The atmospheric contaminants most harmful to human health are designated Criteria Pollutants. To help Maryland attain the national ambient air quality standards (NAAQS) for Criteria Pollutants, and to improve our fundamental understanding of atmospheric chemistry, I conducted aircraft measurements in the Regional Atmospheric Measurement Modeling Prediction Program (RAMMPP). These data are used to evaluate model simulations and satellite observations. I developed techniques for improving airborne observation of two NAAQS pollutants, particulate matter (PM) and nitrogen dioxide (NO2). While structure and composition of organic aerosol are important for understanding PM formation, the molecular speciation of organic ambient aerosol remains largely unknown. The spatial distribution of reactive nitrogen is likewise poorly constrained. To examine water-soluble organic aerosol (WSOA) during an air pollution episode, I designed and implemented a shrouded aerosol inlet system to collect PM onto quartz fiber filters from a Cessna 402 research aircraft. Inlet evaluation conducted during a side-by-side flight with the NASA P3 demonstrated agreement to within 30%. An ion chromatographic mass spectrometric method developed using the NIST Standard Reference Material (SRM) 1649b Urban Dust, as a surrogate material resulted in acidic class separation and resolution of at least 34 organic acids; detection limits approach pg/g concentrations. Analysis of aircraft filter samples resulted in detection of 8 inorganic species and 16 organic acids of which 12 were quantified. Aged, re-circulated metropolitan air showed a greater number of dicarboxylic acids compared to air recently transported from the west. While the NAAQS for NO2 is rarely exceeded, it is a precursor molecule for ozone, America's most recalcitrant pollutant. Using cavity ringdown spectroscopy employing a light emitting diode (LED), I measured vertical profiles of NO¬2 (surface to 2.5 km) west (upwind) of the Baltimore/Washington, area in the morning, and east (downwind) in the afternoon. Column contents (altitude integrals of concentration) were remarkably similar (≈3x1015 molecules cm−2). These measurements indicate that NO2 is widely distributed over the eastern US and help quantify the regional nature of smog events and prove extensive interstate transport of pollutants. These results were used to help shape air pollution control policy based on solid science.