Geochronological and Geochemical Effects of Zircon Chemical Abrasion: Insights from Single-Crystal Stepwise Dissolution Experiments

Abstract

Abstract. Chemical abrasion in hydrofluoric acid (HF) is routinely applied to zircon grains prior to U-Pb dating by isotope dilution thermal ionization mass spectrometry (ID-TIMS) to remove radiation-damaged portions of grains affected by Pb loss. Still, many chemically abraded datasets exhibit evidence of residual Pb loss. Here we test how the temperature and duration of chemical abrasion affects zircon U-Pb and trace element systematics in a series of 4-hour, single-crystal stepwise dissolution experiments at 180 °C and 210 °C. Microtextural data for the zircon samples studied is presented in a complementary paper by McKanna et al. (2023). We find that stepwise dissolution at 210 °C is more effective at eliminating U, common Pb (Pbc), and light rare earth element (LREE) enriched material affected by open system behavior; reduces the presence of leaching-induced artefacts that manifest as reverse discordance; and produces more consistent and concordant results in zircon from the three rocks studied. We estimate that stepwise dissolution in three 4 h steps is roughly equivalent to a single ~8 h leaching step due to the insulating properties of the PTFE sleeve in the Parr pressure dissolution vessel, whereas traditionally labs utilize a single 12-hour leaching step. To better understand the causes of Pb-loss in zircon, we calculate time-integrated alpha dose estimates for leachates and residues from measured radionuclide concentrations to determine: 1) the alpha dose of the material dissolved at the two leaching conditions, and 2) the apparent minimum alpha dose required for Pb loss to occur: ≥ 6 × 1017 α/g. We conclude that a single 8 h leaching step at 210 °C should yield crystallization ages in the majority of zircon and that this can be used as an effective approach for routine analysis. However, Ultimately, the effectiveness of any chemical abrasion protocol will be sample-dependent. By framing Pb loss and zircon solubility in terms of alpha dose, however, workers can better tailor the chemical abrasion process to specific zircon samples to improve the accuracy and precision of U-Pb results.

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“…Reverse discordance is caused by elemental fractionation of U from Pb; in this case, it appears to have occurred without Pb isotope fractionation, resulting in L2 207 Pb/ 206 Pb dates that are in most cases consistent with those of the respective zircon residue. On the basis of acid leaching experiments ( 25 ), we suggest that the presence of this effect in some L2 leachates is an artifact resulting from partial dissolution rather than a natural feature.…”