A climatology of cloud chemistry for the eastern United States derived from the mountain cloud chemistry project

Abstract
The chemical composition of clouds collected in the eastern United States has been intensely monitored over a 4-year period as part of the Mountain Cloud Chemistry Project. On the basis of these measurements we prepared a climatology for cloud chemistry, using simple statistical analyses tools and incorporating meteorological and cloud physical and chemical information. Five mountain stations have been established for cloud collection covering the northern and southern Appalachian Mountain range: Whiteface Mountain, New York; Mount Moosilauke, New Hampshire; Shenandoah Mountain, Virginia; Whitetop Mountain, Virginia; and Mount Mitchell, North Carolina. This review presents the major result from this 4-year measurement program. Cloud cover and cloud base over the eastern United States were deduced from the global real-time nephanalysis archives produced by the U.S. Air Force, augmented by local observations. Both active and passive cloud collectors were deployed to sample cloud water on an hourly basis, i.e., with sufficient time resolution to resolve synoptic scale phenomena. Chemical analysis of cloud water was performed by a central analytical laboratory with occasional on-site analysis to satisfy quality control procedures. Reliable methods now exist for collecting cloud-water samples in sufficient quantities for detailed chemical analysis. The chemical composition of cloud water varied significantly between sites. However, the differences in cloud-water ion concentration do not necessarily establish a geographic gradient between the sites but rather reflect differences in air-mass trajectories associated with the synoptic air-flow pattern and differences in sample location above cloud base. The dependence of cloud-water ion concentrations on synoptic weather type and observed differences in relative frequencies of warm sector, marine flow, and post-cold frontal synoptic types between northern and southern sites suggest that the north–south differences in cloud-water ion concentrations are related to cloud climatology at the northern sites. When air-mass trajectories shift from southwest to northwest, the concentrations of H+, SO42−, NO3 and NH4+ normally decrease but the southern sites continue to receive high concentrations under northwest flow. The height of cloud-water sample collection above cloud base was found to be an additional source of variability in both cloud-water chemistry and liquid-water content. Seasonal variation in cloud-water chemical composition was investigated at one site only. Sulfate levels were found to be significantly lower in supercooled clouds (i.e., during the 'cold' season) than in 'warm' clouds, but nitrate levels remained about the same.Key words: cloud chemistry, cloud frequency, air-mass trajectories, ANOVA.