A new analytical approach for the characterization of organic compounds in size-segregated atmospheric aerosol particles is described. Its potential is demonstrated for samples that were collected during the Second Aerosol Characterization Experiment in Sagres (Portugal) and at the Institut f¿r Troposph¿renforschung research station in Melpitz (Germany). Curie point pyrolysis gas chromatography/mass spectrometry is used to determine semivolatile compounds, capillary electrophoresis for organic acids. The main advantages are low sample amount and almost no sample preparation. Size distributions of alkanes, fatty acids, polycyclic aromatic hydrocarbons (PAHs), oxygenated polycyclic aromatic hydrocarbons (oxy-PAHs), dicarboxylic acids, hydroxylated dicarboxylic acids, organic and elemental carbon, main water soluble ions, and gravimetric mass were determined by impactor measurements and are discussed. Compared to central Europe (hydroxylated) dicarboxylic acids show a higher concentration in marine air influenced by long-range transport through European polluted air masses. Dicarboxylic acids show a maximum concentration in the coarse mode, whereas hydroxylated dicarboxylic acids are mostly found in submicrometer particles. Alkanes are found in higher concentrations and oxy-PAHs are only found in central Europe. For the selected samples, 12--15% of the organic carbon could be assigned to individual species in the case of central Europe, and 20--40% could be assigned in the marine aerosol of Portugal. In all cases, semivolatile organic species such as alkanes and PAHs account for the major fraction of the speciated organic carbon. ¿ 2000 American Geophysical Union