During August 1999 as part of the Southern Oxidants Study Supersite Experiment, our group collected size-resolved measurements of the chemical composition of single ambient aerosol particles with a unique real-time laser desorption/ionization mass spectrometry technique. The rapid single-particle mass spectrometry instrument is capable of analyzing ultrafine particles with aerodynamic diameters ranging from 0.01 to 1.5 ¿m. Under the heaviest loading observed in Atlanta, particles were analyzed at a rate of roughly one per second in sizes ranging from 0.1 to 0.2 ¿m. Nearly 16,000 individual spectra were recorded over the course of the month during both daytime and nighttime sampling periods. Evaluation of the data indicates that the composition of the ultrafine (less than 100 nm) particles is dominated by carbon-containing compounds. Larger particles show varied compositions but typically appeared to have organic carbon characteristics mixed with an inorganic component (e.g., crustal materials, metals, etc.). During the experiment, 70 composition classes were identified. In this paper we report the average spectra and correlations with various meteorological parameters for all major compound classes and a number of minor ones. The major composition classes are identified from the primary peaks in their spectra as organic carbon (about 74% of the particles), potassium (8%), iron (3%), calcium (2%), nitrate (2%), elemental carbon (1.5%), and sodium (1%). Many of these compound classes appeared in repeatable size ranges and quadrants of the wind rose, indicating emission from specific sources.