Atmospheric sulfur cycle elucidated by isotopologue measurements
The formation of atmospheric sulfate(SO42-)aerosols plays an important role in the atmospheric sulfur cycle.However,the mechanisms of chemical formation of SO42-are still elusive.The stable isotope signal of SO42-is an effective method to trace its source and to investigate the mechanisms of atmospheric oxidation reactions.We have developed a novel isotopic analysis method for samples such as ice cores and atmospheric aerosols.We combined this method with experimental data and a three-dimensional atmospheric chemical transport model that contains isotopic information to elucidate the atmospheric sulfur cycle.Particularly,the mass-independent fractionation(MIF)signal of oxygen isotopes(Δ17O)in SO42-provides insight into the source of oxygen during sulfate aerosol formations.In this work,we presented the details of how triple oxygen and quadruple sulfur isotopes can be used to analyze the formation and evolution of atmospheric sulfate aerosols.In addition,we discussed several other examples of isotopic determination to understand the atmospheric sulfur cycle and propose directions for future research.