Connecting the solubility and CCN activation of complex organic aerosols: a theoretical study using solubility distributions

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Riipinen, IlonaStockholms universitet,Institutionen för miljövetenskap och analytisk kemi,Carnegie Mellon University, USA (författare)

Connecting the solubility and CCN activation of complex organic aerosols : a theoretical study using solubility distributions

Artikel/kapitelEngelska2015

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2015-06-10
Copernicus GmbH,2015
printrdacarrier

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LIBRIS-ID:oai:DiVA.org:su-119022
https://urn.kb.se/resolve?urn=urn:nbn:se:su:diva-119022URI
https://doi.org/10.5194/acp-15-6305-2015DOI

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Språk:engelska
Sammanfattning på:engelska

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We present a theoretical study investigating the cloud activation of multicomponent organic particles. We modeled these complex mixtures using solubility distributions (analogous to volatility distributions in the VBS, i.e., volatility basis set, approach), describing the mixture as a set of surrogate compounds with varying water solubilities in a given range. We conducted Khler theory calculations for 144 different mixtures with varying solubility range, number of components, assumption about the organic mixture thermodynamics and the shape of the solubility distribution, yielding approximately 6000 unique cloud condensation nucleus (CCN)-activation points. The results from these comprehensive calculations were compared to three simplifying assumptions about organic aerosol solubility: (1) complete dissolution at the point of activation; (2) combining the aerosol solubility with the molar mass and density into a single effective hygroscopicity parameter kappa; and (3) assuming a fixed water-soluble fraction eff. The complete dissolution was able to reproduce the activation points with a reasonable accuracy only when the majority (70-80 %) of the material was dissolved at the point of activation. The single-parameter representations of complex mixture solubility were confirmed to be powerful semi-empirical tools for representing the CCN activation of organic aerosol, predicting the activation diameter within 10% in most of the studied supersaturations. Depending mostly on the condensedphase interactions between the organic molecules, material with solubilities larger than about 0.1-100 g L-1 could be treated as soluble in the CCN activation process over atmospherically relevant particle dry diameters and supersaturations. Our results indicate that understanding the details of the solubility distribution in the range of 0.1-100 g L-1 is thus critical for capturing the CCN activation, while resolution outside this solubility range will probably not add much information except in some special cases. The connections of these results to the previous observations of the CCN activation and the molecular properties of complex organic mixture aerosols are discussed. The presented results help unravel the mechanistic reasons behind observations of hygroscopic growth and CCN activation of atmospheric secondary organic aerosol (SOA) particles. The proposed solubility distribution framework is a promising tool for modeling the interlinkages between atmospheric aging, volatility and water uptake of atmospheric organic aerosol.

Ämnesord och genrebeteckningar

NATURVETENSKAP Geovetenskap och miljövetenskap hsv//swe
NATURAL SCIENCES Earth and Related Environmental Sciences hsv//eng
miljövetenskap
Environmental Sciences

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Rastak, NargesStockholms universitet,Institutionen för miljövetenskap och analytisk kemi(Swepub:su)nara6543 (författare)
Pandis, S. N. (författare)
Stockholms universitetInstitutionen för miljövetenskap och analytisk kemi (creator_code:org_t)

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Ingår i:Atmospheric Chemistry And Physics: Copernicus GmbH15:11, s. 6305-63221680-73161680-7324

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Atmospheric Chemistry And Physics (Sök värdpublikationen i LIBRIS)

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Av författaren/redakt...: Riipinen, Ilona; Rastak, Narges; Pandis, S. N.

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NATURVETENSKAP: NATURVETENSKAP; och Geovetenskap och ...

Artiklar i publikationen: Atmospheric Chem ...

Av lärosätet: Stockholms universitet

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