The concentration and chemical composition of ambient fine particulate material (PM2.5) is reported for two sampling sites in the Pittsburgh, Pennsylvania metropolitan area: the Department of Energy, National Energy Technology Laboratory (NETL) PM study site south of the city center, and the Carnegie Mellon Pittsburgh Air Quality Study (PAQS) site 5 km east of central Pittsburgh established with funding by the EPA Supersites Program and by DOE-NETL. Data from these sampling sites were characterized by one to three-day episodes with PM2.5 concentrations (constructed from the sum of the chemical components) exceeding 40.0 mug m(-3). The episodes were dominated by high concentrations of ammonium sulfate. The fine particle concentrations were compared with meteorological data from surface weather maps and a Hybrid Single Particle Lagrangian Integrated Trajectory model (HYSPLIT model), with back-trajectories estimated over 24 h. High PM2.5 concentrations were associated with transition from a high pressure to a low pressure regime in advance of an approaching frontal system indicating long-range transport of pollutants. In contrast, fine particulate organic material appeared to be dominated by nearby sources. Distinct differences were observed in the diurnal variations in concentration between the two sites. The NETL site showed clear maximum concentrations of semi-volatile organic material (SVOM) during midday, and minimum concentrations of nonvolatile organic compounds in the afternoon. In contrast, the Carnegie Mellon PAQS site showed an absence of diurnal variation in SVOM, but still with minimum concentrations of nonvolatile organic compounds in the afternoon and evening. Neither site showed significant diurnal variation in ammonium sulfate. (C) 2004 Elsevier Ltd. All rights reserved.