Gas-particle partitioning of atmospheric aerosols: interplay of physical state, non-ideal mixing and morphology

Atmospheric aerosols, comprising organic compounds and inorganic salts, play a key role in air quality and climate. Mounting evidence exists that these particles frequently exhibit phase separation into predominantly organic and aqueous electrolyte-rich phases. As well, the presence of amorphous sem...

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Published inPhysical chemistry chemical physics : PCCP Vol. 15; no. 27; pp. 11441 - 11453
Main Authors SHIRAIWA, Manabu, ZUEND, Andreas, BERTRAM, Allan K, SEINFELD, John H
Format Journal Article
LanguageEnglish
Published Cambridge Royal Society of Chemistry 21.07.2013
Subjects
Aerosols
Aerosols - chemistry
Air quality
Atmosphere - chemistry
Atmospherics
Chemistry
Exact sciences and technology
Gases - chemistry
General and physical chemistry
Glassy
Molecular Structure
Morphology
Partitioning
Phase separation
Semi-solid processing
Climate
Growth
Ozone
Air quality
Solid particle
Laboratory
Equilibrium
Mass transfer
Particle
Ammonium sulfate
Electrolyte
Morphology
Phase separation
Pinene
Chemical composition
Models
Oxidation
Solid phase
Organic compounds
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Summary:Atmospheric aerosols, comprising organic compounds and inorganic salts, play a key role in air quality and climate. Mounting evidence exists that these particles frequently exhibit phase separation into predominantly organic and aqueous electrolyte-rich phases. As well, the presence of amorphous semi-solid or glassy particle phases has been established. Using the canonical system of ammonium sulfate mixed with organics from the ozone oxidation of α-pinene, we illustrate theoretically the interplay of physical state, non-ideality, and particle morphology affecting aerosol mass concentration and the characteristic timescale of gas-particle mass transfer. Phase separation can significantly affect overall particle mass and chemical composition. Semi-solid or glassy phases can kinetically inhibit the partitioning of semivolatile components and hygroscopic growth, in contrast to the traditional assumption that organic compounds exist in quasi-instantaneous gas-particle equilibrium. These effects have significant implications for the interpretation of laboratory data and the development of improved atmospheric air quality and climate models.
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ISSN:1463-9076
1463-9084
DOI:10.1039/c3cp51595h