Uranium-Lead Isotopic Variations in Zircons: a Case Study1

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Uranium-Lead Isotopic Variations in Zircons: a Case Study1 URANIUM-LEAD ISOTOPIC VARIATIONS IN ZIRCONS: A CASE STUDY1 LEON T. SILVER2 AND SARAH DEUTSCH3 ABSTRACT Zircons in a single 250-pound block of Precambrian Johnny Lyon granodiorite from the Dragoon Quad­ rangle in Cochise County, Arizona, have been concentrated with special attention to yield and nature of impurities. Morphology, zoning, color, inclusions, size distribution, radioactivity, refractive indexes, cell dimensions, and other properties have been compared with the isotopic properties in the U-Pb system (and to a less precise degree in the Th-Pb system). It has been observed: (1) Uranothorite impurities, while less than 1 per cent in abundance, contribute much more than 50 per cent of the activity in conventionally pre­ pared concentrates. The presence of uranothorite drastically affects the apparent ages in the zirons. (2) The uranothorite can be satisfactorily removed by an appropriate acid-washing procedure. (3) The uranothorite­ free zircon concentrates are not homogeneous and show systematic variations in radioactivity and various isotopic properties as a function of average crystal size. (4) Individual zircons show internal variation in radioactivity and may differ in specific activity from other individuals by as much as an order of magnitude. (5) It is possible to strip outer layers experimentally from an aggregate of zircons to determine variations in composite internal isotopic properties. (6) The family of uranium-lead systems distinguished in the in­ homogeneous zircon suite may be utilized to establish patterns of isotopic ratio variations that yield much more useful geochronological information than any single system. (7) All systems in this rock appear to have formed 1,655 million years ago and to have been profoundly disturbed by an event 90 million years ago. There is no evidence of any type of disturbance other than this simple episodic pattern. (8) While the mechanism of disturbance is not directly established, it is evident that radioactivity and radiation damage strongly influ­ ence susceptibility of the systems to disturbance. (9) It is possible to offer reasonable explanations for some of the puzzling discrepancies between uranium-lead and thorium-lead ages determined on a single mineral concentrate. (10) Recognition of the existence of families of uranium-lead systems among the variable mem­ bers of a single mineral species, or in associated mineral species, in a single typical granitic rock provides a powerful tool for investigation of the processes and conditions that have influenced the age-dating systems. (11) The systematic variations in U and Th provide interesting information on the role of some trace elements and accessory minerals in the crystallization history of the rock. (12) The Johnny Lyon granodiorite is the oldest igneous rock dated in Arizona thus far and places a minimum age of 1,655 ± 20 million years on the orogeny called Mazatzal Revolution. INTRODUCTION geological setting and history of the ana­ In geochronological investigations of rock lyzed minerals bear directly on the age inter­ systems, methods involving isotope chemis­ pretations made from the carefully meas­ try and mass spectrometry have evolved as ured isotopic relationships. Apparent ages precise and useful techniques for analysis of calculated from several minerals in the same a number of natural radioactivity relation­ host rock commonly have been in significant ships. A vast body of data on parent-daugh­ disagreement. It is to be hoped that some of ter ratios in the systems K 40/ Ar 40, Rb87/Srs7, these contradictory "ages" may be recon­ u2as/pb200, u2as;pb201 and Th2a2/pb2os has ciled, in part, by combining careful minera­ been carefully determined by these tech­ logical and petrological studies of the ana­ niques yielding geochronological informa­ lyzed phases with the isotopic measurements tion of far-reaching importance to studies of to achieve a better understanding of the geo­ the earth. At the same time, it has become logical factors. Few such attempts have been apparent also that numerous factors in the made. Among the several naturally radioactive 1 Contribution No. 1070, Division of Geological isotopes used in geochronology, the constant Sciences, California Institute of Technology, Pasa­ chemical coupling of U238 and U235 with their dena, California. Manuscript received February 21, 206 1962; revised May 25, 1962. chemically similar decay products Pb and 207 2 Division of Geological Sciences, California In­ Pb introduces the fewest assumptions re­ stitute of Technology, Pasadena, California. quired for a comparison of apparent ages. It 232 3 Present address: University of Brussels, Bel­ is fortunate too that Th , a similar actinide gium. element commonly associated with uranium, 721 722 LEON T. SILVER AND SARAH DEUTSCH 208 also decays to a stable lead nuclide, Pb • activity, size, zoning, and other characteris­ Thus it is often possible to compare ages de­ tics. A number of important regularities rived from three systems in the same have been observed. These lead to the con­ analyses. clusion that within these 1! cubic feet of Larsen et al. (1952) suggested that one of granite, there exist a large number of urani­ the most attractive phases in common rock um-thorium-lead systems which, when systems for studying these three isotopic studied as a family, can elucidate some types decay relations was zircon. They proposed of apparent age contradictions and, indeed, the so-called lead-a method, or Larsen meth­ provide some significant additional informa­ od, a non-isotopic method of age determina­ tion on the history of the rock. They also tion. Tilton, Patterson, et al. (1955) and, in raise some questions about accepted as­ particular, Tilton et al. (1957, and numerous sumptions in age interpretations. GEOLOGIC SETTING OF THE ROCK The rock sample was obtained from a large Precambrian granodiorite pluton in the Johnny Lyon Hills in the Dragoon Quadrangle, Cochise County, in southeast­ ern Arizona (figs. 1, 2). Detailed geologic studies have been made of the pluton and its setting by the United States Geological Sur­ vey. Preliminary accounts are available (Silver, 1955; Cooper, 1959), and a full re­ port will be published soon (Cooper and Silver, forthcoming). The regional setting is shown on the geologic map of Cochise Coun­ ty (Arizona Bureau of Mines, 1959). The pluton is a post-tectonic intrusive in its Pre­ cambrian setting but it has been strongly modified locally by younger deformational, intrusive, and alteration processes, many of which are clearly Mesozoic or Cenozoic. This FIG. 1.-Index map of Arizona showing location particular sample (L-312) was selected to be of Johnny Lyon Hills area in Cochise County. as free as possible from detectable metamor­ phic effects, as well as from the extensive other publications) demonstrated that pre­ weathering effects characteristic of this arid cise and significant isotopic measurements region. could be made on the zircons of many differ­ The rock is a medium - to coarse-grained, ent rocks. Tilton's work more than any somewhat porphyritic, hornblende-biotite other to date has defined the applicability granodiorite. In hand specimen, coarse white and problems of U-Th-Pb systems in zircons plagioclase is set in gray quartz, scattered in age-determination studies. The present pink potash feldspar, dark green platy bio­ report is an exploration of some of these tite, greenish-black prismatic hornblende problems. and, more rarely, euhedral brown sphene. The uranium-lead systems and, with less A few very thin epidote-quartz veinlets, a precision, the thorium-lead systems have fraction of a millimeter in thickness, tran­ been examined in zircon concentrates from sect the block. a single block of granitic rock. Variations in In thin section, the rock is hypidiomor­ isotopic properties have been compared with phic-inequigranular with a slightly seriate concentrate purity and homogeneity, radio- porphyritic texture. Tabular and zoned GENERALIZED MAP OF THE LYON HILLS filiii!!ll Tertiary and Quaternary alluvium m Paleozoic or younger rocks .,, ...: u 0... c 0 ~ t?~rt.~ E 0 Zones of 0 Rhyolite porphyry I intrusive sheets ~ lp£pso I Pinal schist (Slates and oraywackes) SCALE IN MILES 0 2 3 FIG. 2.-Generalized geologic map of the Johnny Lyon Hills, showing the stratigraphic and structural relationships of Johnny Lyon granodiorite to both older and younger rocks. Samples L-312 and L-609 were collected to be as free as possible of effects of the three major shear zones and other alteration features in ~he intrusive, 724 LEON T. SILVER AND SARAH DEUTSCH plagioclase crystals vary in composition MINERAL SEPARATIONS from An35 at the cores to An2o at the rims. The original reservoir of samples collected Microcline-microperthite is anhedral, tex­ in the field weighed approximately 250 turally late, and bordered by myrmekite pounds. Almost all of the zircons used in this fringes on the plagioclase. Quartz is scat­ study came from a representative 60-pound tered in anhedral aggregates. The biotite aliquot of the original sample. It was neces­ and hornblende are subhedral to euhedral. sary, however, to process some additional Accessary minerals include magnetite, apa­ TABLE 1B tite, sphene, zircon, allanite, and urano­ thorite in sequence of decreasing abundance. JOHNNY LYON GRANODIORITE Chemical, normative, and modal analyses MODAL ANALYSIS are given in table 1. As in every other speci- (Point Count) TABLE 1A L-312* JOHNNY LYON GRANODIORITE* (Weight Per Cent) CHEMICAL ANALYSIS Quartz ........ 25.84 Plagioclase .... 45.38 Myrmekite .... 1. 93 Average of 80 L-312t Microcline- Granodioritest (Weight perthite ..... 14.20 (Weight Per Cent) Biotite ........ 6.44 Per Cent) Hornblende ... 4.06 Magnetite ..... 1.34 Si02............... 68.89 66.13 Sphene ....... 0.56 Ti02.............. 0.45 0.51 Other accessories 0.25 AbOa. .. 15.02 15.50 Fe20a.............. 1.40 1.62 Total. ...... 100.00 FeO............... 1.89 2.70 MnO.............. 0.08 0.07 Normative Analysis MgO.............. 1.43 1. 73 Salic: Cao.............. 3.44 3.70 Quartz ........ 25.02 Na20.
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