Spherules can be formed by high-temperature processes during volcanic eruptions, lightning strikes and meteorite impacts. Here we report four different types of spherules and spheroidal particles associated with tephra deposits from two separate volcanic fields in the southern Payenia province of Argentina. These silicate and carbonate spherules represent <0.01% of the sampled material, with individual spherules <200 µm in size. Thirty particles were imaged. Only the transparent spherules are smooth, perfect spheres; other morphologies include ellipsoids and aggregated dumbbells. The spheroids are either hollow or solid. Major element analyses show that the spherules and spheroids have silica-rich, Fe-rich, carbonate and basaltic compositions. Chemical analysis of the carbonate spheroids shows some variability in the trace element content between the cores and rims, suggesting element mobility and loss towards the margins. All the analysed carbonate spheroids have elevated Sr/Y, La/Y and La/Ce ratios outside the range for sedimentary carbonates. All four spherule types are considered to be volcanic in origin, with the excess CO2 required for the formation of the carbonate spherules potentially sourced from the basement lithologies. Based on the major and trace element analyses, we conclude that the silica-rich and carbonate spherules formed by instantaneous condensation from supercritical CO2-rich hydrous fluids saturated with dissolved silicates.

Supplementary material: Appendix A, containing the full analytical dataset collected by electron probe microanalysis and secondary ion mass spectrometry, is available at https://doi.org/10.6084/m9.figshare.c.5108689

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