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Fe–Mg diffusion in olivine I: experimental determination between 700 and 1,200°C as a function of composition, crystal orientation and oxygen fugacity

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Abstract

We have determined Fe–Mg diffusion coefficients in olivines from different sources (Nanga Parbat, Pakistan and San Carlos, Arizona, USA) at atmospheric pressure as a function of composition, oxygen fugacity (10−5–10−12 Pa) and temperature (700–1200°C) using thin films produced by pulsed laser deposition and RBS to analyze the concentration profiles. We have characterized the nano-scale structure and composition of the thin films annealed at various conditions and shown that the nature of the film (e.g. crystallinity, wetting behavior) depends strongly on the annealing conditions. If these variations are not taken into account in the form of boundary conditions for modeling the diffusion profiles, artifacts would result in the diffusion data. The diffusion coefficients obtained from 75 experiments reveal that (i) between fO2 of 10−5 and 10−10 Pa, diffusion along all three principal crystallographic directions in olivine, [100], [010] and [001], are described by a constant activation energy of ∼200 kJ/mol, precluding any temperature dependence of diffusion anisotropy and change of mechanism of diffusion at temperatures between 950 and 1200°C, (ii) diffusion coefficients increase with oxygen fugacity at fO2 > 10−10 Pa, with an fO2 exponent that lies between 1/4 and 1/7, and (iii) at fO2 below 10−10 Pa, and consequently at temperatures below ∼900°C, diffusion becomes weakly dependent/independent of fO2, indicating a change of diffusion mechanism. Activation energy of diffusion at these conditions is slightly higher, ∼220 kJ/mol. The data, including the change of mechanism, are analyzed in terms of point defect chemistry in Part II of this work to derive an equation that allows calculation of diffusivities in olivine over its entire field of stability. Availability of directly measured data at temperatures down to 700°C imply that for the first time diffusion coefficients can be interpolated, rather than extrapolated, for modeling most natural systems.

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Acknowledgments

Undergraduate students Julia Halfmann and Daniela Lüttgebüter have provided substantial help in the high temperature furnace laboratory as well as in the thin film deposition laboratory at different stages of this work. In addition, Julia Halfmann helped with white light interference microscopy. Their enthusiasm was contagious. The help of Dr. Rolf Neuser at the SEM and Dr. Hans-Jürgen Bernhardt at the microprobe laboratory were indispensable. Dr. W. Gebert oriented some of the olivine crystals for us. None of the experiments would be possible without the efforts of Tanya Westphal at the polishing lab. The German Science Foundation (DFG) generously sustained this project through material support and by covering the entire salary of the first author. This support was obtained in part within the interdisciplinary program SFB 526 (Rheology of the Earth). We gratefully acknowledge the help from all of these individuals and organizations. Finally, we thank Daniele Cherniak and Bill Carlson for their constructive reviews which helped to revise the manuscript.

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Authors and Affiliations

  1. Institut für Geologie, Mineralogie und Geophysik, Ruhr-Universität Bochum, 44780, Bochum, Germany

    Ralf Dohmen & Sumit Chakraborty

  2. Institut für Physik mit Ionenstrahlen, Ruhr-Universität Bochum, 44780, Bochum, Germany

    Hans-Werner Becker

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  1. Ralf Dohmen
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  2. Hans-Werner Becker
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Correspondence to Ralf Dohmen.

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Dohmen, R., Becker, HW. & Chakraborty, S. Fe–Mg diffusion in olivine I: experimental determination between 700 and 1,200°C as a function of composition, crystal orientation and oxygen fugacity. Phys Chem Minerals 34, 389–407 (2007). https://doi.org/10.1007/s00269-007-0157-7

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