New observations taken in aircraft wakes, including the DLR ATTAS, provide strong constraints on models of aircraft plume aerosols. Using a comprehensive microphysics code, we have performed sensitivity studies to identify the key microphysical mechanisms acting in such plumes. Analysis of these simulations reveals that the largest volatile plume particles-those most likely to contribute to the background abundance of condensation nuclei-are dominated by ion-mode particles when chemiions are included. Moreover, such modeling demonstrates that standard treatments of plume microphysics-in the absence of chemiions-fails to explain field measurements. The principal factor controlling the population of ultrafine plume particles is the number of chemiions emitted by the aircraft engines. Since the ions are a byproduct of the combustion itself, and their abundance in the exhaust stream is controlled by ion-ion recombination, the initial ion concentrations-and so the eventual emission indices for ion-mode particles-are expected to be relatively invariant. Our results indicate that reductions in fuel sulfur content, while not likely to lower the total number of volatile particles emitted, would decrease the size of the ion-mode particles in fresh aircraft wakes, reducing their atmospheric lifetimes and potential environmental effects. ¿ 1998 American Geophysical Union