From Criegee-Intermediates to particle size distributions. Precursor chemistry and aggregation kinetics of sulfuric acid containing clusters in experiment and simulation

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The reaction of Criegee intermediates or carbonyl oxides with sulphur dioxide forming sulphur trioxide and a carbonyl compound is an important atmospheric source of sulphuric acid. Criegee intermediates are produced during alkene ozonolysis by the decomposition of the primary ozonide. The approach followed in this project may allow the detection of in principle all Criegee intermediates in the gas-phase by infrared spectroscopy in time resolved experiments with high reactant concentrations. Alternative methods have been so far restricted to low pressure and small species. In the framework of our studies the kinetic data shall be provided, which are needed to assess the atmospheric influence of the Criegee reaction wit sulphur dioxide. The 2-butene ozonolysis in the presence of sulphur dioxide allows producing high sulphuric acid concentrations in a kinetically controlled experiment. This property we will exploit to study the dynamics of sulphuric acid induced new particle formation.