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

By N. Donahue, A. Robinson, C. Stanier, Spyros N. Pandis. Environmental Science and Technology, 2006

1,456 citations recorded by the source corpus.

A unified framework of semi-volatile partitioning permits models to efficiently treat both semi-volatile primary emissions and secondary organic aerosol production (SOA), and then to treat the chemical evolution (aging) of the aggregate distribution of semi-volatile material. This framework also reveals critical deficiencies in current emissions and SOA formation measurements. The key feature of this treatment is a uniform basis set of saturation vapor pressures spanning the range of ambient organic saturation concentrations, from effectively nonvolatile material at 0.01 microg m(-3) to vapor-phase effluents at 100 mg m(-3). Chemical evolution can be treated by a transformation matrix coupling the various basis vectors. Using this framework, we show that semi-volatile partitioning can be described in a self-consistent way, with realistic behavior with respect to temperature and varying organic aerosol loading. 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.

Subfields: Atmospheric Science, Health, Toxicology and Mutagenesis, Materials Chemistry

View Paper: https://www.semanticscholar.org/paper/4270545cc2c077685b0622b357a1d2dca106545f

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Citations in the corpus

Online coupled regional meteorology chemistry models in Europe: current status and prospects (2013, methodology): “The VBS approach (Donahue et al., 2006) is also an empirical approach, but it differs from the previous one by its definition of surrogate SOA compounds, which also allows the treatment of additional processes such as chemical aging and semi-volatile POA (Donahue et al., 2006).”
A two-dimensional volatility basis set: 1. organic-aerosol mixing thermodynamics (2010, methodology): “Likewise, in the VBS modeling framework (Donahue et al., 2006), we use log10C ∗ explicitly and are thusnot directly sensitive to uncertainties in volatility.”
Microbiology and atmospheric processes: chemical interactions of primary biological aerosols (2008, neutral): “The characterisation, classification, and description of the OC in atmospheric models is a major challenge of current atmospheric and climate research (Kanakidou et al., 2005; Fuzzi et al., 2006; Kalberer et al., 2006; Donahue et al., 2006).”
Impact of organic molecular structure on the estimation of atmospherically relevant physicochemical parameters (2021, background): “…between phases and may vary in their fates, such as the following: semivolatile compounds that partition between the gas and particle phase (Donahue et al., 2006); compounds with moderate reactivity that may last hours or days, depending on oxidant concentrations (Price et al., 2019); or…”
Understanding atmospheric organic aerosols via factor analysis of aerosol mass spectrometry: a review (2011, background): “Furthermore, the composition and properties of both POA and SOA may change dynamically throughout aerosol lifetime, because of intertwined processes including emission, oxidation, fragmentation, oligomerization, gas-to-particle partitioning, and cloud processing [12–18].”
Evolution of organic aerosol mass spectra upon heating: implications for OA phase and partitioning behavior (2010, methodology): “Within the framework of traditional absorptive partitioning theory (Donahue et al., 2006;Odum et al., 1996;Pankow, 1994), OA volatility should be describable from the physical properties and relative abundances of the individual compounds comprising the aerosol.”
Modeling global secondary organic aerosol formation and processing with the volatility basis set: Implications for anthropogenic secondary organic aerosol (2010, methodology): “[15] To describe efficiently the partitioning behavior of SOA, we have used the volatility basis set framework [Donahue et al., 2006].”
A naming convention for atmospheric organic aerosol (2013, methodology): “Donahue et al. (2009) recommended separating species by volatility in line with the VBS framework.”
Aerosol cloud precipitation interactions. Part 1. The nature and sources of cloud-active aerosols (2008, background): “Recently, a conceptual model has been proposed that involves dynamic and bidirectional exchange of semivolatile organic compounds between the gas and condensed phases, allowing for oxidation reactions in both phases (Donahue et al., 2006; Robinson et al., 2007).”
Predicting the glass transition temperature and viscosity of secondary organic material using molecular composition (2017, background): “(1) can be applied in the 232 volatility basis set (VBS) (Donahue et al., 2006; Donahue et al., 2011) and the molecular 233 corridor approach (Shiraiwa et al., 2014; Li et al., 2016) to predict the Tg of SOA particles 234 (Shiraiwa et al., 2017), while the new parameterization may be suitable for co”