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Atom Probe Tomography for Isotopic Analysis: Development of the 34S/32S System in Sulfides

Published online by Cambridge University Press:  12 November 2021

Phillip Gopon Open the ORCID record for Phillip Gopon [Opens in a new window] ,
James O. Douglas ,
Frederick Meisenkothen ,
Jaspreet Singh ,
Andrew J. London  and
Michael P. Moody
Phillip Gopon*
Affiliation:
Department of Applied Geosciences and Geophysics, University of Leoben, Leoben, AT 8700, Austria Department of Materials, University of Oxford, Oxford OX1 3PH, UK Department of Earth Sciences, University of Oxford, Oxford OX1 3AN, UK
James O. Douglas
Affiliation:
Department of Materials, University of Oxford, Oxford OX1 3PH, UK Department of Materials, Imperial College London, London SW7 2AZ, UK
Frederick Meisenkothen
Affiliation:
Materials Measurement Science Division, National Institute of Standards and Technology, Gaithersburg, MD 20889, USA
Jaspreet Singh
Affiliation:
Department of Materials, University of Oxford, Oxford OX1 3PH, UK
Andrew J. London
Affiliation:
Department of Materials, University of Oxford, Oxford OX1 3PH, UK UK Atomic Energy Authority, Culham Science Center, Oxfordshire OX14 3DB, UK
Michael P. Moody
Affiliation:
Department of Materials, University of Oxford, Oxford OX1 3PH, UK
*
*Corresponding author: Phillip Gopon, E-mail: phillip.gopon@unileoben.ac.at
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Abstract

Using a combination of simulated data and pyrite isotopic reference materials, we have refined a methodology to obtain quantitative δ34S measurements from atom probe tomography (APT) datasets. This study builds on previous attempts to characterize relative 34S/32S ratios in gold-containing pyrite using APT. We have also improved our understanding of the artifacts inherent in laser-pulsed APT of insulators. Specifically, we find the probability of multi-hit detection events increases during the APT experiment, which can have a detrimental effect on the accuracy of the analysis. We demonstrate the use of standardized corrected time-of-flight single-hit data for our isotopic analysis. Additionally, we identify issues with the standard methods of extracting background-corrected counts from APT mass spectra. These lead to inaccurate and inconsistent isotopic analyses due to human variability in peak ranging and issues with background correction algorithms. In this study, we use the corrected time-of-flight single-hit data, an adaptive peak fitting algorithm, and an improved deconvolution algorithm to extract 34S/32S ratios from the S2+ peaks. By analyzing against a standard material, acquired under similar conditions, we have extracted δ34S values to within ±5‰ (1‰ = 1 part per thousand) of the published values of our standards.

Keywords

APTatom probe tomographypyritesulfides
Type
Development and Computation
Information
Microscopy and Microanalysis , Volume 28 , Issue 4 , August 2022 , pp. 1127 - 1140
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Copyright
Copyright © The Author(s), 2021. Published by Cambridge University Press on behalf of the Microscopy Society of America

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