Tracing the orogenic sulfur cycle in the Andes using stable isotope composition of dissolved sulfate in thermal springs

Abstract

The cycling of sulfur (S) to the upper crust and surface via thermal springs at convergent margins has not been explored outside areas with active arc volcanism, even though subduction plays a key role in the Earth's long-term S cycle. To address this knowledge gap, we analyzed stable sulfur and oxygen isotope compositions (δ³⁴S and δ¹⁸O values) of dissolved sulfate (SO₄²⁻) in 55 thermal springs from five distinct settings in the Andean orogen. These regions are the Peruvian flat slab and backarc, transition between these two, Argentinian backarc, and Chilean forearc. Although the flat-slab settings had lower SO₄²⁻ concentrations (<2000 mg/L) compared to the steep-slab settings (<12,700 mg/L), there was no significant relationship between isotope composition of SO₄²⁻ and slab geometry. The δ³⁴S and δ¹⁸O values of SO₄²⁻ varied widely across the studied areas (+0.2 to +23.5 ‰ and − 3.3 to +16.0 ‰, respectively) and reflected the isotope compositions of local bedrock endmembers from dissolution of marine evaporites (+5 to +25 ‰ and + 10 to +20 ‰, respectively) and oxidation of magmatic and/or hydrothermal S and ore sulfide minerals with variable δ³⁴S (0 to +16 ‰). The δ¹⁸O and δ²H values of thermal spring water (−18.5 to −3.3 ‰ and − 141.1 to −23.7 ‰, respectively) were consistent with meteoric precipitation, and in most cases decreased with increasing altitude following precipitation in the Andes. Generally, our isotope results do not support the direct transfer of slab-derived S/SO₄²⁻ to thermal springs in the investigated settings. Rather, the δ³⁴S and δ¹⁸O of SO₄²⁻ in the thermal springs are a sensitive indicator of local water-rock interactions that remobilize bedrock S originating from a complex orogenic cycle reflecting tectonic uplift, erosion, weathering, and exhumation history across the duration of Andean Mountain building.