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Evidence suggests that boreal-lake ecosystems are changing rapidly, but with variable ecological responses, due to climate warming. Paleolimnological analysis of 27 undeveloped northern forested lakes showed significant and potentially climate-mediated shifts in diatom communities and increased carbon and biogenic silica burial. We hypothesize the sensitivity of northern forested lakes to climate change will vary along two physical gradients: one reflecting direct, in-lake climate effects (propensity to thermally stratify), the other reflecting indirect watershed effects (watershed to lake-surface area ratio). We focus on the historical response of algal communities to test our two-dimensional sensitivity framework. Historical algal response was summarized by measures of diatom community turnover, changes in species and diagnostic species groups, and measures of siliceous algal and overall primary production (biogenic silica, carbon burial). Measures of algal production increased across all lake types, with carbon burial proportionately higher in polymictic lakes. Greater diatom community change occurred in deep, stratified lakes with smaller watersheds, whereas diatom species groups showed variable responses along our two-dimensional sensitivity framework. Physical characteristics of lakes and watersheds could serve as predictors of sensitivity to climate change based on paleo-indicators that are mechanistically linked to direct and indirect limnological effects of climate change.

The spiny water flea (Bythotrephes cederströmii), a freshwater crustacean considered to be the world’s best-studied invasive zooplankter, was first recorded in North America in the Laurentian Great Lakes during the 1980s. Its arrival is widely considered to be the result of ocean-going cargo ships that translocated contaminated ballast water from Eurasia to the Great Lakes during the 1970–1980s. The subsequent first discovery of the species in inland lakes is consistent with the hypothesis that propagules dispersed initially from established Great Lakes populations. Here we present evidence of exoskeletal remains, including mandibles, tail spines, and resting eggs, in 210Pb-dated lake sediment cores, which suggests that B. cederströmii was already resident in four inland North American lakes (two in Minnesota, USA; two in Ontario, Canada) by at least the early 1900s. Densities of exoskeletal remains were low and relatively steady from first appearance until about 1990, after which time they increased in all cores. The earliest evidence that we found was a mandible at 33-cm depth (pre-1650) in the sediments of Three Mile Lake, Ontario, Canada. These unexpected findings challenge the current paradigm of B. cederströmii invasion, renew uncertainty about the timing and sequence of its colonization of North American lakes, and potentially question our ability to detect invasive species with traditional sampling methods. We attempted to eliminate errors in the dated stratigraphies of the exoskeletal remains that might have been introduced either methodologically (e.g., core-wall smearing) or naturally (e.g., bioturbation). Nonetheless, given the very low numbers of subfossils encountered, questions remain about the possible artifactual nature of our observations and therefore we regard our results as ‘preliminary findings’ at this time.

The strongest evidence for anthropogenic alterations to the global mercury (Hg) cycle comes from historical records of mercury deposition preserved in lake sediments. Hg isotopes have added a new dimension to these sedimentary archives, promising additional insights into Hg source apportionment and biogeochemical processing. Presently, most interpretations of historical changes are constrained to a small number of locally contaminated ecosystems. Here, we describe changes in natural Hg isotope records from a suite of dated sediment cores collected from various remote lakes of North America. In nearly all cases, the rise in industrial-use Hg is accompanied by an increase in δ(202)Hg and Δ(199)Hg values. These trends can be attributed to large scale industrial emission of Hg into the atmosphere and are consistent with positive Δ(199)Hg values measured in modern-day precipitation and modeled increases in δ(202)Hg values from global emission inventories. Despite similar temporal trends among cores, the baseline isotopic values vary considerably among the different study regions, likely attributable to differences in the fractionation produced in situ as well as differing amounts of atmospherically delivered Hg. Differences among the study lakes in precipitation and watershed size provide an empirical framework for evaluating Hg isotopic signatures and global Hg cycling.

Significance Elevated mercury in fish poses risks to fish-consuming wildlife and humans. Tracing sources of mercury by analyzing stable isotope ratios leads to improved source-receptor understanding and natural resource management. This work utilizes fish and sediment archives to trace the response to recent domestic mercury mitigation actions. Fish and sediments rapidly responded to a source perturbation contemporaneous with the reduction of mercury in the late 1980s. Subsequently, energetic pathways were altered due to dreissenid invasions, which dampened the expected decrease in fish mercury concentration. These findings reveal the importance of domestic mercury sources relative to global mercury to the Great Lakes. Results also show methylmercury concentrations in fish are sensitive to changes in trophic structure and diet driven by invasive species., To understand the impact reduced mercury (Hg) loading and invasive species have had on methylmercury bioaccumulation in predator fish of Lake Michigan, we reconstructed bioaccumulation trends from a fish archive (1978 to 2012). By measuring fish Hg stable isotope ratios, we related temporal changes in Hg concentrations to varying Hg sources. Additionally, dietary tracers were necessary to identify food web influences. Through combined Hg, C, and N stable isotopic analyses, we were able to differentiate between a shift in Hg sources to fish and periods when energetic transitions (from dreissenid mussels) led to the assimilation of contrasting Hg pools (2000 to present). In the late 1980s, lake trout δ202Hg increased (0.4‰) from regulatory reductions in regional Hg emissions. After 2000, C and N isotopes ratios revealed altered food web pathways, resulting in a benthic energetic shift and changes to Hg bioaccumulation. Continued increases in δ202Hg indicate fish are responding to several United States mercury emission mitigation strategies that were initiated circa 1990 and continued through the 2011 promulgation of the Mercury and Air Toxics Standards rule. Unlike archives of sediments, this fish archive tracks Hg sources susceptible to bioaccumulation in Great Lakes fisheries. Analysis reveals that trends in fish Hg concentrations can be substantially affected by shifts in trophic structure and dietary preferences initiated by invasive species in the Great Lakes. This does not diminish the benefits of declining emissions over this period, as fish Hg concentrations would have been higher without these actions.

The spiny water flea (Bythotrephes cederströmii), a freshwater crustacean considered to be the world’s best-studied invasive zooplankter, was first recorded in North America in the Laurentian Great Lakes during the 1980s. Its arrival is widely considered to be the result of ocean-going cargo ships that translocated contaminated ballast water from Eurasia to the Great Lakes during the 1970–1980s. The subsequent first discovery of the species in inland lakes is consistent with the hypothesis that propagules dispersed initially from established Great Lakes populations. Here we present evidence of exoskeletal remains, including mandibles, tail spines, and resting eggs, in 210Pb-dated lake sediment cores, which suggests that B. cederströmii was already resident in four inland North American lakes (two in Minnesota, USA; two in Ontario, Canada) by at least the early 1900s. Densities of exoskeletal remains were low and relatively steady from first appearance until about 1990, after which time they increased in all cores. The earliest evidence that we found was a mandible at 33-cm depth (pre-1650) in the sediments of Three Mile Lake, Ontario, Canada. These unexpected findings challenge the current paradigm of B. cederströmii invasion, renew uncertainty about the timing and sequence of its colonization of North American lakes, and potentially question our ability to detect invasive species with traditional sampling methods. We attempted to eliminate errors in the dated stratigraphies of the exoskeletal remains that might have been introduced either methodologically (e.g., core-wall smearing) or naturally (e.g., bioturbation). Nonetheless, given the very low numbers of subfossils encountered, questions remain about the possible artifactual nature of our observations and therefore we regard our results as ‘preliminary findings’ at this time.

© 2020 The Authors. This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/ licenses/by/4.0/. Arctic ecosystems are changing in response to recent rapid warming, but the synergistic effects of other environmental drivers, such as moisture and atmospheric nitrogen (N) deposition, are difficult to discern due to limited monitoring records. Here we use geo- chemical analyses of 210 Pb-dated lake-sediment cores from the North Slope of Alaska to show that changes in landscape nutrient dynamics started over 130 years ago. Lake carbon burial doubled between 1880 and the late-1990s, while current rates (~10 g C m−2 yr−1) represent about half the CO2 emission rate for tundra lakes. Lake C burial reflects increased aquatic production, stimulated initially by nutrients from terrestrial ecosystems due to late- 19 th century moisture-driven changes in soil microbial processes and, more recently, by atmospheric reactive N deposition. These results highlight the integrated response of Arctic carbon cycling to global environmental stressors and the degree to which C–N linkages were altered prior to post-1950 regional warming. Faculty yes

The widespread detection of antibiotics in the environment is concerning because antibiotics are designed to be effective at small doses. The objective of this work was to quantify the accumulation rates of antibiotics used by humans and animals, spanning several major antibiotic classes (sulfonamides, tetracyclines, fluoroquinolones, and macrolides), in Minnesota lake-sediment cores. Our goal was to determine temporal trends, the major anthropogenic source to these lacustrine systems, and the importance of natural production. A historical record of usage trends for ten human and/or animal-use antibiotics (four sulfonamides, three fluoroquinolones, one macrolide, trimethoprim, and lincomycin) was faithfully captured in the sediment cores. Nine other antibiotics were not detected. Ofloxacin, trimethoprim, sulfapyridine, and sulfamethazine were detected in all of the anthropogenically-impacted studied lakes. Maximum sediment fluxes reached 20.5 ng cm− 2 yr− 1 (concentration 66.1 ng/g) for ofloxacin, 1.2 ng cm− 2 yr− 1 (1.2 ng/g) for trimethoprim, 3.3 ng cm− 2 yr− 1 (11.3 ng/g) for sulfapyridine, and 1.0 ng cm− 2 yr− 1 (1.6 ng/g) for sulfamethazine, respectively. Natural production of lincomycin may have occurred in one lake at fluxes ranging from 0.4 to 1.8 ng cm− 2 yr− 1 (0.1 to 5.8 ng/g). Wastewater effluent appears to be the primary source of antibiotics in the studied lakes, with lesser inputs from agricultural activities.

Antibiotic chemicals and antibiotic resistance genes enter the environment via wastewater effluents as well as from runoff from agricultural operations. The relative importance of these two sources, however, is largely unknown. The relationship between the concentrations of chemicals and genes requires exploration, for antibiotics in the environment may lead to development or retention of resistance genes by bacteria. The genes that confer resistance to metal toxicity may also be important in antibiotic resistance. In this work, concentrations of 19 antibiotics (using liquid chromatography tandem mass spectrometry), 14 metals (using inductively coupled plasma-mass spectrometry), and 45 metal, antibiotic, and antibiotic-resistance associated genes (using a multiplex, microfluidic quantitative polymerase chain reaction method) were measured in 13 sediment samples from two large rivers as well as along a spatial transect in a wastewater effluent-impacted lake. Nine of the antibiotics were detected in the rivers and 13 were detected in the lake. Sixteen different resistance genes were detected. The surrounding land use and proximity to wastewater treatment plants are important factors in the number and concentrations of antibiotics detected. Correlations among antibiotic chemical concentrations, metal concentrations, and resistance genes occur over short spatial scales in a lake but not over longer distances in major rivers. The observed correlations likely result from the chemicals and resistance genes arising from the same source, and differences in fate and transport over larger scales lead to loss of this relationship.

Field observations suggest that surface-water sulfate concentrations control the distribution of wild rice, an aquatic grass (Zizania palustris). However, hydroponic studies show that sulfate is not toxic to wild rice at even unrealistically high concentrations. To determine how sulfate might directly or indirectly affect wild rice, potential wild rice habitat was characterized for 64 chemical and physical variables in over 100 sites spanning a relatively steep climatic and geological gradient in Minnesota. Habitat suitability was assessed by comparing the occurrence of wild rice with the field variables, through binary logistic regression. This analysis demonstrated that sulfide in sediment porewater, generated by the microbial reduction of sulfate that diffuses or advects into the sediment, is the primary control of wild rice occurrence. Water temperature and water transparency independently control the suitability of habitat for wild rice. In addition to generating phytotoxic sulfide, sulfate reduction also supports anaerobic decomposition of organic matter, releasing nutrients that can compound the harm of direct sulfide toxicity. These results are important because they show that increases in sulfate loading to surface water can have multiple negative consequences for ecosystems, even though sulfate itself is relatively benign.

Edlund MB, Schottler SP, Reavie ED, Engstrom DR, Baratono NG, Leavitt PR, Heathcote AJ, Wilson B, Paterson AM. 2017. Historical phosphorus dynamics in Lake of the Woods (USA–Canada) — does legacy phosphorus still affect the southern basin? Lake Reserv Manage. 33:386–402. A historical phosphorus (P) budget was constructed for southern Lake of the Woods. Sediment cores from 7 bays were radioisotopically dated and analyzed for loss-on-ignition, P, Si, diatoms, and pigments. Geochemical records for cores were combined using focusing factors for whole-basin estimates of sediment, total P, and P fraction accumulation. Although historical monitoring shows that external P loads decreased since the 1950s, sediment P has continued to increase since the mid-20th century. Much sediment P is labile and may be mobile within the sediments and/or available for internal loading and resuspension. Two mass-balance models were used to explore historical P loading scenarios and in-lake dynamics, a static one-box model and a dynamic multi-box model. The one-box model predicts presettlement external loads were slightly less than modern loads. The dynamic model shows that water-column P was higher in the 1950s–1970s than today, that the lake is sensitive to external loads because P losses from burial and outflow are high, and that the lake is moving to a new steady state with respect to water-column P and size of the active sediment P pool. The active sediment pool built up in the mid-20th century has been depleted through outflow and burial, such that its legacy effects are now minimal. Comparison of historical nutrient dynamics and sediment records of algal production showed a counterintuitive increase in production after external P loads decreased, suggesting other drivers may now regulate modern limnoecology, including seasonality of P loading, shifting nutrient limitation, and climate warming.

In Chap. 2 of this volume Lange and Frederick evaluate changes in mercury (Hg) concentrations in Everglades biota to identify the occurrence of temporally coherent trends that ideally can be understood and related to changing process dynamics. To the extent such trends occur in the Everglades, processes that are potentially causative include atmospheric deposition of Hg, changing dynamics in key water quality variables such as sulfate and dissolved organic carbon, and changing hydrology. This overall process of trend identification and elucidation of underlying factors can in turn provide insight on possible strategies for mitigating the problem of excessive biota Hg concentrations in the Everglades. This chapter evaluates whether changes in atmospheric deposition of Hg to the Everglades have occurred in recent years using direct evidence from measured wet deposition and gaseous elemental mercury (GEM). The chapter also considers changes in mercury concentrations recorded in bottom sediments as a proxy for longer-term changes in atmospheric deposition. This latter analysis includes a review of changes observed in aquatic ecosystems from North America and Europe as well as south Florida and the Everglades, and whether recent changes in south Florida reflect large scale processes or reductions in local emissions of Hg.

For the Western North America Mercury Synthesis, we compiled mercury records from 165 dated sediment cores from 138 natural lakes across western North America. Lake sediments are accepted as faithful recorders of historical mercury accumulation rates, and regional and sub-regional temporal and spatial trends were analyzed with descriptive and inferential statistics. Mercury accumulation rates in sediments have increased, on average, four times (4×) from 1850 to 2000 and continue to increase by approximately 0.2μg/m(2) per year. Lakes with the greatest increases were influenced by the Flin Flon smelter, followed by lakes directly affected by mining and wastewater discharges. Of lakes not directly affected by point sources, there is a clear separation in mercury accumulation rates between lakes with no/little watershed development and lakes with extensive watershed development for agricultural and/or residential purposes. Lakes in the latter group exhibited a sharp increase in mercury accumulation rates with human settlement, stabilizing after 1950 at five times (5×) 1850 rates. Mercury accumulation rates in lakes with no/little watershed development were controlled primarily by relative watershed size prior to 1850, and since have exhibited modest increases (in absolute terms and compared to that described above) associated with (regional and global) industrialization. A sub-regional analysis highlighted that in the ecoregion Northwestern Forest Mountains

Eutrophication can initiate sudden ecosystem state change either by slowly pushing lakes toward a catastrophic tipping point beyond which self-reinforcing mechanisms establish an alternate stable state, or through rapid but persistent changes in external forcing mechanisms. In principle, these processes can be distinguished by determining whether historical changes in focal parameters (phytoplankton) exhibit transient (rising then declining) or continuously-elevated variability characteristic of alternate stable states or a “paradox of enrichment,” respectively. We tested this hypothesis in the south basin of Lake Winnipeg, Canada, a site with intense blooms of N2-fixing cyanobacteria since 1990, but for which little is known of earlier limnological conditions, causes of eutrophication, or whether modern conditions represent a alternate stable state. Paleolimnological analysis revealed that the basin was naturally mesotrophic (∼15–20 μg P L−1) with diazotrophic cyanobacteria, productive diatoms, and phosphorus-rich sediments. Eutrophication accelerated during ca.1900–ca.1990, when sedimentary nitrogen, phosphorus and carbon contents increased 10–50%, δ15N enriched 3–4‰, and concentrations of many fossil pigments increased 300–500%. Nearly 75% of 20th century variability was explained by concomitant increases in production of livestock and crops, but not by climate. After ca.1990, the basin exhibited a rapid threefold increase in akinetes from Aphanizomenon and Anabaena spp. and 50% declines in pigments from chlorophytes and cyanobacteria because of sudden socio-economic reorganization of agriculture. Phytoplankton variability quantified using Gaussian generalized additive models increased continuously since the onset of agriculture for bloom-forming taxa, did not decline after state change, and suggested that recovery should not be affected by stable-state hysteresis.

Herbert (‘Herb’) E. Wright, Jr. stands among the most productive and highly recognized Quaternary scientists of all time. Professionally active nearly to the end of his 98 years, he led an amazing scientific career that touched on many of the key questions of recent earth history. He mentored and inspired a very long list of graduate students and visiting scholars. He received some of the highest awards of his scientific discipline, including a Lifetime Achievement Award from the International Paleolimnology Association. All of these accomplishments were coupled with a characteristically quiet and modest style that was both generous and genuine.

Atmospheric deposition is a primary source of reactive nitrogen (Nr) to undisturbed watersheds of the Great Lakes region of the U.S., raising concerns over whether enhanced delivery over recent decades has affected lake ecosystems. The National Atmospheric Deposition Program (NADP) has been measuring Nr deposition in this region for over 35 years. Here we explore the relationships among NADP-measured Nr deposition, nitrogen stable isotopes (δ15N) in lake sediments, and the response of algal communities in 28 lakes situated in national parks of the western Great Lakes region of the U.S. We find that 36% of the lakes preserve a sediment δ15N record that is statistically correlated with some form of Nr deposition (total dissolved inorganic N, nitrate, or ammonium). Furthermore, measured long-term (since 1982) nitrogen biogeochemistry and inferred critical nitrogen loads suggest that watershed nitrogen retention and climate strongly affect whether sediment δ15N is related to Nr deposition in lake sediment records. Measurements of algal change over the last ~ 150 years suggest that Nr deposition, in-lake nutrient cycling, and watershed inputs are important factors affecting diatom community composition, in addition to direct climatic effects on lake physical limnology. The findings suggest that bulk sediment δ15N does reflect Nr deposition in some instances. In addition, this study highlights the interactive effects of Nr deposition and climate variability.

Historical reconstruction of mercury (Hg) accumulation in natural archives, especially lake sediments, has been essential to understanding human perturbation of the global Hg cycle. Here we present a high-resolution chronology of Hg accumulation between 1727 and 1996 in a varved sediment core from the Pettaquamscutt River Estuary (PRE), Rhode Island. Mercury accumulation is examined relative to (1) historic deposition of polycyclic aromatic hydrocarbons (PAHs) and lead (Pb) and its isotopes (206Pb/207Pb) in the same core, and (2) other reconstructions of Hg deposition in urban and remote settings. Mercury deposition in PRE parallels the temporal patterns of PAHs, and both track industrialization and regional coal use between 1850 and 1950 as well as rising petroleum use after 1950. There is little indication of increased Hg deposition from late 19th-century silver and gold mining in the western U.S. A broad maximum of Hg deposition during 1930–1980, and not found in remote sites, is consistent with the pr...

Increased deposition of atmospheric sulfate exacerbates methylmercury (MeHg) production in freshwater wetlands by stimulating methylating bacteria, but it is unclear how methylation in sub-boreal wetlands is impacted by chronically elevated sulfate inputs, such as through mine discharges. The purpose of our study is to determine how sulfate discharges to wetlands from iron mining activities impact MeHg production. In this study, we compare spatial and temporal patterns in MeHg and associated geochemistry in two wetlands receiving contrasting loads of sulfate. Two orders of magnitude less sulfate in the un-impacted wetland create significant differences in acid-volatile sulfide and porewater sulfide; however, dissolved and solid-phase MeHg concentrations and methylation rate potentials (Kmeth) are statistically similar in both wetlands. Permitted mine pumping events flood the sulfate-impacted wetland with very high sulfate waters during the fall. In contrast to observations in sulfate-limited systems, this large input of sulfate to a chronically sulfate-impacted system led to significantly lower potential relative methylation rates, suggesting a predominance of demethylation processes over methylation processes during the sulfate loading. Overall, short-term measurements of methylation and demethylation potential are unrelated to gross measures of long-term MeHg accumulation, indicating a decoupling of short- and long-term process measurements and an overall disequilibrium in the systems. High sulfide accumulation, above ∼600-800 μg l(-1) sulfide, in the sulfate-impacted system lowers long-term MeHg accumulation, perhaps as a result of less bioavailable Hg-S complexes. Although continued research is required to determine how sulfate-limited freshwater wetlands might respond to new, large inputs of high-sulfate runoff from mining operations, chronically impacted wetlands do not appear to continually accumulate or produce MeHg at rates different from wetlands unimpacted by mining.

A series of severe droughts during the course of a long-term, atmospheric sulfate-deposition experiment in a boreal peatland in northern Minnesota created a unique opportunity to study how methylmercury (MeHg) production responds to drying and rewetting events in peatlands under variable levels of sulfate loading. Peat oxidation during extended dry periods mobilized sulfate, MeHg, and total mercury (HgT) to peatland pore waters during rewetting events. Pore water sulfate concentrations were inversely related to antecedent moisture conditions and proportional to past and current levels of atmospheric sulfate deposition. Severe drying events caused oxidative release of MeHg to pore waters and resulted in increased net MeHg production likely because available sulfate stimulated the activity of sulfate-reducing bacteria, an important group of Hg-methylating bacteria in peatlands. Rewetting events led to increased MeHg concentrations across the peatland, but concentrations were highest in peat receiving elevated atmospheric sulfate deposition. Dissolved HgT concentrations also increased in peatland pore waters following drought but were not affected by sulfate loading and did not appear to be directly controlled by dissolved organic carbon mobilization to peatland pore waters. Peatlands are often considered to be sinks for sulfate and HgT in the landscape and sources of MeHg. Hydrologic fluctuations not only serve to release previously sequestered sulfate and HgT from peatlands but may also increase the strength of peatlands as sources of MeHg to downstream aquatic systems, particularly in regions that have experienced elevated levels of atmospheric sulfate deposition.

Lakes may store globally significant quantities of organic carbon (OC) in their sediments, but the extent to which burial rates vary across space and time is not well described. Using 210Pb-dated sediment cores, we explored patterns of OC burial in 116 lakes spanning several ecoregions and land use regimes in Minnesota, USA during the past 150–200 years. Rates for individual lakes (across all time periods) range from 3 to 204 g C m−2 yr−1 (median 33 g C m−2 yr−1) and show strong geographic separation in accordance with the degree of catchment disturbance and nutrient enrichment. Climate and basin morphometry exercise subordinate control over OC burial patterns, and diagenetic gradients introduce little bias to estimated temporal trends. Median burial rates in agricultural lakes exceed urban lakes and have increased fourfold since Euro-American settlement. The greatest increase in OC burial occurred prior to the widespread adoption of industrial fertilizers, during an era of land clearance and farmland expansion. Northern boreal lakes, impacted by historical logging and limited cottage development yet comparatively undisturbed by human activity, bury OC at rates 3X lower than agricultural lakes and exhibit much smaller increases in OC burial. Scaling up modern OC burial estimates to the entire state, we find that Minnesota lakes annually store 0.40 Tg C in their sediments, equal to 1.5% of annual statewide CO2 emissions from fossil fuel combustion. During the period of Euro-American settlement (circa 1860–2000), cumulative OC burial amounted to 36 Tg C, 40% of which can be attributed to anthropogenic enhancement.

Ongoing changes in disturbance regimes are predicted to cause acute changes in ecosystem structure and function in the coming decades, but many aspects of these predictions are uncertain. A key challenge is to improve the predictability of postdisturbance biogeochemical trajectories at the ecosystem level. Ecosystem ecologists and paleoecologists have generated complementary data sets about disturbance (type, severity, frequency) and ecosystem response (net primary productivity, nutrient cycling) spanning decadal to millennial timescales. Here, we take the first steps toward a full integration of these data sets by reviewing how disturbances are reconstructed using dendrochronological and sedimentary archives and by summarizing the conceptual frameworks for carbon, nitrogen, and hydrologic responses to disturbances. Key research priorities include further development of paleoecological techniques that reconstruct both disturbances and terrestrial ecosystem dynamics. In addition, mechanistic detail from disturbance experiments, long-term observations, and chronosequences can help increase the understanding of ecosystem resilience.

Intensive agricultural practices can dramatically change the landscape, thereby increasing the concentrations and rates at which nutrients are delivered to aquatic ecosystems. In the United States, concerns about accelerating rates of lake eutrophication related to increases in nutrient loading require a method of quantifying ecological changes that have occurred since European settlement. Because the application of traditional quantitative total phosphorus transfer functions in paleolimnology has proven difficult in shallow, hypereutrophic lakes, we used several approaches in this study to assess ecosystem changes associated with eutrophication of 32 natural lakes in the state of Iowa, USA. In addition to traditional transfer function methods, we estimated changes in primary productivity from the flux of biogenic silica (BSi) and organic carbon accumulation rates (OC AR). Additionally, we compared pre-disturbance diatom communities to modern diatom communities, i.e. floristic change, using non-metric multi-dimensional scaling and square chord distance. OC AR and BSi fluxes increased over time and were positively correlated with the time period of agricultural intensification in the region (post-1940). Ninety-one percent of the lakes in this study showed evidence for eutrophication based on geochemical proxies, and 88 % of lakes showed major floristic change in the diatom community. Whereas geochemical indicators showed consistent increases in productivity across most lakes, floristic changes reflected more complex interactions between other environmental drivers. The magnitude of floristic change did not directly correlate to nutrient-driven increases in primary production, but was driven by ecological diatom assembly related to lake depth. Transfer functions consistently perform poorly, especially for shallow lakes, and other techniques that combine geochemistry and diatom ecology are recommended for reconstructions of eutrophication.

Human activities over the last several centuries have transferred vast quantities of mercury (Hg) from deep geologic stores to actively cycling earth-surface reservoirs, increasing atmospheric Hg deposition worldwide. Understanding the magnitude and fate of these releases is critical to predicting how rates of atmospheric Hg deposition will respond to future emission reductions. The most recently compiled global inventories of integrated (all-time) anthropogenic Hg releases are dominated by atmospheric emissions from preindustrial gold/silver mining in the Americas. However, the geophysical evidence for such large early emissions is equivocal, because most reconstructions of past Hg-deposition have been based on lake-sediment records that cover only the industrial period (1850-present). Here we evaluate historical changes in atmospheric Hg deposition over the last millennium from a suite of lake-sediment cores collected from remote regions of the globe. Along with recent measurements of Hg in the deep ocean, these archives indicate that atmospheric Hg emissions from early mining were modest as compared to more recent industrial-era emissions. Although large quantities of Hg were used to extract New World gold and silver beginning in the 16th century, a reevaluation of historical metallurgical methods indicates that most of the Hg employed was not volatilized, but rather was immobilized in mining waste.

Sedimentary diatom profiles from saline lakes are frequently used to reconstruct lakewater salinity as an indicator of drought. However, diatom-inferred salinity (DI-salinity) reconstructions from geographically proximal sites in the Great Plains (USA) have yielded disparate results. This study explores how physical changes in lake habitat resulting from drought may affect climate inferences from salinity reconstructions. Differences in relationships among drought, lake-level change, and diatom community structure over the last century were examined for three saline lakes in the northern Great Plains with dissimilar DI-salinity records. At each site, models were developed relating available planktic:benthic (P:B) habitat area to lake-level change, and models were compared with instrumental drought records and fossil diatoms to understand how drought conditions were recorded in sedimentary diatom assemblages. The degree to which DI-salinity tracked drought variation was affected by site-specific physical characteristics that influenced the relationship between lake-level change and P:B habitat zonation within each lake. Moon Lake showed the strongest correlation between drought and DI-salinity, although this relationship was weaker during wetter conditions, as highstands resulted in a larger influx of benthic diatoms. At Coldwater Lake, a dual-basin system, P:B varied depending on lake level, which apparently reduced the correlation between DI-salinity and drought. At Lake Cochrane, the simplest and freshest of the three basins, the P:B of fossil diatoms was a better proxy for drought than DI-salinity. The integration of additional ecological characteristics into interpretations of paleoclimate records, particularly for biologically-based proxies, may improve reconstructions of regional patterns of climate variation.

Southeastern Alaska is a remote coastal-maritime ecosystem that is experiencing increased deposition of mercury (Hg) as well as rapid glacier loss. Here we present the results of the first reported survey of total and methyl Hg (MeHg) concentrations in regional streams and biota. Overall, streams draining large wetland areas had higher Hg concentrations in water, mayflies, and juvenile salmon than those from glacially-influenced or recently deglaciated watersheds. Filtered MeHg was positively correlated with wetland abundance. Aqueous Hg occurred predominantly in the particulate fraction of glacier streams but in the filtered fraction of wetland-rich streams. Colonization by anadromous salmon in both glacier and wetland-rich streams may be contributing additional marine-derived Hg. The spatial distribution of Hg in the range of streams presented here shows that watersheds are variably, yet fairly predictably, sensitive to atmospheric and marine inputs of Hg.

Transfer of nutrients from terrestrial to aquatic ecosystems is a natural process with climatic, biotic, and geologic controls. Recently, increasing concern about human manipulation of global nutrient cycles has required a long-term approach to assessing the nutrient status of aquatic systems. Data available in palaeorecords can assess current trophic status, baseline conditions, and long-term processes controlling nutrient fluxes on decadal to millennial timescales. Here, we review three palaeolimnological methods used to reconstruct nutrient cycling: (1) chemical compounds preserved in lacustrine sediment, (2) aquatic biotic indicators (often using a quantitative transfer function), and (3) quantitative empirical sediment flux estimates. The millennial-scale regulation of nutrient cycling by climate and catchment geochemistry leads to a gradual trajectory of dystrophication over the Holocene in many temperate lakes. In many systems, the magnitude of recent anthropogenic changes to nutrient cycling is la...

It can be advantageous to revisit coring locations in lakes years after an initial paleolimnological study is completed, to assess environmental changes in the intervening time interval. We revisited sediment core sites in Lake Pepin (Minnesota, Wisconsin) more than a decade after an original set of 10 cores was collected, dated radiometrically, and studied in 1996. Prominent magnetic susceptibility features were used to align the new core set with the older set, such that traditional radiometric dating was not necessary to obtain a chronology for the new cores. The procedure used to align the two core sets accounted for compaction of former surface sediments by burial with new sediment. The amount of new sediment, mercury, and phosphorus accumulated at each core site was determined and extrapolated to the depositional area of the lake to estimate recent (1996–2008) whole-basin loads. Recent sediment accumulation in Lake Pepin compared well (within 3%) with monitored inflow data from a gauging station on the upper Mississippi River just before it enters the lake. Bulk sediment accumulation rate remained very high (772,000 t/year) for the recent period (1996–2008), down slightly from the peak in 1990–1996 (876,000 t/year), and almost an order of magnitude above pre-settlement rates. Total phosphorus deposition remained constant since a peak in the 1960s, but was also well above pre-settlement rates. Mercury continued its precipitous decline since peaking in the 1960s.

Rivers in watersheds dominated by agriculture throughout the US are impaired by excess sediment, a significant portion of which comes from non-field, near-channel sources. Both land-use and climate have been implicated in altering river flows and thereby increasing stream-channel erosion and sediment loading. In the wetland-rich landscapes of the upper Mississippi basin, 20th century crop conversions have led to an intensification of artificial drainage, which is now a critical component of modern agriculture. At the same time, much of the region has experienced increased annual rainfall. Uncertainty in separating these drivers of streamflow fuels debate between agricultural and environmental interests on responsibility and solutions for excess riverine sediment. To disentangle the effects of climate and land-use, we compared changes in precipitation, crop conversions, and extent of drained depressional area in 21 Minnesota watersheds over the past 70 years. Watersheds with large land-use changes had increases in seasonal and annual water yields of >50% since 1940. On average, changes in precipitation and crop evapotranspiration explained less than one-half of the increase, with the remainder highly correlated with artificial drainage and loss of depressional areas. Rivers with increased flow have experienced channel widening of 10–40% highlighting a source of sediment seldom addressed by agricultural best management practices. Copyright © 2013 John Wiley & Sons, Ltd.

Our previous work has documented a correlation between Hg concentrations and 210 Pb activity measured in wet deposition that might be used to help apportion sources of Hg in precipitation. Here we present the results of a 27-month precipitation collection effort using co-located samplers for Hg and 210 Pb designed to assess this hypothesis. Study sites were located on the east and west coasts of North America, in the continental interior, and on the Florida Peninsula. Relatively high variability in Hg/ 210 Pb ratios was found at all sites regionally and seasonally (e.g., overall: 0.99–9.13 ng dpm − 1 ). The ratio of average volume-weighted Hg concentrations and 210 Pb activities showed consistent trends (higher in impacted area), with Glacier Bay in southeast Alaska, exhibiting the lowest value. Assuming that Glacier Bay represents a benchmark for a site with no regional contribution, we estimate less than 50% of the Hg input was “global” at the Seattle and Florida sites. Differences in Hg/ 210 Pb in wet deposition could be due to either a regional/local source contribution of Hg, or a regional/local enhancement in the removal of Hg from the atmosphere (i.e., oxidants), however, this approach is not capable of discerning between these two possibilities. Thus, this method of source apportionment represents an estimate of the maximal amount of Hg contributed by regional sources and may be limited in regions of deep convective mixing.

Reavie ED, Edlund MB, Andresen NA, Engstrom DR, Leavitt PR, Schottler S, Cai M. 2017. Paleolimnology of the Lake of the Woods southern basin: continued water quality degradation despite lower nutrient influx. Lake Reserv Manage. 33:369–385. Despite decades of reduced nutrient inputs, Lake of the Woods, a large, shallow boreal lake on the US-Canadian border, shows little evidence of water quality improvements in the pelagic system. Here we analyzed sediments from 6 sites in the southern basin for diverse biogeochemical (loss-on-ignition, biogenic silica, pigments) and microfossil (diatoms, chrysophytes) remains to reconstruct the environmental history of the lake. Our objectives were to quantify the magnitude and direction of historical trophic change and evaluate reasons for an apparent lack of basin recovery following documented nutrient diversion. Evidence came from fossil indicator profiles and comparisons of these long-term trends with historical land use and monitoring data. Results indicate major changes in algal communities during and following peak nutrient loading in the mid-20th century as well as more recent increases in colonial cyanobacteria and high-nutrient diatom taxa. Combined, fossil indicators reflect an anthropogenically enriched system that has undergone substantial ecological change, particularly since ∼1980, due to multiple drivers. Physical changes in lake thermal regime resulting from climate warming may be exacerbating internal phosphorus release from sediments, thereby lowering nitrogen:phosphorus ratios and enhancing cyanobacterial abundance. These drivers of lake condition in the lake may apply to other large shallow lakes that exhibit only limited biological recovery from reduced external nutrient loading.

When discharged into surface waters via wastewater effluents, triclosan, the antimicrobial agent in handsoaps, and chlorinated triclosan derivatives (CTDs, formed during disinfection with chlorine) react photochemically to form polychlorinated dibenzo-p-dioxins. To evaluate the historical exposure of waters to these compounds, the levels of triclosan, CTDs, and their derived dioxins were determined in sediment cores collected from wastewater-impacted Minnesota lakes. The accumulation rates and temporal trends of triclosan, CTDs, and dioxins in aquatic sediments were found to be a function of historical wastewater treatment operations and lake system scale. Cores collected from large-scale riverine systems with many wastewater sources recorded increasing concentrations of triclosan, CTDs, and their derived dioxins since the patent of triclosan in 1964. In small-scale lakes with a single wastewater source, the trends were directly attributed to increased triclosan use, local improvements in treatment, and changes in wastewater disinfection since the 1960s. In the lake with no wastewater input, no triclosan or CTDs were detected. Overall, concentrations of triclosan, CTDs, and their dioxins were higher in small-scale systems, reflecting a greater degree of wastewater impact. In cores collected in northern MN, the four dioxins derived from triclosan are present prior to the patent of triclosan, suggesting a secondary source. It is clear, however, that triclosan and CTDs are the dominant source of these congeners after 1965 in systems impacted by wastewater.

Lake sediments record the flux of materials (nutrients, pollutants, particulates) through a lake system both qualitatively, as changes in the composition of geochemical and biological tracers, as well as quantitatively, through changes in their rate of burial. Burial rates provide a direct link to contemporary (neo-) limnological studies as well as management efforts aimed at load reductions, but are difficult to reconstruct accurately from single cores owing to the spatial and temporal variability of sediment deposition in most lakes. The accurate determination of whole-lake burial rates from analysis of multiple cores, though requiring more effort per lake, can help resolve such problems and improve our understanding of sediment heterogeneity at multiple scales. Partial solutions to these problems also include focusing corrections based on 210Pb flux, co-evaluation of concentration profiles, trend analysis using multiple lakes, and trend replication based on a small number of cores from the same lake. Recent multi-core studies demonstrate that no single core site faithfully records the whole-lake time-resolved input of materials, but that as few as five well-placed cores can provide a reliable record of whole-lake sediment flux for morphometrically simple basins. Lake-wide sediment fluxes can be coupled with reconstructed outflow losses to calculate historical changes in watershed and atmospheric loading of nutrients, metals, and other constituents. The ability of paleolimnology to accurately assess the sedimentary flux and extend the period of reference into the distant past represents an important contribution to the understanding of biogeochemical processes and their response to human and natural disturbance.

In low-sulfate and sulfate-limited freshwater sediments, sulfate loading increases the production of methylmercury (MeHg), a potent and bioaccumulative neurotoxin. Sulfate loading to anoxic sediments leads to sulfide production that can inhibit mercury methylation, but this has not been commonly observed in freshwater lakes and wetlands. In this study, sediments were collected from sulfate-impacted, neutral pH, surface water bodies located downstream from ongoing and historic mining activities to examine how chronic sulfate loading produces porewater sulfide, and influences MeHg production and transport. Sediments were collected over two years, during several seasons from lakes with a wide range of overlying water sulfate concentration. Samples were characterized for in-situ solid phase and porewater MeHg, Hg methylation potentials via incubations with enriched stable Hg isotopes, and sulfur, carbon, and iron content and speciation. Porewater sulfide reflected historic sulfur loading and was strongly related to the extractable iron content of sediment. Overall, methylation potentials were consistent with the accumulation of MeHg on the solid phase, but both methylation potentials and MeHg were significantly lower at chronically sulfate-impacted sites with a low solid-phase Fe:S ratio. At these heavily sulfate-impacted sites that also contained elevated porewater sulfide, both MeHg production and partitioning are influenced: Hg methylation potentials and sediment MeHg concentrations are lower, but occasionally porewater MeHg concentrations in sediment are elevated, particularly in the spring. The dual role of sulfide as a ligand for inorganic mercury (decreasing bioavailability) and methylmercury (increasing partitioning into porewater) means that elucidating the role of iron and sulfur loads as they define porewater sulfide is key to understanding sulfate's influence on MeHg production and partitioning in sulfate-impacted freshwater sediment.

As part of a long-term, peatland-scale sulfate addition experiment, the impact of varying sulfate deposition on bacterial community responses was assessed using 16S tag encoded pyrosequencing. In three separate areas of the peatland, sulfate manipulations included an eight year quadrupling of atmospheric sulfate deposition (experimental), a 3-year recovery to background deposition following 5years of elevated deposition (recovery), and a control area. Peat concentrations of methylmercury (MeHg), a bioaccumulative neurotoxin, were measured, the production of which is attributable to a growing list of microorganisms, including many sulfate-reducing Deltaproteobacteria. The total bacterial and Deltaproteobacterial community structures in the experimental treatment differed significantly from those in the control and recovery treatments that were either indistinguishable or very similar to one another. Notably, the relatively rapid return (within three years) of bacterial community structure in the recovery treatment to a state similar to the control, demonstrates significant resilience of the peatland bacterial community to changes in atmospheric sulfate deposition. Changes in MeHg accumulation between sulfate treatments correlated with changes in the Deltaproteobacterial community, suggesting that sulfate may affect MeHg production through changes in the community structure of this group.

Summary 1. In cultural landscapes, lake response to climate can be masked by land-use change and nutrient loss from their catchments. Palaeolimnological methods were used to reconstruct the ecological response of diatoms in a eutrophic lowland lake (White Lough, Co. Tyrone, Northern Ireland) to altered nutrient P loading and precipitation variability over c. 100 years. 2. 210Pb-dated sediment cores were analysed to determine diatom assemblage variability, biogenic silica concentration, geochemical phosphorus concentration and accumulation rate. Manure P and agricultural N surplus data were collated from documentary sources. Long-term trends in annual temperature and precipitation were derived from the Armagh Observatory. 3. Diatom community turnover from 1890 until c. 1960 was limited, and assemblages were dominated by Aulacoseira subarctica; after this date, changes primarily reflected a eutrophication sequence owing to increased diffuse nutrient inputs associated with intensification of land use (external P loading increased by a factor of three). 4. Diatom and biogenic Si profiles were compared with North Atlantic Oscillation (NAO) records, an index of regional weather patterns. Biogenic Si exhibited a c. 7-year cycle, which tracked a cycle of similar timescale in the Armagh climate record for dry summers. In turn, this cycle was related to the variation in the NAO. 5. Monitoring data from 1971 to 2007 of nitrate exports from the Blackwater River showed that these too followed a roughly 7-year cycle at least up to 2000, in which dry summers were followed by sharp increases in nitrate export. It is argued that diatom production in White Lough reflects the cyclic behaviour in nitrate loading and the constraints that nitrogen availability places on the spring diatom bloom in a lake that is dominated by cyanobacteria.

Data from 104 sediment cores from the Great Lakes and "inland lakes" in the region were compiled to assess historical and recent changes in mercury (Hg) deposition. The lower Great Lakes showed sharp increases in Hg loading c. 1850-1950 from point-source water dischargers, with marked decreases during the past half century associated with effluent controls and decreases in the industrial use of Hg. In contrast, Lake Superior and inland lakes exhibited a pattern of Hg loading consistent with an atmospheric source - gradual increases followed by recent (post-1980) decreases. Variation in sedimentary Hg flux among inland lakes was primarily attributed to the ratio of watershed area:lake area, and secondarily to a lake's proximity to emission sources. A consistent region-wide decrease (∼20%) of sediment-Hg flux suggests that controls on local and regional atmospheric Hg emissions have been effective in decreasing the supply of Hg to Lake Superior and inland lakes.

The effect of eutrophication on particulate amorphous silica (ASi) sequestration was isolated and quantified in Lake St. Croix and Lake Pepin, two natural, human-impacted impoundments of the upper Mississippi River. In contrast to impoundments behind engineered dams, where silica (Si) fluxes may be changed by various aspects of dam construction, these two riverine lakes have long (9,000+ years) sedimentary sequences that record the entire span of cultural eutrophication and the resulting silica sequestration. The concentrations of dissolved silicate (DSi) and ASi in the lake inflows were measured for 1 year to obtain the total flux of bioavailable silica (TSib = DSi + ASi) to each impoundment. Historical rates of Si sequestration in each lake were determined using ASi burial in multiple sediment cores and modeled estimates of historical TSib fluxes. The Si trapping efficiency of each lake was found to have increased exponentially with cultural eutrophication (estimated two- to fivefold increase in Lake St. Croix and 9- to 16-fold increase in Lake Pepin over the last 100 years), indicating the degree to which eutrophication of impoundments can reduce silica export to downstream coastal and marine ecosystems. Because these two lakes presently exhibit different degrees of eutrophication, together they depict a relationship between phosphorus concentration and Si trapping efficiency that may be applied to other impoundments, including human-made reservoirs.

We dated a continuous, similar to 22-m long sediment sequence from Lake Challa (Mt. Kilimanjaro area, Kenya/Tanzania) to produce a solid chronological framework for multi-proxy reconstructions of climate and environmental change in equatorial East Africa over the past 25,000 years. The age model is based on a total of 168 AMS C-14 dates on bulk-organic matter, combined with a Pb-210 chronology for recent sediments and corrected for a variable old-carbon age offset. This offset was estimated by i) pairing bulk-organic C-14 dates with either Pb-210-derived time markers or C-14 dates on grass charcoal, and ii) wiggle-matching high-density series of bulk-organic C-14 dates. Variation in the old-carbon age offset through time is relatively modest, ranging from similar to 450 yr during glacial and late glacial time to similar to 200 yr during the early and mid-Holocene, and increasing again to similar to 250 yr today. The screened and corrected C-14 dates were calibrated sequentially, statistically constrained by their stratigraphical order. As a result their constrained calendar-age distributions are much narrower, and the calibrated dates more precise, than if each C-14 date had been calibrated on its own. The smooth-spline age-depth model has 95% age uncertainty ranges of similar to 50-230 yr during the Holocene and similar to 250-550 yr in the glacial section of the record. The delta C-13 values of paired bulk-organic and grass-charcoal samples, and additional C-14 dating on selected turbidite horizons, indicates that the old-carbon age offset in Lake Challa is caused by a variable contribution of old terrestrial organic matter eroded from soils, and controlled mainly by changes in vegetation cover within the crater basin. (C) 2011 Elsevier Ltd. All rights reserved.

The Nebraska Sand Hills are a distinctive eco-region in the semi-arid Great Plains of the western United States. The water table underlying the Sand Hills is part of the High Plains/Ogallala aquifer, an important water resource for the central Great Plains. Lake levels are affected directly by fluctuations in the water table, which is recharged primarily by local precipitation and responds quickly to climatically induced changes in regional water balance. Instrumental records are available for only 50–100 years, and paleolimnological data provide important insights into the extremes and variability in moisture balance over longer time scales. A set of 69 lakes from across Nebraska was used to establish a statistical relationship between diatom community composition and water depth. This relationship was then used to develop a diatom-based inference model for water depth using weighted averaging regression and calibration techniques. Development of the inference model was complicated by strong intra-seasonal variability in water depth and the linkages between depth and other limnologic characteristics, including alkalinity, water clarity and nutrient concentrations. Analysis of historical diatom communities from eight lakes allowed for the reconstruction of lake-level fluctuations over the past several thousand years. Comparisons of the more recent portion of these reconstructions with the instrumental Palmer Drought Severity Index (PDSI) showed that sediment records may not faithfully reflect short-term fluctuations in water level, except where sedimentation rates are very high. However, large and persistent changes in moisture availability were discernible even in longer, low-resolution records. Thus, diatoms are a useful addition to the tools available for understanding past drought in the central Great Plains, especially when trajectories of change are constrained by data from multiple sites or other proxies.

Tropical alpine areas may be highly sensitive to climate change. Yet, because high-resolution palaeoenvironmental studies in these regions are scant, patterns of environmental change over the last few centuries, and linkages with regional changes, remain poorly resolved. This article presents a 400-year palaeolimnological record from Lower Kitandara Lake (3,989 m above m.a.s.l.), located in the Rwenzori Mountains of Uganda, where marked glacial recession has been recorded over much of the twentieth century. An age model is produced for a 57.5 cm sediment core based on 210Pb and 14C dating, suggesting a basal date of approximately 1600 AD. Diatom and organic geochemistry (%TOC, C/N ratios, δ13C) analyses are carried out at an approximately decadal resolution. Twentieth-century glacial recession does not appear to have significantly impacted either the diatom or geochemical records. However, large ecological changes have occurred during the past 400 years, particularly shown by the diatom fluxes and geochemical data. Throughout the core, the diatom record reveals only minor changes in assemblage composition, which may be related to the dominance of Staurosira construens var. venter in the lake’s diatom flora, a tychoplanktonic taxon which is highly adaptive to environmental change. Geochemical analyses, however, reveal a marked change at around the end of the eighteenth century, when C/N ratios suggest an increase in the dominance of algal aquatic sources to lacustrine organic matter, concomitant with a stabilisation of catchment inputs and increased diatom productivity, which may have been caused by reduced glacial inputs. The relationship between these changes at Lower Kitandara Lake and wider regional climate change that occurred at the end of the eighteenth century is not well understood, but this study highlights the need for additional research to link drivers of alpine ecosystem change with those operating at low altitudes.

We report estimates of mercury (Hg) flux to the sediments of Lake Tahoe, California–Nevada: 2 and 15–20 µg/m2/year in preindustrial and modern sediments, respectively. These values result in a modern to preindustrial flux ratio of 7.5–10, which is similar to flux ratios recently reported for other alpine lakes in California, and greater than the value of 3 typically seen worldwide. We offer plausible hypotheses to explain the high flux ratios, including (1) proportionally less photoreduction and evasion of Hg with the onset of cultural eutrophication and (2) a combination of enhanced regional oxidation of gaseous elemental Hg and transport of the resulting reactive gaseous Hg to the surface with nightly downslope flows of air. If either of these mechanisms is correct, it could lead to local/regional solutions to lessen the impact of globally increasing anthropogenic emissions of Hg on Lake Tahoe and other alpine ecosystems.