The chemistry of cloud multiphase systems was studied within the Klein
er Feldberg Cloud Experiment 1990. The clouds encountered during this
experimental campaign could be divided into two categories according t
o the origin of air masses in which the clouds formed. From the chemic
al point of view, clouds passing the sampling site during the first pe
riod of the campaign (26 October-4 November) were characterized by low
er pollutant loading and higher pH, as compared to clouds during the f
inal period of the experimental campaign (10-13 November). The study o
f multiphase partitioning of the main chemical constituents of the clo
ud systems and of atmospheric acidity within the multiphase systems th
emselves (gas + interstitial aerosol + liquid droplets) are presented
in this paper. A general lack of gaseous NH3 was found in these cloud
systems, which caused a lack of buffer capacity toward acid addition.
Evidence supports the hypothesis that the higher acidity of the cloud
systems during this final period of the campaign was due to input of H
NO3. Our measurements, however, could not determine whether the observ
ed input was due to scavenging of gaseous HNO3 from the air feeding in
to the cloud, or to heterogeneous HNO3 formation via NO2 oxidation by
O-3 to NO3 and N2O5. Sulfate in cloud droplets mainly originated from
aerosol SO42- scavenging, since S(IV) to S(VI) liquid phase conversion
was inhibited due to both lack of H2O2 and low pH of cloud droplets,
which made O-3 and metal catalyzed S(IV) oxidation inefficient.