2 results
Search Results
Now showing 1 - 2 of 2
- ItemIn-cloud sulfate addition to single particles resolved with sulfur isotope analysis during HCCT-2010(München : European Geopyhsical Union, 2014) Harris, E.; Sinha, B.; van Pinxteren, D.; Schneider, J.; Poulain, L.; Collett, J.; D'Anna, B.; Fahlbusch, B.; Foley, S.; Fomba, K.W.; George, C.; Gnauk, T.; Henning, S.; Lee, T.; Mertes, S.; Roth, A.; Stratmann, F.; Borrmann, S.; Hoppe, P.; Herrmann, H.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.
- ItemA new method to determine the mixing state of light absorbing carbonaceous using the measured aerosol optical properties and number size distributions(München : European Geopyhsical Union, 2012) Ma, N.; Zhao, C.S.; Müller, T.; Cheng, Y.F.; Liu, P.F.; Deng, Z.Z.; Xu, W.Y.; Ran, L.; Nekat, B.; van Pinxteren, D.; Gnauk, T.; Müller, K.; Herrmann, H.; Yan, P.; Zhou, X.J.; Wiedensohler, A.In this paper, the mixing state of light absorbing carbonaceous (LAC) was investigated with a two-parameter aerosol optical model and in situ aerosol measurements at a regional site in the North China Plain (NCP). A closure study between the hemispheric backscattering fraction (HBF) measured by an integrating nephelometer and that calculated with a modified Mie model was conducted. A new method was proposed to retrieve the ratio of the externally mixed LAC mass to the total mass of LAC (rext-LAC) based on the assumption that the ambient aerosol particles were externally mixed and consisted of a pure LAC material and a core-shell morphology in which the core is LAC and the shell is a less absorbing material. A Monte Carlo simulation was applied to estimate the overall influences of input parameters of the algorithm to the retrieved rext-LAC. The diurnal variation of rext-LAC was analyzed and the PartMC-MOSAIC model was used to simulate the variation of the aerosol mixing state. Results show that, for internally mixed particles, the assumption of core-shell mixture is more appropriate than that of homogenous mixture which has been widely used in aerosol optical calculations. A significant diurnal pattern of the retrieved rext-LAC was found, with high values during the daytime and low values at night. The consistency between the retrieved rext-LAC and the model results indicates that the diurnal variation of LAC mixing state is mainly caused by the diurnal evolution of the mixing layer.