Recent studies have linked atmospheric particulate matter with human health problems. In many urban areas, mobile sources are a major source of particulate matter (PM) and the dominant source of fine particles or PM2.5 (PM smaller than 2.5 pm in aerodynamic diameter). Dynamometer studies have implicated diesel engines as being a significant source of ultrafine particles (< 0.1 microm), which may also exhibit deleterious health impacts. In addition to direct tailpipe emissions, mobile sources contribute to ambient particulate levels by brake and tire wear and by resuspension of particles from pavement. Information about particle emission rates, size distributions, and chemical composition from in-use light-duty (LD) and heavy-duty (HD) vehicles is scarce, especially under real-world operating conditions. To characterize particulate emissions from a limited set of in-use vehicles, we studied on-road emissions from vehicles operating under hot-stabilized conditions, at relatively constant speed, in the Tuscarora Mountain Tunnel along the Pennsylvania Turnpike from May 18 through 23, 1999. There were five specific aims of the study. (1) obtain chemically speciated diesel profiles for the source apportionment of diesel versus other ambient constituents in the air and to determine the chemical species present in real-world diesel emissions; (2) measure particle number and size distribution of chemically speciated particles in the atmosphere; (3) identify, by reference to data in years past, how much change has occurred in diesel exhaust particulate mass; (4) measure particulate emissions from LD gasoline vehicles to determine their contribution to the observed particle levels compared to diesels; and (5) determine changes over time in gas phase emissions by comparing our results with those of previous studies. Comparing the results of this study with our 1992 results, we found that emissions of C8 to C20 hydrocarbons, carbon monoxide (CO), and carbon dioxide (CO2) from HD diesel emissions substantially decreased over the seven-year period. Particulate mass emissions showed a similar trend. Considering a 25-year period, we observed a continued downward trend in HD particulate emissions from approximately 1,100 mg/km in 1974 to 132 mg/km (reported as PM2.5) in this study. The LD particle emission factor was considerably less than the HD value, but given the large fraction of LD vehicles, emissions from this source cannot be ignored. Results of the current study also indicate that both HD and LD vehicles emit ultrafine particles and that these particles are preserved under real-world dilution conditions. Particle number distributions were dominated by ultrafine particles with count mean diameters of 17 to 13 nm depending on fleet composition. These particles appear to be primarily composed of sulfur, indicative of sulfuric acid emission and nucleation. Comparing the 1992 and 1999 HD emission rates, we observed a 48% increase in the NOx/CO2 emissions ratio. This finding supports the assumption that many new-technology diesel engines conserve fuel but increase NOx emissions.