1Leibniz Institute for Tropospheric Research, Permoserstr. 15, 04318 Leipzig, Germany
2Atmospheric Chemistry Division, Max Planck Institute for Chemistry, P.O. Box 3060, 55020 Mainz, Germany
3Institute of Atmospheric Physics, German Aerospace Center, Oberpfaffenhofen, 82230 Wessling, Germany
4Institute for Meteorology and Climate Research, Karlsruhe Institute of Technology, P.O. Box 3640, 76021 Karlsruhe, Germany
5Royal Netherlands Meteorological Institute, P.O. Box 201, 3730 AE de Bilt, The Netherlands
Received: 25 May 2009 – Published in Atmos. Chem. Phys. Discuss.: 18 Jun 2009
Abstract. The origin of aerosol particles in the upper troposphere and lowermost stratosphere over the Eurasian continent was investigated by applying cluster analysis methods to in situ measured data. Number concentrations of submicrometer aerosol particles and trace gas mixing ratios derived by the CARIBIC (Civil Aircraft for Regular Investigation of the Atmosphere Based on an Instrument Container) measurement system on flights between Germany and South-East Asia were used for this analysis. Four cluster analysis methods were applied to a test data set and their capability of separating the data points into scientifically reasonable clusters was assessed. The best method was applied to seasonal data subsets for summer and winter resulting in five cluster or air mass types: stratosphere, tropopause, free troposphere, high clouds, and boundary layer influenced. Other source clusters, like aircraft emissions could not be resolved in the present data set with the used methods. While the cluster separation works satisfactory well for the summer data, in winter interpretation is more difficult, which is attributed to either different vertical transport pathways or different chemical lifetimes in both seasons. The geographical distribution of the clusters together with histograms for nucleation and Aitken mode particles within each cluster are presented. Aitken mode particle number concentrations show a clear vertical gradient with the lowest values in the lowermost stratosphere (750–2820 particles/cm3 STP, minimum of the two 25% – and maximum of the two 75%-percentiles of both seasons) and the highest values for the boundary-layer-influenced air (4290–22 760 particles/cm3 STP). Nucleation mode particles are also highest in the boundary-layer-influenced air (1260–29 500 particles/cm3 STP), but are lowest in the free troposphere (0–450 particles/cm3 STP). The given submicrometer particle number concentrations represent the first large-scale seasonal data sets for the upper troposphere and lowermost stratosphere over the Eurasian continent.
Revised: 25 Sep 2009 – Accepted: 07 Oct 2009 – Published: 05 Nov 2009
Citation: Köppe, M., Hermann, M., Brenninkmeijer, C. A. M., Heintzenberg, J., Schlager, H., Schuck, T., Slemr, F., Sprung, D., van Velthoven, P. F. J., Wiedensohler, A., Zahn, A., and Ziereis, H.: Origin of aerosol particles in the mid-latitude and subtropical upper troposphere and lowermost stratosphere from cluster analysis of CARIBIC data, Atmos. Chem. Phys., 9, 8413-8430, doi:10.5194/acp-9-8413-2009, 2009.