Rethinking organic aerosols: semivolatile emissions and photochemical aging |
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Authors: | Robinson Allen L Donahue Neil M Shrivastava Manish K Weitkamp Emily A Sage Amy M Grieshop Andrew P Lane Timothy E Pierce Jeffrey R Pandis Spyros N |
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Institution: | Center for Atmospheric Particle Studies, Carnegie Mellon University, Pittsburgh, PA 15213, USA. alr@andrew.cmu.edu |
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Abstract: | Most primary organic-particulate emissions are semivolatile; thus, they partially evaporate with atmospheric dilution, creating substantial amounts of low-volatility gas-phase material. Laboratory experiments show that photo-oxidation of diesel emissions rapidly generates organic aerosol, greatly exceeding the contribution from known secondary organic-aerosol precursors. We attribute this unexplained secondary organic-aerosol production to the oxidation of low-volatility gas-phase species. Accounting for partitioning and photochemical processing of primary emissions creates a more regionally distributed aerosol and brings model predictions into better agreement with observations. Controlling organic particulate-matter concentrations will require substantial changes in the approaches that are currently used to measure and regulate emissions. |
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