Strontium and oxygen isotope decoupling in the Hercynian Trois Seigneurs Massif,Pyrenees: evidence for fluid circulation in a brittle regime

Systematic shifts of oxygen isotopic compositions in the higher grade parts of the high temperature-low pressure Hercynian metamorphic sequence, exposed in the Trois Seigneurs Massif, have previously been explained as a result of an influx of surface-derived water during the prograde part of the metamorphic cycle. It has been suggested that this caused a regional lowering of ⁸⁷Sr/⁸⁶Sr in the metamorphic sequence. Mapping of strontium isotopic compositions across a 15 m meta-carbonate horizon in the higher grade pelite-psammite sequence shows that strontium isotopic compositions were homogenised over length scales of metres or less during the Hercynian metamorphism, which brought the carbonate and pelite-psammite to oxygen isotopic equilibrium with a common fluid. Comparison of model pre-Hercynian ⁸⁷Sr/⁸⁶Sr profiles across the carbonate (based on a depositional/diagenetic age of 450 Ma and initial ⁸⁷Sr/⁸⁶Sr ratio of 0.7086 given by 10 m length scale averaging) with the post-Hercynian ⁸⁷Sr/⁸⁶Sr profile (calculated from analysed ⁸⁷Sr/⁸⁶Sr and Rb/Sr compositions) implies strontium isotopic diffusion distances of ca. 0.4 m in the carbonate and ca. 7 m in the pelite-psammite. The limited Sr-isotopic diffusion distance of 0.4–0.7 m within the carbonate is compatible with pervasive oxygen-isotopic exchange over distances restricted to 4–15 m if fluid strontium concentrations were between 4 and 50 ppm. The strontium isotopic transport distances are not compatible with pervasive oxygen isotopic alteration over the observed 5 km regional scale. Either the flow was perfectly layer-parallel or, more probably, the regional-scale alteration of oxygen took place by fluid circulation in the brittle regime early in, or prior to, the Hercynian metamorphic event. Flow along cracks with incomplete diffusive exchange between fluid and wall rock would allow greater decoupling of oxygen and strontium isotopic transport than pervasive advective transport with local fluid-solid equilibrium.