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SO2 oxidation products other than H2SO4 as a trigger of new particle formation. Part 1: Laboratory investigations
2008, Berndt, T., Stratmann, F., Bräsel, S., Heintzenberg, J., Laaksonen, A., Kulmala, M.
Mechanistic investigations of atmospheric H2SO4 particle formation have been performed in a laboratory study taking either H2SO4 from a liquid reservoir or using the gas-phase reaction of OH radicals with SO2. Applying both approaches for H2SO4 generation simultaneously it was found that H2SO4 evaporated from the liquid reservoir acts considerably less effective for the process of particle formation and growth than the products originating from the reaction of OH radicals with SO2. Furthermore, for NOx concentrations >5×1011 molecule cm−3 the formation of new particles from the reaction of OH radicals with SO2 is inhibited. This suggests that substances other than H2SO4 (potentially products from sulphur-containing peroxy radicals) trigger lower tropospheric new particle formation and growth. The currently accepted mechanism for SO2 gas-phase oxidation does not consider the formation of such substances. The analysis of new particle formation for different reaction conditions in our experiment suggests that a contribution of impurities to the nucleation process is unlikely.
New-particle formation events in a continental boundary layer: First results from the SATURN experiment
2003, Stratmann, F., Siebert, H., Spindler, G., Wehner, B., Althausen, D., Heintzenberg, J., Hellmuth, O., Rinke, R., Schmieder, U., Seidel, C., Tuch, T., Uhrner, U., Wiedensohler, A., Wandinger, U., Wendisch, M., Schell, D., Stohl, A.
During the SATURN experiment, which took place from 27 May to 14 June 2002, new particle formation in the continental boundary layer was investigated. Simultaneous ground-based and tethered-balloon-borne measurements were performed, including meteorological parameters, particle number concentrations and size distributions, gaseous precursor concentrations and SODAR and LIDAR observations. Newly formed particles were observed inside the residual layer, before the break-up process of the nocturnal inversion, and inside the mixing layer throughout the break-up of the nocturnal inversion and during the evolution of the planetary boundary layer.
LACIS-measurements and parameterization of sea-salt particle hygroscopic growth and activation
2008, Niedermeier, D., Wex, H., Voigtländer, J., Stratmann, F., Brüggemann, E., Kiselev, A., Henk, H., Heintzenberg, J.
The Leipzig Aerosol Cloud Interaction Simulator (LACIS) was used to investigate the hygroscopic growth and activation of sea-salt particles which were generated from three different sea-water samples. The measurements showed that the sea-salt particles exhibit a slightly reduced hygroscopic growth compared to pure NaCl particles. Köhler theory was utilized to model the hygroscopic growth of these particles. Some parameters used in this model are unknown for sea-salt. These parameters are combined in an "ionic density" ρion. For each sea-salt sample an average ρion was determined by fitting the Köhler equation to the data from the hygroscopic growth measurements. LACIS was also used to measure the activation of the sea-salt particles at three different supersaturations: 0.11%, 0.17% and 0.32%. A CCN-closure was tested by calculating the critical diameters Dcrit for the sea-salt particles at these supersaturations, using the Köhler model and the corresponding ρion as derived from the hygroscopic growth data. These calculated critical diameters were compared to the measured ones. Measured and calculated values of Dcrit agree within the level of uncertainty. Based on this successful closure, a new parameterization to describe sea-salt-particle hygroscopic growth (at RH>95%) and activation has been developed.