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Rethinking Organic Aerosols: Semivolatile Emissions and Photochemical Aging

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TLDR
Accounting for partitioning and photochemical processing of primary emissions creates a more regionally distributed aerosol and brings model predictions into better agreement with observations, attribute this unexplained secondary organic-aerosol production to the oxidation of low-volatility gas-phase species.
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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Citations
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Journal ArticleDOI

Bounding the role of black carbon in the climate system: A scientific assessment

TL;DR: In this paper, the authors provided an assessment of black-carbon climate forcing that is comprehensive in its inclusion of all known and relevant processes and that is quantitative in providing best estimates and uncertainties of the main forcing terms: direct solar absorption; influence on liquid, mixed phase, and ice clouds; and deposition on snow and ice.
Journal ArticleDOI

Evolution of Organic Aerosols in the Atmosphere

Jose L. Jimenez, +66 more
- 11 Dec 2009 - 
TL;DR: A unifying model framework describing the atmospheric evolution of OA that is constrained by high–time-resolution measurements of its composition, volatility, and oxidation state is presented, which can serve as a basis for improving parameterizations in regional and global models.
References
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Journal ArticleDOI

Organic aerosol and global climate modelling: a review

TL;DR: In this article, the authors reviewed existing knowledge with regard to organic aerosol (OA) of importance for global climate modelling and defined critical gaps needed to reduce the involved uncertainties, and synthesized the information to provide a continuous analysis of the flow from the emitted material to the atmosphere up to the point of the climate impact of the produced organic aerosols.
Journal ArticleDOI

Gas/Particle Partitioning and Secondary Organic Aerosol Yields

TL;DR: In this paper, Pankow expressions for the fractional SOA yield (Y) were developed within this framework and shown to be a function of the organic aerosol mass concentration, M_o.
Journal ArticleDOI

Source apportionment of airborne particulate matter using organic compounds as tracers

TL;DR: In this paper, a chemical mass balance receptor model based on organic compounds was developed that relates sours; contributions to airborne fine particle mass concentrations and revealed source contributions to the concentrations of specific organic compounds.
Journal ArticleDOI

Coupled partitioning, dilution, and chemical aging of semivolatile organics.

TL;DR: The time evolution strongly suggests that neglected oxidation of numerous "intermediate volatility" vapors (IVOCs, with saturation concentrations above approximately 1 mg m(-3)) may contribute significantly to ambient SOA formation.
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Evolution of Organic Aerosols in the Atmosphere

Jose L. Jimenez, +66 more
- 11 Dec 2009 -