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| Titel |
In-cloud sulfate addition to single particles resolved with sulfur isotope analysis during HCCT-2010 |
| VerfasserIn |
E. Harris, B. Sinha, D. van Pinxteren, J. Schneider, L. Poulain, J. Collett, B. D'Anna, B. Fahlbusch, S. Foley, K. W. Fomba, C. George, T. Gnauk, S. Henning, T. Lee, S. Mertes, A. Roth, F. Stratmann, S. Borrmann, P. Hoppe, H. Herrmann |
| Medientyp |
Artikel
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| Sprache |
Englisch
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| ISSN |
1680-7316
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| Digitales Dokument |
URL |
| Erschienen |
In: Atmospheric Chemistry and Physics ; 14, no. 8 ; Nr. 14, no. 8 (2014-04-28), S.4219-4235 |
| Datensatznummer |
250118642
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| Publikation (Nr.) |
 copernicus.org/acp-14-4219-2014.pdf |
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| Zusammenfassung |
In-cloud production of sulfate modifies aerosol size distribution, with
important implications for the magnitude of indirect and direct aerosol
cooling and the impact of SO2 emissions on the environment. We investigate
which sulfate sources dominate the in-cloud addition of sulfate to different
particle classes as an air parcel passes through an orographic cloud. Sulfate
aerosol, SO2 and H2SO4 were collected upwind, in-cloud and downwind
of an orographic cloud for three cloud measurement events during the Hill Cap
Cloud Thuringia campaign in autumn 2010 (HCCT-2010). Combined SEM and
NanoSIMS analysis of single particles allowed the δ34S of
particulate sulfate to be resolved for particle size and type.
The most important in-cloud SO2 oxidation pathway at HCCT-2010 was aqueous
oxidation catalysed by transition metal ions (TMI catalysis), which was shown
with single particle isotope analyses to occur primarily in cloud droplets
nucleated on coarse mineral dust. In contrast, direct uptake of H2SO4
(g) and ultrafine particulate were the most important sources modifying fine
mineral dust, increasing its hygroscopicity and facilitating activation.
Sulfate addition to "mixed" particles (secondary organic and inorganic
aerosol) and coated soot was dominated by in-cloud aqueous SO2 oxidation
by H2O2 and direct uptake of H2SO4 (g) and ultrafine particle
sulfate, depending on particle size mode and time of day. These results
provide new insight into in-cloud sulfate production mechanisms, and show the
importance of single particle measurements and models to accurately assess
the environmental effects of cloud processing. |
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