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Elemental Carbon (EC) has significant impact on human health and climate change. In order to evaluate the size segregation of EC emission and investigation of its influence on atmospheric transport processes in Europe, we used the fully coupled online Weather Research and Forecasting/Chemistry model (WRF-Chem) at a resolution of 2 km focusing on a region in Germany, in conjunction with a high-resolution EC emission inventory. The ground meteorology conditions, vertical structure and wind pattern were well reproduced by the model. The simulations of particle number/mass size distributions were evaluated by observations taken at the central European background site Melpitz. The fine mode aerosol was reasonably well simulated, but the coarse mode was substantially overestimated by the model. We found that it was mainly due to the nearby point source plume emitting a high amount of EC in the coarse mode. The comparisons between simulated EC and Multi-angle Absorption Photometers (MAAP) measurements at Melpitz, Leipzig-TROPOS and Bösel indicated that coarse mode EC (ECc) emission in the nearby point sources might be overestimated by a factor of 2-10. The emission fraction of EC in coarse mode was overestimated by about 10-30% for Russian and 5-10% for Eastern Europe (e.g.: Poland and Belarus), respectively. This overestimation in ECc emission fraction makes EC particles having less opportunity to accumulate in the atmosphere and participate to the long range transport, due to the shorter lifetime of coarse mode aerosol. The deposition concept model showed that the transported EC mass from Warsaw and Moskva to Melpitz may be reduced by 25-35 and 25-55% respectively, due to the overestimation of ECc emission fraction. This may partly explain the underestimation of EC concentrations for Germany under eastern wind pattern in some other modelling research. [ABSTRACT FROM AUTHOR]

In the fine-particle mode (aerodynamic diameter < 1 pm) non-volatile material has been associated with black carbon (BC) and low-volatile organics and, to a lesser extent, with sea salt and mineral dust. This work analyzes nonvolatile particles at the tropospheric research station Melpitz (Germany), combining experimental methods such as a mobility particle-size spectrometer (3-800nm), a thermodenuder operating at 300 °C, a multi-angle absorption photometer (MAAP), and an aerosol mass spectrometer (AMS). The data were collected during two atmospheric field experiments in May-June 2008 as well as February-March 2009. As a basic result, we detected average non-volatile particlevolume fractions of 11 ± 3% (2008) and 17 ± 8% (2009). In both periods, BC was in close linear correlation with the nonvolatile fraction, but not sufficient to quantitatively explain the non-volatile particle mass concentration. Based on the assumption that BC is not altered by the heating process, the non-volatile particle mass fraction could be explained by the sum of black carbon (47% in summer, 59% in winter) and a non-volatile organic contribution estimated as part of the low-volatility oxygenated organic aerosol (LV-OOA) (53% in summer, 41% in winter); the latter was identified from AMS data by factor analysis. Our results suggest that LVOOA was more volatile in summer (May-June 2008) than in winter (February-March 2009) which was linked to a difference in oxidation levels (lower in summer). Although carbonaceous compounds dominated the sub-pm non-volatile particle mass fraction most of the time, a cross-sensitivity to partially volatile aerosol particles of maritime origin could be seen. These marine particles could be distinguished, however from the carbonaceous particles by a characteristic particle volume-size distribution. The paper discusses the uncertainty of the volatility measurements and outlines the possible merits of volatility analysis as part of continuous atmospheric aerosol measurements. [ABSTRACT FROM AUTHOR]

A recent parcel model study (Reutter et al., 2009) showed three deterministic regimes of initial cloud droplet formation, characterized by different ratios of aerosol concentrations (NCN) to updraft velocities. This analysis, however, did not reveal how these regimes evolve during the subsequent cloud development. To address this issue, we employed the Active Tracer High Resolution Atmospheric Model (ATHAM) with full microphysics and extended the model simulation from the cloud base to the entire column of a single pyro-convective mixed-phase cloud. A series of 2-D simulations (over 1000) were performed over a wide range of NCN and dynamic conditions. The integrated concentration of hydrometeors over the full spatial and temporal scales was used to evaluate the aerosol and dynamic effects. The results show that: (1) the three regimes for cloud condensation nuclei (CCN) activation in the parcel model (namely aerosol-limited, updraft-limited, and transitional regimes) still exist within our simulations, but net production of raindrops and frozen particles occurs mostly within the updraft-limited regime. (2) Generally, elevated aerosols enhance the formation of cloud droplets and frozen particles. The response of raindrops and precipitation to aerosols is more complex and can be either positive or negative as a function of aerosol concentrations. The most negative effect was found for values of NCN of ~1000 to 3000 cm-3. (3) The involvement of nonlinear (dynamic and microphysical) processes leads to a more complicated and unstable response of clouds to aerosol perturbation compared with the parcel model results. Therefore, conclusions drawn from limited case studies might require caveats regarding their representativeness, and high-resolution sensitivity studies over a wide range of aerosol concentrations and updraft velocities are strongly recommended. [ABSTRACT FROM AUTHOR]

In the fine particle mode (aerodynamic diameter < 1 μm) refractory material has been associated with black carbon (BC) and low-volatile organics and, to a lesser extent, with sea salt and mineral dust. This work analyses refractory particles at the tropospheric research station Melpitz (Germany), combining experimental methods such as a mobility particle size spectrometer (3-800 nm), a thermodenuder operating at 300°C, a multiangle absorption photometer (MAAP), and an aerosol mass spectrometer (AMS). The data were collected during two atmospheric field experiments in May/June 2008 as well as February/March 2009. As a basic result, we detected average refractory particle volume fractions of 11±3% (2008) and 17±8% (2009). In both periods, BC was in close linear correlation with the refractory fraction, but not sufficient to quantitatively explain the refractory particle mass concentration. Based on the assumption that BC is not altered by the heating process, the refractory particle mass fraction could be explained by the sum of black carbon BC (47% in summer, 59% in winter) and a refractory organic contribution estimated as part of the Low-Volatility Oxygenated Organic Aerosol (LV-OOA) (53% in summer, 41% in winter); the latter was identified from AMS data by factor analysis. Our results suggest that organics were more volatile in summer (May-June 2008) than in winter (February/March 2009). Although carbonaceous compounds dominated the sub-μm refractory particle mass fraction most of the time, a cross-sensitivity to partially volatile aerosol particles of maritime origin could be seen. These marine particles could be distinguished, however, from the carbonaceous particles by a characteristic particle volume size distribution. The paper discusses the uncertainty of the volatility measurements and outlines the possible merits of volatility analysis as part of continuous atmospheric aerosol measurements. [ABSTRACT FROM AUTHOR]

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