Abstract
To evaluate the mechanisms driving nanoscale trace element mobility in radiation-damaged zircon, we analyzed two well-characterized Archean zircons from the Kaapvaal Craton (southern Africa): one zircon remained untreated and the other was experimentally heated in the laboratory at 1450 °C for 24 h. Atom probe tomography (APT) of the untreated zircon reveals homogeneously distributed trace elements. In contrast, APT of the experimentally heated zircon shows that Y, Mg, Al, and Pb+Yb segregate to a set of two morphologically and crystallographically distinct cluster populations that range from 5 nm tori to 25 nm toroidal polyhedra, which are confirmed to be dislocation loops by transmission electron microscopy (TEM). The dislocation loops lie in {100} and {001} planes; the edges are aligned with <100>, <101>, and <001>. The largest loops (up to 25 nm diameter) are located in {100} and characterized by high concentrations of Mg and Al, which are aligned with <001>. The 207Pb/206Pb measured from Pb atoms located within all of the loops (0.264 ± 0.025; 1σ) is consistent with present-day segregation and confirms that the dislocation loops formed during our experimental treatment. These experimentally induced loops are similar to clusters observed in zircon afected by natural geologic processes. We interpret that diferences in cluster distribution, density, and composition between experimentally heated and geologically afected zircon are a function of the radiation dose, the pressure-temperature-time history, and the original composition of the zircon. These findings provide a framework for interpreting the significance of clustered trace elements and their isotopic characteristics in zircon. Our findings also suggest that the processes driving cluster formation in zircon can be replicated under laboratory conditions over human timescales, which may have practical implications for the mineralogical entrapment of significant nuclear elements.
Funding statement: This work was supported in part by Bowdoin College Research Funds. The SEMs at Bowdoin College and Curtin University were supported by NSF MRI-1530963 to E. Peterman and R. Beane and ARC LE 190100176 to S. Reddy and Z. Quadir, respectively. The development of the Geoscience Atom Probe Facility was supported by the Science and Industry Endowment Fund (SIEF) through Grant SIEF RI13-01 to S. Reddy. D. Fougerouse is supported by the Australian Research Council (ARC DE190101307).
Acknowledgments
The authors thank Callum Hetherington for editorial handling and Lee White and two anonymous reviewers for providing constructive comments. Peterman thanks Jaclyn Baughman (Humboldt State University) for providing the zircon separate, Jonathan Stebbins (Stanford) for the use of his high-temperature furnaces, Marty Grove (Stanford) for supporting Peterman’s Blaustein appointment at Stanford, and the Blaustein Visiting Researcher fund at Stanford University.
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