Variability in pesticide deposition and source contributions to snowpack in Western U.S. national parks.

Fifty-six seasonal snowpack samples were collected at remote alpine, subarctic, and arctic sites in eight Western U.S. national parks during three consecutive years (2003-2005). Four current-use pesticides (CUPs) (dacthal (DCPA), chlorpyrifos, endosulfans, and gamma-hexachlorocyclohexane (HCH)) and four historic-use pesticides (HUPs) (dieldrin, alpha-HCH, chlordanes, and hexachlorobenzene (HCB)) were commonly measured at all sites, during all years. The mean coefficient of variation for pesticide concentrations was 15% for site replicate samples, 41% for intrapark replicate samples, and 59% for interannual replicate samples. The relative pesticide concentration profiles were consistent from year to year but unique for individual parks, indicating a regional source effect. HUP concentrations were well-correlated with regional cropland intensity when the effect of temperature on snow-air partitioning was considered. The mass of individual CUPs used in regions located one-day upwind of the parks was calculated using air mass back trajectories, and this was used to explain the distribution of CUPs among the parks. The percent of the snowpack pesticide concentration due to regional transport was high (>75%) for the majority of pesticides in all parks. These results suggest that the majority of pesticide contamination in U.S. national parks is due to regional pesticide use in North America.

Effects of wind and air trajectory directions on atmospheric concentrations of persistent organic pollutants near the Great Lakes.

Three different regression models involving air temperature, time, and either wind direction or parametric or nonparametric air trajectory direction were used with concentrations of four representative persistent organic pollutants to quantitate the atmospheric transport of these compounds to the Great Lakes. The local wind and parametric trajectory models predicted an optimal source direction for each compound, whereas the nonparametric trajectory model was based on a hypothesized source region. All three regressions were used to calculate the factor by which the partial pressures of each compound measured at five sampling sites increased when the air came from a particular source direction. Dieldrin, chlordane, polychlorinated biphenyl, and polycyclic aromatic hydrocarbon partial pressures were used with each of these regressions, and the correlation coefficients (r2) were evaluated for each model, for each compound, and for each regression term. In general, with the exception of polycyclic aromatic hydrocarbons at some sites, the explanatory powers of the regressions were not improved by the inclusion of any of these directional terms.

Influence of local human population on atmospheric polycyclic aromatic hydrocarbon concentrations.

Literature values of atmospheric polycyclic aromatic hydrocarbon (PAH) concentrations from sampling sites around the world were found, and using a high-resolution human population grid, the population within a 25-km radius of each sampling site was calculated. A regression of concentration vs population revealed much about PAH concentration differences among regions as well as site locations within a continent. The best fit for the regression was for sampling locations in North America. A small amount of scatter was present for the regression of all developed countries indicating slight differences in emission regulations or energy usage. The regression from this plot was used as a benchmark for the expected relationship between PAHs and human population. Sites located within 25 km of a coasttended to have concentrations lower than expected, due to dilution with clean ocean air, while sites near industrial outputs or other point sources had higher than expected concentrations. Sites from developing countries typically had PAH concentrations that were far higher than those of the rest of the world.

Potential sources of pesticides, PCBs, and PAHs to the atmosphere of the Great Lakes.

A probabilistic model called the potential source contribution function (PSCF) has been used to estimate atmospheric source regions of polycyclic aromatic hydrocarbons (PAHs), chlorinated pesticides, and polychlorinated biphenyls (PCBs) to the Great Lakes. This model allows us to map each compound's source region on a 0.5 degrees x 0.5 degrees latitude/longitude grid centered over the Great Lakes basin. PCBs primarily have urban sources, the strengths of which vary. Like PCBs, PAHs show a strong urban signature, but these compounds also seem to come from rural sites. The source regions of PAH become less distinct as the molecular weight of the compound increases. Since reactivity increases with PAH size, this diminishing trend may be an indication that atmospheric degradation plays a large role in PAH transport. The pesticides have the strongest source regions and are typically transported the farthest, often from areas distant from the Great Lakes basin.