Technical note: Investigation into the relationship between zircon structural damage and Pb mobility using chemical abrasion, SIMS, Raman spectroscopy, and atom probe tomography

Abstract

Chemical abrasion (CA), a two-step process of annealing and partial dissolution, is routinely applied to zircon grains prior to U-Pb geochronology to dissolve portions of the grains affected by Pb loss prior to analysis. Despite the utility of the technique, it is not clear what the more HF-soluble material produced in the annealing step is, what degree of lattice damage causes it to form instead of zircon, how to predict if a specific sub-volume of a zircon will survive CA, or how any of these processes relate to Pb mobility. In this study, we use secondary ion mass spectrometry (SIMS), Raman spectroscopy, and atom probe tomography (APT) to constrain what happens to both concordant and discordant zircon during each step of the CA process. We find that zircon in SIMS sputter craters which have undergone Pb loss generally have more heterogeneous Raman band widths than in those sputter craters where Pb has been retained. Annealing drastically reduces Raman band widths, but some heterogeneity is still present in discordant sputter craters. APT results from all samples which successfully ran were homogeneous in U, Pb, Th, and most other elements in all cases. This makes it hard to link Pb loss and lattice damage at the submicrometre scale by direct imaging in this study. However, as the zircon sputter craters with Pb loss show homogeneous APT results, we recommend against using homogeneous APT results as an indicator of closed-system U-Pb behaviour.