Date of Award

8-2007

Level of Access Assigned by Author

Campus-Only Dissertation

Degree Name

Doctor of Philosophy (PhD)

Department

Ecology and Environmental Sciences

Advisor

Cynthia S. Loftin

Second Committee Member

Jeffrey S. Kahl

Third Committee Member

Ivan J. Fernandez

Abstract

This dissertation examined major ion and mercury (Hg) atmospheric deposition and winter Hg mobility in forested watersheds at Acadia National Park. Throughfall fluxes of Hg and major ions were estimated using several methods in paired research watersheds with contrasting vegetation, and compared the results to the literature. Conifer forested sites had greater snow Hg concentration (19.5±7.7 ng/L) and deposition (27.8±11.7 ng/m2/yr) than deciduous (concentration: 5.85±2.6 ng/L, deposition: 9.77±6.4 ng/m2/yr) or non-vegetated (concentration: 4.33±2.1 ng/L, deposition: 6.39±4.3 ng/m2/yr) sites. The ratios of Hg in throughfall to open deposition in snowpack (ratio=2.1) and snow events (ratio=3.8) were greater than the throughfall to wet deposition ratio (1.8) during growing season as reported in the literature. This unexpected result indicates that enhancement of dry deposition by forest canopies is at least as important during winter months as during the growing season. However, estimates of Hg in snow throughfall deposition varied by up to a factor of two depending on the frequency of sampling and collection method. Individually sampled snow events had the greatest Hg deposition (3.11±0.54 ng/m2/cold season), and snow left open to the atmosphere for the entire winter (“seasonal” snow) had the least (1.16±0.21 ng/m2/cold season). Using labeled Hg tracer additions, we found that snowpack contained Hg contributed from underlying litter and soils, and its Hg burden was intermediate (2.38±0.68 ng/m2/cold season) between seasonal and event snow Hg. These findings suggest that previous research at other sites has documented low Hg burdens in snow because of un-measured losses to the atmosphere. To place these winter Hg findings in context, I developed a conceptual model explaining throughfall flux at Acadia using marine tracers, coherence analysis, and spatial autocorrelation. In winter, throughfall chemistry showed a strong a marine air mass signal (wet-only precipitation sulfate: chloride=1.36), which contrasted dramatically with the summer signal sulfate: chloride=10.2). Spatial analysis indicated that precipitation amount was more variable and had a different spatial pattern in winter than in summer. The coherence analysis indicated that vegetation type was the primary influence on concentration and throughfall flux of most analytes during the growing season.

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