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Size-segregated atmospheric aerosols were collected from urban and rural locations in Massachusetts using a micro-orifice impactor. The samples were analyzed for polycyclic aromatic hydrocarbons (PAH) with molecular weights between 178 and 302, using gas chromatography/mass spectrometry. Fifteen PAH were quantified in the urban samples and nine in the rural samples. The quantification results are in good agreement with available ambient monitoring data. In the urban samples, PAH were distributed among aerosol size fractions based on molecular weight. PAH with molecular weights between 178 and 202 were approximately evenly distributed between the fine (aerodynamic diameter <2 μm) and coarse (aerodymanic diameter >2 μm) aerosols. PAH with molecular weights greater than 228 were associated primarily with the fine aerosol fraction. In the rural samples, low and high molecular weight PAH were associated with both the fine and coarse aerosols. Slow mass transfer by vaporization and condensation is proposed to explain the observed PAH partitioning among aerosol size fractions.