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- 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.
- ItemModeling the global emission, transport and deposition of trace elements associated with mineral dust(München : European Geopyhsical Union, 2015) Zhang, Y.; Mahowald, N.; Scanza, R.A.; Journet, E.; Desboeufs, K.; Albani, S.; Kok, J.F.; Zhuang, G.; Chen, Y.; Cohen, D.D.; Paytan, A.; Patey, M.D.; Achterberg, E.P.; Engelbrecht, J.P.; Fomba, K.W.Trace element deposition from desert dust has important impacts on ocean primary productivity, the quantification of which could be useful in determining the magnitude and sign of the biogeochemical feedback on radiative forcing. However, the impact of elemental deposition to remote ocean regions is not well understood and is not currently included in global climate models. In this study, emission inventories for eight elements primarily of soil origin, Mg, P, Ca, Mn, Fe, K, Al, and Si are determined based on a global mineral data set and a soil data set. The resulting elemental fractions are used to drive the desert dust model in the Community Earth System Model (CESM) in order to simulate the elemental concentrations of atmospheric dust. Spatial variability of mineral dust elemental fractions is evident on a global scale, particularly for Ca. Simulations of global variations in the Ca / Al ratio, which typically range from around 0.1 to 5.0 in soils, are consistent with observations, suggesting that this ratio is a good signature for dust source regions. The simulated variable fractions of chemical elements are sufficiently different; estimates of deposition should include elemental variations, especially for Ca, Al and Fe. The model results have been evaluated with observations of elemental aerosol concentrations from desert regions and dust events in non-dust regions, providing insights into uncertainties in the modeling approach. The ratios between modeled and observed elemental fractions range from 0.7 to 1.6, except for Mg and Mn (3.4 and 3.5, respectively). Using the soil database improves the correspondence of the spatial heterogeneity in the modeling of several elements (Ca, Al and Fe) compared to observations. Total and soluble dust element fluxes to different ocean basins and ice sheet regions have been estimated, based on the model results. The annual inputs of soluble Mg, P, Ca, Mn, Fe and K associated with dust using the mineral data set are 0.30 Tg, 16.89 Gg, 1.32 Tg, 22.84 Gg, 0.068 Tg, and 0.15 Tg to global oceans and ice sheets.
- ItemLong-term chemical characterization of tropical and marine aerosols at the Cape Verde Atmospheric Observatory (CVAO) from 2007 to 2011(München : European Geopyhsical Union, 2014) Fomba, K.W.; Müller, K.; Van Pinxteren, D.; Poulain, L.; Van Pinxteren, M.; Herrmann, H.The first long-term aerosol sampling and chemical characterization results from measurements at the Cape Verde Atmospheric Observatory (CVAO) on the island of São Vicente are presented and are discussed with respect to air mass origin and seasonal trends. In total 671 samples were collected using a high-volume PM10 sampler on quartz fiber filters from January 2007 to December 2011. The samples were analyzed for their aerosol chemical composition, including their ionic and organic constituents. Back trajectory analyses showed that the aerosol at CVAO was strongly influenced by emissions from Europe and Africa, with the latter often responsible for high mineral dust loading. Sea salt and mineral dust dominated the aerosol mass and made up in total about 80% of the aerosol mass. The 5-year PM10 mean was 47.1 ± 55.5 μg m−2, while the mineral dust and sea salt means were 27.9 ± 48.7 and 11.1 ± 5.5 μg m−2, respectively. Non-sea-salt (nss) sulfate made up 62% of the total sulfate and originated from both long-range transport from Africa or Europe and marine sources. Strong seasonal variation was observed for the aerosol components. While nitrate showed no clear seasonal variation with an annual mean of 1.1 ± 0.6 μg m−3, the aerosol mass, OC (organic carbon) and EC (elemental carbon), showed strong winter maxima due to strong influence of African air mass inflow. Additionally during summer, elevated concentrations of OM were observed originating from marine emissions. A summer maximum was observed for non-sea-salt sulfate and was connected to periods when air mass inflow was predominantly of marine origin, indicating that marine biogenic emissions were a significant source. Ammonium showed a distinct maximum in spring and coincided with ocean surface water chlorophyll a concentrations. Good correlations were also observed between nss-sulfate and oxalate during the summer and winter seasons, indicating a likely photochemical in-cloud processing of the marine and anthropogenic precursors of these species. High temporal variability was observed in both chloride and bromide depletion, differing significantly within the seasons, air mass history and Saharan dust concentration. Chloride (bromide) depletion varied from 8.8 ± 8.5% (62 ± 42%) in Saharan-dust-dominated air mass to 30 \textpm 12% (87 ± 11%) in polluted Europe air masses. During summer, bromide depletion often reached 100% in marine as well as in polluted continental samples. In addition to the influence of the aerosol acidic components, photochemistry was one of the main drivers of halogenide depletion during the summer; while during dust events, displacement reaction with nitric acid was found to be the dominant mechanism. Positive matrix factorization (PMF) analysis identified three major aerosol sources: sea salt, aged sea salt and long-range transport. The ionic budget was dominated by the first two of these factors, while the long-range transport factor could only account for about 14% of the total observed ionic mass.
- ItemAerosol size-resolved trace metal composition in remote northern tropical atlantic marine environment: Case study cape verde islands(München : European Geopyhsical Union, 2013) Fomba, K.W.; Müller, K.; van Pinxteren, D.; Herrmann, H.Size-resolved trace metal concentrations of 15 elements in aerosol particles at the Cape Verde Atmospheric Observatory (CVAO) under remote background conditions were investigated through analysis of aerosol samples collected during intensive field studies from January 2007 to November 2011 using total reflection x-ray fluorescence (TXRF). The identification of the main air mass origin that influence remote marine aerosol in the northern tropical Atlantic has been investigated. In total, 317 samples were collected. The dataset was analyzed according to the main air mass inflow at the station. We found that remote conditions make up about 45% of the meteorological conditions in a year at CVAO and thus the northern tropical Atlantic. Surprisingly, air masses from North America are often responsible for higher trace metal concentrations in this region. Elements such as Zn, Pb, Cu, Cr, Ni, and V were mostly found in the submicron size fractions, while elements with dominant crustal or oceanic origin such as Fe, Ti, Mn, Sr, and Rb were found in the coarse fractions (>1 μm). The highest metal concentrations, especially for Zn (3.23 ng m−3), Cu (0.81 ng m−3), Sr (2.63 ng m−3), and Cr (0.53 ng m−3), were observed in air masses originating from North America and the concentrations were within the same concentration range to those reported previously in the literature for remote marine aerosols. Fe (12.26 ng m−3), Ti (0.91 ng m−3), and Mn (0.35 ng m−3) showed higher concentrations when air mass came from Europe and the Canary Islands. Pb concentration was low (<0.20 ng m−3) and did not vary significantly with air mass direction. The low Pb concentration is indicative of the complete phase-out of leaded gasoline even in African countries. Crustal enrichment factor values decreased from fine to coarse-mode particles with low values (<4) observed for Fe, Mn, and Rb, and high values (>20) for Zn, Cu, Ni, Cr, Pb, and Se. The observed enrichment of the elements was attributed to crustal, marine, anthropogenic, and biogenic sources, as well as long-range transport and resuspension. Zn, Cu and Pb were indicators of anthropogenic activities, while Ti and Sr were indicators of crustal and marine origin, respectively. Oceanic and biogenic emissions might have contributed to most of the Se observed. This work provides the first long-term size-resolved trace metals study for remote tropical northern Atlantic marine aerosols and the dataset could serve as good initiation of yearly flux estimates.
- ItemMass deposition fluxes of Saharan mineral dust to the tropical northeast Atlantic Ocean: An intercomparison of methods(München : European Geopyhsical Union, 2014) Niedermeier, N.; Held, A.; Müller, T.; Heinold, B.; Schepanski, K.; Tegen, I.; Kandler, K.; Ebert, M.; Weinbruch, S.; Read, K.; Lee, J.; Fomba, K.W.; Müller, K.; Herrmann, H.; Wiedensohler, A.Mass deposition fluxes of mineral dust to the tropical northeast Atlantic Ocean were determined within this study. In the framework of SOPRAN (Surface Ocean Processes in the Anthropocene), the interaction between the atmosphere and the ocean in terms of material exchange were investigated at the Cape Verde atmospheric observatory (CVAO) on the island Sao Vicente for January 2009. Five different methods were applied to estimate the deposition flux, using different meteorological and physical measurements, remote sensing, and regional dust transport simulations. The set of observations comprises micrometeorological measurements with an ultra-sonic anemometer and profile measurements using 2-D anemometers at two different heights, and microphysical measurements of the size-resolved mass concentrations of mineral dust. In addition, the total mass concentration of mineral dust was derived from absorption photometer observations and passive sampling. The regional dust model COSMO-MUSCAT was used for simulations of dust emission and transport, including dry and wet deposition processes. This model was used as it describes the AOD's and mass concentrations realistic compared to the measurements and because it was run for the time period of the measurements. The four observation-based methods yield a monthly average deposition flux of mineral dust of 12–29 ng m−2 s−1. The simulation results come close to the upper range of the measurements with an average value of 47 ng m−2 s−1. It is shown that the mass deposition flux of mineral dust obtained by the combination of micrometeorological (ultra-sonic anemometer) and microphysical measurements (particle mass size distribution of mineral dust) is difficult to compare to modeled mass deposition fluxes when the mineral dust is inhomogeneously distributed over the investigated area.
- ItemTrace metal characterization of aerosol particles and cloud water during HCCT 2010(München : European Geopyhsical Union, 2015) Fomba, K.W.; van Pinxteren, D.; Müller, K.; Iinuma, Y.; Lee, T.; Collett Jr., J.L.; Herrmann, H.Trace metal characterization of bulk and size-resolved aerosol and cloud water samples were performed during the Hill Cap Cloud Thuringia (HCCT) campaign. Cloud water was collected at the top of Mt. Schmücke while aerosol samples were collected at two stations upwind and downwind of Mt. Schmücke. Fourteen trace metals including Ti, V, Fe, Mn, Co, Zn, Ni, Cu, As, Sr, Rb, Pb, Cr, and Se were investigated during four full cloud events (FCEs) that fulfilled the conditions of a continuous air mass flow through the three stations. Aerosol particle trace metal concentrations were found to be lower than those observed in the same region during previous field experiments but were within a similar range to those observed in other rural regions in Europe. Fe and Zn were the most abundant elements with concentration ranges of 0.2–111.6 and 1.1–32.1 ng m−3, respectively. Fe, Mn, and Ti were mainly found in coarse mode aerosols while Zn, Pb, and As were mostly found in the fine mode. Correlation and enrichment factor analysis of trace metals revealed that trace metals such as Ti and Rb were mostly of crustal origin while trace metals such as Zn, Pb, As, Cr, Ni, V, and Cu were of anthropogenic origin. Trace metals such as Fe and Mn were of mixed origins including crustal and combustion sources. Trace metal cloud water concentration decreased from Ti, Mn, Cr, to Co with average concentrations of 9.18, 5.59, 5.54, and 0.46 μg L−1, respectively. A non-uniform distribution of soluble Fe, Cu, and Mn was observed across the cloud drop sizes. Soluble Fe and Cu were found mainly in cloud droplets with diameters between 16 and 22 μm, while Mn was found mostly in larger drops greater than 22 μm. Fe(III) was the main form of soluble Fe especially in the small and larger drops with concentrations ranging from 2.2 to 37.1 μg L−1. In contrast to other studies, Fe(II) was observed mainly in the evening hours, implying its presence was not directly related to photochemical processes. Aerosol–cloud interaction did not lead to a marked increase in soluble trace metal concentrations; rather it led to differences in the chemical composition of the aerosol due to preferential loss of aerosol particles through physical processes including cloud drop deposition to vegetative surfaces.