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Isotope mixing models require individual isotopic tracer content for correct quantification of sediment source contributions
Authors:Hari Ram Upadhayay  Samuel Bodé  Marco Griepentrog  Roshan Man Bajracharya  William Blake  Wim Cornelis  Pascal Boeckx
Institution:1. Isotope Bioscience Laboratory – ISOFYS, Faculty of Bioscience Engineering, Ghent University, Ghent, Belgium;2. Aquatic Ecology Center (AEC), School of Science, Kathmandu University, Dhulikhel, Nepal;3. Biogeoscience, Department of Earth Sciences, ETH Zurich, Zurich, Switzerland;4. School of Geography, Earth and Environmental Sciences, Plymouth University, Plymouth, Devon, UK;5. Soil Physics Group, Department of Environment, Faculty of Bioscience Engineering, Ghent University, Ghent, Belgium
Abstract:The use of isotopic tracers for sediment source apportionment is gaining interest with recent introduction of compound‐specific stable isotope tracers. The method relies on linear mixing of source isotopic tracers, and deconvolution of a sediment mixture initially quantifies the contribution of sources to the mixture's tracer signature. Therefore, a correction to obtain real sediment source proportions is subsequently required. As far as we are aware, all published studies to date have used total isotopic tracer content or a proxy (e.g., soil carbon content) for this post‐unmixing correction. However, as the relationship between the isotopic tracer mixture and the source mixture is different for each isotopic tracer, post‐unmixing corrections cannot be carried out with one single factor. This contribution presents an isotopic tracer model structure—the concentration‐dependent isotope mixing model (CD‐IMM)—to overcome this limitation. Herein, we aim to clarify why the “conventional” approach to converting isotopic tracer proportions to source proportions using a single factor is wrong. In an initial mathematical assessment, error incurred by not using CD‐IMM (NCD‐IMM) in unmixing two sources with two isotopic tracers showed a complex relation as a function of relative tracer contents. Next, three artificial mixtures with different proportions of three soil sources were prepared and deconvoluted using 13C of fatty acids using CD‐IMM and NCD‐IMM. Using NCD‐IMM affected both accuracy (mean average error increased up to a threefold compared with the CD‐IMM output) and precision (interquartile range was up to 2.5 times larger). Finally, as an illustrative example, the proportional source contribution reported in a published study was recalculated using CD‐IMM. This resulted in changes in estimated source proportions and associated uncertainties. Content of isotopic tracers is seldom reported in published work concerning use of isotopic tracers for sediment source partitioning. The magnitude of errors made by miscalculation in former studies is therefore difficult to assess. With this contribution, we hope the community will acknowledge the limitations of prior approaches and use a CD‐IMM in future studies.
Keywords:compound‐specific stable isotope (CSSI)  isotope mixing model  isotopic tracer content  MixSIAR  sediment source apportionment
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