Ultrafine aerosols, with diameters less than 10 nm, nucleate from gas phase species. The composition of newly formed ultrafine atmospheric aerosols is not known with certainty; new particles have variously been conjectured to be sulfates, organic compounds, and sulfate/organic mixtures. The 1993 Tropospheric OH Photochemistry Experiment at Idaho Hill, Colorado, provided an opportunity to examine the question of which class of compounds, i.e., sulfates or organics, make the major contribution to new particle formation in the unpolluted troposphere. This study compared the production rates of sulfuric acid (from the oxidation of sulfur dioxide) and oxidized organic compounds to gauge their relative contributions to the formation of ultrafine particles. Potential organic precursor species examined in this study were the naturally occurring terpenes α- and β pinene, and the anthropogenic hydrocarbons toluene, m-xylene, ethyl benzene, 1,2,4 trimethyl benzene, and methylcyclohexane. The calculated production of oxidized organics appeared well correlated with total particle surface area and volume, suggesting that at least some of the organic compounds formed in gas phase reactions condensed upon the preexisting aerosol. New particle formation was found to be more highly associated with elevated production of gas phase sulfuric acid (via the SO2-OH reaction) than with production of oxidized organic products, although data from one day, during which sulfuric acid production and total aerosol surface area were both lower than usual, provided evidence for the involvement of terpene species in new particle formation. The results suggest that for this continental site, sulfuric acid was probably responsible for most of the observed new ultrafine particle formation. Low-volatility organic compounds may have caused particle formation under the right conditions, but were more likely to condense upon preexisting particles.¿ 1997 American Geophysical Union <