The modification of physical and chemical properties of aerosols passi
ng through clouds has received considerable attention over recent year
s. Some of these transformations are related to in-cloud chemical reac
tions, particularly the oxidation of sulphur dioxide (SO2) to sulphate
(SO42-). The Great Dun Fell experiment provided an opportunity to inv
estigate the connection between the chemistry within cloud droplets an
d the processing of an aerosol population. We have noted significant i
ncreases in SO42- in the aerosol population downstream of the cloud co
mpared to the aerosol entering the cloud. These increases are connecte
d to both S(IV) oxidation in the liquid phase and to the entrainment o
f new air into the cloud, supplying reactants such as H2O2 to the syst
em. The addition of SO42- mass to the aerosol is also associated with
changes in the NH4+ aerosol concentrations, possibly as a result of ne
utralisation of the acidified cloud droplets by NH3. The study was per
formed taking into account dynamical mixing of air masses as well as p
ossible sampling artefacts. (C) 1997 Elsevier Science Ltd.