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Lability of secondary organic particulate matter
Liu P.1; Li Y.J.1,2; Wang Y.1,3; Gilles M.K.4; Zaveri R.A.5; Bertram A.K.6; Martin S.T.1,7
Source PublicationProceedings of the National Academy of Sciences of the United States of America
Other Abstract

The energy flows in Earth's natural and modified climate systems are strongly influenced by the concentrations of atmospheric particulate matter (PM). For predictions of concentration, equilibrium partitioning of semivolatile organic compounds (SVOCs) between organic PM and the surrounding vapor has widely been assumed, yet recent observations show that organic PM can be semisolid or solid for some atmospheric conditions, possibly suggesting that SVOC uptake and release can be slow enough that equilibrium does not prevail on timescales relevant to atmospheric processes. Herein, in a series of laboratory experiments, the mass labilities of films of secondary organic material representative of similar atmospheric organic PM were directly determined by quartz crystal microbalance measurements of evaporation rates and vapor mass concentrations. There were strong differences between films representative of anthropogenic comparedwith biogenic sources. For films representing anthropogenic PM, evaporation rates and vapor mass concentrations increased above a threshold relative humidity (RH) between 20% and 30%, indicating rapid partitioning above a transition RH but not below. Below the threshold, the characteristic time for equilibration is estimated as up to 1 wk for a typically sized particle. In contrast, for films representing biogenic PM, no RH threshold was observed, suggesting equilibrium partitioning is rapidly obtained for all RHs. The effective diffusion rate Dorgfor the biogenic case is at least 103times greater than that of the anthropogenic case. These differences should be accounted for in the interpretation of laboratory data as well as in modeling of organic PMin Earth's atmosphere.

KeywordAtmospheric Chemistry Secondary Organic Aerosol Evaporation
URLView the original
Indexed BySCI
WOS Research AreaScience & Technology - Other Topics
WOS SubjectMultidisciplinary Sciences
WOS IDWOS:000388073300045
The Source to ArticleScopus
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Cited Times [WOS]:45   [WOS Record]     [Related Records in WOS]
Document TypeJournal article
Corresponding AuthorMartin S.T.
Affiliation1.John A. Paulson School of Engineering and Applied Sciences, Harvard University, Cambridge, MA 02138
2.Department of Civil and Environmental Engineering, Faculty of Science and Technology, University of Macau, Macau 999078, China
3.T. H. Chan School of Public Health, Harvard University, Boston, MA 02115
4.Chemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA 94720
5.Atmospheric Sciences and Global Change Division, Pacific Northwest National Laboratory, Richland, WA 99354
6.Department of Chemistry, University of British Columbia, Vancouver, BC, Canada, VT6 1Z1
7.Department of Earth and Planetary Sciences, Harvard University, Cambridge, MA 02138
Recommended Citation
GB/T 7714
Liu P.,Li Y.J.,Wang Y.,et al. Lability of secondary organic particulate matter[J]. Proceedings of the National Academy of Sciences of the United States of America,2016,113(45):12643-12648.
APA Liu P..,Li Y.J..,Wang Y..,Gilles M.K..,Zaveri R.A..,...&Martin S.T..(2016).Lability of secondary organic particulate matter.Proceedings of the National Academy of Sciences of the United States of America,113(45),12643-12648.
MLA Liu P.,et al."Lability of secondary organic particulate matter".Proceedings of the National Academy of Sciences of the United States of America 113.45(2016):12643-12648.
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