Proceedings of the National Academy of Sciences · 2014 · 565 citations · 24 references
Natural SciencesChemistryEnvironmental SciencesAtmospheric ChemistryAtmospheric ScienceEnvironmental ChemistryAerosol ChemistryAerosol ScienceAir QualityParticulate MatterSecondary Aerosol FormationSecondary Organic AerosolsAerosol ModelingAtmospheric Particulate Matter ChemistryCoupled Climate ModelsLaboratory Chamber StudiesOrganic AerosolsSecondary Aerosol Formation ModelingSecondary Organic Aerosol FormationWall Loss Effects
Secondary organic aerosol (SOA) constitutes a major fraction of submicrometer atmospheric particulate matter. Quantitative simulation of SOA within air-quality and climate models--and its resulting impacts--depends on the translation of SOA formation observed in laboratory chambers into robust parameterizations. Worldwide data have been accumulating indicating that model predictions of SOA are substantially lower than ambient observations. Although possible explanations for this mismatch have been advanced, none has addressed the laboratory chamber data themselves. Losses of particles to the walls of chambers are routinely accounted for, but there has been little evaluation of the effects on SOA formation of losses of semivolatile vapors to chamber walls. Here, we experimentally demonstrate that such vapor losses can lead to substantially underestimated SOA formation, by factors as much as 4. Accounting for such losses has the clear potential to bring model predictions and observations of organic aerosol levels into much closer agreement.
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