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Published June 2014 | Supplemental Material
Journal Article Open

Introducing a Comprehensive Data Reduction and Uncertainty Propagation Algorithm for U‐Th Geochronometry with Extraction Chromatography and Isotope Dilution MC‐ICP‐MS

Abstract

We present an open‐source algorithm in Mathematica application (Wolfram Research) with a transparent data reduction and Monte Carlo simulation of systematic and random uncertainties for U‐Th geochronometry by multi‐collector ICP‐MS. Uranium and thorium were quantitatively separated from matrix elements through a single U/TEVA extraction chromatography step. A rigorous calibrator‐sample bracketing routine was adopted using CRM‐112A and IRMM‐035 standard solutions, doped with an IRMM‐3636a ^(233)U/^(236)U 'double‐spike' to account for instrumental mass bias and deviations of measured isotope ratios from certified values. The mean of ^(234)U/^(238)U and ^(230)Th/^(232)Th in the standard solutions varied within 0.42 and 0.25‰ (permil) of certified ratios, respectively, and were consistent with literature values within uncertainties. Based on multiple dissolutions with lithium metaborate flux fusion, U and Th concentrations in USGS BCR‐2 CRM were updated to 1739 ± 2 and 5987 ± 50 ng g^(−1) (95% CI), respectively. The measurement reproducibility of our analytical technique was evaluated by analysing six aliquots of an in‐house reference material, prepared by homogenising a piece of speleothem (CC3A) from Cathedral Cave, Utah, which returned a mean age of 21483 ± 63 years (95% CI, 2.9‰). Replicate analysis of ten samples from CC3A was consistent with ages previously measured at the University of Minnesota by single‐collector ICP‐MS within uncertainties.

Additional Information

© 2013 The Authors. Geostandards and Geoanalytical Research © 2013 International Association of Geoanalysts. Received 10 Jun 13 – Accepted 14 Oct 13. We would like to thank Nicolas Dauphas for providing the CRM‐112A U metal reference material, IRMM3636a spike and his generous input on development of the code and the Monte Carlo simulation. We thank David McGee for providing us with the CCA3 speleothem. We are also grateful to Ted Zateslo, Lary Ball and Franco Marcantonio for their feedback on mass spectrometry and thank Aaron Pietruszka for providing the ^(229)Th spike. Hai Cheng and Larry Edwards's contributions were instrumental in the initial dating of the CC3 sample at UMN. The authors appreciate the constructive comments from the journal editor Jon Woodhead, Noah McLean and two other anonymous reviewers. This study was in part funded by NSF Grant #1103489.

Attached Files

Supplemental Material - ggr12018-sup-0001-u_data_appendix_a.xls

Supplemental Material - ggr12018-sup-0002-th_data_appendix_a.xls

Supplemental Material - ggr12018-sup-0003-u_th_data_appendix_a.xls

Supplemental Material - ggr12018-sup-0004-u_th_age_appendix_a.xls

Supplemental Material - ggr12018-sup-0005-supplementarydata.xlsx

Supplemental Material - ggr12018-sup-0006-supplementary_flow_chart.xlsx

Supplemental Material - ggr12018-sup-0007-th_input_appendix_a.xlsx

Supplemental Material - ggr12018-sup-0008-u_input_appendix_a.xlsx

Supplemental Material - ggr12018-sup-0009-u-thdatareductionprogram.nb

Supplemental Material - ggr12018-sup-0010-u-th-data-reduction-program.cdf

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