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Titel |
Sensitivity of global cloud condensation nuclei concentrations to primary sulfate emission parameterizations |
VerfasserIn |
G. Luo, F. Yu |
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 ; 11, no. 5 ; Nr. 11, no. 5 (2011-03-03), S.1949-1959 |
Datensatznummer |
250009440
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Publikation (Nr.) |
copernicus.org/acp-11-1949-2011.pdf |
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Zusammenfassung |
The impact of primary sulfate emissions on cloud condensation nuclei (CCN)
concentrations, one of the major uncertainties in global CCN predictions,
depends on the fraction of sulfur mass emitted as primary sulfate particles
(fsulfate), the fraction of primary sulfate mass distributed into the
nucleation mode particles (fnucl), and the nucleation and growth
processes in the ambient atmosphere. Here, we use a global size-resolved
aerosol microphysics model recently developed to study how the different
parameterizations of primary sulfate emission affect particle properties and
CCN abundance. Different from previous studies, we use the ion-mediated
nucleation scheme to simulate tropospheric particle formation. The kinetic
condensation of low volatile secondary organic gas (SOG) (in addition to
H2SO4 gas) on nucleated particles is calculated based on our new
scheme that considers the SOG volatility changes arising from the oxidation
aging. Our simulations show a compensation effect of nucleation to primary
sulfate emission. We find that the change of fnucl from 5% to 15%
has a more significant impact on the simulated particle number budget than
that of fsulfate within the range of 2.5–5%. Based on our model
configurations, an increase of fsulfate from 0% to 2.5% (with
fnucl = 5%) does not improve the agreement between simulated and
observed annual mean number concentrations of particles >10 nm at 21
stations but further increase of either fsulfate from 2.5% to 5%
(with fnucl = 5%) or fnucl from 5% to 15% (with
fsulfate = 2.5%) substantially deteriorates the agreement. For
fsulfate of 2.5%–5% and fnucl of 5%, our simulations
indicate that the global CCN at supersaturation of 0.2% increases by
8–11% in the boundary layer and 3–5% in the whole troposphere
(compared to the case with fsulfate=0). |
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