Vertically uniform formation pathways of tropospheric sulfate aerosols in East China detected from triple stable oxygen and radiogenic sulfur isotopes
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Abstract
Abstract Sulfate aerosols (SO 4 2− ) in the continental outflow from East China significantly alter the atmospheric sulfur budget across the Pacific Rim, but its formation pathways, especially in the free troposphere (FT), remain poorly understood. Here we analyze stable oxygen (δ 17 O and δ 18 O) and radiogenic sulfur ( 35 S) isotopes in SO 4 2− collected at a mountain site in East China to investigate SO 4 2− formation pathways at varying altitudes. We find that Δ 17 O (=δ 17 O‐0.52 × δ 18 O) in SO 4 2− is not correlated with 35 S (a direct measure of high‐altitude air masses). This pattern notably differs from the currently known 35 S‐Δ 17 O relation. The result implies that the formation pathway of tropospheric SO 4 2− in East China is vertically uniform, likely due to large emissions and active convection in this region. Our measurements provide unambiguous isotopic constraints for reducing uncertainties in modeling SO 4 2− in the FT over East China, which greatly affects regional climate but current models fail to accurately estimate.
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