The cycle of waterborne methylmercury (meHg) in Little Rock Lake is characterized by a period of accumulation during summertime (when the lake is warm and open to the atmosphere) and a period of decline during winter (when the lake is sealed by ice). We followed this cycle for 16 yr, during which time the lake was acidified with H 2 SO 4 and then allowed to recover naturally as part of a long-term field experiment on acidic rain. Mass balance was used to quantify meHg sources and sinks during acidification and recovery. Although year-to-year variability in the summertime accumulation of meHg was high during both acidified and de-acidified years (C.V. ϭ 0.7 and 0.5, respectively), on average 65% more meHg accumulated in the water column during acidification. Most of the meHg mass accumulated in the anoxic hypolimnion (Ͼ70%), even though the hypolimnion constituted Ͻ5% of the lake volume. In hypolimnetic waters, we observed a direct correlation between the maximum meHg concentration and the sulfate deficit for each year (r 2 ϭ 0.5-0.9) and a direct correlation between meHg and sulfide concentrations (r 2 ϭ 0.7). Sulfide was directly related to dissolved organic carbon at concentrations between 300 and 600 mol L Ϫ1 carbon (C). Seasonal changes in waterborne Hg (II) , meHg, and sulfate reduction covaried with the atmospheric deposition of Hg (II) and SO . Across all years, the interaction term [SO ϫ Hg (II) ] explained 70% of the variationin the meHg accumulation rate during summer. These results indicate that meHg production was co-mediated by several simultaneously occurring processes that affect the supply of Hg (II) substrate to the anoxic hypolimnion and the activity of methylating bacteria that are present there. They imply that meHg levels in lakes may respond to future changes in atmospheric Hg deposition in a rapid but complex way, modulated by environmental variables that can interact synergistically with Hg (II) supply. Such variables include sulfate in acid rain, organic carbon in terrestrial runoff, and temperature.Acid rain and methylmercury (meHg) contamination emerged as limnological issues during the 1970s, but it was not until the late 1980s that both were linked to atmospheric deposition and widespread human perturbation of the sulfur and mercury cycles. A direct connection between acid deposition and the aquatic meHg cycle was first indicated by early synoptic surveys that documented strong negative correlations between lake water pH and the concentration of meHg in fish (Spry and Wiener 1991; Wiener and Spry 1996). Today, pH remains the strongest environmental cor-1 Corresponding author (cjwatras@wisc.edu).
AcknowledgmentsWe thank Nick Bloom, Emily Greenberg, Steve Claas, Beth Kuhn, Rick Back, Vanessa Visman, Jeff Rubsam, Lana Fanberg, Bruce Rodger, and many others for assistance throughout this longterm project. Mercury analyses prior to 1993 were conducted at Frontier Geosciences, Seattle, Washington.