The legacy of crystal-plastic deformation in olivine: high-diffusivity pathways during serpentinization

Crystal-plastic olivine deformation to produce subgrain boundaries composed of edge dislocations is an inevitable consequence of asthenospheric mantle flow. Although crystal-plastic deformation and serpentinization are spatio-temporally decoupled, we identified compositional readjustments expressed on the micrometric level as a striped Fe-enriched ((X) over bar (Fe) = 0.24 +/- 0.02 (zones); 0.12 +/- 0.02 (bulk)) or Fe-depleted ((X) over bar Fe = 0.10 +/- 0.01 (zones); 0.13 +/- 0.01 (bulk)) zoning in partly serpentinized olivine grains from two upper mantle sections in Norway. Focused ion beam sample preparation combined with transmission electron microscopy (TEM) and aberration-corrected scanning TEM, enabling atomic-level resolved electron energy-loss spectroscopic line profiling, reveals that every zone is immediately associated with a subgrain boundary. We infer that the zonings are a result of the environmental Fe2+Mg-1 exchange potential during antigorite serpentinization of olivine and the drive toward element exchange equilibrium. This is facilitated by enhanced solid-state diffusion along subgrain boundaries in a system, which otherwise re-equilibrates via dissolution-reprecipitation. Fe enrichment or depletion is controlled by the silica activity imposed on the system by the local olivine/orthopyroxene mass ratio, temperature and the effect of magnetite stability. The Fe-Mg exchange coefficients K-D(Atg/Ol) between both types of zoning and antigorite display coalescence toward exchange equilibrium. With both types of zoning, Mn is enriched and Ni depleted compared with the unaffected bulk composition. Nanometer-sized, heterogeneously distributed antigorite precipitates along olivine subgrain boundaries suggest that water was able to ingress along them. Crystallographic orientation relationships gained via electron backscatter diffraction between olivine grain domains and different serpentine vein generations support the hypothesis that serpentinization was initiated along olivine subgrain boundaries.