The isotope effect for Mg-Fe interdiffusion in olivine and its dependence on crystal orientation, composition and temperature

Sio, Corliss K.; Roskosz, Mathieu; Dauphas, Nicolas; Bennett, Neil R.; Mock, Timothy; Shahar, Anat
2018
GEOCHIMICA ET COSMOCHIMICA ACTA
DOI
10.1016/j.gca.2018.06.024
Isotopic fractionation associated with diffusion in crystals is the most reliable means of understanding the origin of mineral zoning in igneous and metamorphic rocks. We have experimentally determined the relative diffusivities of iron isotopes in olivine as a function of crystallographic orientation, composition, and temperature. For two isotopes i and j of an element, the isotope effect for diffusion is parameterized as D-i/D-j = (m(j)/m(i))(beta), where beta is a dimensionless parameter, and D and m stand for diffusivity and mass, respectively. A series of single crystal diffusion couple experiments were conducted at an oxygen fugacity of QFM - 1.5 at temperatures of 1200, 1300, and 1400 degrees C. For the Fo(83.4)-Fo(88.8) composition pair, beta(Fe) is isotropic and a value of 0.16 +/- 0.09 can be used to describe diffusion along all major crystallographic axes in olivine. Based on our experiments and previously reported coupled Mg-Fe isotopic data, we also estimate beta(Mg) = 0.09 +/- 0.05 for this range of olivine composition. For the Fo(88.8)-Fo(100) composition pair, beta(Fe) becomes anisotropic with beta(Fe [100]) = 0.11 +/- 0.03, beta(Fe [010]) = 0.14 +/- 0.03 (both within error of the value measured for the Fo(83.4)-Fo(88.8) pair), and beta(Fe [001]) = 0.03 +/- 0.03. For Fo# between 83.4 and 100, beta(Fe [100]) and beta(Fe [010]) are thus independent of composition. The reason why beta(Fe) ([001]) transitions from similar to 0.16 to similar to 0.03 close to the Mg-endmember is unclear. Over the temperature range studied, a dependence of beta(Fe) on temperature was not resolved. General analytical expressions are introduced to calculate isotopic fractionation as a function of distance, time, beta, and the concentration contrast between the diffusing media for spherical, cylindrical, and planar geometries. (C) 2018 Elsevier Ltd. All rights reserved.