Foliar accumulation of mercury has been demonstrated to occur as plants leaf out, yet the primary source of this mercury is not known. Using closed-system growth chambers, uptake of mercury by quaking aspen (Populus tremuloides) foliage was measured over time as a function of soil mercury concentrations (0.01, 6.2, and 25.6 microg/g) and atmospheric mercury exposure concentrations (1.4, 14.9, and 68.5 ng/m3). Foliar mercury concentrations increased as a function of time for all exposures. Twice during the experiment, leaf washes were analyzed for mercury to assess surface deposition, and little mercury was removed (0.02-0.04 ng/m2), suggesting that direct deposition to the leaf surface was not significant during this experiment. At the end of the four-month experiment, whole-plant mercury concentrations were determined. It was found that whereas mercury in the atmosphere primarily influenced foliar uptake, root concentrations were related to the soil mercury concentration. The implication of this study is that litterfall may serve as a pathway for new, atmospherically derived mercury to be deposited to forest soils. This has significant implications for watershed management of ecosystems where mercury is of concern.