Colin A. Cooke

Over three millennia of mercury pollution in the Peruvian Andes

We present unambiguous records of preindustrial atmospheric mercury (Hg) pollution, derived from lake-sediment cores collected near Huancavelica, Peru, the largest Hg deposit in the New World. Intensive Hg mining first began ca. 1400 BC, predating the emergence of complex Andean societies, and signifying that the region served as a locus for early Hg extraction. The earliest mining targeted cinnabar (HgS) for the production of vermillion. Pre-Colonial Hg burdens peak ca. 500 BC and ca. 1450 AD, corresponding to the heights of the Chavín and Inca states, respectively. During the Inca, Colonial, and industrial intervals, Hg pollution became regional, as evidenced by a third lake record ≈225 km distant from Huancavelica. Measurements of sediment-Hg speciation reveal that cinnabar dust was initially the dominant Hg species deposited, and significant increases in deposition were limited to the local environment. After conquest by the Inca (ca. 1450 AD), smelting was adopted at the mine and Hg pollution became more widely circulated, with the deposition of matrix-bound phases of Hg predominating over cinnabar dust. Our results demonstrate the existence of a major Hg mining industry at Huancavelica spanning the past 3,500 years, and place recent Hg enrichment in the Andes in a broader historical context.

Recent changes in a remote Arctic lake are unique within the past 200,000 years

The Arctic is currently undergoing dramatic environmental transformations, but it remains largely unknown how these changes compare with long-term natural variability. Here we present a lake sediment sequence from the Canadian Arctic that records warm periods of the past 200,000 years, including the 20th century. This record provides a perspective on recent changes in the Arctic and predates by approximately 80,000 years the oldest stratigraphically intact ice core recovered from the Greenland Ice Sheet. The early Holocene and the warmest part of the Last Interglacial (Marine Isotope Stage or MIS 5e) were the only periods of the past 200,000 years with summer temperatures comparable to or exceeding todays at this site. Paleoecological and geochemical data indicate that the past three interglacial periods were characterized by similar trajectories in temperature, lake biology, and lakewater pH, all of which tracked orbitally-driven solar insolation. In recent decades, however, the study site has deviated from this recurring natural pattern and has entered an environmental regime that is unique within the past 200 millennia.

Are Current Rates of Atmospheric Nitrogen Deposition Influencing Lakes in the Eastern Canadian Arctic

Abstract Although arctic lakes rank among the most pristine ecosystems remaining on Earth, widespread paleoecological analyses have revealed rapid recent changes in lake ecology that largely surpass Holocene natural variability and that are generally attributed to climate warming since the end of the Little Ice Age. However, the possibility that climate is only one dimension of these unprecedented ecological shifts remains an untested possibility, especially given that current warming may not yet exceed maximum, naturally mediated, postglacial warmth. In this paper, we assess whether increased anthropogenic nitrogen (N) deposition from distant sources is contributing to directional changes in the biogeochemistry and ecology of two remote lakes on Baffin Island in the eastern Canadian Arctic. Paleolimnological analyses, including diatom assemblages and a suite of biogeochemical proxies (total organic matter, biogenic silica, organic N and C contents, and stable isotopic ratios) reveal a complex suite of progressive changes that are coherently expressed in both lakes. Diatom assemblages began to change as early as the mid-19th century, but major inflections in the biogeochemical proxies occurred significantly later, being most pronounced after 1950. Among these changes are increases in sediment organic matter, depletions of 2‰ in sediment δ15N, and decoupling of δ13C and δ15N signatures. It seems likely that climate warming, subsequently coupled to anthropogenic N deposition, is synergistically driving these ecosystems towards states for which no prior natural analogs exist.

Use and Legacy of Mercury in the Andes

Both cinnabar (HgS) and metallic mercury (Hg(0)) were important resources throughout Andean prehistory. Cinnabar was used for millennia to make vermillion, a red pigment that was highly valued in pre-Hispanic Peru; metallic Hg(0) has been used since the mid-16th century to conduct mercury amalgamation, an efficient process of extracting precious metals from ores. However, little is known about which cinnabar deposits were exploited by pre-Hispanic cultures, and the environmental consequences of Hg mining and amalgamation remain enigmatic. Here we use Hg isotopes to source archeological cinnabar and to fingerprint Hg pollution preserved in lake sediment cores from Peru and the Galápagos Islands. Both pre-Inca (pre-1400 AD) and Colonial (1532-1821 AD) archeological artifacts contain cinnabar that matches isotopically with cinnabar ores from Huancavelica, Peru, the largest cinnabar-bearing district in Central and South America. In contrast, the Inca (1400-1532 AD) artifacts sampled are characterized by a unique Hg isotopic composition. In addition, preindustrial (i.e., pre-1900 AD) Hg pollution preserved in lake sediments matches closely the isotopic composition of cinnabar from the Peruvian Andes. Industrial-era Hg pollution, in contrast, is distinct isotopically from preindustrial emissions, suggesting that pre- and postindustrial Hg emissions may be distinguished isotopically in lake sediment cores.

Late-Holocene atmospheric lead deposition in the Peruvian and Bolivian Andes

The analysis of lead (Pb) in lake-sediment cores is a useful method to reconstruct local histories of Pb pollution. Here, we use Pb concentration profiles from lake sediments to reconstruct local trajectories of pre-Colonial smelting from three metallurgical centres in the South American Andes: the Morococha mining district, Peru; the Bolivian Altiplano around Lake Titicaca; and the silver-mining centre of Potosí, Bolivia. The earliest evidence for Pb enrichment from smelting is on the Altiplano beginning ~AD 400, coincident with the rise of the pre-Incan Tiwanaku and Wari Empires. Coeval with the collapse of these Empires ~AD 1000, there is a dramatic decrease in Pb pollution on the Altiplano, suggesting metallurgical activity was closely tied to the Tiwanaku state. In contrast, metallurgy at Morococha, Peru and Potosí, Bolivia began ~AD 1000—1200, likely as the result of the diaspora generated by the collapses of Tiwanaku and Wari. The independent chronologies of these records suggest asynchronous metallurgical activity between mining centres, and local-scale control of mineral resources. Following Inca conquest of the Andes ~AD 1450, strong increases in Pb are noted at all three study sites, suggesting an increase in silver production to meet Inca imperial demand. Following Hispanic conquest (AD 1532), large increases in Pb pollution are noted at Morococha and Potosí, only to be superseded by industrial development. The records presented here have implications for the reconstruction of Andean prehistory, and demonstrate the sensitivity of lake sediment geochemistry to pre-Colonial smelting activity. The technique has much potential for exploring the timing and magnitude of pre-industrial metallurgy in the New World.

Climate Change Forces New Ecological States in Tropical Andean Lakes

Air temperatures in the tropical Andes have risen at an accelerated rate relative to the global average over recent decades. However, the effects of climate change on Andean lakes, which are vital to sustaining regional biodiversity and serve as an important water resource to local populations, remain largely unknown. Here, we show that recent climate changes have forced alpine lakes of the equatorial Andes towards new ecological and physical states, in close synchrony to the rapid shrinkage of glaciers regionally. Using dated sediment cores from three lakes in the southern Sierra of Ecuador, we record abrupt increases in the planktonic thalassiosiroid diatom Discostella stelligera from trace abundances to dominance within the phytoplankton. This unprecedented shift occurs against the backdrop of rising temperatures, changing atmospheric pressure fields, and declining wind speeds. Ecological restructuring in these lakes is linked to warming and/or enhanced water column stratification. In contrast to seasonally ice-covered Arctic and temperate alpine counterparts, aquatic production has not increased universally with warming, and has even declined in some lakes, possibly because enhanced thermal stability impedes the re-circulation of hypolimnetic nutrients to surface waters. Our results demonstrate that these lakes have already passed important ecological thresholds, with potentially far-reaching consequences for Andean water resources.

Increased mercury loadings to western Canadian alpine lakes over the past 150 years.

We reconstructed historical trends in mercury (Hg) accumulation over the past ∼ 150 years in nine western Canadian alpine lakes. Recent Hg accumulation rates (fluxes) ranged between ∼ 7 and 75 μg m(-2) yr(-1), which were an average of 1.8 times higher than preindustrial (i.e., pre-1850) fluxes. Increased Hg fluxes in these lakes were less than at lower elevation sites, showing that despite the potential for increased deposition, alpine lakes are no more susceptible to Hg accumulation. Unlike other studies, we found that geographic setting, changes in chlorophyll-inferred algal production, and climate were not significant predictors of [Hg] or Hg flux in lakes. Instead, our findings highlight how a combination of atmospheric deposition and site-specific processes, including organic matter supply and catchment weathering, better explain sequestration of Hg in alpine lakes.

Pre-Colombian Mercury Pollution Associated with the Smelting of Argentiferous Ores in the Bolivian Andes

The development of the mercury (Hg) amalgamation process in the mid-sixteenth century triggered the onset of large-scale Hg mining in both the Old and New Worlds. However, ancient Hg emissions associated with amalgamation and earlier mining efforts remain poorly constrained. Using a geochemical time-series generated from lake sediments near Cerro Rico de Potosí, once the world’s largest silver deposit, we demonstrate that pre-Colonial smelting of Andean silver ores generated substantial Hg emissions as early as the twelfth century. Peak sediment Hg concentrations and fluxes are associated with smelting and exceed background values by approximately 20-fold and 22-fold, respectively. The sediment inventory of this early Hg pollution more than doubles that associated with extensive amalgamation following Spanish control of the mine (1574–1900 AD). Global measurements of [Hg] from economic ores sampled world-wide indicate that the phenomenon of Hg enrichment in non-ferrous ores is widespread. The results presented here imply that indigenous smelting constitutes a previously unrecognized source of early Hg pollution, given naturally elevated [Hg] in economic silver deposits.

Northern peatland initiation lagged abrupt increases in deglacial atmospheric CH4

Peatlands are a key component of the global carbon cycle. Chronologies of peatland initiation are typically based on compiled basal peat radiocarbon (14C) dates and frequency histograms of binned calibrated age ranges. However, such compilations are problematic because poor quality 14C dates are commonly included and because frequency histograms of binned age ranges introduce chronological artefacts that bias the record of peatland initiation. Using a published compilation of 274 basal 14C dates from Alaska as a case study, we show that nearly half the 14C dates are inappropriate for reconstructing peatland initiation, and that the temporal structure of peatland initiation is sensitive to sampling biases and treatment of calibrated 14C dates. We present revised chronologies of peatland initiation for Alaska and the circumpolar Arctic based on summed probability distributions of calibrated 14C dates. These revised chronologies reveal that northern peatland initiation lagged abrupt increases in atmospheric CH4 concentration at the start of the Bølling–Allerød interstadial (Termination 1A) and the end of the Younger Dryas chronozone (Termination 1B), suggesting that northern peatlands were not the primary drivers of the rapid increases in atmospheric CH4. Our results demonstrate that subtle methodological changes in the synthesis of basal 14C ages lead to substantially different interpretations of temporal trends in peatland initiation, with direct implications for the role of peatlands in the global carbon cycle.

Reliance on 210Pb chronology can compromise the inference of preindustrial Hg flux to lake sediments.

Lake sediments are frequently used to reconstruct the rate and magnitude of human impacts on the biogeochemical cycle of mercury (Hg). The vast majority of these studies rely on excess (210)Pb inventories in short cores to temporally constrain recent trends in Hg deposition, revealing an approximately 3-fold increase in Hg deposition since preindustrial times. However, the exhaustion of unsupported (210)Pb and the onset of widespread global Hg pollution converge temporally in the late 19th century, raising the possibility that preindustrial Hg fluxes are poorly constrained. Here, we combine (210)Pb and accelerator mass spectrometry (AMS) (14)C dated lake sediment records from arctic and Andean lakes to assess the reliability of (210)Pb-derived chronologies in the estimation of preindustrial Hg fluxes. For all four studied lakes, relying on (210)Pb chronologies results in an overestimate of preindustrial Hg fluxes, because extrapolated basal (210)Pb sedimentation rates are systematically overestimated in comparison to accumulation models that include (14)C dates. In the Andes, the use of (14)C dates is critical toward assessing the full history of Hg pollution, which extends beyond the industrial era. In the Arctic, (14)C dating suggests that Hg deposition may have increased >10-fold since the Industrial Revolution, rather than the commonly quoted 3-fold increase. The incorporation of (14)C dates may therefore be necessary if accurate Hg flux histories are sought from oligotrophic lake sediments.