Testing a new combined (U,Th)–He and U/Th dating approach on Plio-Pleistocene calcite speleothems

The geochronology of cave deposits in the Cradle of Humankind UNESCO World Heritage Site in South Africa provides a timeframe essential for the interpretation of its fossils. The uranium-lead (U–Pb) and uranium-thorium disequilibrium (U/Th) dating of speleothems, mostly flowstones that underlie and blanket the fossil-bearing sediments, have been effective in this sense, but U–Pb is limited by the requirement of ∼1 ppm U concentrations and low common Pb contents, and U/Th has a c. 500 ka limit of applicability. Here we report age results for calcite-aragonite speleothems obtained using a new combined uranium-thorium-helium ((U,Th)–He) and U/Th dating routine. We reproduced within analytical uncertainty, the published U–Pb or U/Th ages for (a) flowstone in three drill core samples in the range 2000–3000 ka, (b) a flowstone hand sample taken at surface with an age of 1800 ka, and (c) five underground flowstone samples in the range 100–800 ka. Calcite retentivity for He under cave conditions is thus demonstrated. In the few cases where helium loss was observed in speleothems, only some of the subsamples were affected, and to varying degrees, suggesting loss by lattice damage not related to diagenetic processes, rather than volume diffusion. In the 100 to 800 ka range, the combined U/Th disequilibrium and (U,Th)–He method also yielded reliable values for initial (230Th/238U) and (234U/238U) activity ratios. Importantly, most subsamples had high initial (230Th/238U) values, ranging from 1.0 to 19.7, although having low Th/U ratios. This is probably due to incorporation of Fe–Mn oxides-hydroxides dust, on which 230Th was previously adsorbed. Such samples are mostly not dateable by U/Th without the additional input from the He analysis. If not detected and corrected for, such high initial (230Th/238U) values can lead to inaccurate U/Th and U–Pb ages. Our study shows that the incorporation of He analysis in U/Th dating has broad potential application, with four methods for calculating the ages, in carbonates from different environments where U-Pb or U/Th dating would not work.