Samples of fog and cloud drops were collected by drop size from severa
l locations around the United States. Sites were selected to represent
a variety of cloud types (coastal stratus clouds, frontal clouds, and
radiation fog) as well as both clean and polluted environments. A siz
e-fractionating version of the Caltech Active Strand Cloudwater Collec
tor (sf-CASCC) and a two-stage Eidgenossische Technische Hochschule (E
TH) cloud impactor were each used to simultaneously collect small and
large cloud drop fractions. The sf-CASCC is designed to collect drops
> 23 mu m in diameter in the large fraction and drops between 4 and 23
mu m in the small fraction, while the ETH impactor is typically confi
gured to collect drops > 10 mu m in diameter and drops between 3 and 1
0 mu m in diameter in its two size fractions. Concentrations of sulfat
e and ammonium were typically observed to be enriched in small cloud d
rops. A similar pattern was observed for nitrate at several locations.
Coarse mode aerosol species were often observed to be enriched in lar
ge cloud drops. These findings suggest that the size-dependent chemica
l signature of the precursor aerosol particle size distribution is at
least partially maintained in the cloud drop size spectrum. The observ
ed size dependence of the cloud drop composition can enhance rates of
aqueous phase sulfate production relative to expectations based on ave
rage cloud drop composition, bias efficiencies with which individual c
hemical species are incorporated into precipitation within clouds, and
affect patterns of chemical deposition to plant canopies or within th
e respiratory tract.