Zircon crystallization and the lifetimes of ore-forming magmatichydrothermal systems

Albrecht von Quadt, Michaela Erni, Klara Martinek, Melanie Moll, Irena Peytcheva, and Christoph A. Heinrich
Institute of Geochemistry and Petrology, Department of Earth Sciences, ETH Zurich, Clausiusstrasse 25, 8092 Zurich, Switzerland ABSTRACT Magmatic-hydrothermal copper ore formation involves multiple pulses of subvolcanic porphyry intrusion, vein opening, and hydrothermal ore deposition. It is driven by larger subjacent magma reservoirs, acting as the source of uid and ore-forming components. High-precision U-Pb ages of individual zircon crystals from porphyries immediately predating and postdating Cu-Au mineralization at Bingham Canyon (Utah, United States) and Bajo de la Alumbrera (northwestern Argentina) show a signicant spread of reliably concordant ages. This demonstrates zircon crystal formation over a protracted period of ~1 m.y., which is interpreted to record the lifetime of the magma reservoir from which porphyries and ore uids were extracted. The youngest zircons in all pre-ore and post-ore intrusions overlap within a much shorter time interval of 0.32 m.y. at Bingham Canyon and 0.090 m.y. at Alumbrera; these youngest zircons of each intrusion are interpreted to bracket the maximum duration of porphyry emplacement and ore formation to short periods, consistent with thermal constraints. This study illustrates that age brackets based on individual magmatic zircon grains are geologically more informative than the calculation of means and standard deviations based on apparently normal age distributions in zircon populations. at the temperature of hydrothermal mineralization (>350 C) for more than a few tens of thousands of years, even with massive heat advection by magmatic uids (Driesner and Geiger, 2007). Diffusive equilibration between uids and altered rocks is even faster, which was used to suggest that a large porphyry deposit like Bajo de la Alumbrera (northwestern Argentina) may form within <100 yr (Cathles and Shannon, 2007). These rapid time scales contrast with interpretations of geochronological data, suggesting that multiple pulses of porphyry emplacement and mineralization may be separated by as much as 1 m.y. (e.g., Ballard et al., 2001; Harris et al., 2008), which implies that each porphyry cooled to ambient crustal temperatures prior to the next pulse of porphyry emplacement and mineralization. To better dene these contrasting time scales, we present high-precision U-Pb zircon age data (see the GSA Data Repository1) from two world-class porphyry Cu-Au deposits, where geological mapping has documented an intrusion sequence of several porphyry phases that truncate, and therefore bracket in time, distinct pulses of hydrothermal veining and Cu-Au mineralization (Fig. 2). Concordant zircon ages were obtained by isotope dilutionthermal ionizationmass spectrometry (ID-TIMS) of single crystals, after chemical abrasion of disturbed domains using thermal annealing and selective leaching of each grain (Mattinson, 2005). Results show that geologically constrained interpretation of high-precision zircon geochronology can differentiate between the characteristic lifetimes of processes contributing to magmatic-hydrothermal ore formation. ALUMBRERA: TWO MINERALIZATION PULSES IN SHORT SUCCESSION The porphyry-Cu-Au deposit of Bajo de la Alumbrera (Ulrich et al., 1999, 2002; Proffett, 2003; Halter et al., 2005; Harris et al., 2003) and its geological context in the Faralln Negro Volcanic Complex of northwestern Argentina were previously studied by Ar-Ar step-heating and U-Pb laser ablationinductively coupled

INTRODUCTION Porphyry Cu Mo Au deposits form by hydrothermal metal enrichment from uids that immediately follow the emplacement of porphyritic stocks and dikes at 28 km depth. Ore-generating uids originate from water-rich magma chambers underlying the pervasively fractured and altered porphyry stocks. Mass balance of ore metals and sulfur in the deposits (Dilles, 1987; Cline and Bodnar, 1991) and knowledge of the concentration of ore-forming components in the uids (Ulrich et al., 1999; Audtat et al., 2008) constrain the minimum size of the uidgenerating magma volume to tens to hundreds of cubic kilometers for a major deposit. The processes of generating and differentiating hydrous magmas, establishing a major hydrous magma reservoir in the upper crust, emplacing a composite porphyry stock in its roof, exsolving uids from the magma reservoir, and focusing them through a narrow porphyry stock are key steps in the formation of an economic ore deposit (Fig. 1; Candela, 1991; Hedenquist and Lowenstern, 1994; Shinohara et al., 1995; Richards, 2003; Sillitoe, 2010). Thermal constraints impose characteristic time scales on these interacting physical processes. Large magma chambers in the hot lower crust may grow and retain partial melt over millions of years (Rohrlach and Loucks, 2005; Annen, 2009), whereas upper crustal magma chambers without open magma throughput have a maximum lifetime of <1 m.y. (e.g., Michel et al., 2008). Small porphyry stocks emplaced at shallow depth crystallize within 0.01 m.y. or less (Cathles, 1977). They are difcult to keep

0 km

Porphyry Cu-Au deposit Hydrothermal veining Fluid focusing Upper-crustal magma chamber Fluid exsolution Magma mixing

10

20

Crustal-scale magmatichydrothermal system

Lower-crustal magma chamber Fractionation - assimilation

30

Crust Mantle

40

Magma pod Mantle melt

Figure 1. Illustration of ore-forming magmatic-hydrothermal system, emphasizing scale and transient nature of hybrid magma with variable mantle (black) and crustal (gray) components. Interacting processes operate at different time scales, depending on rate of melt generation in mantle, variable rate of heat loss controlled by ambient temperature gradients, and exsolution of hydrothermal uids and their focused ow through vein network, where Cu, Au, or Mo are enriched 100 fold to 1000 fold compared to magmas and crustal rocks (combining Dilles, 1987; Hedenquist and Lowenstern, 1994; Hill et al., 2002; Richards, 2003).

1 GSA Data Repository item 2011222, zircon crystallization and the lifetimes of magmatic-hydrothermal ore systems, is available online at www.geosociety .org/pubs/ft2011.htm, or on request from editing@ geosociety.org or Documents Secretary, GSA, P.O. Box 9140, Boulder, CO 80301, USA.

2011 Geological Society of America. For permission to copy, contact Copyright Permissions, GSA, or editing@geosociety.org. GEOLOGY, August 2011 Geology , August 2011; v. 39; no. 8; p. 731734; doi:10.1130/G31966.1; 4 gures; Data Repository item 2011222.

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Figure 2. Rock slab from Bajo de la Alumbrera, showing early andesite porphyry (P2, left part of picture and xenolith in lower right corner) that solidied before becoming intensely veined and pervasively mineralized by hydrothermal magnetite + quartz with disseminated chalcopyrite and gold. After this rst pulse of hydrothermal mineralization, a dacite porphyry intruded along an irregular subvertical contact (EP3, right part of picture), before both rocks were cut by second generation of quartz veins (diagonal toward lower right).

shown in Figure 2. This intrusion truncates the rst generation of hydrothermal quartz-magnetite veinlets associated with P2, and is in turn cut by a second generation of quartz veins. Figure 3A compares ID-TIMS results on a concordia diagram with previously published LA-ICP-MS measurements (Harris et al., 2004, 2008; Figs. 3B and 3C). The TIMS data resolve an overlapping range of LA-ICP-MS results into a suite of concordant but distinct zircon ages. Grain ages from the earlier P2 porphyry range from 7.772 0.135 Ma (2) to 7.212 0.027 Ma. A group of three grains overlaps the younger age bracket within their individual uncertainties (P29, P211, P213), and six additional, discernably different grain ages are distributed between this group and the oldest age. Since most grains show simple oscillatory zoning, there is no doubt that individual zircons crystallized from the parent magma of the P2 porphyry as late as 7.216 0.018 Ma (P211, the most precise of the young group), which is therefore interpreted as the maximum age for subvolcanic intrusion, solidication, and rst hydrothermal veining of the P2 porphyry. The EP3 porphyry truncating these veins also yielded a group of three overlapping and perfectly concordant single-grain ages, ranging from
0.00132

7.126 0.016 Ma to 7.164 0.057 Ma (EP31, EP313, EP314). As the two most precise measurements from each group do not overlap within their individual uncertainties, we may interpret them as the most likely solidication ages of P2 and EP3, respectively, and conclude that the two intrusions were separated in time by 0.090 0.034 m.y. (P211 minus EP313 the sum of individual uncertainties). As a more cautious interpretation, we might emphasize that the two clusters overlap if the less precise grains are included, and therefore conclude that both porphyries intruded within a period of 0.124 m.y. (taking the two most precise points plus their error brackets; Fig. 3A). This more conservative interpretation allows that the two events may have occurred within a much shorter time span. Both porphyries contain concordant zircon grains that are as much as 0.56 m.y. (P2) and 1.08 m.y. (EP3) older than the maximum emplacement ages. These are interpreted to have grown as antecrysts (Miller et al., 2007) from the evolving parent magma reservoir, from which both porphyries were nally extracted in rapid succession. Million-year age spreads among zircons and other accessory minerals have previously been documented in lower crustal granitoid plutons (Oberli et al., 2004;

plasmamass spectrometry (LA-ICP-MS) geochronology (Halter et al., 2004; Harris et al., 2004, 2008). There is agreement that the volcanic complex had a long lifetime, probably at least 2.7 m.y. from the oldest lavas, ca. 9.7 Ma, to cooling below 300 C of the last Cu-Au mineralized intrusion in the Alumbrera deposit ca. 7.0 Ma. Debate centers on the time of initiation and the duration of porphyry mineralization. Halter et al. (2004) argued that all porphyries were emplaced and mineralized in rapid succession at 7.0 0.2 Ma, after a period of closed magma chamber evolution following the last volcanic eruption at 7.35 0.16 Ma. By contrast, Harris et al. (2004, 2008) used LA-ICP-MS analyses of zircons to conclude that the earliest and most intensely mineralized porphyry (P2) was emplaced at 7.92 0.14 Ma, followed by a later pulse of intrusion (P3) and mineralization at 6.96 0.09 Ma, 1 m.y. after the rst mineralization event. We redated the two mineralizing porphyry intrusions, based on samples that show unambiguous eld relations in a continuous open-pit outcrop (Fig. 2; see the Data Repository). Sample BLA-P2 is pervasively quartz-magnetite (K-feldsparbiotite) altered P2 porphyry (Proffett, 2003), as shown on the left side of the slab in Figure 2, but sampled 5 m away from the EP3 contact to exclude contamination. Sample BLAEP3 was taken from the right side of the slab

ID-TIMS Data Alumbrera

0.00128

0.00124

8.0

ACH9998 (LP3)
6.96 0.09 Ma MSWD 1.01 after filtering 24 of 47 by Harris et al. (2008)
206 Pb/ 238 U ages by LA-ICP-MS

BLA-P2
0.00120
206Pb/238 U

0.00116

0.00112
t = 0.124 m.y. t = 0.090 0.034 m.y.

0.00108

7.0

ACHP2
7.92 0.14 Ma MSWD 1.67 after filtering 21 of 37 by Harris et al. (2004)

0.00104

BLA-EP3

0.00100 0.001 0.003 0.005 0.007 0.009 0.011 0.013

207Pb/235 U

Figure 3. A: Concordia diagram with isotope dilutionthermal ionization mass spectrometry (ID-TIMS) results from the rst (red ellipses, P2) and second (blue ellipses, EP3) Cu-Au mineralizing porphyry of Bajo de la Alumbrera. B, C: For comparison, published laser ablationinductively coupled plasmamass spectrometry (LA-ICP-MS) analyses and their interpreted mean ages and uncertainties on the same age scale (replotted from Harris et al., 2004, 2008; LP3 is petrographically indistinguishable from EP3, but cuts also second phase of ore veins). All errors are 2. MSWDmean square of weighted deviates.

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Miller et al., 2007). Age differences of as much as 1 m.y. are also resolved by zircon populations from upper crustal intrusions and extrusive volcanic complexes (Bacon and Lowenstern, 2005; Charlier et al., 2005; Bachmann et al., 2007; Crowley et al., 2007; Schaltegger et al., 2009). These observations and our new data show that zircon crystals of datable size generally grow at depth, together with other rock-forming phenocrysts and antecrysts, and not during rapid quenching of extrusive rocks or subvolcanic porphyries. PORPHYRY INTRUSIONS BRACKETING CU-AU MINERALIZATION AT BINGHAM CANYON A similar spread in zircon ages and overlap of the youngest zircon grains was found in pre-ore, syn-ore, and post-ore porphyry intrusions of the giant Cu-Au-Mo deposit of Bingham Canyon (Utah, USA; Fig. 4). Most intense veining and Cu-Au introduction was associated with the quartz monzonite porphyry. A second pulse of mineralization followed the latite porphyry. Quartz latite porphyry nally truncated nearly all Cu-Au mineralized veins and was crosscut only by a distinct late generation of quartz-molybdenite veins (Redmond and Einaudi, 2004, 2010). We dated all three porphyries, obtaining 31 ages that are mostly concordant except for a few highly discordant grains pointing to Paleoproterozoic upper intercepts. Six of the youngest and most precisely dated grains from all three porphyries overlap entirely within the age range of 38.1037.78 Ma, including their 2 uncertainty. Seven additional grains overlap this range within their larger uncertainties, ignoring a single younger outlier from the geologically oldest intrusion (KM24; young age possibly due to residual Pb loss). We therefore interpret that all three porphyry intru0.0063 0.0062

sions and the two Cu-Au mineralization pulses occurred within a time window of 0.32 m.y., but possibly in more rapid succession. In each intrusion, several concordant grains are signicantly older, ranging to at least 38.5 Ma but possibly as far back as ca. 40.5 Ma. This variation is interpreted as a minimum lifetime of the subjacent magma reservoir of at least 0.8 m.y., but possibly more than 2 m.y. Four published Re-Os mineral ages indicate that hydrothermal molybdenum veins formed at 37.0 0.27 Ma (Chesley and Ruiz, 1997), distinctly later than the cluster of young highprecision ages from the latite dikes that are cut by these veins (Fig. 4). AGE BRACKETS OR POPULATION STATISTICS? A PLEA FOR GEOLOGICAL UNCERTAINTY INTERPRETATION High-precision concordant U-Pb dates from two porphyry copper deposits and published data from magmatic complexes show that individual zircon grains can crystallize in a magma reservoir over a protracted period, and that each grain can retain its crystallization age through subsequent magma evolution. This implies that the mean of all zircon grain ages for each porphyry shown in Figures 3A and 4 has no direct physical signicance, and is certainly not a good estimator for the age of porphyry emplacement. The standard error of this mean has even less geological signicance if age variations are real. It is no measure of uncertainty, and it bears no relation to the duration of zircon crystallization in the long-lived magma reservoir; note that the value of the standard error of the mean would decrease if greater numbers of zircons were measured, contrary to Figure 3A and geological expectation from a zircon-precipitating magma system with a nite lifetime. These limitations to statistical data interpretation also apply to

the overlapping zircon populations shown in Figures 3B and 3C, obtained by Harris et al. (2004, 2008) using LA-ICP-MS microanalyses. Without outlier ltering, statistical population analysis, and computation of means and their unrealistically small standard errors (following Ballard et al., 2001), Harris et al. (2008) would not have reached the incorrect conclusion that the mineralized porphyries at Bajo de la Alumbrera were emplaced during two main epochs separated by ~1 m.y. These observations carry a more general message for the reporting of geological uncertainties in igneous zircon geochronology, especially for young magmatic rocks. We propose that a set of analyses of different grains should only be averaged if their ages overlap within analytical uncertainty. Geological age uncertainty in this case is most realistically estimated from the variance or standard deviation of the sample of ages. Interpreting the smaller standard error of the mean as a geological uncertainty for the age of magma solidication is only correct if its value is small compared with the duration of zircon crystallization. This assumption cannot be validated by population statistics alone; it must be geologically justied case by case. If individual zircon grain ages do not overlap, the age range may carry signicant geological information, and the youngest reliably magmatic and analytically concordant ages yield the maximum age of emplacement of rapidly cooled magmatic rocks, provided that crystal portions that had undergone lead loss were avoided or removed by chemical abrasion. CONCLUSIONS Critical interpretation of high-precision zircon ages, based on clear eld relations and a careful distinction between analytical sampling uncertainty and real age variation, can differentiate between the characteristic lifetimes of processes contributing to the formation of giant magmatic-hydrothermal ore deposits. Crustal magma reservoirs evolve over hundreds of thousands or even a few million years, which may be recorded by individual zircon grains of signicantly variable age within a single sample. This long-lasting process is probably essential in preparation for a major event of large-scale uid saturation (Halter et al., 2005). By contrast, the emplacement of one or several mineralized porphyries from the roof of the magma chamber and the focusing of a large uid ux through the fractured stock occurs on a time scale of <100 k.y., and possibly much faster. With further improvement of analytical precision of IDTIMS and its geologically critical application, we can hope to further constrain the lifetime of a single porphyry mineralization event. This will be essential for testing alternative physical models for magmatic-hydrothermal ore formation,

ID-TIMS data Bingham Canyon

KM10

B
Latite Porphyry
Truncates first veins, cut by second Cu-Au pulse

C
40 39

206Pb/238 U

0.0061 0.0060 0.0059 0.0058 0.0057 0.0056 0.030 0.0325 0.035 0.0375 0.040 207Pb/235 U
Immediately predating main Cu-Au mineralization

KM2

5091-400

KM5

D310

37

ReOs ages
0.0425 0.035 0.0375 0.040 0.035 0.0375 0.040 0.0425

36

Figure 4. Concordia diagrams with isotopic dilutionthermal ionization mass spectrometry (ID-TIMS) results from three porphyries (A: KM10, KM2, 5091-400; B: KM5; C: D310) bracketing two main pulses of Cu-Au mineralization at Bingham Canyon (Utah, USA); Re-Os (molybdenite) data are from Chesley and Ruiz (1997).

GEOLOGY, August 2011

206Pb/238 U

Postdates Cu-Au veining, only weak potassic 38 alteration

age

Quartz Monzonite Prophyry

Quartz Latite Porphyry

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which predict even shorter time scales ranging between 100 yr and tens of thousands of years.
ACKNOWLEDGMENTS We thank Julio Bruna, Florencia Mrquez-Zavala, Dimitri Meier, and Kim Schroeder for help with eld work; John Dilles, Thomas Driesner, and Urs Schaltegger for discussions; and the reviewers for constructive comments on this manuscript. This research was supported by Swiss National Science Foundation grants 200020-116639 and 200020-124906. REFERENCES CITED Annen, C., 2009, From plutons to magma chambers: Thermal constraints on the accumulation of eruptible silicic magma in the upper crust: Earth and Planetary Science Letters, v. 284, p. 409416, doi:10.1016/j.epsl.2009.05.006. Audtat, A., Pettke, T., Heinrich, C.A., and Bodnar, R.J., 2008, The composition of magmatichydrothermal uids in barren and mineralized intrusions: Economic Geology and the Bulletin of the Society of Economic Geologists, v. 103, p. 877908, doi:10.2113/gsecongeo.103.5.877. Bachmann, O., Charlier, B.L.A., and Lowenstern, J.B., 2007, Zircon crystallization and recycling in the magma chamber of the rhyolitic Kos Plateau Tuff (Aegean arc): Geology, v. 35, p. 7376, doi:10.1130/G23151A.1. Bacon, C.R., and Lowenstern, J.B., 2005, Late Pleistocene granodiorite source for recycled zircon and phenocrysts in rhyodacite lava at Crater Lake, Oregon: Earth and Planetary Science Letters, v. 233, p. 277293, doi:10.1016/j.epsl .2005.02.012. Ballard, J.R., Palin, J.M., Williams, I.S., Campbell, I.H., and Faunes, A., 2001, Two ages of porphyry intrusion resolved for the super-giant Chuquicamata copper deposit of northern Chile by ELA-ICP-MS and SHRIMP: Geology, v. 29, p. 383386, doi:10.1130/0091-7613 (2001)029<0383:TAOPIR>2.0.CO;2. Candela, P.A., 1991, Physics of aqueous phase evolution in plutonic environments: American Mineralogist, v. 76, p. 10811091. Cathles, L.M., 1977, An analysis of the cooling of intrusives by ground-water convection which includes boiling: Economic Geology and the Bulletin of the Society of Economic Geologists, v. 72, p. 804826, doi:10.2113/gsecongeo.72.5.804. Cathles, L.M., and Shannon, R., 2007, How potassium silicate alteration suggests the formation of porphyry ore deposits begins with the nearly explosive but barren expulsion of large volumes of magmatic water: Earth and Planetary Science Letters, v. 262, p. 92108, doi:10.1016/j .epsl.2007.07.029. Charlier, B.L.A., Wilson, C.J.N., Lowenstern, J.B., Blake, S., Van Calsteren, P.W., and Davidson, J.P., 2005, Magma generation at a large, hyperactive silicic volcano (Taupo, New Zealand) revealed by U-Th and U-Pb systematics in zircons: Journal of Petrology, v. 46, p. 332, doi:10.1093/petrology/egh060. Chesley, J.T., and Ruiz, J., 1997, Preliminary Re-Os dating on molybdenite mineralization from the Bingham Canyon porphyry copper deposit, Utah, in John, D.A., and Ballantyne, G.H., eds., Geology and ore deposits of the Oquirrh and Wasatch Mountains, Utah: Society of Economic Geologists Guidebook Series 29, p. 165169. Cline, J.S., and Bodnar, R.J., 1991, Can economic porphyry copper mineralization be generated by a typical calc-alkaline melt?: Journal of

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