Systematic changes in serpentine Si isotope signatures across the Mariana forearc – a new proxy for slab dehydration processes

Highlights • Si was measured with micrometer resolution in mantle wedge serpentinites. • Serpentine Si varies depending on w/r ratios and Si of interacting fluids. • Si in veins formed under high w/r ratios mirror that of subducted sediments. • Across-forearc changes in Si fingerprint prograde slab dehydration reactions. • Si isotopes provide a new tool for tracing slab dehydration processes. Abstract The Mariana forearc is a unique location for exploring the role serpentinization plays in the marine Si cycle by means of Si stable isotope variations. Here, active mud volcanism transports deep, serpentinized mantle wedge material to the surface and thus offers a natural window to slab dehydration processes in dependence of changing temperature and pressure with depth. Si isotopes were measured in situ by femtosecond laser ablation MC-ICPMS in serpentine within ultramafic clasts from three mud volcanoes (Yinazao, Fantangisña, and Asùt Tesoru) sampled during International Ocean Discovery Program Expedition 366. To corroborate the results, serpentinization of olivine was studied in batch experiments. The Si isotope ratios show large variations between the mud volcanoes and between individual serpentine generations within a given mud volcano. Serpentine that formed early under low water/rock ratios exhibits Si of −0.41 ± 0.04‰ (1SD) similar to unaltered olivine which agrees well with experimental findings predicting no significant isotope fractionation during early serpentinization. In contrast, late serpentine veins formed under higher water/rock ratios span a wide range of Si isotope ratios that differ significantly between the individual mud volcanoes. With increasing distance to the trench, Si of late veins are −0.10 ± 0.07‰, −1.94 ± 0.13‰, and −0.80 ± 0.22‰ and −0.93 ± 0.21‰. These Si values are interpreted to record the isotopic composition of the fluid source, namely subducted biogenic silica and pore fluids, clays, and altered oceanic crust that dehydrate as consequence of rising pressure and temperature with depth. We show that Si isotopes of mantle wedge serpentinites can be used as a reliable new proxy for slab dehydration processes. They may be used in paleo-forearc systems to unravel oceanic sediment and silica biomineralization evolution through geological time