Short Communication: Nanoscale heterogeneity of U and Pb in baddeleyite – implications for nanogeochronology and ²³⁸U series alpha recoil effects

Abstract. Atom probe tomography (APT) of ²³⁸U and ²⁰⁶Pb has been applied to baddeleyite crystals from the Hart Dolerite (1791 ± 1 Ma) and the Great Dyke of Mauritania (2732 ± 2 Ma) in an effort to map U and Pb concentration at the nanometre scale. The purpose was to constrain the average nuclear recoil distance of ²³⁸U-series daughter nuclei in order to correct U-Pb ages determined on small baddeleyite crystals for alpha-recoil loss of Pb. Both crystals were thought to expose natural crystal surfaces providing a boundary where maximum effects of recoil loss could be observed. The Hart Dolerite sample showed no variations in Pb concentrations near the edge. The Great Dyke sample shows U zoning and the associated ²⁰⁶Pb zoning is affected by alpha recoil, apparently adjacent to a natural grain surface. The sample also shows 10 nm-scale apparently primary clusters of U atoms that contain about 40 % of the U. These are too small to constrain alpha recoil distance beyond a few nm but are apparently primary and their formation mechanism poses a dilemma. To constrain alpha recoil distance, a forward modelling approach is presented where ²⁰⁶Pb redistribution functions were determined for a range of possible distances and synthetic ²⁰⁶Pb/²³⁸U profiles were determined from the convolution of the observed U profile with the redistribution functions that were compared to the observed ²⁰⁶Pb/²³⁸U profile. A complication is the fact that the 40 by 400 nm size of the sample is lower than the range of possible alpha recoil redistribution effects so it was necessary to extrapolate the observed U zoning. An oscillatory pattern gives the best fit to the observed profile but any reasonable extrapolation constrains the average alpha recoil distance to be close to 80–90 nm, which is much larger than previous estimates using other methods. Either recoil distances can be highly anisotropic within small crystal samples or surface roughness was a factor that modified the recoiled Pb distribution. APT is a potentially useful approach to determining average alpha recoil distance but requires sampling of primary, smooth crystal faces.