The impacts of whole-lake acidification and eutrophication on the accumulation of lead in sediments from manipulated lakes in the Experimental Lakes Area (IISD-ELA).

Acidification and eutrophication are common limnological stressors impacting many water bodies across the globe. While the negative impacts of these stressors on limnetic communities are generally known, their influence on the accumulation of specific sediment constituents, such as metals, remains unclear. Benefitting from past research and long-term monitoring, lakes at the International Institute for Sustainable Development - Experimental Lakes Area (IISD-ELA) in northwestern Ontario, Canada are invaluable to understand the extent to which these two common lake stressors can influence the accumulation of metals in lacustrine sediment. To address these issues, sediment cores were retrieved from six lakes: four were subjected to past experimental acidification or eutrophication and two were reference lakes. Focusing on elemental lead (Pb), a metal known to have accumulated in lake sediments worldwide and generally exhibiting a relatively small fraction of terrigenous input, we assessed the hypothesis that greater accumulation of Pb would be observed in lakes subjected to eutrophication, while the reverse was expected for lakes subjected to acidification experiments. Our analyses support this hypothesis, whereby relatively low enrichment was recorded in sediments deposited in the acidified lake during the manipulation era. On the other hand, eutrophied lakes demonstrated a strong enrichment in Pb during experimental manipulation. When investigating the mechanisms behind these divergent responses, we found epilimnetic dissolved organic carbon (DOC) and conductivity were associated with a relative increase in Pb accumulation in sediments. Acidic pH is also expected to mediate these responses by decreasing epilimnetic DOC concentrations leading to reduced Pb accumulation in the sediment.

Developing diatom-based inference models to assess lake ecosystem change along a gradient of metal smelting impacts: Sudbury lakes revisited.

Mining and smelting activities have strongly influenced the Sudbury region (Ontario, Canada) since the late 19th century, leading to acidification and metal contamination in many local ecosystems. Regulations on restricting acidic emissions were enacted in the 1970s, after which a considerable volume of paleolimnological work was completed to study the impacts of acidification on Sudbury-region lakes and their subsequent biological recovery. Twenty years after the last regional diatom-based assessment, many lakes have undergone large changes in limnological variables, including increases in pH and dissolved organic carbon concentrations, as well as decreases in metal concentrations. Additionally, these lakes are under the potential impacts of newly emerging environmental stressors such as climate warming and road salt contamination. Here, we revisited a suite of Sudbury-region lakes (n = 80) to examine the relationships between their current water chemistry and diatom assemblages preserved in surface sediments using a canonical correspondence analysis. Although the pH gradient in our study lakes is shorter (pH ~1.4) than in earlier calibration studies conducted in this region, lake water pH was still identified as the strongest environmental variable shaping diatom distributions and was used to construct a robust inference model (R2boot = 0.73; RMSEP = 0.32). By assessing ecological changes experienced by a subset of these Sudbury-region lakes (n = 33) over the past few decades, we identified two major trends: an overall increase in diatom-inferred pH and a rise in the relative abundance of planktonic taxa. Our study provides useful insights into the autecology of major diatom taxa in acidified waters and highlights the importance of considering other anthropogenic stressors when assessing the recovery response of acid-impacted systems.

Climate oscillations drive millennial-scale changes in seabird colony size.

Seabird population size is intimately linked to the physical, chemical, and biological processes of the oceans. Yet, the overall effects of long-term changes in ocean dynamics on seabird colonies are difficult to quantify. Here, we used dated lake sediments to reconstruct ~10,000-years of seabird dynamics in the Northwest Atlantic to determine the influences of Holocene-scale climatic oscillations on colony size. On Baccalieu Island (Newfoundland and Labrador, Canada)-where the world's largest colony of Leach's storm-petrel (Hydrobates leucorhous Vieillot 1818) currently breeds-our data track seabird colony growth in response to warming during the Holocene Thermal Maximum (ca. 9000 to 6000 BP). From ca. 5200 BP to the onset of the Little Ice Age (ca. 550 BP), changes in colony size were correlated to variations in the North Atlantic Oscillation (NAO). By contrasting the seabird trends from Baccalieu Island to millennial-scale changes of storm-petrel populations from Grand Colombier Island (an island in the Northwest Atlantic that is subjected a to different ocean climate), we infer that changes in NAO influenced the ocean circulation, which translated into, among many things, changes in pycnocline depth across the Northwest Atlantic basin where the storm-petrels feed. We hypothesize that the depth of the pycnocline is likely a strong bottom-up control on surface-feeding storm-petrels through its influence on prey accessibility. Since the Little Ice Age (LIA), the effects of ocean dynamics on seabird colony size have been altered by anthropogenic impacts. Subsequently, the colony on Baccalieu Island grew at an unprecedented rate to become the world's largest resulting from favorable conditions linked to climate warming, increased vegetation (thereby nesting habitat), and attraction of recruits from other colonies that are now in decline. We show that although ocean dynamics were an important driver of seabird colony dynamics, its recent influence has been modified by human interference.

Metal contamination in alkaline Phantom Lake (Flin Flon, Manitoba, Canada) generates strong responses in multiple paleolimnological proxies.

The copper-zinc smelter at Flin Flon (Manitoba) operated between 1930 and 2010 and emitted large amounts of metal(loid)s and sulphur dioxide into the atmosphere, damaging the surrounding terrestrial landscapes and depositing airborne industrial pollutants into aquatic ecosystems. However, the extent of biological impairment in regional lakes is largely unknown. Here, we analysed biological and geochemical proxies preserved in a dated sediment core from Phantom Lake, collected seven years after the smelter closed in 2010. Our objectives were to determine how smelting history affected long-term trends in (1) sedimentary elements, (2) biota across multiple trophic levels, and (3) spectrally-inferred chlorophyll a and lake-water total organic carbon. The effects of smelting activities were clearest in the diatom record, in concordance with modest responses in chironomid and cladoceran assemblages. Several metal(loid)s were naturally high and exceeded sediment quality guidelines during the pre-smelting era. With the opening of the smelter, metal(loid) concentrations in sediments increased through the 1930s, peaked in the 1960s, and declined thereafter with technological improvements but remained above background to this day. Although modest declines in inferred lake-water total organic carbon indicate reduced terrestrial carbon supply following sulphate deposition in the catchment, the diatom record showed no evidence of acidification as the lake was and remained well-buffered. Pre-smelting diatom and invertebrate assemblages were diverse and indicated oligo-mesotrophic conditions. Smelting was associated with the loss of metal-sensitive biological indicators and the emergence of assemblages dominated by metal-tolerant, generalist taxa. Diatoms tracked substantial reductions in aerial emissions since the 1990s, particularly after the smelter closed, but also indicated that the biological effects of metal pollution persist in Phantom Lake. Examining the effects of a base metal smelter on a well-buffered lake offered insights into multi-trophic level responses to severe metal contamination and potential recovery without the confounding effects of concurrent changes in lake acidity.

Land-use and climate controls on aquatic carbon cycling and phototrophs in karst lakes of southwest China.

Land-use and climate changes have been repeatedly identified as important factors affecting terrestrial carbon budgets, however little is known about how deforestation and catchment development affect aquatic systems in carbonate-rich regions. Multi-proxy analyses of 210Pb-dated sediment cores from two hard-water lakes with different land-use histories were applied for assessing carbon cycling and limnological changes in response to land-use changes over the past century in southwest China. Logging of primary forests in the catchment of Lugu Lake, starting in the 1950s, led to a significant increase of catchment erosion, as well as a consistent decline in inferred lake-water total organic carbon (TOC) levels and sediment carbonate accumulation. This process of recent deforestation may significantly reduce the role of lake systems to act as carbon sinks through hampering of both the soil organic carbon flux and the dissolution of catchment carbonate. The decline in lake-water TOC in Lugu Lake further increased algal production (i.e. tracked through sediment trends in chlorophyll a and its main diagenetic products) and changes in diatom composition. In comparison, there was little variation of sediment carbonate content in Chenghai Lake, which has a long history of catchment deforestation, while both primary production and lake-water TOC increased following cultural eutrophication during the last three decades. Furthermore, regional warming was associated with an increase in small-sized diatoms in both deep lakes, likely due to enhanced thermal stability. This study highlights the significant role of vegetation cover and land use in driving aquatic carbon cycling and phototrophs, revealing that deforestation can strongly reduce both inorganic and organic carbon export to lakes and thus aquatic carbon storage in karst landscapes.

Re-browning of Sudbury (Ontario, Canada) lakes now approaches pre-acid deposition lake-water dissolved organic carbon levels.

Since the implementation of large-scale lake monitoring in the ~1980s, water color and dissolved organic carbon (DOC) concentrations have increased in many northern lakes (i.e., lake browning), impacting the functioning of aquatic ecosystems. In regions that formerly experienced high levels of acid deposition, this browning trend has been largely attributed to the recovery from the impacts of past acid deposition. However, the extent to which DOC levels have now returned to naturally higher, pre-industrial conditions is still poorly understood. In this study, we assessed whether DOC levels are still influenced by acid deposition in lakes near Sudbury, Ontario, a region that has been heavily affected by sulfur dioxide emissions from local metal smelting during the 20th century. We analyzed water chemistry monitoring data (1981-2018), together with comparisons between modern and pre-industrial DOC levels inferred from sediment spectroscopy, for 51 acid-sensitive and 24 buffered reference lakes across the Sudbury landscape. Since 1981, DOC concentrations doubled in acid-sensitive lakes, with a mean increase of +1.6 mg/L, whereas in more buffered reference lakes, mean DOC levels increased by only 0.8 mg/L. Similarly, sediment-inferred DOC trends indicate that current DOC levels are, on average, ~22% below pre-industrial levels in acid sensitive systems compared to only ~10% in buffered lakes. Weakening correlations between DOC and acidification-related water chemistry variables (e.g., pH, alkalinity, metals) further indicate a diminishing influence of acid deposition on DOC in Sudbury lakes. These results highlight the strong impact that acid deposition has historically had on lake-water DOC dynamics in this region, but also suggest that DOC levels are approaching natural baseline levels in less acid-sensitive lakes, and that other drivers, such as changes in climate or vegetation cover, are now becoming the dominant controls on changes in DOC concentrations.

The browning and re-browning of lakes: Divergent lake-water organic carbon trends linked to acid deposition and climate change.

Dissolved organic carbon (DOC) concentrations and water colour are increasing in many inland waters across northern Europe and northeastern North America. This inland-water "browning" has profound physical, chemical and biological repercussions for aquatic ecosystems affecting water quality, biological community structures and aquatic productivity. Potential drivers of this "browning" trend are complex and include reductions in atmospheric acid deposition, changes in land use/cover, increased nitrogen deposition and climate change. However, because of the overlapping impacts of these stressors, their relative contributions to DOC dynamics remain unclear, and without appropriate long-term monitoring data, it has not been possible to determine whether the ongoing "browning" is unprecedented or simply a "re-browning" to pre-industrial DOC levels. Here, we demonstrate the long-term impacts of acid deposition and climate change on lake-water DOC concentrations in low and high acid-deposition areas using infrared spectroscopic techniques on ~200-year-long lake-sediment records from central Canada. We show that acid deposition suppressed naturally higher DOC concentrations during the 20th century, but that a "re-browning" of lakes is now occurring with emissions reductions in formerly high deposition areas. In contrast, in low deposition areas, climate change is forcing lakes towards new ecological states, as lake-water DOC concentrations now often exceed pre-industrial levels.

Inferring Past Trends in Lake Water Organic Carbon Concentrations in Northern Lakes Using Sediment Spectroscopy.

Changing lake water total organic carbon (TOC) concentrations are of concern for lake management because of corresponding effects on aquatic ecosystem functioning, drinking water resources and carbon cycling between land and sea. Understanding the importance of human activities on TOC changes requires knowledge of past concentrations; however, water-monitoring data are typically only available for the past few decades, if at all. Here, we present a universal model to infer past lake water TOC concentrations in northern lakes across Europe and North America that uses visible-near-infrared (VNIR) spectroscopy on lake sediments. In the orthogonal partial least-squares model, VNIR spectra of surface-sediment samples are calibrated against corresponding surface water TOC concentrations (0.5-41 mg L-1) from 345 Arctic to northern temperate lakes in Canada, Greenland, Sweden and Finland. Internal model-cross-validation resulted in a R2 of 0.57 and a prediction error of 4.4 mg TOC L-1. First applications to lakes in southern Ontario and Scotland, which are outside of the model's geographic range, show the model accurately captures monitoring trends, and suggests that TOC dynamics during the 20th century at these sites were primarily driven by changes in atmospheric deposition. Our results demonstrate that the lake water TOC model has multiregional applications and is not biased by postdepositional diagenesis, allowing the identification of past TOC variations in northern lakes of Europe and North America over time scales of decades to millennia.

Early land use and centennial scale changes in lake-water organic carbon prior to contemporary monitoring.

Organic carbon concentrations have increased in surface waters across parts of Europe and North America during the past decades, but the main drivers causing this phenomenon are still debated. A lack of observations beyond the last few decades inhibits a better mechanistic understanding of this process and thus a reliable prediction of future changes. Here we present past lake-water organic carbon trends inferred from sediment records across central Sweden that allow us to assess the observed increase on a centennial to millennial time scale. Our data show the recent increase in lake-water carbon but also that this increase was preceded by a landscape-wide, long-term decrease beginning already A.D. 1450-1600. Geochemical and biological proxies reveal that these dynamics coincided with an intensification of human catchment disturbance that decreased over the past century. Catchment disturbance was driven by the expansion and later cessation of widespread summer forest grazing and farming across central Scandinavia. Our findings demonstrate that early land use strongly affected past organic carbon dynamics and suggest that the influence of historical landscape utilization on contemporary changes in lake-water carbon levels has thus far been underestimated. We propose that past changes in land use are also a strong contributing factor in ongoing organic carbon trends in other regions that underwent similar comprehensive changes due to early cultivation and grazing over centuries to millennia.

Pliocene warmth, polar amplification, and stepped Pleistocene cooling recorded in NE Arctic Russia.

Understanding the evolution of Arctic polar climate from the protracted warmth of the middle Pliocene into the earliest glacial cycles in the Northern Hemisphere has been hindered by the lack of continuous, highly resolved Arctic time series. Evidence from Lake El'gygytgyn, in northeast (NE) Arctic Russia, shows that 3.6 to 3.4 million years ago, summer temperatures were ~8°C warmer than today, when the partial pressure of CO2 was ~400 parts per million. Multiproxy evidence suggests extreme warmth and polar amplification during the middle Pliocene, sudden stepped cooling events during the Pliocene-Pleistocene transition, and warmer than present Arctic summers until ~2.2 million years ago, after the onset of Northern Hemispheric glaciation. Our data are consistent with sea-level records and other proxies indicating that Arctic cooling was insufficient to support large-scale ice sheets until the early Pleistocene.