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Isotope fractionation in silicate melts by thermal diffusion

Nature volume 464, pages 396–400 (2010)Cite this article

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Abstract

The phenomenon of thermal diffusion (mass diffusion driven by a temperature gradient, known as the Ludwig–Soret effect1,2) has been investigated for over 150 years, but an understanding of its underlying physical basis remains elusive. A significant hurdle in studying thermal diffusion has been the difficulty of characterizing it. Extensive experiments over the past century have established that the Soret coefficient, ST (a single parameter that describes the steady-state result of thermal diffusion), is highly sensitive to many factors3,4,5,6,7,8,9. This sensitivity makes it very difficult to obtain a robust characterization of thermal diffusion, even for a single material. Here we show that for thermal diffusion experiments that span a wide range in composition and temperature, the difference in ST between isotopes of diffusing elements that are network modifiers (iron, calcium and magnesium) is independent of the composition and temperature. On the basis of this finding, we propose an additive decomposition for the functional form of ST and argue that a theoretical approach based on local thermodynamic equilibrium3,5,10 holds promise for describing thermal diffusion in silicate melts and other complex solutions. Our results lead to a simple and robust framework for characterizing isotope fractionation by thermal diffusion in natural and synthetic systems.

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Figure 1: Thermal-diffusion isotopic sensitivity and concentration steady state of time-series experiments (ZM70 and ZM71)6.
Figure 2: Cross-correlations of magnesium, iron and calcium isotope ratios for both the thermal diffusion experiments of refs 6, 16 and previous work.
Figure 3: Distribution of isotope concentrations and isotope ratios against Δ T for thermal diffusion experiments with a wide range of melt compositions and bulk temperatures.

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Acknowledgements

This work is supported by US National Science Foundation grants NSF EAR 0609726 and NSF EAR 0944169 (C.C.L.), and NSF EAR 0943991 (C.E.L.). The multi-collector inductively-coupled-plasma mass spectrometry laboratory at the University of Illinois at Urbana-Champaign is supported by NSF EAR 0732481. P.C. acknowledges support from a Roscoe G. Jackson II Research Fellowship. P.C. and S.W.K. acknowledge support from S.W.K.’s Walgreen Chair funds. We thank B. Fouke for use of his micro-drilling system, Z. Zhang and X. Li for analytical assistance, V. Kariwala for help with references and Y. Zhang for a review of this work.

Author Contributions F.H. led the analytical effort and P.C. led the theoretical treatment of the results. C.E.L. performed the laboratory thermal diffusion experiments. J.J.G.G. assisted with iron and magnesium isotope analyses and C.H. measured calcium isotopes. P.C. and F.H. wrote the manuscript and Supplementary Information with contributions from C.C.L., C.H., S.W.K., J.J.G.G. and C.E.L.

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Author notes

  1. F. Huang

    Present address: Present address: Institute of Geochemistry and Petrology, ETH Zurich, CH-8092 Zurich, Switzerland.,

  2. F. Huang and P. Chakraborty: These authors contributed equally to this work.

Authors and Affiliations

  1. Department of Geology, University of Illinois, Urbana, Illinois 61801, USA,

    F. Huang, P. Chakraborty, C. C. Lundstrom, J. J. G. Glessner & S. W. Kieffer

  2. Department of Geological Sciences, University of Saskatchewan, Saskatoon, Saskatchewan S7N 5E2, Canada,

    C. Holmden

  3. Department of Geology, University of California, Davis, California 95616, USA,

    C. E. Lesher

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  1. F. Huang
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Correspondence to C. C. Lundstrom.

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Huang, F., Chakraborty, P., Lundstrom, C. et al. Isotope fractionation in silicate melts by thermal diffusion. Nature 464, 396–400 (2010). https://doi.org/10.1038/nature08840

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