Heterogeneous chemistry in aircraft wakes: Constraints for uptake coefficients

Recent in situ measurements in subsonic and supersonic aircraft plumes show the presence of high aerosol abundances. Given the large initial surface areas of the exhaust particles (volatile aerosols, soot, and ice) of 10(3) - 10(5) mu m(2) cm(-3) or more, heterogeneous processing can potentially become important. Based on an analytical model to predict the temporal evolution of the surface areas, the potential for heterogeneous chemistry during the lifetime of single aircraft wakes is investigated. The model surface areas are constrained by plume observations and compared to numerical simulations of aerosol formation and growth. Efficient heterogeneous processing on volatile aerosols and soot on timescales below I day generally requires uptake coefficients greater than or similar to 0.003 - 0.007, depending on the specific surface area of soot. For low available surface areas and slow reactions, the lifetime of emitted exhaust species sensitively depends on the wake mixing properties. Shutting off uptake by volatile particles inhibits heterogeneous processing unless high soot surface areas and reaction probabilities are prescribed. Depending on the lifetime of ice contrails, uptake coefficients greater than or similar to 0.1 are required for rapid uptake of exhaust species on the ice particles. This lower limit becomes relaxed if contrails are long-lived or develop into persistent cirrus or polar stratospheric clouds, rendering activation of chlorine potentially important. The model is applied to investigate the uptake of gaseous HNO2 and SO2 by the observed particles in the plume of the Concorde in the lower stratosphere.