a b s t r a c tThe global atmospheric distribution and long-range transport (LRT) potential of three polycyclic aromatic hydrocarbons (PAH) -anthracene, fluoranthene and benzo [a]pyrene -are studied. The model used is a global aerosol-chemistry-transport-model, which is based on an atmospheric general circulation model. The model includes an in-built dynamic aerosol model coupled to two-dimensional surface compartments. Several parameterisations of gas/particle partitioning and different assumptions of degradation in the aerosol particulate phase were tested.PAHs are mostly distributed in the source regions but reach the Arctic and the Antarctic. The Canadian Arctic is predicted to be significantly less affected by mid-latitude PAH emissions than the European Arctic. Re-volatilisation is significant for semivolatile PAHs. Accumulation of semivolatile PAHs in polar regions, however, is not indicated. The model study suggests that gas/particle partitioning in air drastically influences the atmospheric cycling, the total environmental fate (e.g. compartmental distributions) and the LRT potential of the substances studied. A parameterisation which calculates the gas/particle partitioning assuming absorption into organic matter and adsorption to black carbon (soot) agrees best with the observations at remote sites. The study provides evidence that the degradation in the particulate phase must be slower than that in the gas-phase. The predicted concentrations of the semivolatile PAHs anthracene and fluoranthene in near-ground air at remote sites in mid and high northern latitudes are in line with measured concentrations, if adsorption of the substances to soot combined with absorption in particulate organic matter is assumed to determine gas/particle partitioning, but cannot be explained by adsorption alone (Junge-Pankow parameterisation of gas/particle partitioning). The results suggest that PAHs absorbed in the organic matrix of particulate matter is shielded from the gas-phase.
An overview of the two FEBUKO aerosol-cloud interaction field experiments in the Thu¨ringer Wald (Germany) in October 2001 and 2002 and the corresponding modelling project MODMEP is given. Experimentally, a variety of measurement methods were deployed to probe the gas phase, particles and cloud droplets at three sites upwind, downwind and within an orographic cloud with special emphasis on the budgets and interconversions of organic gas and particle phase constituents. Out of a total of 14 sampling periods within 30 cloud events three events (EI, EII and EIII) are selected for detailed analysis. At various occasions an impact of the cloud process on particle chemical composition such as on the organic compounds content, sulphate and nitrate and also on particle size distributions and particle mass is observed. Moreover, direct phase transfer of polar organic compound from the gas phase is found to be very important for the understanding of cloudwater composition.For the modelling side, a main result of the MODMEP project is the development of a cloud model, which combines a complex multiphase chemistry with detailed microphysics. Both components are described in a fine-resolved particle/ drop spectrum. New numerical methods are developed for an efficient solution of the entire complex model. A further development of the CAPRAM mechanism has lead to a more detailed description of tropospheric aqueous phase organic chemistry. In parallel, effective tools for the reduction of highly complex reaction schemes are provided. Techniques are provided and tested which allow the description of complex multiphase chemistry and of detailed microphysics in multidimensional chemistry-transport models. r
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