Chronologies of Pb, polycyclic aromatic hydrocarbons (PAHs), Al, carbon, and n-alkanes in pelagic sediments of Crystal Lake, a precipitation-dominated seepage lake in north-central Wisconsin, were determined to investigate the geochemistry of sediments derived from atmospheric deposition and to evaluate the impact of environmental changes in the region on the geochemistry of this oligotrophic lake. Concentrations of Pb and combustion-derived PAHs in Crystal Lake sediments have increased by factors of 8 and 3, respectively, over the past 150 years. In contrast, levels of perylene increased with depth in the sediment, indicating that postdepositional formation of this PAH might be occurring. Atmospheric fluxes of anthropogenic Pb and combustion-derived PAHs were estimated to be 10,000 g m Ϫ2 a Ϫ1 and 34 g m Ϫ2 a Ϫ1 , respectively. The settling sediment fluxes of planktonic n-alkanes (⌺ C 15 , C 17 , C 19 ) and terrestrial n-alkanes (⌺ C 25 , C 27 , C 29 , C 31 ) in Crystal Lake were 4,400 g m Ϫ2 a Ϫ1 and 10,500 g m Ϫ2 a Ϫ1 , respectively, whereas their accumulation rates in pelagic sediments were 270 g m Ϫ2 a Ϫ1 and 7,100 g m Ϫ2 a Ϫ1 , respectively. The large difference between the settling sediment flux and the accumulation rate of the planktonic n-alkanes in the sediments is ascribed to microbial degradation during or soon after deposition. In contrast, the terrestrial n-alkanes are incorporated in a wax matrix and are protected from degradation. The contribution of terrestrial n-alkanes to the organic carbon of the sediments has remained relatively constant over the past 150 years. About 20% of the organic carbon that is incorporated in the present-day sediments of Crystal Lake can be attributed to the deposition of pine pollen in the lake. Deforestation of the region in the late 1800s apparently caused terrigenous inputs and primary productivity of nonsiliceous plankton to increase, because planktonic and terrestrial n-alkane concentrations in the sediment increased at about the same time. However, since about 1900 concentrations of organic carbon and of terrestrial and planktonic n-alkanes in Crystal Lake sediments have decreased, and concentrations of Al and combustion-derived PAH have increased. These occurrences might reflect a decrease in pollen dispersal in the region and an increase in the atmospheric deposition of fly ash from coal-burning power plants.The pelagic sediments of precipitation-dominated seepage lakes provide a unique opportunity to study the chronology and preservation of atmospherically and internally derived chemical species. Seepage lakes have no surface water inlets or outlets and receive water exclusively from precipitation and groundwater, so that allochthonous (external) sources of organic matter are restricted to the atmosphere, surface runoff, and groundwater. Autochthonous (internal) sources of organic matter in seepage lakes include plankton, bacteria, 1 Corresponding author (pvdoskey@anl.gov).
AcknowledgmentsWe thank the Trout Lake Biological Station of the University ...