Daniel R. Engstrom

Evaluation of large lake response to centennial changes in land use and climate can be complicated by high spatial and hydrological complexity within their catchments, particularly in regions of low relief. Furthermore, large lakes can exhibit abrupt changes in structure and function that obscure causes of eutrophication. We provide the first quantification of historical trends in lake production, cyanobacterial abundance, sediment geochemistry and diatom composition since c. 1800 in Lake Manitoba, the 29th largest lake in the world, and compared them to Lake Winnipeg, a morphologically similar, adjacent basin with a 10‐fold larger catchment and an abrupt increase in production around 1990. Before 1900, Lake Manitoba was mesotrophic, with low sedimentary concentrations of carbon, phosphorus, nitrogen, cyanobacteria and algal pigments, as well as assemblages of low‐light‐adapted benthic diatoms. Analysis of pigment time‐series with hierarchical generalised additive models revealed that Lake Manitoba eutrophied during 1900–1930 as a consequence of the development of intensive agriculture within its local catchment, but thereafter exhibited stable cyanobacterial densities with limited expansion of N₂‐fixing cyanobacteria despite persistent eutrophication. Lake Manitoba did not undergo an abrupt change as seen in Lake Winnipeg. These findings suggest that catchment size had little influence on water quality degradation and that nutrient influx from proximal agricultural sources was sufficient to initially degrade these large prairie lakes. The abrupt change in Lake Winnipeg around 1990 required additional intensification of local land use that did not occur in the Lake Manitoba catchment.

Changes in sulfate (SO₄^2-) deposition have been linked to changes in mercury (Hg) methylation in peatlands and water quality in freshwater catchments. There is little empirical evidence, however, of how quickly methyl-Hg (MeHg, a bioaccumulative neurotoxin) export from catchments might change with declining SO₄^2- deposition. Here, we present responses in total Hg (THg), MeHg, total organic carbon, pH, and SO₄^2- export from a peatland-dominated catchment as a function of changing SO₄^2- deposition in a long-term (1998-2011), whole-ecosystem, control-impact experiment. Annual SO₄^2- deposition to half of a 2-ha peatland was experimentally increased 6-fold over natural levels and then returned to ambient levels in two phases. Sulfate additions led to a 5-fold increase in monthly flow-weighted MeHg concentrations and yields relative to a reference catchment. Once SO₄^2- additions ceased, MeHg concentrations in the outflow streamwater returned to pre-SO₄^2- addition levels within 2 years. The decline in streamwater MeHg was proportional to the change in the peatland area no longer receiving experimental SO₄^2- inputs. Importantly, net demethylation and increased sorption to peat hastened the return of MeHg to baseline levels beyond purely hydrological flushing. Overall, we present clear empirical evidence of rapid and proportionate declines in MeHg export from a peatland-dominated catchment when SO₄^2- deposition declines.

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 geochemical analyses of ²¹⁰Pb-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.

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 δ²⁰²Hg and Δ¹⁹⁹Hg values. These trends can be attributed to large-scale industrial emission of Hg into the atmosphere and are consistent with positive Δ¹⁹⁹Hg values measured in modern-day precipitation and modeled increases in δ²⁰²Hg 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.

Lakes have a disproportionate effect on the global carbon (C) cycle relative to their area, mediating C transfer from land to atmosphere, and burying organic-C in their sediments. The magnitude and temporal variability of C burial is, however, poorly constrained, and the degree to which humans have influenced lake C cycling through landscape alteration has not been systematically assessed. Here, we report global and biome specific trajectories of lake C sequestration based on 516 lakes and show that some lake C burial rates (i.e., those in tropical forest and grassland biomes) have quadrupled over the last 100 years. Global lake C-sequestration (~0.12 Pg year⁻¹) has increased by ~72 Tg year⁻¹ since 1900, offsetting 20% of annual CO₂ freshwater emissions rising to ~30% if reservoirs are included and contributing to the residual continental C sink. Nutrient availability explains ~70% of the observed increase, while rising temperatures have a minimal effect.

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.

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 predicted influence of additional industrial sources and commercial products. Our results imply that a significant portion of global anthropogenic Hg emissions during the 20th century was deposited locally, near urban and industrial centers of Hg use and release.

Climate disrupts aquatic ecosystems directly through changes in temperature, wind, and precipitation, and indirectly through watershed effects. Climate-induced changes in northern lakes include longer ice-free season, stronger stratification, browning, shifts in algae, and more cyanobacterial blooms. We compared retrospective temperature-depth relationships modeled using MINLAKE2012 with biogeochemical changes recorded in sediment cores. Four lakes in Voyageurs National Park (VOYA) and four lakes in Isle Royale National Park (ISRO) were studied. Meteorological data from International Falls and Duluth, Minnesota, were used for VOYA and ISRO, respectively. Model output was processed to analyze epilimnetic and hypolimnetic water temperatures and thermal gradients between two periods (1962–1986, 1987–2011). Common trends were increased summer epilimnion temperatures and, for deep lakes, increased frequency and duration of thermoclines. Changes in diatom communities differed between shallow and deep lakes and the parks. Based on changes in benthic and tychoplanktonic communities, shallow lake diatoms respond to temperature, mixing events, pH, and habitat. Changes in deep lakes are evident in the deep chlorophyll layer community of Cyclotella and Discostella species, mirroring modeled changes in thermocline depth and stability, and in Asterionella and Fragilaria species, reflecting the indirect effects of in-lake and watershed nutrient cycling and spring mixing.