Number and sulfur derived 3-parameter aerosol size distributions in the tropopause region from CARIBIC flights between Germany and the Indic

Aerosol number concentrations in three size ranges (dp>4,dp>12,18 dp 135 nm) and sulfur mass from impactor samples were collected over a total of about 120 sampling hours on 18 long-range commercial flights between the northern mid-latitudes and the equatorial region covering an altitude range between 8.8 and 11.2 km. The data were evaluated with a new random search algorithm to derive monomodal lognormal particle size distributions. Through tests of the algorithm using synthetic data and size distributions from mountain stations the retrieval capabilities of the fitting algorithm are established. The fitting of aerosol data yields three parameters of the submicrometer size distribution. Their latitudinal trends indicate the influence of tropical and mid-latitudinal source regions on the tropopause aerosol. Total particle numbers show maxima near tropical biomass burning and over the European regions. Geometric mean diameters decrease north of 35°N while the width of the distribution increases, indicating a move towards more frequent recent nucleation events or more frequent bimodal size distributions.