493300 1 7.1 0.083 42.3 10.9 0.49 7.65 0.42 2.70 –51 Froland 469890 6494100 1 32.2 0.079 84.7 11.7 0.94 5.61 0.91 1.98 0. 03652 Froland 470540 6496270 1 12.8 0.067 50.9 10.4 1.66 4.85 5.30 1.64 0. 02453 Froland 467540 6491090 4 6.0 0.199 178.8 22.9 1.36 6.00 0.53 1.05 0. 01554 Froland 469830 6496810 1 12.9 0.057 48.9 15.4 2.37 7.74 0.69 1.57 0. 02755 Froland 467920 6495460 4 12.6 0.091 35.8 19.3 – 7.50 – 0.66 –

621

All together, Geqz, Pqz, Beqz and Tiqz are most con-sistent in their correlation with Rbkfs and partially withPbkfs and Gakfs. Therefore, the Ge/Ti and the Be/Tiratios, for example, may be sensitive to the igneousevolution of the granitic melts.

To test this hypothesis, the Ga, Pb and Rb concen-trations of K-feldspar were compared to the Ge/Ti andthe Ge/Be ratios of quartz (Fig. 6a–f) and, apparently,the concentration of the incompatible elements in K-feldspar is well correlated with these ratios. The P/Be orthe P/Ti ratios would be other choices of differentiationindex, however, Ge, Ti and Be are analysed with a muchhigher precision than P because, in the plasma processduring ICP-MS, P does not ionise as well as Ge, Ti andBe. In the end, the Ge/Ti ratio was prioritised in thepresent study since Be may be mobile during subsolidusprocesses. Another advantage in choosing the Ge/Tiratio is that both ions are simple substitutional ionshence compete for the same structural position inquartz. Accordingly, their incorporation in quartz isindependent upon the availability of charge compensa-tors, lattice defects and vacancies.

Discussion

Igneous geochemistry of quartz

The current study implies that early formed quartzfeatures a relative enrichment of Ti, Be and K whereas

Ge and P and, partially, Li and Al are enriched atlower temperatures during late crystallization graniticsystems. Accordingly, Ti, Be and K are predominantlycompatible elements whereas Ge, P, Li, and Al maybe regarded as incompatible. Based on the relativechange in the concentration of trace elements fromprimitive to more evolved granites, the trace elementsmay tentatively be organised in the following fashion:

Relatively compatible Relatively incompatibleK¼>Fe¼>Be¼>Ti¼>P¼>Ge¼>Li¼>A1

Where the elements become progressively moreincompatible towards the right.

Furthermore, the total concentration of stuffedderivatives, i.e. element pairs of Li and Al, increases atlower temperatures. At higher temperatures in earlierformed quartz, the proportion of coupled- and single-substitutions is higher (Fig. 4a,b).

Particularly Al, Li and K show a somewhat irregulartrend during igneous evolution of the granitic melts(Fig. 5f–h), whereas Ge, P, Ti and Be are more wellconstrained. The underlying reasons for this distributionpattern is probably two-fold.

The oxidation state of Ge, Ti, P and Be ions does notchange throughout common geological conditions andthey occur at only one structural site in the atomic latticeof quartz. Secondly, as substitutions for Si, they arestrongly confined to the atomic lattice structure ofquartz hence are not easily influenced by subsolidusprocesses (except for Be).

Table 2 (Contd.)

Location Area UTM-East UTM-North n Li Be Al P K Ti Fe Ge Sr

56 Froland 467650 6490560 13 12.7 0.083 56.4 11.9 – 5.17 – 1.25 –57 Froland 470020 6495990 1 6.7 0.041 25.8 16.3 – 8.85 – 1.31 –58 Froland 469860 6495600 1 14.6 0.039 35.2 4.2 – 3.94 – 0.76 –59 Froland 471700 6496420 1 15.0 0.015 35.6 8.2 – 5.29 – 0.16 –61 Froland 471540 6500370 1 11.6 0.063 39.5 12.4 – 11.47 – 0.64 –63 Froland 472190 6500290 2 15.0 0.097 69.6 10.3 – 5.23 – 1.17 –64 Froland 468550 6494450 3 12.2 0.122 36.0 8.7 – 4.67 – 1.17 –65 Froland 470900 6498370 1 4.0 0.008 24.2 15.3 – 9.82 – 0.66 –66 Froland 470040 6495640 1 17.6 0.097 5.0 1.0 – 4.86 – 1.73 –67 Froland 471530 6496570 1 10.3 0.099 7.2 0.3 – 2.84 – 1.92 –68 Froland 472090 6496670 1 4.0 0.065 29.3 1.0 – 4.64 – 1.18 –70 Froland 462250 6485580 1 13.7 0.116 25.5 0.9 – 14.93 – 2.20 –72 Froland 465320 6494100 1 4.0 0.079 12.8 1.0 – 20.05 – 0.73 –73 Froland 464150 6492030 1 4.0 0.144 79.7 1.0 – 14.08 – 1.30 –94 Froland 436112 6487535 23 9.8 0.202 63.3 64.4 – 31.67 – 2.04 –95 Froland 435546 6488751 1 11.3 0.363 48.6 53.4 – 30.70 – 1.93 –96 Froland 435522 6488767 1 12.3 0.169 48.6 53.4 – 30.70 – 1.14 –98 Froland 450650 6477060 3 13.6 0.087 180.8 22.2 83.87 140.11 41.35 1. 06 0.67199 Froland 461350 6479125 6 12.7 0.088 99.9 13.8 21.15 23.22 1.80 2.10 0. 385100 Froland 466900 6487500 6 14.2 0.111 39.2 14.3 4.42 4.85 2.96 3.71 0. 041101 Froland 466200 6488350 3 17.0 0.046 53.0 10.0 8.25 5.75 1.01 1.84 0. 057102 Froland 467300 6495500 3 10.2 0.101 42.1 10.6 19.41 8.25 1.42 2.02 0. 071103 Froland 467325 6494850 6 15.6 0.072 44.1 9.8 1.01 4.44 0.71 1.45 0. 004108 Froland 469350 6495125 6 15.5 0.112 57.3 10.7 8.86 3.63 1.33 2.02 0. 048109 Froland 469375 6495250 3 17.3 0.155 48.1 7.1 0.13 2.17 1.15 1.18 0. 003110 Froland 469550 6495100 6 23.9 0.083 99.8 11.4 15.48 8.02 1.10 2.00 0. 059

()) Either, not analysed or falling below the limit of detection. Cr, Mg, Mn, Na, Pb, Rb, Th and U were included in the analytical packagebut mostly fell below the LOD, hence are omitted from the table. All concentrations are in ppm

622

On the contrary, Al and Fe3+ may be assigned aseither coupled substitutions with P or stuffed derivativeswith a charge compensator, typically Li. Accordingly,Fe and Al are more versatile during igneous differenti-ation. Either, Al and Fe3+ may be enriched in quartzthat crystallised at low temperatures where it predomi-nantly is charge compensated by Li, which is an

incompatible element, or they may be enriched at hightemperatures if they are coupled with P, which is morecompatible.

Iron features the added complexity that it may bepresent in two oxidation states hence may occur as eithersingle substitutions for Si or in vacancies. Finally, somerecent studies imply that iron has the ability to diffusethroughout the quartz atomic lattice (Penniston-Dor-land 2001; Muller et al. 2002a,b).

Given these chemical properties, it is not surprisingthat the distribution of Al and Fe, throughout theigneous differentiation of granitic melts is more incon-sistent than Ge, Ti, P and Be.

Based on the previous rationale, Li and K, beingstrictly monovalent cations that are adapted in the

Fig. 4 Composition of quartz compared to the igneous evolutionof K-feldspar. The Sr/Rb and the Rb/Ba ratios express the igneousevolution of K-feldspar. The composition of quartz is classifiedaccording to structural sites i.e. ‘‘Simple substitutions’’ includesmol Ge + Ti, coupled substitutions largely comprises mol P +and an equivalent mol proportion of Al. Stuffed derivativesprimarily includes mol Al + Li with accessory contributionsfrom Na, K and B. Mol contributions of other ions are insignificant

623

same structural settings in the quartz atomic lattice (i.e.atomic channels, lattice defects), should change sys-tematically and predictably throughout the igneous

evolution of the granitic system. Agreeing with thispresumption, the K-concentrations in quartz aredecreasing systematically throughout differentiation. Liis mostly enriched in late-formed quartz, however, thetrajectories that Li follows throughout igneous differ-entiation is not as well defined as with Ge and Ti(Fig. 5). Either, the behaviour of Li during igneousprocesses is more erratic than the other elements or the

Fig. 5 Absolute concentration of Ge, P, Ti, Be, Fe, K, Al and Li inquartz compared to the concentration of three incompatibleelements in granitic K-feldspar (Rb, Pb and Ga). All samples arefrom the Evje pegmatite field. Arrows define the direction ofigneous differentiation

624

Fig. 6 Concentration of Rb,Ga and Pb in K-feldsparcompared to the Ge/Ti and theGe/Be ratio of quartz. Allsamples are from the Evjepegmatite field. Arrows definethe direction of igneousdifferentiation

Table 3 Effects of hydrothermal recrystallization of primary igneous quartz (all values in ppm)

Sample Type Li Be B Na Al P K Ti Mn Ge Rb Sr Ba

97047-1 Primary 4.5 0.054 0.35 6.47 15.6 0.23 4.02 37.98 0.30 1.18 0.002 0.063 0.0697047-2 Early secondary 1.6 0.058 0.44 9.20 16.1 1.92 4.04 44.46 0.20 1.30 0.018 0. 068 0.0797047-3 Late secondary 0.2 0.049 0.45 – 21.2 30.71 – – 0.36 1.32 0.027 0.083 0. 2897111A-1 Primary 5.0 0.091 2.72 11.07 21.1 5.22 4.02 9.28 0.45 3.54 0.239 0.108 0.0897111A-2 Early secondary 2.4 0.106 2.16 70.17 18.1 6.09 6.85 9.32 0.30 3.31 0.185 0. 115 0.1397111A-3 Late secondary 0.7 0.061 0.51 15.78 12.4 10.59 – 9.88 0.42 3.27 0.029 0. 129 0.0897111B-1 Primary 7.2 0.115 1.37 25.92 4.5 0.97 4.24 9.84 0.30 3.09 0.077 0.146 0.1097111B-2 Secondary 3.1 0.116 2.09 41.33 19.1 4.49 10.15 6.71 0.41 3.35 0.167 0.157 0.2097115-1 Primary 9.4 0.111 0.30 2.26 17.9 2.90 3.25 5.89 0.21 1.49 0.007 0.163 0.0697115-2 Early secondary 5.1 0.095 0.41 8.54 25.0 3.49 5.05 5.05 0.19 1.52 0.030 0. 169 0.1397132A-1 Primary 5.3 0.096 1.27 14.95 28.5 10.18 9.04 9.32 0.11 1.37 0.038 0.230 0.0997132A-2 Early secondary 3.2 0.006 1.16 27.72 25.3 9.99 4.31 10.84 0.21 1.07 0.018 0. 291 0.0897132B-1 Primary 5.6 0.095 2.34 47.83 26.1 9.58 17.21 9.42 0.32 1.62 0.085 0.336 0.1097132B-2 Early secondary 1.5 0.022 1.86 87.29 46.9 8.90 268.28 10.54 0.64 1.62 0.093 0. 366 0.17

625

chemical properties of this element together with itsassignment to the quartz lattice make it more prone tosubsolidus processes than Ge and Ti.

Subsolidus remobilisation

In order to test the sensitivity of Li and other monova-lent cations to subsolidus processes, we analysed Evjeand Froland quartz that had recrystallized repetitivelyduring subsolidus conditions (Figs. 3d and 7). Theseanalyses consistently imply that Ge and Ti maintainconstant concentrations even through episodes of per-vasive recrystallization (Table 3, Fig. 7a,b). On thecontrary, the concentration of Li is falling with the de-gree of recrystallization whereas the concentrations ofNa and K respectively, are increasing (Na) or nearlyconstant (K) (Fig. 7c–e). Accordingly, Na partition infavour of quartz whereas Li partition in favour of theaqueous fluids that are associated with subsolidusrecrystallization. Potassium is apparently undisturbedby the infiltrating aqueous fluids.

With these results it is implied that Li and Na has theability to partially migrate in and out of the quartz lat-tice during subsolidus hydrothermal alteration.

Igneous evolution of granitic pegmatites

Normally when evaluating the origin, igneous evolutionand the petrogenetic links of granitic pegmatites in alarge and complex igneous field, the traditional choicehas been to look at the composition of feldspar (e.g.Heier and Taylor 1959; Shearer et al. 1985, 1992; AbadOrtega et al. 1993; Icenhower and London 1996; Kontakand Martin 1997; Larsen 2002). However, when severalparent melts are involved in the genesis of the pegma-tites, the major and trace element composition of thefeldspars does not adequately distinguish the differentgenerations of granitic pegmatites (e.g. Larsen 2002).Accordingly, when for example the Rb/K ratio is plottedagainst the Sr/Rb ratio, granitic pegmatites with differ-ent parent melts follow overlapping trajectories duringtheir igneous evolution (Larsen 2002).

Fig. 7 Mobility of trace elements in quartz during subsolidus fluidinfiltration and recrystallization of igneous quartz. Primary, earlysecondary and late secondary quartz refers to the types of quartzshown on Fig. 3d. Each line comprises a pegmatite locality

Fig. 8 Igneous evolution of granitic quartz. The trace elementdistribution in igneous quartz follows distinctively different trendsduring their igneous evolution from primitive to progressively moreevolved quartz. Arrows define the direction of igneous differenti-ation

626

On the contrary the trace element distribution inquartz distinctively document the contrasting origin ofthese two fields in South Norway (Fig. 8a,b). Particu-larly when Geqz and Beqz are plotted against the Ge/Tiqzratio, it is clear that the fields follow distinctively dif-ferent trends during their igneous evolution.Accordingly the concentrations of these elements areincreasing along a much steeper slope in the Evje field asthe igneous evolution develops towards progressivelymore evolved compositions.

Conclusions

– The dominant trace elements in igneous quartz in theEvje and Froland pegmatite fields comprises Al, P, Li,Ti, Ge, Fe and K in that order of abundance and inconcentrations greater than 1 ppm. Be, B, Ba and Srare common in concentrations from a few ppb to1 ppm.

– Structural bound trace elements in quartz are highlysensitive to petrogenetic processes. Particularly Ge, P,Ti and Be record both the origin and evolution of thegranitic rocks and efficiently discriminate betweenmelts of different origin. Compared to K-feldspar,quartz is more efficient in distinguishing igneous rockswith different petrogenetic histories.

– K, Fe, Be and Ti are the most compatible trace ele-ments, P is transitional whereas Ge, Li, and Al pre-dominantly are incompatible.

– Ge and Ti are immobile during subsolidus recrystal-lization of igneous quartz. Li partition in favour of theinfiltrating aqueous fluids whereas Na partition infavour of quartz.

– In distinguishing igneous processes and petrogeneticlinks in a pegmatite field, any of the ratios Ge/Ti, Ge/Be, P/Ti and P/Be may be utilised. However, the Ge/Ti ratio is more robust to subsolidus processes andboth Ge and Ti features good analytical behaviourduring LA-ICP-MS analysis.

Acknowledgements The authors are indebted to the NorwegianResearch Council (Project: The value chain of quartz from bedrockto beneficiated product) and North Cape Minerals for partialfunding of this study. Careful and constructive reviews by Dr. A.Muller and Dr. K. Simon are much appreciated.

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