Barium isotope behavior during interaction between serpentinite-derived fluids and metamorphic rocks in the continental subduction zone

Serpentinites in subduction zones are important fluid reservoirs for crust-mantle interaction and arc magma formation. The serpentinite-derived fluids can carry fluid-mobile elements such as Ba and potentially affect the geochemical composition of the metamorphic rocks in the subduction zones. However, the Ba isotope behavior during interaction between serpentinite-derived fluids and metamorphic rocks is still poorly understood. The whiteschists of the Dora-Maira Massif in the Western Alps have experienced fluid infiltration by serpentinite-derived fluids during deep subduction. Here we report the Ba isotope data of the whiteschist and its protolith metagranite to investigate the Ba isotope behavior during fluid-rock interaction. The metagranites, which have experienced ultrahigh-pressure metamorphism, have a small variation of δ138Ba (−0.25 to 0.26‰), while the whiteschists display a large Ba isotope variation from −0.99‰ to 0.48‰. Such a large variation in whiteschists cannot be explained by chemical weathering, protolith heterogeneity, or kinetic effects. Instead, considering the negative correlations of δ138Ba with Ba and other fluid-mobile elements (e.g., Sr, Cs, Zn, and Cu) and the geochemical composition features of serpentinite-derived fluids, the large Ba isotope variation in whiteschists is inferred to be induced by the interaction between serpentinite-derived fluid and metagranite during intense fluid infiltration. This is consistent with the observation that the whiteschists with low Ba contents tend to exhibit heavier Mg-Fe isotope compositions but lighter Li isotope compositions, which indicates that the related fluids were derived from the dehydration of mantle wedge serpentinite. The fluid infiltrating process is well explained by a numerical model with high fluid-rock ratios of 4 to 12. Our modeling further suggests that serpentinite-derived fluid has a distinctly higher δ138Ba value than the depleted upper mantle. During fluid-rock interaction, heavy Ba isotopes prefer to be infiltrated into fluids with an apparent fractionation factor (Δ138Barock-fluid) of mostly −0.5‰ to −0.1‰ but can be down to −0.8‰ to −0.7‰ required for a few samples. A two-stage dehydration and metasomatism model at different depths can well explain the formation of Dora-Maira whiteschists. Whereas the Ba isotope composition of mantle wedge serpentinite is mainly dictated by crust-derived fluids from the subducting slab, an interaction between the serpentinite-derived fluids and the metagranite protolith resulted in a large Ba isotope variation of whiteschists. In case of a general involvement of serpentinites in subduction zones, serpentinite-derived fluids would significantly affect the Ba isotope compositions of subarc mantle peridotites and also arc lavas.