Open Access
On the Evaporation Kinetics and Phase of Laboratory and Ambient Secondary Organic Aerosol
A. Zelenyuk,T. Vaden,Dan Imre,Josef Beranek,M. Shrivastava +4 more
- Vol. 2010
TLDR
It is found that even when gas phase organics are removed, it takes ∼24 h for pure α-pinene SOA particles to evaporate 75% of their mass, which is in sharp contrast to the ∼10 min time scale predicted by current kinetic models.Abstract:
Field measurements of secondary organic aerosol (SOA) find significantly higher mass loads than predicted by models, sparking intense effort focused on finding additional SOA sources but leaving the fundamental assumptions used by models unchallenged. Current air-quality models use absorptive partitioning theory assuming SOA particles are liquid droplets, forming instantaneous reversible equilibrium with gas phase. Further, they ignore the effects of adsorption of spectator organic species during SOA formation on SOA properties and fate. Using accurate and highly sensitive experimental approach for studying evaporation kinetics of size-selected single SOA particles, we characterized room-temperature evaporation kinetics of laboratory-generated α-pinene SOA and ambient atmospheric SOA. We found that even when gas phase organics are removed, it takes ∼24 h for pure α-pinene SOA particles to evaporate 75% of their mass, which is in sharp contrast to the ∼10 min time scale predicted by current kinetic models. Adsorption of “spectator” organic vapors during SOA formation, and aging of these coated SOA particles, dramatically reduced the evaporation rate, and in some cases nearly stopped it. Ambient SOA was found to exhibit evaporation behavior very similar to that of laboratory-generated coated and aged SOA. For all cases studied in this work, SOA evaporation behavior is nearly size-independent and does not follow the evaporation kinetics of liquid droplets, in sharp contrast with model assumptions. The findings about SOA phase, evaporation rates, and the importance of spectator gases and aging all indicate that there is need to reformulate the way SOA formation and evaporation are treated by models.read more
Citations
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Journal ArticleDOI
A large source of low-volatility secondary organic aerosol
Mikael Ehn,Joel A. Thornton,Einhard Kleist,Mikko Sipilä,Heikki Junninen,Iida Pullinen,Monika Springer,Florian Rubach,Ralf Tillmann,Ben H. Lee,Felipe D. Lopez-Hilfiker,S. Andres,Ismail-Hakki Acir,Matti P. Rissanen,Tuija Jokinen,Siegfried Schobesberger,Juha Kangasluoma,Jenni Kontkanen,Tuomo Nieminen,Theo Kurtén,Lasse B. Nielsen,Solvejg Jørgensen,Henrik G. Kjaergaard,Manjula R. Canagaratna,Miikka Dal Maso,Torsten Berndt,Tuukka Petäjä,Andreas Wahner,Veli-Matti Kerminen,Markku Kulmala,Douglas R. Worsnop,Juergen Wildt,Thomas F. Mentel +32 more
TL;DR: It is found that a direct pathway leads from several biogenic VOCs, such as monoterpenes, to the formation of large amounts of extremely low-volatility vapours, helping to explain the discrepancy between the observed atmospheric burden of secondary organic aerosol and that reported by many model studies.
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Gas uptake and chemical aging of semisolid organic aerosol particles
TL;DR: The findings demonstrate that the occurrence and properties of amorphous semisolid phases challenge traditional views and require advanced formalisms for the description of organic particle formation and transformation in atmospheric models of aerosol effects on air quality, public health, and climate.
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Effects of aging on organic aerosol from open biomass burning smoke in aircraft and laboratory studies
Michael J. Cubison,Michael J. Cubison,Amber M. Ortega,Amber M. Ortega,Patrick L. Hayes,Patrick L. Hayes,Delphine K. Farmer,Delphine K. Farmer,Douglas A. Day,Douglas A. Day,M. J. Lechner,William H. Brune,Eric C. Apel,Glenn S. Diskin,Jenny A. Fisher,Henry E. Fuelberg,Arsineh Hecobian,D. J. Knapp,Tomas Mikoviny,Daniel D. Riemer,Glen W. Sachse,W. R. Sessions,Rodney J. Weber,Andrew J. Weinheimer,Armin Wisthaler,Jose L. Jimenez,Jose L. Jimenez +26 more
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Multiphase chemistry at the atmosphere-biosphere interface influencing climate and public health in the anthropocene.
Ulrich Pöschl,Manabu Shiraiwa +1 more
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A two-dimensional volatility basis set - Part 2: Diagnostics of organic-aerosol evolution
TL;DR: In this article, the authors use a 2D-Voxidation space to describe organic-aerosol chemical evolution, based on two coordinates, volatility and the degree of oxidation, which can be constrained observationally or specified for known molecules.
References
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Journal ArticleDOI
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Allen L. Robinson,Neil M. Donahue,Manish Shrivastava,Emily A. Weitkamp,Amy M. Sage,Andrew P. Grieshop,Timothy E. Lane,Jeffrey R. Pierce,Spyros N. Pandis,Spyros N. Pandis +9 more
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Journal ArticleDOI
Chemistry of secondary organic aerosol: Formation and evolution of low-volatility organics in the atmosphere
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Journal ArticleDOI
Gas/Particle Partitioning and Secondary Organic Aerosol Yields
Jay R. Odum,Thorsten Hoffmann,Frank M. Bowman,Don R. Collins,Richard C. Flagan,John H. Seinfeld +5 more
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.
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