Preamble: The 'National Geochemical Survey of Australia: The Geochemical Atlas of Australia' was published in July 2011 along with a digital copy of the NGSA geochemical dataset (http://dx.doi.org/10.11636/Record.2011.020). The NGSA project is described here: www.ga.gov.au/ngsa. The present dataset contains additional geochemical data obtained on NGSA samples: the Lead Isotopes Dataset. Abstract: Over 1200 new lead (Pb) isotope analyses were obtained on catchment outlet sediment samples from the NGSA regolith archive to document the range and patterns of Pb isotope ratios in the surface regolith and their relationships to geology and anthropogenic activity. The selected samples included 1204 NGSA Top Outlet Sediment (TOS) samples taken from 0 to 10 cm depth and sieved to <2 mm (or ‘coarse’ fraction); three of these were analysed in duplicate for a total of 1207 Pb isotope analyses. Further, 12 Northern Australia Geochemical Survey (NAGS; http://dx.doi.org/10.11636/Record.2019.002) TOS samples from within a single NGSA catchment, also sieved to <2 mm, were analysed to provide an indication of smaller scale variability. Combined, we thus present 1219 new TOS coarse, internally comparable data points, which underpin new national regolith Pb isoscapes. Additionally, 16 NGSA Bottom Outlet Sediment (BOS; ~60 to 80 cm depth) samples, also sieved to <2 mm, and 16 NGSA TOS samples sieved to a finer grainsize (<75 um, or ‘fine’) fraction from selected NGSA catchments were also included to inform on Pb mobility and residence. Lead isotope analyses were performed by Candan Desem as part of her PhD research at the School of Geography, Earth and Atmospheric Sciences, University of Melbourne. After an initial ammonium acetate (AmAc) leach, the samples were digested in aqua regia (AR). Although a small number of samples were analysed after the AmAc leach, all samples were analysed after the second, AR digestion, preparation step. The analyses were performed without prior matrix removal using a Nu Instruments Attom single collector Sector Field-Inductively Coupled Plasma-Mass Spectrometer (SF-ICP-MS). The dried soil digests were redissolved in 2% HNO3 run solutions containing high-purity thallium (1 ppb Tl) and diluted to provide ~1 ppb Pb in solution. Admixture of natural, Pb-free Tl (with a nominal 205Tl/203Tl of 2.3871) allowed for correction of instrumental mass bias effects. Concentrations of matrix elements in the diluted AR digests are estimated to be in the range of 1–2 ppm. The SF-ICP-MS was operated in wet plasma mode using a Glass Expansion cyclonic spray chamber and glass nebuliser with an uptake rate of 0.33 mL/min. The instrument was tuned for maximum sensitivity and provided ~1 million counts per second/ppb Pb while maintaining flat-topped peaks. Each analysis, performed in the Attom’s ‘deflector peak jump’ mode, consists of 30 sets of 2000 sweeps of masses 202Hg, 203Tl, 204Pb, 205Tl, 206Pb, 207Pb and 208Pb, with dwell times of 500 μs and a total analysis time of 4.5 min. Each sample acquisition was preceded by a blank determination. All corrections for baseline, sample Hg interference (202Hg/204Pb ratios were always <0.043) and mass bias were performed online, producing typical in-run precisions (2 standard errors) of ±0.047 for 206Pb/204Pb, ±0.038 for 207Pb/204Pb, ±0.095 for 208Pb/204Pb, ±0.0012 for 207Pb/206Pb and ±0.0026 for 208Pb/206Pb. A small number of samples with low Pb concentrations exhibited very low signal sizes during analysis resulting in correspondingly high analytical uncertainties. Samples producing within-run uncertainties of >1% relative (measured on the 207Pb/204Pb ratio) were discarded as being insufficiently precise to contribute meaningfully to the dataset. Data quality was monitored using interspersed analyses of Tl-doped ~1 ppb solutions of the National Institute of Standards and Technology (NIST) SRM981 Pb standard, and several silicate reference materials: United States Geological Survey ‘BCR-2’ and ‘AGV-2’, Centre de Recherches Pétrographiques et Géochimiques ‘BR’ and Japan Geological Survey ‘JB-2’. In a typical session, up to 50 unknowns plus 15 standards were analysed using an ESI SC-2 DX autosampler. Although previous studies using the Attom SF-ICP-MS used sample-standard-bracketing techniques to correct for instrumental Pb mass bias, Tl doping was found to produce precise, accurate and reproducible results. Based upon the data for the BCR-2 and AGV-2 secondary reference materials, for which we have the most analyses, deviations from accepted values (accuracy) were typically <0.17%. Data for the remaining silicate standards appear slightly less accurate but these results may, to some extent, reflect uncertainty in the assigned literature values for these materials. Replicate runs of selected AR digests yielded similar reproducibility estimates. The results show a wide range of Pb isotope ratios in the NGSA (and NAGS) TOS <2 mm fraction samples across the continent (N = 1219): 206Pb/204Pb: Min = 15.558; Med ± Robust SD = 18.844 ± 0.454; Mean ± SD = 19.047 ± 1.073; Max = 30.635 207Pb/204Pb; Min = 14.358; Med ± Robust SD = 15.687 ± 0.091; Mean ± SD = 15.720 ± 0.221; Max = 18.012 208Pb/204Pb; Min = 33.558; Med ± Robust SD = 38.989 ± 0.586; Mean ± SD = 39.116 ± 1.094; Max = 48.873 207Pb/206Pb; Min = 0.5880; Med ± Robust SD = 0.8318 ± 0.0155; Mean ± SD = 0.8270 ± 0.0314; Max = 0.9847 208Pb/206Pb; Min = 1.4149; Med ± Robust SD = 2.0665 ± 0.0263; Mean ± SD = 2.0568 ± 0.0675; Max = 2.3002 These data allow the construction of the first continental-scale regolith Pb isotope maps (206Pb/204Pb, 207Pb/204Pb, 208Pb/204Pb, 207Pb/206Pb, and 208Pb/206Pb isoscapes) of Australia and can be used to understand contributions of Pb from underlying bedrock (including Pb-rich mineralisation), wind-blown dust and possibly from anthropogenic sources (industrial, transport, agriculture, residential, waste handling). The complete dataset is available to download as a comma separated values (CSV) file from Geoscience Australia's website (http://dx.doi.org/10.26186/5ea8f6fd3de64). Isoscape grids (inverse distance weighting interpolated grids with a power coefficient of 2 prepared in QGis using GDAL gridding tool based on nearest neighbours) are also provided for the five Pb isotope ratios (IDW2NN.TIF files in zipped folder). Alternatively, the new Pb isotope data can be downloaded from and viewed on the GA Portal (https://portal.ga.gov.au/).

<div>We present the first national-scale lead (Pb) isotope maps of Australia based on surface regolith for five isotope ratios, ²⁰⁶Pb/²⁰⁴Pb, ²⁰⁷Pb/²⁰⁴Pb, ²⁰⁸Pb/²⁰⁴Pb, ²⁰⁷Pb/²⁰⁶Pb, and ²⁰⁸Pb/²⁰⁶Pb, determined by single collector Sector Field-Inductively Coupled Plasma-Mass Spectrometry after an Ammonium Acetate leach followed by Aqua Regia digestion. The dataset is underpinned principally by the National Geochemical Survey of Australia (NGSA) archived floodplain sediment samples. We analysed 1219 ‘top coarse’ (0-10 cm depth, &lt;2 mm grain size) samples, collected near the outlet of 1098 large catchments covering 5.647 million km2 (~75% of Australia). This paper focusses on the Aqua Regia dataset. The samples consist of mixtures of the dominant soils and rocks weathering in their respective catchments (and possibly those upstream) and are therefore assumed to form a reasonable representation of the average isotopic signature of those catchments. This assumption was tested in one of the NGSA catchments, within which 12 similar ‘top coarse’ samples were also taken; results show that the Pb isotope ratios of the NGSA catchment outlet sediment sample are close to the average of the 12 sub-catchment, upstream samples. National minimum, median and maximum values reported for ²⁰⁶Pb/²⁰⁴Pb were 15.558, 18.844, 30.635; for ²⁰⁷Pb/²⁰⁴Pb 14.358, 15.687, 18.012; for ²⁰⁸Pb/²⁰⁴Pb 33.558, 38.989, 48.873; for ²⁰⁷Pb/²⁰⁶Pb 0.5880, 0.8318, 0.9847; and for ²⁰⁸Pb/²⁰⁶Pb 1.4149, 2.0665, 2.3002, respectively. The new dataset was compared with published bedrock and ore Pb isotope data, and was found to dependably represent crustal elements of various ages from Archean to Phanerozoic. This suggests that floodplain sediment samples are a suitable proxy for basement and basin geology at this scale, despite various degrees of transport, mixing, and weathering experienced in the regolith environment, locally over protracted periods of time. An example of atmospheric Pb contamination around Port Pirie, South Australia, where a Pb smelter has operated since the 1890s, is shown to illustrate potential environmental applications of this new dataset. Other applications may include elucidating detail of Australian crustal evolution and mineralisation-related investigations.&nbsp;</div> <b>Citation:</b> Desem, C. U., de Caritat, P., Woodhead, J., Maas, R., and Carr, G.: A regolith lead isoscape of Australia, <o>Earth Syst. Sci. Data</i>, 16, 1383–1393, https://doi.org/10.5194/essd-16-1383-2024, 2024.