Atmospheric sulfur isotopic anomalies recorded at Mt. Everest across the Anthropocene

Increased anthropogenic-induced aerosol concentrations over the Himalayas and Tibetan Plateau have affected regional climate, accelerated snow/glacier melting, and influenced water supply and quality in Asia. Although sulfate is a predominant chemical component in aerosols and the hydrosphere, the contributions from different sources remain contentious. Here, we report multiple sulfur isotope composition of sedimentary sulfates from a remote freshwater alpine lake near Mount Everest to reconstruct a two-century record of the atmospheric sulfur cycle. The sulfur isotopic anomaly is utilized as a probe for sulfur source apportionment and chemical transformation history. The nineteenthcentury record displays a distinct sulfur isotopic signature compared with the twentieth-century record when sulfate concentrations increased. Along with other elemental measurements, the isotopic proxy suggests that the increased trend of sulfate is mainly attributed to enhancements of dust-associated sulfate aerosols and climate-induced weathering/erosion, which overprinted sulfur isotopic anomalies originating from other sources (e.g., sulfates produced in the stratosphere by photolytic oxidation processes and/or emitted from combustion) as observed in most modern tropospheric aerosols. The changes in sulfur cycling reported in this study have implications for better quantification of radiative forcing and snow/glacier melting at this climatically sensitive region and potentially other temperate glacial hydrological systems. Additionally, the unique Delta S-33-delta S-34 pattern in the nineteenth century, a period with extensive global biomass burning, is similar to the Paleoarchean (3.6-3.2 Ga) barite record, potentially providing a deeper insight into sulfur photochemical/thermal reactions and possible volcanic influences on the Earth's earliest sulfur cycle.