Author's personal copy Earth and Planetary Science Letters 286 (2009) 208–218 Contents lists available at ScienceDirect Earth and Planetary Science Letters j o u r n a l h o m e p a g e : w w w. e l s ev i e r. c o m / l o c a t e / e p s l Zircon and titanite recording 1.5 million years of magma accretion, crystallization and initial cooling in a composite pluton (southern Adamello batholith, northern Italy) Urs Schaltegger a,⁎, Peter Brack b, Maria Ovtcharova a, Irena Peytcheva a,b,c, Blair Schoene a, Andreas Stracke b, Marta Marocchi d, Giuseppe M. Bargossi d a Section des Sciences de la Terre et de l'environnement, Université de Genève, 1205 Genève, Switzerland Departement Erdwissenschaften, ETH Zürich, 8092 Zürich, Switzerland Geological Institute, Bulgarian Academy of Science, Sofia, Bulgaria d Dipartimento di Scienze della Terra e Geologico-Ambientali, Università di Bologna, P.zza P.ta S. Donato,1-40126, Bologna, Italy b c a r t i c l e i n f o Article history: Received 4 February 2009 Received in revised form 15 June 2009 Accepted 20 June 2009 Available online 17 July 2009 Editor: R.W. Carlson Keywords: Adamello batholith U–Pb dating zircon titanite hafnium isotopes zircon residence time a b s t r a c t The southern part of the Adamello batholith (the so-called “Re di Castello unit”) is an example of a composite pluton, ranging from gabbro to granodiorite in composition. U–Pb dating of single-zircon crystals from four tonalitic to granodioritic lithologies reveals that zircon crystallization is protracted in all studied lithologies, showing apparent durations of growth between 90 and 700 ka. The youngest zircons crystallized near the solidus and yield identical or slightly older ages than titanite. The formation of these autocrystic zircons is considered to approximate the age of emplacement of the melt and its final crystallization, in contrast to antecrystic zircons present in the same sample, which had formed earlier in the magmatic column or were derived from re-mobilized earlier magma. The autocryst-derived “emplacement” ages range from 42.43 ± 0.09 Ma to 40.90 ± 0.05 Ma, recording 1.5 Ma of intrusion and crystallization history. We anticipate that extended periods of zircon crystallization may be common in silicic rocks, whereas the zircons from residual melts from initially undersaturated mafic liquids should yield far more precise emplacement ages within our present analytical uncertainties of 0.1–0.2% in 206Pb/238U age. Decreasing Th/U ratios of dated zircons within one melt batch document the depletion of the residual melt portion in Th due to the contemporaneous crystallization of titanite. Preliminary Hf isotopic compositions of the dated zircon grains suggest that the early stage melts of the southern Re di Castello unit represent hybrid melts with an important crustal component (εHf between − 2.8 and +3.0). Subsequently emplaced melts are more juvenile at εHf values at +6.4 to +8.9 and may thus reflect the addition of large volumes of mafic melt to the magmatic system. © 2009 Elsevier B.V. All rights reserved. 1. Introduction Middle-to-upper crustal plutons provide a complex integrated picture of tens of thousands to million year-long evolution of melt accretion, melt depletion and crystallization. This often complex history can be reconstructed from analyzing magmatic mineral textures and syn-magmatic deformation structures at micro-to-macroscale. A growing body of age determinations provide evidence that the emplacement of even apparently homogeneous plutons occurs by the sequential injection of multiple magma pulses, as well as lateral or vertical accretion of magma batches, both in the subvolcanic environment (Bacon et al., 2007, Charlier et al., 2008) and in the middle-to-upper crustal level (Coleman et al., 2004; Matzel et al., 2006; Michel et al., 2008). Zircon is a suitable mineral to reconstruct these processes, since it records crystallization at different stages of magmatic evolution: in the source, during the ascent and at the final level of emplacement, starting ⁎ Corresponding author. Tel.: +41 22 379 66 38; fax: +41 22 379 32 10. E-mail address: [email protected] (U. Schaltegger). 0012-821X/$ – see front matter © 2009 Elsevier B.V. All rights reserved. doi:10.1016/j.epsl.2009.06.028 at the moment the melt has reached zircon saturation (e.g., Belousova et al., 2006). The emplacement of magmatic liquids in the intermediate and upper crust occurs over variable timescales: batholiths can grow over hundred thousands to millions of years (e.g., Matzel et al., 2006) and be composed of individual magmatic pulses that intruded over much shorter time spans, i.e. in the range of several tens to hundred thousand years (e.g., Michel et al., 2008). Can we quantify the timescale during which an individual pluton is assembled? A challenge of modern high-precision U–Pb geochronology is to resolve the emplacement ages of individual magma pulses within a larger magmatic context by analysis of single-zircon crystals. We assume that zircon may crystallize over a considerable time in the same batch of magma, even prior to the final emplacement. This may be startling for people who used to think of the emplacement “age” of a pluton. It has been made possible by recent improvement in analytical precision and accuracy in U–Pb zircon dating: development of annealing–leaching (chemical abrasion) techniques (Mattinson, 2005) to mitigate the problem of lead loss, improved precision by using a new 205Pb–233U– 235 U tracer solution (Condon and Members of the Earthtime Working Author's personal copy U. Schaltegger et al. / Earth and Planetary Science Letters 286 (2009) 208–218 Group, 2005) and reducing tracer calibration uncertainties (Schoene et al., 2006; Schmitz and Schoene, 2007), and thorough monitoring of analytical conditions during mass spectrometric analysis (described in Sláma et al., 2008). Part of this effort is a community-wide intercalibra- 209 tion effort for removing inter-laboratory biases (Condon and Members of the Earthtime Working Group, 2005; Sláma et al., 2008; see most recent status on www.earth-time.org). Furthermore, we are able to quantify the initial subsolidus cooling of a crystallized magma body Fig. 1. Geological map of the Adamello batholith in N Italy. Inset: Map of Re di Castello unit, southern Adamello, with (1) Western Adamello tonalite, (2) Mte. Re di Castello tonalites, (3) Lago d'Arno/Lago Boazza leucotonalites, (4) Badile granodiorite, (5) Bruffione granodiorite, (6) Listino tonalite, (6a) Listino poprphyry ring structure, (7) Galliner tonalite, (8) Passo del Termine/Val Paghera leucotonalites, (9) Lage della Vacca tonalites, (10) Blumone gabbros and quartz-diorites, (11) Alta Guardia tonalite, (12) Val Fredda tonalite. Sample localities are indicated by asterisks. Author's personal copy 210 U. Schaltegger et al. / Earth and Planetary Science Letters 286 (2009) 208–218 Table 1 U, Pb isotopic results and ages for zircons from Southern Adamello. Samplea Monte 1 2 3 4 5 6 7 8 9 10 11 12 13 Weight Concentrations (mg) U Th/Ub Pb Pb Rad. (ppm) Nonrad. (pg) Frerone aplite granite dykes (GMF) z 0.0070 954 6.75 0.42 z 0.0020 785 7.78 0.47 z 0.0016 861 6.12 0.39 z 0.0049 1094 7.43 0.53 z 0.0049 1061 8.33 0.48 z 0.0028 726 5.23 0.86 z 0.0014 983 6.94 1.43 z 0.0023 1451 10.39 0.20 z 0.0022 1207 8.17 0.54 z 0.0023 941 8.78 0.56 z 0.0009 878 6.20 0.53 z 0.0013 1188 8.42 2.37 t 0.0125 85 0.83 13.50 Atomic ratios Apparent ages 206/ 204c 207/ 235d,e Error 0.62 0.48 0.64 0.43 0.46 0.54 0.60 0.43 0.44 0.43 0.61 0.62 2.08 6926 2114 1564 4444 5425 1065 418 59,148 2073 2204 642 289 52 0.04275 0.06544 0.04270 0.04337 0.05051 0.04468 0.04296 0.05235 0.04294 0.06249 0.04255 0.04240 0.04232 206/ 238d Error 0.23 0.33 0.44 0.25 0.22 0.31 1.06 0.10 0.26 0.31 0.90 1.64 5.21 0.00661 0.00951 0.00660 0.00667 0.00762 0.00685 0.00663 0.00686 0.00663 0.00909 0.00662 0.00663 0.00662 2σ (%) Error 206/238 2σ (%) Corrected for disequilibrium 0.20 0.20 0.20 0.20 0.19 0.20 0.10 0.06 0.06 0.09 0.10 0.13 0.37 0.04688 0.04988 0.04689 0.04719 0.04804 0.04727 0.04696 0.05539 0.04701 0.04989 0.04659 0.04635 0.04639 0.11 0.25 0.38 0.15 0.11 0.23 0.99 0.08 0.24 0.29 0.85 1.54 4.89 42.50 61.05 42.43 42.82 48.97 44.04 42.63 44.04 42.57 58.30 42.56 42.63 42.51 42.50 64.36 42.45 43.11 50.03 44.38 42.71 51.81 42.69 61.55 42.31 42.16 42.09 43.06 189.43 43.64 58.86 101.20 62.86 47.18 427.98 49.70 189.89 28.30 15.83 18.16 0.87 0.65 0.51 0.80 0.87 0.67 0.73 0.62 0.44 0.36 0.55 0.79 0.88 2σ (%) 207/235 207/206 Error corr. 207/ 206d,e Leucotonalite of Alta Guardia (TAG) 14* z 0.0031 1163 7.78 15* z 0.0069 354 3.29 16* z 0.0075 418 3.13 17* z 0.0064 438 3.07 18* z 0.0046 634 4.24 19 z 0.0034 694 4.84 20 z 0.0074 356 2.35 21 z 0.0090 308 2.09 22 z 0.0097 511 3.39 23 z 0.0130 292 1.98 24 z 0.0102 301 2.02 25 z 0.0092 513 3.49 26 t 0.0226 329 1.99 27 t 0.0204 453 3.50 28 t 0.0275 709 4.40 29 t 0.0186 897 3.60 30 t 0.0377 616 3.74 2.56 2.13 1.10 2.50 2.60 0.71 0.72 0.63 0.94 0.89 1.50 1.13 53.20 45.44 56.85 43.31 43.49 0.47 0.10 0.87 0.48 0.47 0.64 0.46 0.55 0.46 0.36 0.44 0.55 0.14 1.07 0.22 0.14 0.13 596 697 1238 492 478 1414 1570 1901 2148 1837 859 1708 76 103 160 124 241 0.04186 0.06436 0.04202 0.04342 0.04174 0.04169 0.04176 0.04191 0.04187 0.04447 0.04263 0.04200 0.04237 0.04218 0.04202 0.04192 0.04203 0.83 0.74 0.70 1.11 1.11 0.38 0.40 0.37 0.33 0.28 0.56 0.32 0.89 0.76 1.87 1.05 0.38 0.00649 0.00935 0.00650 0.00668 0.00647 0.00645 0.00644 0.00646 0.00646 0.00680 0.00657 0.00646 0.00643 0.00643 0.00644 0.00642 0.00649 0.35 0.37 0.38 0.35 0.35 0.27 0.21 0.20 0.06 0.07 0.08 0.07 0.07 0.08 0.12 0.09 0.07 0.04681 0.04992 0.04689 0.04715 0.04679 0.04684 0.04699 0.04702 0.04697 0.04746 0.04710 0.04715 0.04781 0.04755 0.04733 0.04732 0.04694 0.71 0.62 0.57 1.01 1.01 0.26 0.33 0.30 0.30 0.26 0.52 0.30 0.84 0.72 1.76 0.99 0.35 41.67 59.99 41.76 42.91 41.58 41.48 41.41 41.54 41.54 43.66 42.18 41.52 41.31 41.34 41.38 41.28 41.73 41.64 63.33 41.79 43.16 41.52 41.47 41.54 41.69 41.65 44.18 42.39 41.78 42.14 41.95 41.80 41.70 41.80 39.56 191.36 43.79 56.71 38.33 41.20 48.67 50.27 47.70 72.47 54.28 56.65 89.80 77.01 65.88 65.60 45.98 0.53 0.55 0.58 0.43 0.43 0.73 0.55 0.59 0.43 0.40 0.55 0.41 0.73 0.54 0.89 0.71 0.50 Tonalite of Malga Listino (TML) 31* z 0.0015 847 32* z 0.0040 500 33 z 0.0026 192 34 z 0.0010 325 35 z 0.0012 563 36 z 0.0014 607 37 z 0.0024 420 38 z 0.0040 312 39 z 0.0036 213 40 z 0.0025 232 41 z 0.0028 600 42 z 0.0015 816 43 t 0.0253 332 44 t 0.0184 353 45 t 0.0169 444 46 t 0.0273 396 47 t 0.0298 393 5.68 4.83 1.33 2.21 3.69 4.20 2.67 2.18 1.49 1.70 3.99 5.74 3.51 3.60 4.00 3.90 3.92 2.09 7.79 0.65 0.59 0.55 0.88 0.34 0.79 0.79 0.92 0.87 0.86 28.19 20.73 30.31 29.21 38.58 0.53 0.52 0.63 0.56 0.45 0.66 0.36 0.69 0.68 0.83 0.51 0.72 2.74 2.52 1.83 2.28 2.38 265 123 249 339 528 420 1265 656 406 274 793 589 141 146 119 170 142 0.04126 0.04166 0.04178 0.04170 0.04133 0.04121 0.04152 0.04141 0.04175 0.04242 0.04127 0.04119 0.04118 0.04129 0.04180 0.04156 0.04150 1.59 2.42 1.79 1.66 0.92 0.61 0.53 0.76 1.15 1.91 0.64 0.81 0.84 0.68 0.89 0.76 1.16 0.00639 0.00644 0.00638 0.00644 0.00637 0.00638 0.00637 0.00642 0.00643 0.00647 0.00640 0.00641 0.00637 0.00637 0.00636 0.00638 0.00638 0.35 0.36 0.22 0.87 0.45 0.24 0.21 0.08 0.10 0.16 0.08 0.08 0.09 0.08 0.08 0.07 0.18 0.04680 0.04694 0.05 0.04692 0.04704 0.04683 0.04731 0.04675 0.04706 0.04753 0.04673 0.04658 0.04691 0.04702 0.04770 0.04722 0.04721 1.49 2.27 1.70 1.29 0.75 0.52 0.48 0.71 1.08 1.79 0.60 0.76 0.80 0.64 0.85 0.72 1.09 41.08 41.36 41.02 41.48 40.95 41.01 40.90 41.28 41.34 41.60 41.16 41.21 40.91 40.93 40.85 41.03 40.97 41.05 41.44 41.56 41.48 41.12 41.01 41.30 41.20 41.53 42.18 41.06 40.98 40.98 41.08 41.58 41.35 41.29 39.26 46.00 72.59 45.30 51.30 40.60 64.92 36.43 52.22 75.91 35.40 27.73 44.69 50.07 84.20 60.13 59.90 0.38 0.48 0.62 0.46 0.59 0.54 0.43 0.66 0.72 0.77 0.55 0.68 0.54 0.54 0.53 0.58 0.46 Leucotonalite of Cima di Vallone 48 z 0.0038 653 49 z 0.0011 1143 50 z 0.0013 674 51 z 0.0046 271 52 z 0.0044 267 53 z 0.0042 239 54 z 0.0049 306 55 z 0.0042 321 56 z 0.0040 178 57 z 0.0080 92 (VAL) 5.04 7.59 4.52 1.86 1.83 1.61 2.09 2.33 1.17 0.62 0.88 0.80 0.62 2.36 0.76 0.79 0.64 0.68 1.07 1.39 0.50 0.52 0.55 0.66 0.64 0.56 0.63 0.71 0.48 0.57 1323 645 585 228 636 526 956 832 284 229 0.04916 0.04141 0.04144 0.04123 0.04138 0.04132 0.04116 0.04309 0.04137 0.04177 0.34 0.75 0.99 2.34 0.80 0.90 0.46 0.55 1.52 2.08 0.00739 0.00637 0.00637 0.00637 0.00636 0.00638 0.00636 0.00659 0.00637 0.00638 0.06 0.09 0.12 0.17 0.09 0.09 0.07 0.07 0.13 0.16 0.04822 0.04711 0.04715 0.04691 0.04716 0.04694 0.04691 0.04740 0.04707 0.04745 0.32 0.71 0.94 2.23 0.75 0.84 0.43 0.52 1.43 1.94 47.49 40.96 40.96 40.96 40.90 43.14 40.90 42.37 40.96 41.03 48.73 41.20 41.23 40.96 40.90 41.03 40.90 42.37 41.16 41.56 110.07 54.85 56.80 44.67 57.37 46.15 44.67 69.38 52.79 71.90 0.41 0.55 0.51 0.65 0.62 0.68 0.51 0.49 0.71 0.88 a b c d e z = zircon, t = titanite; all zircons annealed-leached, all single grains, titanites are multigrain fractions; * = measured with Calculated on the basis of radiogenic Pb208/Pb206 ratios, assuming concordancy. Corrected for fractionation and spike. Corrected for fractionation, spike, blank and common lead (Stacey and Kramers, 1975). Corrected for initial Th Disequilibrium, using an estimated Th/U ratio of 4 for the melt. 205 Pb–235U tracer. Author's personal copy U. Schaltegger et al. / Earth and Planetary Science Letters 286 (2009) 208–218 211 down to 600 °C (Cherniak, 1993) by dating titanite with the same technique. The results presented here are from a study of rocks from the Re di Castello (RdC) pluton in the southern Adamello batholith (northern Italy), and provide a first accurate quantification of the duration of zircon growth in individual magma pulses of a composite magmatic unit. The RdC pluton is a complex assembly of up to several km3-sized bodies of gabbros, diorites, tonalites, granodiorites and minor granites (Brack, 1985; Ulmer et al., 1985), showing spectacular field evidence for the sequential emplacement of distinct magmatic units, mingling and mixing of magma at variable volume fractions of crystals (crystallinity) as well as syn-magmatic ductile-to-brittle deformation features (Brack, 1985; Blundy and Sparks, 1992; John and Blundy, 1993). The present data demonstrate that state-of-the-art singlezircon preparation techniques and analytical precision are capable of resolving the residence time and/or the period of zircon growth in a given population. Titanite U–Pb ages allow assessing whether the youngest zircon dates indeed represent the youngest zircon growth in the cooling magma or if data are biased by lead loss. We also combine the hafnium isotope composition of zircon with their crystallization age in order to characterize the source of melts as a function of time. sediments up to several kilometers wide and exhibiting features of emplacement-related deformation (Brack, 1981). Limbs of the same sediments also separate different magmatic bodies. The main magmatic lithologies are fine-grained tonalites to granodiorites that are in some cases homogenous and abut sharply against one another. Elsewhere, however, contacts between individual magmatic pulses can only be discerned through subtle differences in texture and mineralogy. Gabbros and diorites occur as coherent and often sheetlike intrusive bodies especially along the margins of the RdC, but are also present as small enclaves in the acidic rocks (Blundy and Sparks, 1992). Structures of syn-intrusive (forceful) deformation are observed in several magmatic bodies in the southern RdC (Brack, 1985; John and Blundy, 1993). The mutual relationships in outcrop suggest that immediately after their emplacement the different intrusions at least locally coexisted as largely crystallized and cooling bodies, with residual interstitial liquid, deforming in a plastic way during the emplacement of subsequent melt batches (e.g., John et al., 1997). Radiometric ages available to date (Del Moro et al., 1985; Villa, 1985; Hansmann, 1986, Hansmann and Oberli, 1991) fully overlap and indicate a narrow time span of less than 4 Ma for the emplacement and cooling of the southern RdC intrusive rocks. 2. The Adamello batholith 3. U–Pb and Hf isotope results The Adamello batholith is exposed over an area of ~670 km2 with up to 3 km of vertical relief in northern Italy (Fig. 1; see Callegari and Brack, 2002 for further references). It is the largest of the Tertiary Periadriatic intrusions of the Alps and the Adamello magmas were emplaced during the Middle/Late Eocene–Early Oligocene into the South Alpine Variscan basement and its non-metamorphic PermoTriassic cover rocks. The outer borders of the igneous complex are largely primary intrusive contacts. Along its north-eastern corner the batholith is tectonically bound, i.e. by the late- to post-magmatic Tonale Line and by the Miocene Giudicarie Line, and its interior parts are crossed by only a few late to post-magmatic fault zones (Pennacchioni et al., 2006). The Adamello Batholith is divided into four plutons (Re di Castello, Adamello, Avio, and Presanella plutons; Callegari, 1985; Callegari and Brack, 2002) that encompass around 10 Ma of magmatic activity (43 to 33 Ma). The individual plutons are composite bodies and were emplaced sequentially from the oldest units in the south (~43 Ma) to the youngest units in the north (Del Moro et al., 1985). Geochemical (Dupuy et al., 1982; Macera et al., 1985) and isotopic (Cortecci et al., 1979; Del Moro et al., 1985) results demonstrate a roughly northward increase of the initial 87Sr/86Sr (Sri) and 18O/16O (δ18O) ratios, along with the concentrations of incompatible elements such as U, Cs and K, with maximal values in the Avio pluton. This points to increasing crustal contamination during the interval of magmatism. Mafic rocks of the southern Re di Castello unit (cumulate olivine–pyroxene wherlites to hornblendites to hornblende gabbros and diorites; Ulmer et al., 1985; Blundy and Sparks, 1992) have Sri and δ18O close to mantle values (Sri: 0.7036–0.7038, δ18O: +5.9–6.0), overlapping with those of the associated tonalitic–granodioritic rocks, whereas Sri ratios in the north range up to 0.711 (Cortecci et al., 1979; Del Moro et al., 1985). Altogether, the basic and felsic rocks define a typical calcalkaline fractionation trend (e.g., Macera et al., 1985; Ulmer et al., 1985). On the basis of these results Taylor (1980), Macera et al. (1985), Bigazzi et al. (1986) and Thompson et al. (2002) proposed and refined an assimilation fractional crystallization (AFC) model for the derivation and evolution of the Adamello, with the digestion of progressively larger amounts of lower to middle crustal material into fractionating mantle-derived magmas. The southernmost unit of the Adamello batholith, i.e. the Re di Castello (RdC) pluton, is a complex assembly of gabbros, diorites, tonalites, granodiorites and minor granites, (Fig. 1, lower panel). These magmatic units are bordered by rims of contact-metamorphic Triassic Four lithologies have been sampled for this study, which cover the entire age range of the southern RdC unit and most of which exhibit unequivocal relative age relationships with the neighbouring rocks and each other (Fig. 1; descriptions and coordinates in Table S1). Zircon separation was carried out at the University of Bologna following the procedure of Marocchi et al. (2008). Analytical techniques of the U–Pb age determinations of zircon follow those described in Schaltegger et al. (2008), those of titanite are outlined in Chiaradia et al. (2009). Part of the analyses were carried out using the 205Pb–233U–235U tracer solution (Condon and Members of the Earthtime Working Group, 2005), which has been internationally intercalibrated and proven to yield 206Pb/238U inter-laboratory reproducibility to better than 0.1% (see Sláma et al., 2008), the other part with a 205Pb–235U spike from ETH Zürich (analyses marked in Table 1 by asterisks). All analyses were carried out on the Triton thermal ionization mass spectrometer at University of Geneva, using a discrete-dynode MasCom® secondary electron multiplier in ion counting mode for the analysis of Pb. Uncertainty ellipses of individual analyses in Fig. 2 are at 2σ level and do not include the uncertainty of tracer calibration or non-blank common Pb composition. For the calculation of average 206Pb/238U titanite ages, an additional estimated uncertainty for the initial Pb composition has been added to analytical uncertainty of the 206Pb/238U ratio (2% for 206Pb/204Pb, 1% for 207Pb/ 204 Pb, 2% for 208Pb/204Pb). The Hf fraction was isolated using Eichrom™ Ln-spec resin, and measured in static mode on a NuPlasma™ multi-collector ICP-MS using an Aridus nebulizer for sample introduction. 176Lu/177Hf ratios of analyzed zircons were not determined but 176Hf/177Hf ratios were age corrected for a typical value of 176Lu/177Hf in zircon of 0.0005 (compare, e.g., to values in Kemp et al., 2008; or in Miskovic and Schaltegger, 2009). The 176Lu decay constant of Scherer et al. (2001) was used for calculation; the correction stayed within limits of analytical precision of the measured 176Hf/177Hf ratios in all cases. The Hf isotopic ratios were corrected for mass fractionation using a 179Hf/177Hf value of 0.7325 and normalized to 176 Hf/177Hf =0.282160 of the JMC-475 standard (Blichert-Toft et al. 1997). The JMC-475 standard was measured every fourth position in similar measurement conditions as the zircon samples and yielded values between 176Hf/177Hf =0.282130 to 0.282190 according to the daily instrument tuning. 176Lu and 176Yb present in analysis never amounted to more than 0.0003% or 0.01%, respectively, of the intensity of the 176Hf beam and were corrected for using isotopic ratios for 176Lu/175Lu=0.02656 and 176 Yb/172Yb=0.586155. Errors of the measured 176Hf/177Hf ratios are either given as external 2 σ reproducibility of standard measurements (i.e. Author's personal copy 212 U. Schaltegger et al. / Earth and Planetary Science Letters 286 (2009) 208–218 Author's personal copy U. Schaltegger et al. / Earth and Planetary Science Letters 286 (2009) 208–218 ±0.5 ε units) or individual 2 σ errors, whichever is larger. εHf values and TDM model ages were calculated with (176Hf/177Hf)CHUR(0) =0.282785 (Bouvier et al., 2008) and use present-day depleted mantle values of 176Hf/ 177 Hf =0.28325 (Nowell et al., 1998), 176Lu/177Hf =0.0385 (Griffin et al., 2000), and a crustal 176Lu/177Hf =0.015 (Griffin et al., 2002). Prior to the selection of zircon crystals for analysis, a morphological classification into acicular, long prismatic, prismatic, short-prismatic and equant morphologies was applied. In addition, the selected zircons were shortly described in terms of inclusions, milky-translucent vs. transparent crystal domains, presence of cracks, and/or even characterized by simple drawings. Despite this effort, no clear dependence between external morphology and apparent 206Pb/238U age can be recognized, except for indications of inherited material in the core (circular round inclusions, central milky domain, or radial cracks). For better characterization of the dated material, a micro-photographic documentation will have to be established for such detailed studies in future. Granitic aplite dykes of the Monte Frerone granite (GMF) are found as a complex network of apophyses emerging from a several hundred meter long body crossing the pre-Adamello folds of the carbonates and hornfelses of the inner contact aureole in the southwestern flank of Monte Frerone. The central body of GMF is cut by an outlier of the Valfredda leucotonalite (Brack, 1984) and peripheral aplitic dykes are locally affected by deformation induced by a subsequent intrusion. The GMF is hitherto the oldest magmatic lithology that can be clearly assigned to the southern RdC pluton and accordingly it is the oldest known magmatic product of the entire Adamello batholith. Apart from an Early Paleozoic inheritance (analyses 2, 5, 6 and 10 yielding an upper intercept age at 469±45 Ma), analytically concordant zircon data of GMF yield a scatter of 206Pb/238U dates from 42.43 to 42.63 Ma, i.e. record an age dispersion of 200 ka (Fig. 2a). From 6 clustering analyses a mean 206Pb/238U age of 42.57±0.05 Ma may be calculated; the MSWD value of 5, however, indicates that the points are not equivalent. Therefore, the youngest age of 42.43±0.09 Ma is taken as a first approximation for the age of autocrystic zircon growth and of emplacement, whereas the other analyses date prolonged crystallization of autocrystic zircon (crystallized in the same magma at an earlier stage), or of antecrystic zircon (earlier crystallization in the same magmatic system), see discussion below. There is no relation between external morphology and 206Pb/238U age. The sample yielded very few titanite crystals, one of which could be dated at a 206Pb/238U age of 42.51± 0.16 Ma; it is thus coeval with the youngest zircon within analytical uncertainties. The tonalite of Alta Guardia (TAG; nr. 11 in Fig. 1) is a peripheral intrusion, lithologically similar to but possibly distinct from the Val Fredda leucotonalite. The latter unit very likely predates the formation of the Listino ring (see Fig. 1) and its interior. Apart from Paleozoic inherited components yielding an upper intercept age of 437 ± 37 Ma (analyses 15, 17, 24), eight TAG zircons crystallized over 350 ka (between 41.41 and 41.76 Ma; Fig. 2b). A mean 206Pb/238U date of 41.53 ± 0.04 Ma with an MSWD of 3.1 may be derived from these analyses; we assume, however, that the youngest date of 41.41 ± 0.09 Ma (analysis 19) reflects autocrystic zircon growth and approximates the age of emplacement. Four out of five titanite analyses yield an average 206Pb/238U date of 41.31 ± 0.03 Ma (MSWD = 1.03; with enhanced Pb common uncertainty), which is insignificantly younger than the age for the youngest zircon. A fifth titanite analysis plots at an older age of 41.73 ± 0.03 Ma. There is no relation between external morphology and 206Pb/238U zircon age. The tonalite of Malga Listino (TML; nr. 6 in Fig. 1) forms the core of the enigmatic Listino ring structure, a zone of highly deformed tonalite with abundant mafic enclaves and sediment inclusions, crosscut by syn-magmatic dykes (Brack, 1984, 1985). The TML core, 213 however, is composed of an undeformed tonalite which shows some variation in grain-size (fine to medium grained) and containing comparably few mafic enclaves but no sedimentary xenoliths. The results of 14 zircon crystals scatter between 40.90 and 41.60 Ma, indicating apparent prolonged zircon growth over 700 ka (Fig. 2c). Analyses 29 and 31 yielded 206Pb/238U dates of 40.90 and 40.95 ± 0.09 Ma and are thus considered to represent autocrystic zircon growth and approximate the age of emplacement of this tonalite. The lack of enclaves and xenoliths is also reflected by the lack of inheritance in the analyzed zircon grains. Five titanite analyses scatter between 41.03 and 40.85 Ma, averaging at 40.94 ± 0.09 Ma (MSWD = 4.3; with 0.1% enhanced Pb common uncertainty). Excluding the oldest or youngest of the analyses does not yield a significantly different result (40.97 ± 0.10 and 40.90 ± 0.07 Ma, respectively). The titanite dates thus agree with the date of the youngest zircons. There is a tendency that the youngest zircon 206Pb/238U ages are found in longprismatic to acicular zircon grains (analyses 31, 33, 35–37). The leucotonalite of Cima Vallone (VAL; nr. 3 in Fig. 1) crosscuts the Listino ring structure and its tonalitic core (TML) and likely belongs to the youngest plutonic rocks in the southern part of the RdC pluton. Two zircons from VAL incorporated a Paleozoic inherited component (analyses 53 and 55; upper intercept age of 405 ± 54 Ma), whereas 7 concordant grains cluster around a mean 206Pb/238U date of 40.93 ± 0.04 Ma (Fig. 2d). The elevated MSWD of 4.4, however, indicates that the ages are not equivalent and in turn record zircon growth over a timespan of 130 ka (41.03–40.90 Ma). The youngest zircons at 40.90 ± 0.03 Ma (analyses 41 and 43) record growth of autocrystic zircon and thus approximate the age of emplacement. There is no relation between external morphology and 206Pb/238U age. Initial Hf isotopic compositions of magmatic zircons from TML and VAL range between εHf values of +6.4 and +8.9, characterizing a rather juvenile source for these two intrusions. The zircons of GMF and TAG, however, have initial Hf isotopic composition equal to εHf values between − 2.8 and +3.0, indicating a more hybrid character of those melts (Table 2). These values provide evidence for the existence of different magma sources within the same magmatic system. The Hf Table 2 Hf isotopic compositions of dated zircons. 176Hf/ 177Hf ±2 σ 176Hf/177Hf eps Hf (T) (T) ±2 σ T2 (DM) (Ga) GMF Granite Monte Frerone 1 0.282825 0.000004 3 0.282782 0.000021 4 0.282829 0.000008 0.282824 0.282782 0.282829 2.8 1.3 3.0 0.5 0.5 0.5 0.87 0.95 0.86 TAG Leucotonalite Alta Guardia 14 0.282832 0.000008 15 0.282722 0.000005 16 0.282744 0.000006 23 0.282803 0.000004 24 0.282667 0.000004 25 0.282808 0.000003 0.282832 0.282722 0.282744 0.282803 0.282667 0.282808 3.0 − 0.8 − 0.1 2.0 − 2.8 2.2 0.5 0.5 0.5 0.5 0.5 0.5 0.85 1.08 1.03 0.91 1.19 0.90 TML Tonalite Malga Listino 31 0.282993 0.000013 32 0.282980 0.000013 38 0.282926 0.000006 41 0.282948 0.000023 0.282993 0.282980 0.282926 0.282948 8.7 8.3 6.4 7.1 0.5 0.5 0.5 0.5 0.52 0.54 0.66 0.61 VAL Leucotonalite Cima di Vallone 48 0.282999 0.000006 49 0.282993 0.000006 50 0.282970 0.000012 0.282999 0.282993 0.282970 8.9 8.7 7.9 0.5 0.5 0.5 0.50 0.52 0.56 Fig. 2. Concordia diagrams and ranked 206Pb/238U age plots containing the results of zircon U–Pb dating of four samples from the southern Re di Castello unit, Southern Adamello. (a) GMF, granite of Monte Frerone, (b) TAG, tonalite of Alta Guardia, (c) TML, tonalite of Malga Listino, (d) VAL, leucotonalite of Cima di Vallone. Gray ellipses and black bars denote titanite analyses, open ellipses and bars zircon analyses. Author's personal copy 214 U. Schaltegger et al. / Earth and Planetary Science Letters 286 (2009) 208–218 Fig. 3. Epsilon Hf versus 206Pb/238U age diagram for selected zircons. isotopic values could point to an evolution towards more juvenile compositions with time (Fig. 3). 4. Discussion of the isotopic data and their implications 4.1. Age range of magmatism The new age data cover the majority of the lifetime of the multicomponent southern RdC pluton, which was assembled during some 1.5 Ma. The leucocratic dykes of GMF were emplaced at 42.43 ± 0.09 Ma and likely predate the Lago della Vacca intrusive body (Fig. 1; Brack, 1984; John and Blundy, 1993). Our emplacement age of 41.41 ± 0.09 Ma for the peripheral TAG intrusion is younger than the U–Pb thorite age of 42.9 ± 0.2 Ma (Hansmann, 1986) for the Vacca tonalite. The intrusions of Vacca and Galliner tonalites, and the Blumone gabbros and diorites are clearly cut by the Listino ring structure and its core, the TML tonalite at 40.90 ± 0.09 Ma. The VAL leucotonalite is coeval with the latter at 40.90 ± 0.03 Ma and crosscuts deformed tonalites of the Listino ring; TML and VAL ages are thus in line with field relationships. 4.2. How to treat precise U–Pb age data? The data reveal that age dispersions of up to several 100 ka exist among a zircon population from the same rock, which may indicate prolonged growth of autocrystic zircon in the same magma batch, or incorporation of older, antecrystic zircon from different magma batches of the same magma system, and may additionally be biased by incorporation of small inherited cores in the magmatic zircon. Such a result may be achieved by higher precision through the new and improved analytical techniques described above, and foster some fundamental questions of how to interpret high-precision zircon U–Pb ages from magmatic rocks. Zircon forms in complex magmatic systems at different levels of the crust. Small melt portions in the source area within the lower crust may already saturate and crystallize zircon due to feldspar crystallization lowering the K and Na activity in the melt (Watson and Harrison, 1983), whereas other melt batches do so only during the ascent through lower and middle crust, during further crystallization and cooling. Such zircon has been termed “antecrystic” (see Miller et al., 2007 and further references therein); it gets entrained and incorporated into the magma emplaced at a shallow crustal level and will record the integrated history of melt extraction, ascent, possibly intermediate crystallization at N50% crystallinity and subsequent re-mobilization of such “proto-plutons” before final emplacement. Since magma is emplaced with less than 50% crystals (convection threshold; Marsh, 1981; Lejeune and Richet, 1995), there will be further zircon formation in the stagnant interstitial melt, leading to mantling of preexisting grains as well as possible nucleation of new, smaller grains (Charlier and Zellmer, 2000). The last autocrystic zircons crystallizing at the final level of emplacement would date or at least approximate the emplacement, or possibly even be slightly younger. The age dispersion that we will determine by using a representative suite of zircons therefore depends on what moment the system reaches saturation for zircon. Since we have analyzed entire grains, integrating growth over a certain period of time, we will only get a maximum age for the youngest autocrystic zircon. Furthermore, we have to be aware that we may still record subordinate effects of lead loss, despite our efforts of chemical abrasion pre-treatment. The U–Pb results of magmatic titanite from TAG and TML lithologies (Fig. 2b, c) demonstrate that titanite ages may serve as a test for this hypothesis: titanite has been shown to have a closure temperature of ca. 650 ± 50 °C for grains with an effective diffusion radius between 100 and 1000 µm and 2–10 °C/Ma cooling rate (Cherniak, 1993); magmatic titanite therefore records its crystallization close to the solidus or initial cooling below the solidus. In both samples TAG and TML the titanites are within analytical uncertainty of the youngest zircon (Fig. 2b, c), arguing that our annealing–leaching pre-treatment is indeed effective at minimizing the post-crystallization lead loss. One older titanite analysis of sample TAG (Fig. 2b) asks, however, for caution and indicates that titanite may grow earlier and be possibly mantled by refractory phases in order to keep its isotopic system closed over 105 a. Our results of zircon U–Pb dating in fact roughly represent absolute durations of zircon growth. Since we are dealing with single grain analyses recording an integrated signal across all growth zones, we may consider it as a minimum duration of growth. On the other hand, since we cannot rule out that an antecrystic or even xenocrystic component is affecting the apparent age range, we may also consider obtaining periods of time that are longer than the durations of zircon crystallization. In the case of samples GMF, TAG and VAL (Fig. 2a, b, d, respectively) inherited Pb is evidenced by significantly higher 206Pb/ 238 U ages (analyses 2, 5, 6, 8, 10, 15, 17, 24, 48, 53 and 55). Sample TML, however, does not show any sign of a significantly older inherited component that would contribute to the apparent c. 700 ka-long zircon growth period. Generally speaking, most intermediate and acid rocks will reach zircon saturation early in magma evolution, zircon will record a prolonged period of growth (possibly biased by ante- and xenocrystic components) and the emplacement age may be best approximated by the youngest dates only. With a significant number of analyses we may use the value of mean square of weighted deviates (MSWD) of the mean 206Pb/238U age to assess whether the observed scatter is beyond purely analytical variation. It is self-understanding that ID-TIMS techniques are too difficult and time-consuming to ever achieve a number of analyses from one sample that is representative for the entire population. If a dataset of seven concordant analyses – e.g., in case of the sample VAL (Fig. 2d) – already shows nonequivalency of points and a MSWD of 4.4, we can be sure that there is geological complexity beyond analytical scatter. Such information for rocks of similar age cannot be obtained from low-precision U–Pb analyses such as by LA-ICP-MS or SIMS, because their large uncertainty on individual data points would suggest equivalency of points (with MSWD's around unity) and hence yield a potentially inaccurate weighted mean age for the emplacement, even outside of ICP-MS or SIMS analytical uncertainty. 4.3. Implications for zircon crystallization and survival of xenocrystic zircon Through crystallization, initially zircon-undersaturated mafic magma batches become volatile-saturated and eventually rise to intermediate crustal levels due to the lowered viscosity and higher buoyancy. They may only saturate zircon due to cooling and oversaturation of the interstitial Author's personal copy U. Schaltegger et al. / Earth and Planetary Science Letters 286 (2009) 208–218 fluid-saturated residual melt. The first precipitating zircons date in such a case the moment of zircon saturation. Only these kinds of samples are anticipated to yield perfect clusters of zircon 206Pb/238U ages within present analytical errors and confirm that analytical reproducibility is indeed within the claimed analytical uncertainty (see examples in Schoene et al., 2006). Such a case has not been found among the four studied Adamello rocks, which all show age variation largely in excess of analytical scatter (130 to 700 ka) with an analytical uncertainty of ±30–90 ka in the 206Pb/238U age of an individual analysis. The studied tonalites and granodiorites have saturated zircon already at an early stage of their geochemical evolution, because Zr acts as an incompatible element during crystallization of pyroxene, amphibole and plagioclase. Maximum bulk rock Zr concentrations are reached at around 64% SiO2 (Ulmer, 1986). We can envisage that some melt portions already started to crystallize zircon at lower crustal levels, despite the continuous influx of mafic magma batches. In these rocks we anticipate finding an extended history of zircon crystallization over 200–300 ka, as has been shown for various volcanic cases, e.g., by Brown and Fletcher (1999), Charlier and Zellmer (2000), Bacon and Lowenstern (2005), Bachmann et al. (2007), Simon et al. (2008), and many others. For longer durations of autocrystic zircon growth (as displayed by sample TML, if we assume that the age range is not due to ante- and xenocrystic material; Fig. 2c), it would only be possible if the necessary heat is sustained by repeated influx of hot mafic magma into the source region, keeping temperatures above the solidus and adding more and more juvenile material (Annen et al. 2006). We would find even more likely that the antecrystic zircons may be derived from already partly solidified magma at different crustal levels of the magmatic system (“proto-plutons”) that became (possibly repeatedly) remelted and with zircon crystals that were entrained into the leaving melt fraction. Such a hypothesis may be supported by field observations (antecrystic amphibole and plagioclase crystals entrained in later liquids), but is, however, not supported by our U–Pb and chemical data. Furthermore, we would assume that residual liquid (residual from basalt fractionation) would very likely mix with partial crustal melts and carry their zircon xenocrysts in suspension; in samples GMF, TAG and VAL xenocrystic zircons were indeed detected. In sample TML, however, they were not. The nature of the digested crustal component in the RdC pluton did not change during the 1.5 Ma lifetime of the studied magmatic system, as shown by the similar age for the inherited component in GMF, TAG and VAL (upper intercept ages of 469 ± 45, 437 ± 37 and 405 ± 54 Ma, respectively). This age range is typical for ubiquitous Ordovician metamorphism and magmatism in the Southalpine basement (Boriani et al. 1995; Zurbriggen et al. 1997) and also coincides with an Rb–Sr isochron age of 460 Ma for the Edolo schists, used to calculate AFC models of Adamello intrusive rocks (Bigazzi et al. 1986). Our Hf isotope analyses, however, distinguish between a more hybrid crustal component for GMF and TAG (with intermediate, partly negative εHf), and a rather juvenile source for TML and VAL (with εHf around +8). 215 age between GMF and TML (between 42.4 and 40.9 Ma; Fig. 1b): They were repeatedly injected by gabbroic to dioritic dykes and sills, namely the Cadino and Mattoni gabbros intruding into the Val Fredda tonalites (Blundy and Sparks, 1992) or the stocks and dykes of the Blumone gabbros (Ulmer et al. 1985). As a result of this massive and geochemically more juvenile mafic input, the following batches of evolved magma (samples TML and VAL) have significantly more juvenile Hf isotopic compositions (εHf values up to +8.9, see Fig. 3). This is, however, not true for sample TAG, an intrusion more peripheral to the magmatic center of the pluton, which is displaying less radiogenic Hf isotopic values and therefore obviously remained unaffected by the juvenile input. According to the “hot-zone” model of Annen et al. (2006, 2008) we may argue that the onset of magma production in the RdC unit was dominated by partial crustal melts (sample GMF) which may be regarded as low-degree partial melts in the lower crust produced by hot and dry mantle melts; this peak in crustal melting would have been followed by pulses of wetter mantle melts and resulting hybrid liquids became more and more juvenile. This source evolution is only valid for the southern Re di Castello unit, in that the more northern units of the Adamello batholith show increasing crustal influence (or of more radiogenic/older crust) as traced by Sr and O isotopes with ongoing magmatism between 38 and 33 Ma (Cortecci et al., 1979; Del Moro et al., 1985). 4.5. Zircon as a tracer for magma fractionation processes We have shown that zircon crystals form during a certain period of time during magma assembly, ascent and final emplacement at intermediate to shallow crustal level. By using the variable initial Hf isotope composition of individual zircons we may be able to trace the magma mingling of hybrid melt batches and/or exchange of antecrystic zircon between melt batches in certain cases. In complement to Hf isotopes that serve as a source indicator, we may additionally use the model Th/U ratio (Th concentration calculated on the basis of 208Pb rad. assuming concordancy between 206Pb/238U and 208Pb/232Th) of single-zircon crystals to trace magma fractionation. Fig. 4 shows Th/U ratios of zircon and titanite of all 4 samples dated in this study and leads to the following conclusions: GMF and VAL show restricted variations of the Th/U from 0.65 to 0.45 that are independent of measured age, probably indicating short-lived crystallization without significant fractionation due to precipitation of concurrent U and Th-bearing phases, respectively. TAG and TML show much larger scatter (between 0.85 and 0.35), which in the case of sample TML is age dependent, pointing to decreasing Th/U during 4.4. Heat and magma mingling Field relationships between some of the magma pulses suggest that the intrusion of each respective pulse at the present-day observable structural level occurred while the previous batches had already cooled and mostly solidified. This interpretation is in line with our U–Pb titanite ages indicating rapid cooling down to 600 °C within the analytical uncertainty of the U–Pb age of the youngest autocrystic zircon (c. ±0.09 Ma; Fig. 2b, c). We therefore consider the intrusions of GMF, TAG and TML + VAL, respectively, as three separate magma batches, which did not mingle with the previous magmas. Mingling is recognized in lithologies of the Blumone and the Val Fredda Complexes, which are intermediate in Fig. 4. Th/U versus 206Pb/238U age diagram for dated magmatic zircons and titanites; the latter are labelled “ti”. Author's personal copy 216 U. Schaltegger et al. / Earth and Planetary Science Letters 286 (2009) 208–218 zircon crystallization. Uranium is known to be four times more compatible in the zircon lattice than is Th (Mahood and Hildreth 1983). A reduction of the Th/U ratio in the crystallizing zircon and in the magma therefore asks for contemporaneous precipitation of a Thbearing phase. The TML titanites incorporated Th/U at ratios up to 2.7 (Fig. 4 and Table 1), suggesting that concurrent titanite crystallization may have led to melt depletion in Th. We therefore may interpret the largest spread and the lowest values for Th/U in zircon in sample TML by the highest Th concentrations (790–910 ppm) and highest Th/U ratios of co-precipitating titanite in this lithology. The situation is somewhat reversed in the case of sample TAG: zircon Th/U are elevated at 0.0.36–0.87, whereas titanite has, with one exception, very low Th/U of 0.22–0.13, concurrent with a trend towards higher Th/U in co-precipitating zircon. 5. Description of CL textures of dated samples Cathodoluminescence imaging (or backscattered electron imaging) is often used to visualize in an empiric way the result of growth processes in zircons (e.g., Corfu et al. 2003). Do the cathodoluminescence images of zircons analyzed in this study really reflect the observed differences in the crystallization/ fractionation paths? With our U–Pb zircon dataset from the southern Re di Castello unit we try to reconstruct the history of zircon growth and pluton assembly in great detail and may test the validity of the empirically interpreted CL information (Fig. 5). Sample GMF shows well-defined and undisturbed oscillatory zoning over most of the growth zones (Fig. 5a, b), possibly reflecting the observed (minimum) 200 ka of uninterrupted crystallization. Some grains show clear inherited cores (C in Fig. 5a), in accordance to the isotopic results (analyses 2, 5, 10 with inheritance of old lead; see Table 1), as well as nonplanar, chaotic textures at the interface between core and rim (Fig. 5a). The latter may be related to post-crystallization processes mobilizing radiogenic Pb; significant Pb loss is, however, excluded by the titanite analysis. Sample TAG shows the same uninterrupted oscillatory textures integrating 350 ka of growth (Fig. 5c,d), ending with a high–U zone in case of Fig. 5c, and very likely featuring small inherited cores in both Fig. 5c, d, which is in line with the detected inheritance (analyses 15, 17, and 23). A clearly different picture is presented by zircons of sample TML. Many zircon grains of this sample contain a sector-zoned central part, which was formed at high temperatures in deep crustal levels. Sector zoning is typical for high-T melts, such as in granulites (e.g., Vavra et al. 1999, Schaltegger et al. 1999), gabbros (Peressini et al. 2007), or, more generally speaking, in high-temperature mantle-derived residual liquids (examples of zircon in oceanic arc melts in Heuberger et al. 2007). Sector zoning is produced by an equilibrium process partitioning heavy ions between prism and pyramid faces (see summary of models in Corfu et al. Fig. 5. Cathodoluminescence images of representative zircons from sample GMF (a, b), TAG (c, d), TML (e, f), and VAL (g, h). C = core; F = post-crystallization surface-bound replacement front; P = abrupt change of growth rate for a U-rich (low-CL) prism face; R = resorption interface. Scale bars = 50 µm. Author's personal copy U. Schaltegger et al. / Earth and Planetary Science Letters 286 (2009) 208–218 2003). The prism faces in Fig. 5e show enrichment in U and acceleration of growth (P in Fig. 5e) until the moment when sector zoning gets replaced by oscillatory (rapid) growth, and grain morphology changing from a more equant shape with {211} pyramids to a prismatic shape with {101} pyramids. These observations agree with our observation that zircon grew over prolonged periods of time; crystallization started a deeper level, the magma of TML thus saturated deeper in the crust than the other samples. However, we do not have a direct age control on such sector-zoned crystals. The zircon imaged in Fig. 5f shows oscillatory zoning from center to rim, but disturbed by phases of resorption (R) and surface-bound replacement fronts (F). Both crystals end their growth in high-U rims. The crystals of VAL (Fig. 5g, h) show very fine-banded oscillatory growth, indistinguishable from TAG. The zircon in Fig. 5 h has a small inherited core, whereas the zircon on Fig. 5g is representative for abundant secondary replacement structures (F) in zircons of this sample. The observed age dispersion may therefore be explained by either prolonged growth of autocrystic zircon or (and?) disturbance of the lattice during or shortly after crystallization and may be at the origin of age variation at the 10 ka level. The conclusion from the CL imaging is that we may find useful information for the crystallization sequence of the dated zircon population and these are in line with the results of the age determinations. A direct application will, however, only be possible once we have direct CL information on the very dated zircon grains. 6. Conclusions Mid-to-upper crustal intrusions are assembled incrementally by individual magma pulses rather than being single batches of magma intruding at one time (see e.g., Michel et al 2008). Our data demonstrate that the composite southern RdC pluton of the Adamello batholith was emplaced over 1.5 Ma, with each magma batch of 10− 1 to 100 km3 volume recording single-crystal zircon ages spanning from 130 to 700 ka. This age span may be interpreted in terms of i) prolonged growth of autocrystic zircon, ii) incorporation of antecrystic zircon from the same magmatic system, iii) incorporation of minute amounts of inheritance, or – most likely – a combination of all. It is very likely that each magma pulse (yielding a coherent lithological unit) consists of a series of even smaller increments only visible through careful observation of magmatic fabrics. The availability of precise U–Pb dates from magmatic zircon with permil analytical uncertainties in 206Pb/238U age forces us to better understand the systematics of the zircon crystals that are present in a magmatic rock, in order to define the date of the youngest autocryst as a best approximation for the emplacement age of the respective magma batch. Each of the dated intrusions from the southernmost part of the Adamello Batholith (from oldest to youngest: Granite of Monte Frerone – GMF; Tonalite of Alta Guardia – TAG; Tonalite of Malga Listino – TML; Granodiorite of Cima Vallone – VAL) was emplaced into already fully crystallized rocks, as indicated by the titanite ages of TAG and TML, which are coeval or only slightly younger than the youngest zircon age and date cooling to 650±50 °C, i.e. below the solidus. Substantial mingling phenomena are known from the southernmost RdC pluton, from intrusions intermediate in age between GMF and TML (Valfredda and Vacca to Blumone suites; Blundy and Sparks 1992; John and Blundy 1993). Hf isotopes of individual, dated zircons act as a source indicator and, between the intrusion of GMF and TML, document a drastic change in source and/or in the ratio of partial crustal versus residual mantle melt in the Re di Castello unit. The geochemical evolution of the melts can be described in terms of the hot-zone model of Annen et al. (2006, 2008). The first basaltic magmas intruding into the lower crust lead to a pulse of crustal partial melts that mix with mafic residual melts to produce the strongly hybrid GMF, and later TAG magmas. As indicated by juvenile Hf isotopic values, the mantle component increases during the subsequent evolution of the system, possibly due to the influx of large volumes of 217 mafic melts into the magmatic system, which triggers the intrusion of the Blumone gabbro intermediate in age between GMF and TML. The increased precision in U–Pb ID-TIMS dating allows observation and documentation of magmatic processes at the 104–105 yr level and starts to form an observational link between geological processes acting in the past over 106–108 Ma, and timescales of melt assembly in large modern volcanic centers. Acknowledgements Support of the Geneva isotope laboratory through several projects of the Swiss National Research Fund is acknowledged. M. Senn and M. Chiaradia contributed with technical help and advice to the success of this research. Comments of C. Annen (Geneva) on an early version were very helpful. The two journal reviews of M. Schmitz and F. Corfu were extremely thoughtful and are highly appreciated. This study was initially supported by a APAT (CARG, RL-PAT) for the 079 Bagolino Sheet funded to G.B and M.M. Appendix A. Supplementary data Supplementary data associated with this article can be found, in the online version, at doi:10.1016/j.epsl.2009.06.028. References Annen, C., Blundy, J.D., Sparks, R.S.J., 2006. The genesis of intermediate and silicic magmas in deep crustal hot zones. J. Petrol. 47, 505–539. Annen, C., Blundy, J.D., Sparks, R.S.J., 2008. The sources of granitic melt in Deep Hot Zones. Trans. Royal Soc. Edinburgh; Earth Sci. 97, 297–309. Bachmann, O., Charlier, B.L.A., Lowenstern, J.B., 2007. Zircon crystallization and recycling in the magma chamber of the rhyolitic Kos Plateau Tuff (Aegean arc). Geology 35, 73–76. Bacon, C.R., Lowenstern, J.B., 2005. Late Pleistocene granodiorite source for recycled zircon and phenocrysts in rhyodacite lava at Crater Lake. Oregon. Earth Planet. Sci. Lett. 233, 277–293. 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