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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.
- ItemNumerical simulations of optical properties of Saharan dust aerosols with emphasis on lidar applications(Milton Park : Taylor & Francis, 2017) Wiegner, M.; Gasteiger, J.; Kandler, K.; Weinzierl, B.; Rasp, K.; Esselborn, M.; Freudenthaler, V.; Heese, B.; Toledano, C.; Tesche, M.; Althausen, D.In the framework of the Saharan Mineral Dust Experiment (SAMUM) for the first time the spectral dependence of particle linear depolarization ratios was measured by combining four lidar systems. In this paper these measurements are compared with results from scattering theory based on the T-matrix method. For this purpose, in situ measurements—size distribution, shape distribution and refractive index—were used as input parameters; particle shape was approximated by spheroids. A sensitivity study showed that lidar-related parameters—lidar ratio Sp and linear depolarization ratio δp—are very sensitive to changes of all parameters. The simulated values of the δp are in the range of 20% and 31% and thus in the range of the measurements. The spectral dependence is weak, so that it could not be resolved by the measurements. Calculated lidar ratios based on the measured microphysics and considering equivalent radii up to 7.5μm show a range of possible values between 29 and 50 sr at λ = 532 nm. Larger Sp might be possible if the real part of the refractive index is small and the imaginary part is large. A strict validation was however not possible as too many microphysical parameters influence Sp and δp that could not be measured with the required accuracy.
- ItemEvaluation of long-range transport and deposition of desert dust with the CTM MOCAGE(Milton Park : Taylor & Francis, 2017) Martet, M.; Peuch, V-H.; Laurent, B.; Marticorena, B.; Bergametti, G.Desert dust modelling and forecasting attract growing interest, due to the numerous impacts of dusts on climate, numerical weather prediction, health, ecosystems, transportation, as well as on many industrial activities. The validation of numerical tools is a very important activity in this context, and we present here an example of such an effort, combining in situ (horizontal visibility in SYNOP messages, IMPROVE database) and remote-sensing data (satellite imagery, AERONET aerosol optical thickness data). Interestingly, these measurements are available routinely, and not only in the context of dedicated measurements campaign; thus, they can be used in an operational context to monitor the performances of operational forecasting systems. MOCAGE is the chemistry-transport model of Météo-France, used operationally to forecast the three-dimensional transport of dusts and their deposition. Two very long-range transport episodes of dust have been studied: one case of Saharan dust transported to East America through Asia and Pacific observed in November 2004 and one case of Saharan dust transported from West Africa to Caribbean Islands in May 2007. Episodes of geographical extension had seldom been studied, and they provide a very selective reference to compare the modelled desert dusts with. The representation of dusts in MOCAGE appears to be realistic in these two very different cases. In turn, the model simulations are used to make the link between the complementary information provided by the different measurements tools, providing a fully consistent picture of the entire episodes. The evolution of the aerosol size distribution during the episodes has also been studied. With no surprise, our study underlines that deposition processes are very sensitive to the size of dust particles. If the atmospheric cycle, in terms of mass, is very much under the influence of larger particles (some micrometres and above), only the finer particles actually travel over thousands of kilometres. This illustrates the need for an accurate representation of size distributions for this aerosol component in numerical models and advocates for using a size-resolved (bin) approach as sinks, and particularly, deposition do not affect the emitted log-normal distributions symmetrically on both sides of the median diameter. Overall, the results presented in this study provide an evaluation of Météo-France operational dust forecasting system MOCAGE.