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Abstract The nearly continuous volcanic eruption record at Mt. Etna dating back ~700 years provides an excellent opportunity to investigate the geochemical evolution of a highly active volcano. Of particular interest is elucidating the cause of selective enrichment in alkali elements (K and Rb) and 87Sr/86Sr observed in various episodes of past activity. More recently, this alkali enrichment trend started to manifest in the 17th century and accelerated after 1971, and was accompanied by an increase in the volume, frequency, and explosivity of eruptions. Explanations for this signature include recharge of alkali-enriched magmas and/or crustal contamination from the subvolcanic basement. This study quantitatively examines the role of crustal contamination in post-1971 Etnean magma compositions via hundreds of open-system phase equilibria and trace element calculations based upon whole-rock major oxides, trace elements, 87Sr/86Sr ratios, and mineral compositional data. Available pre-1971 petrochemical data are satisfactorily reproduced by fractional crystallization of a high whole-rock MgO (12–17 wt.%), Ni (135–285 ppm), and Cr (920–1330 ppm) parental magma composition that is documented in Etna's ~4-ka fall-stratified deposit. Observed post-1971 whole-rock and glass trends and phase equilibria are reproduced via modeled assimilation of a skarn and flysch mixture, lithologies that represent the uppermost 10 to 15 km of sedimentary rocks beneath Etna. Notably, models show that K2O (wt.%) and Rb (ppm) behave incompatibly during partial melting of skarn/flysch. Additionally, the observed elevation of 87Sr/86Sr in post-1971 samples is consistent with the addition of radiogenic Sr from wallrock partial melts. In best-fit models, which yield observed post-1971 K2O, Rb, and 87Sr/86Sr trends, ~17% anatectic melt is assimilated and there may be a subordinate stoped wallrock component of ≤2% (percentage is relative to the starting mass of pristine magma). Previous work has shown that metasomatized spinel lherzolite and garnet pyroxenite can be melted in different proportions to reproduce long- and short-term changes observed in Etna’s geochemical products. We propose that the alkali enrichment signature observed after 1971 can be fully explained through the combination of mantle heterogeneity and crustal contamination. In particular, up to ~20% crustal input coupled with mantle heterogeneity of primitive melts explains the geochemical signals quite well. The influence of crustal contamination on post-1971 lavas is, in part, the result of frequent recharge of magmas that thermally primed the middle to upper crust and enhanced its partial melting. 

Several times in the past 60 ka, Mount Etna has erupted lavas with variable alkaline character. The most recent chemical excursion began in 1971, accompanied by an increase in explosivity and eruption frequency. The origin of the alkaline signature remains enigmatic, with endmember hypotheses involving dominant contributions from mantle vs. crust. For lavas that erupted between 1329 and 2016, we used thermodynamic modeling to test if post-1971 anomalous alkalinity is dominated by mantle processes. First, we assessed mantle melting conditions required to reproduce the chemistry of potential parental magmas. Second, we examined the differentiation of partial melts as they underwent closed-system crustal storage and ascent. The mantle melting conditions explored via ~300 models include source compositions (peridotite + pyroxenite ± metasomatic phases), pressure, extent of melting, and fO2. Best-fit models that reproduce the major element chemistry of volcanics interpreted as parental magmas involve 20 to 30% melting of a peridotite-pyroxenite mantle source that contained phlogopite, pargasite, and CO2 (~1 wt.%) between ~1-1.5 GPa (~30-45 km) along the QFM+1 buffer. Subsequent isentropic decompression (adiabatic and reversible) of mantle partial melts + crystallization at shallower pressures (0.8-0.2 GPa) were modeled to test the effects of closed system ascent and storage. Isentropic decompression models yield no crystallization although temperature decreases ~3°C/0.1 GPa. Decompression + closed system crystallization fail to replicate post-1971 glass samples and do not explain observed post-1971 alkali enrichments. We conclude that partial melting of a metasomatized source produced Etna parental magmas, but closed system crustal ascent and storage cannot fully account for alkali enrichment highlighted in post-1971 products at Etna. Open system modeling suggests that assimilation and crystallization (e.g., Takach et al. 2024) play a critical role, and ongoing modeling is testing the contributions of recharge (magma replenishment) and entrainment of previously formed mushes to the high alkalinity excursions.