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ReportsRethinking Organic Aerosols: Semivolatile Emissions and Photochemical Aging
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.
1 Center for Atmospheric Particle Studies, Carnegie Mellon University, Pittsburgh, PA 15213, USA.
2 Department of Chemical Engineering, University of Patras, Patra 26500, Greece. * To whom correspondence should be addressed. E-mail: alr{at}andrew.cmu.edu (A.L.R.); nmd{at}andrew.cmu.edu (N.M.D.)
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Science. ISSN 0036-8075 (print), 1095-9203 (online)