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  Molecular corridors and parameterizations of volatility in the chemical evolution of organic aerosols

Li, Y., Pöschl, U., & Shiraiwa, M. (2015). Molecular corridors and parameterizations of volatility in the chemical evolution of organic aerosols. Atmospheric Chemistry and Physics Discussions, 15, 27877-27915. doi:10.5194/acpd-15-27877-2015.

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 Creators:
Li, Y.1, Author              
Pöschl, U.1, Author              
Shiraiwa, M.1, Author              
Affiliations:
1Multiphase Chemistry, Max Planck Institute for Chemistry, Max Planck Society, ou_1826290              

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 Abstract: The formation and aging of organic aerosols (OA) proceed through multiple steps of chemical reaction and mass transport in the gas and particle phases, which is challenging for the interpretation of field measurements and laboratory experiments as well as accurate representation of OA evolution in atmospheric aerosol models. Based on data from over 30 000 compounds, we show that organic compounds with a wide variety of functional groups fall into molecular corridors, characterized by a tight inverse correlation between molar mass and volatility. We developed parameterizations to predict the saturation mass concentration of organic compounds containing oxygen, nitrogen, and sulfur from the elemental composition that can be measured by soft-ionization high-resolution mass spectrometry. Field measurement data from new particle formation events, biomass burning, cloud/fog processing, and indoor environments were mapped into molecular corridors to characterize the chemical nature of the observed OA components. We found that less-oxidized indoor OA are constrained to a corridor of low molar mass and high volatility, whereas highly oxygenated compounds in atmospheric water extend to high molar mass and low volatility. Among the nitrogen- and sulfur-containing compounds identified in atmospheric aerosols, amines tend to exhibit low molar mass and high volatility, whereas organonitrates and organosulfates follow high O : C corridors extending to high molar mass and low volatility. We suggest that the consideration of molar mass and molecular corridors can help to constrain volatility and particle-phase state in the modeling of OA particularly for nitrogen- and sulfur-containing compounds.

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Language(s): eng - English
 Dates: 2015-10-15
 Publication Status: Published online
 Pages: 38
 Publishing info: -
 Table of Contents: -
 Rev. Type: -
 Identifiers: DOI: 10.5194/acpd-15-27877-2015
 Degree: -

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Title: Atmospheric Chemistry and Physics Discussions
  Abbreviation : Atmos. Chem. Phys. Discuss.
Source Genre: Journal
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Publ. Info: Katlenburg-Lindau, Germany : European Geophysical Society
Pages: - Volume / Issue: 15 Sequence Number: - Start / End Page: 27877 - 27915 Identifier: ISSN: 1680-7367
CoNE: https://pure.mpg.de/cone/journals/resource/111076360006006