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RESEARCH PRODUCT

230Th/U-dating of carbonate deposits from ancient aqueducts

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Abstract Carbonate deposits in aqueducts, known as calcareous sinter, can reach a considerable thickness and are commonly annually laminated. Environmental and palaeoclimate proxies measured in calcareous sinter samples, such as stable oxygen and carbon isotopes and trace elements, can provide important high-resolution information on hydrological conditions, temperature, and local precipitation in the catchment area of an aqueduct. In order to utilize the proxy data for palaeoclimate reconstruction, the sinter deposits must be dated by annual laminae counting and more precisely by 230 Th/U-dating. The major problem of 230 Th/U-dating of calcareous sinter in aqueducts is the relatively large amount of initial detrital Th contained in the deposits, leading to apparently wrong 230 Th/U-ages. Here we present the first systematic approach to date sinter deposits from various locations in western and eastern Europe using the 230 Th/U-method. Calcareous sinter samples from eight Roman aqueducts in France, Germany, Greece, and Turkey were investigated. Preliminary screening for the U and Th content of the samples by LA-MC-ICPMS revealed that the 238 U/ 232 Th isotope ratio of the samples is highly variable, with values ranging from 0.03 to >11. The four samples with the largest 238 U/ 232 Th ratios were selected for MC-ICPMS 230 Th/U-dating, even though they still contain substantial amounts of detrital 232 Th. The uncorrected 230 Th/U-ages are between 2.9 and 46 ka and thus all significantly older than required by the Roman origin of the samples (ca. 2 ka). Application of the conventional correction for detrital contamination, assuming a bulk Earth 232 Th/ 238 U weight ratio of 3.8 (±50%) and 230 Th, 234 U, and 238 U in secular equilibrium, results in younger ages that are in agreement within error with a Roman origin. However, the resulting errors are very large, and the ages are therefore not very reliable. Application of three-dimensional isochrons yields both younger ages and smaller age uncertainties than the conventional detrital correction. However, the isochron age uncertainties are still between 0.8 and 1 ka and thus not as precise as required for paleoclimate and archaeological studies. Precise and accurate 230 Th/U-dating of these relatively young Roman sinter deposits is therefore challenging. The observed high MSWD values ( Mean Square of Weighted Deviates ) and low Probabilities of Fit of all isochrons show that the isochron assumptions are not fulfilled for our samples. However, it is possible to estimate the degree of scatter around the isochron produced by different processes and simulate the different scenarios in Monte-Carlo simulations. These simulations show that the scatter observed in our isochron data cannot be explained by different ages and initial ( 234 U/ 238 U) activity ratios of different sub-samples, but also requires variable ( 230 Th/ 232 Th) activity ratios of the detrital component.