Interhemispheric antiphasing of neotropical precipitation during the past millennium.

Uncertainty about the influence of anthropogenic radiative forcing on the position and strength of convective rainfall in the Intertropical Convergence Zone (ITCZ) inhibits our ability to project future tropical hydroclimate change in a warmer world. Paleoclimatic and modeling data inform on the timescales and mechanisms of ITCZ variability; yet a comprehensive, long-term perspective remains elusive. Here, we quantify the evolution of neotropical hydroclimate over the preindustrial past millennium (850 to 1850 CE) using a synthesis of 48 paleo-records, accounting for uncertainties in paleo-archive age models. We show that an interhemispheric pattern of precipitation antiphasing occurred on multicentury timescales in response to changes in natural radiative forcing. The conventionally defined "Little Ice Age" (1450 to 1850 CE) was marked by a clear shift toward wetter conditions in the southern neotropics and a less distinct and spatiotemporally complex transition toward drier conditions in the northern neotropics. This pattern of hydroclimatic change is consistent with results from climate model simulations indicating that a relative cooling of the Northern Hemisphere caused a southward shift in the thermal equator across the Atlantic basin and a southerly displacement of the ITCZ in the tropical Americas, with volcanic forcing as the principal driver. These findings are at odds with proxy-based reconstructions of ITCZ behavior in the western Pacific basin, where changes in ITCZ width and intensity, rather than mean position, appear to have driven hydroclimate transitions over the last millennium. This reinforces the idea that ITCZ responses to external forcing are region specific, complicating projections of the tropical precipitation response to global warming.

Annually resolved Atlantic sea surface temperature variability over the past 2,900 y.

Global warming due to anthropogenic factors can be amplified or dampened by natural climate oscillations, especially those involving sea surface temperatures (SSTs) in the North Atlantic which vary on a multidecadal scale (Atlantic multidecadal variability, AMV). Because the instrumental record of AMV is short, long-term behavior of AMV is unknown, but climatic teleconnections to regions beyond the North Atlantic offer the prospect of reconstructing AMV from high-resolution records elsewhere. Annually resolved titanium from an annually laminated sedimentary record from Ellesmere Island, Canada, shows that the record is strongly influenced by AMV via atmospheric circulation anomalies. Significant correlations between this High-Arctic proxy and other highly resolved Atlantic SST proxies demonstrate that it shares the multidecadal variability seen in the Atlantic. Our record provides a reconstruction of AMV for the past ∼3 millennia at an unprecedented time resolution, indicating North Atlantic SSTs were coldest from ∼1400-1800 CE, while current SSTs are the warmest in the past ∼2,900 y.

The Donora Smog Revisited: 70 Years After the Event That Inspired the Clean Air Act.

At a storefront museum approximately 25 miles southeast of Pittsburgh, Pennsylvania, a sign reads, "Clean Air Started Here." This is not hyperbole. At the end of October 1948, the communities of Donora and Webster in Pennsylvania were visited by a smog that changed the face of environmental protection in the United States. Conservative estimates showed that 20 individuals died, while an additional 5900-43% of the population of Donora-were affected by the smog. This event led to the first large-scale epidemiological investigation of an environmental health disaster in the United States. Questions remain about the long-term effects of the smog, because higher rates of cardiovascular disease and cancer than were expected were observed in the region in the decade following the smog. Recent work has suggested that environmental contaminants from a bygone era in Donora might have an impact even today. In addition, reports regarding air pollution have indicated that levels of pollutants similar to those estimated to have occurred in Donora are currently present in some rapidly industrializing regions of China and India. Seventy years after the smog, this event still resonates.

Climate, Fire, and Vegetation Mediate Mercury Delivery to Midlatitude Lakes over the Holocene.

The rise in mercury concentrations in lake sediment deposited over the last ∼150 years is widely recognized to have resulted from human activity. However, few studies in the Great Lakes region have used lake sediment to reconstruct atmospheric mercury deposition on millennial time scales. Here we present a 9000-year mercury record from sediment in Copper Falls; a small closed-basin lake on the Keweenaw Peninsula. Prior to abrupt increases in the 19th and 20th centuries, mercury remains at relatively low concentrations for the last 9000 years. Higher mercury fluxes in the early Holocene (3.4 ± 1.1 µg m-2 yr-1) are attributed to drier conditions and greater forest fire occurrence. The gradual decline in mercury flux over the middle to late Holocene (1.9 ± 0.2 µg m-2 yr-1) is interpreted to reflect a transition to wetter conditions, which reduced forest fires, and promoted the development of soil organic matter and deciduous forests that sequestered natural sources of mercury. The Copper Falls Lake record highlights the sensitivity of watersheds to changes in mercury inputs from both human and natural forcings, and provides millennial-scale context for recent mercury contamination that will aid in establishing baseline values for restoration efforts.

Reconstructing Early Industrial Contributions to Legacy Trace Metal Contamination in Southwestern Pennsylvania.

Early industrial trace metal loadings are poorly characterized but potentially substantial sources of trace metals to the landscape. The magnitude of legacy contamination in southwestern Pennsylvania, the cradle of North American fossil fuel industrialization, is reconstructed from trace metal concentrations in a sediment core with proxies including major and trace metal chemistry, bulk density, and magnetic susceptibility. Trace metal chemistry in this sediment record reflects 19th and 20th century land use and industry. In particular, early 19th century arsenic loadings to the lake are elevated from pesticides used by early European settlers at a lakeside tannery. Later, sediment barium concentrations rise, likely reflecting the onset of acidic mine drainage from coal operations. Twentieth century zinc, cadmium, and lead concentrations are dominated by emissions from the nearby, infamous Donora Zinc Works yet record both the opening of a nearby coal-fired power plant and amendments to the Clean Air Act. The impact of early industry is substantial and rivals more recent metal fluxes, resulting in a significant potential source of contaminated sediments. Thus, modern assessments of trace metal contamination cannot ignore early industrial inputs, as the potential remobilization of legacy contamination would impact ecosystem and human health.

Synchronous interhemispheric Holocene climate trends in the tropical Andes.

Holocene variations of tropical moisture balance have been ascribed to orbitally forced changes in solar insolation. If this model is correct, millennial-scale climate evolution should be antiphased between the northern and southern hemispheres, producing humid intervals in one hemisphere matched to aridity in the other. Here we show that Holocene climate trends were largely synchronous and in the same direction in the northern and southern hemisphere outer-tropical Andes, providing little support for the dominant role of insolation forcing in these regions. Today, sea-surface temperatures in the equatorial Pacific Ocean modulate rainfall variability in the outer tropical Andes of both hemispheres, and we suggest that this mechanism was pervasive throughout the Holocene. Our findings imply that oceanic forcing plays a larger role in regional South American climate than previously suspected, and that Pacific sea-surface temperatures have the capacity to induce abrupt and sustained shifts in Andean climate.

Environmental legacy of copper metallurgy and Mongol silver smelting recorded in Yunnan Lake sediments.

Geochemical measurements on well-dated sediment cores from Lake Er (Erhai) are used to determine the timing of changes in metal concentrations over 4500 years in Yunnan, a borderland region in southwestern China noted for rich mineral deposits but with inadequately documented metallurgical history. Our findings add new insight into the impacts and environmental legacy of human exploitation of metal resources in Yunnan history. We observe an increase in copper at 1500 BC resulting from atmospheric emissions associated with metallurgy. These data clarify the chronological issues related to links between the onset of Yunnan metallurgy and the advent of bronze technology in adjacent Southeast Asia, subjects that have been debated for nearly half a century. We also observe an increase from 1100 to 1300 AD in a number of heavy metals including lead, silver, zinc, and cadmium from atmospheric emissions associated with silver smelting. Culminating during the rule of the Mongols, known as the Yuan Dynasty (1271-1368 AD), these metal concentrations approach levels three to four times higher than those from industrialized mining activity occurring within the catchment today. Notably, the concentrations of lead approach levels at which harmful effects may be observed in aquatic organisms. The persistence of this lead pollution over time created an environmental legacy that likely contributes to known issues in modern day sediment quality. We demonstrate that historic metallurgical production in Yunnan can cause substantial impacts on the sediment quality of lake systems, similar to other paleolimnological findings around the globe.

1,500 year quantitative reconstruction of winter precipitation in the Pacific Northwest.

Multiple paleoclimate proxies are required for robust assessment of past hydroclimatic conditions. Currently, estimates of drought variability over the past several thousand years are based largely on tree-ring records. We produced a 1,500-y record of winter precipitation in the Pacific Northwest using a physical model-based analysis of lake sediment oxygen isotope data. Our results indicate that during the Medieval Climate Anomaly (MCA) (900-1300 AD) the Pacific Northwest experienced exceptional wetness in winter and that during the Little Ice Age (LIA) (1450-1850 AD) conditions were drier, contrasting with hydroclimatic anomalies in the desert Southwest and consistent with climate dynamics related to the El Niño Southern Oscillation (ENSO) and the Pacific Decadal Oscillation (PDO). These findings are somewhat discordant with drought records from tree rings, suggesting that differences in seasonal sensitivity between the two proxies allow a more compete understanding of the climate system and likely explain disparities in inferred climate trends over centennial timescales.

A 2,300-year-long annually resolved record of the South American summer monsoon from the Peruvian Andes.

Decadal and centennial mean state changes in South American summer monsoon (SASM) precipitation during the last 2,300 years are detailed using an annually resolved authigenic calcite record of precipitation δ(18)O from a varved lake in the Central Peruvian Andes. This unique sediment record shows that δ(18)O peaked during the Medieval Climate Anomaly (MCA) from A.D. 900 to 1100, providing evidence that the SASM weakened considerably during this period. Minimum δ(18)O values occurred during the Little Ice Age (LIA) between A.D. 1400 and 1820, reflecting a prolonged intensification of the SASM that was regionally synchronous. After the LIA, δ(18)O increased rapidly, particularly during the current warm period (CWP; A.D. 1900 to present), indicating a return to reduced SASM precipitation that was more abrupt and sustained than the onset of the MCA. Diminished SASM precipitation during the MCA and CWP tracks reconstructed Northern Hemisphere and North Atlantic warming and a northward displacement of the Intertropical Convergence Zone (ITCZ) over the Atlantic, and likely the Pacific. Intensified SASM precipitation during the LIA follows reconstructed Northern Hemisphere and North Atlantic cooling, El Niño-like warming in the Pacific, and a southward displacement of the ITCZ over both oceans. These results suggest that SASM mean state changes are sensitive to ITCZ variability as mediated by Western Hemisphere tropical sea surface temperatures, particularly in the Atlantic. Continued Northern Hemisphere and North Atlantic warming may therefore help perpetuate the recent reductions in SASM precipitation that characterize the last 100 years, which would negatively impact Andean water resources.

Drought variability in the Pacific Northwest from a 6,000-yr lake sediment record.

We present a 6,000-yr record of changing water balance in the Pacific Northwest inferred from measurements of carbonate δ(18)O and grayscale on a sediment core collected from Castor Lake, Washington. This subdecadally resolved drought record tracks the 1,500-yr tree-ring-based Palmer Drought Severity Index reconstructions of Cook et al. [Cook ER, Woodhouse CA, Eakin CM, Meko DM, Stahle DW (2004) Science 306:1015-1018] in the Pacific Northwest and extends our knowledge back to 6,000 yr B.P. The results demonstrate that low-frequency drought/pluvial cycles, with occasional long-duration, multidecadal events, are a persistent feature of regional climate. Furthermore, the average duration of multidecadal wet/dry cycles has increased since the middle Holocene, which has acted to increase the amplitude and impact of these events. This is especially apparent during the last 1,000 yr. We suggest these transitions were driven by changes in the tropical and extratropical Pacific and are related to apparent intensification of the El Niño Southern Oscillation over this interval and its related effects on the Pacific Decadal Oscillation. The Castor Lake record also corroborates the notion that the 20th century, prior to recent aridity, was a relatively wet period compared to the last 6,000 yr. Our findings suggest that the hydroclimate response in the Pacific Northwest to future warming will be intimately tied to the impact of warming on the El Niño Southern Oscillation.

Lake sediments record prehistoric lead pollution related to early copper production in North America.

The mining and use of copper by prehistoric people on Michigan's Keweenaw Peninsula is one of the oldest examples of metalworking. We analyzed the concentration of lead, titanium, magnesium, iron, and organic matter in sediment cores recovered from three lakes located near mine pits to investigate the timing, location, and magnitude of ancient copper mining pollution. Lead concentrations were normalized to lithogenic metals and organic matter to account for processes that can influence natural (or background) lead delivery. Nearly simultaneous lead enrichments occurred at Lake Manganese and Copper Falls Lake ∼8000 and 7000 years before present (yr BP), indicating that copper extraction occurred concurrently in at least two locations on the peninsula. The poor temporal coherence among the lead enrichments from ∼6300 to 5000 yr BP at each lake suggests that the focus of copper mining and annealing shifted through time. In sediment younger than ∼5000 yr BP, lead concentrations remain at background levels at all three lakes, excluding historic lead increases starting ∼150 yr BP. Our work demonstrates that lead emissions associated with both the historic and Old Copper Complex tradition are detectable and can be used to determine the temporal and geographic pattern of metal pollution.

Pond Sediments Reveal the Increasing Importance of Road Runoff as a Source of Metal Contamination in Industrialized Urban Environments Downwind of Pittsburgh, Pennsylvania (USA).

Toxic levels of trace metals from human activities accumulate in natural environments, yet these metal mixtures are rarely characterized or quantified. Metal mixtures accumulate in historically industrial urban areas and change as economies shift. Previous research has often focused on the sources and fate of a specific element, which limits our understanding of metal contaminant interactions in our environment. Here, we reconstruct the history of metal contamination in a small pond downstream of an interstate highway and downwind of fossil fuel and metallurgical industries that have been active since the middle of the nineteenth century. Metal contamination histories were reconstructed from the sediment record using metal ratio mixing analysis to attribute the relative contributions of contamination sources. Cadmium, copper, and zinc concentrations in sediments accumulated since the construction of major road arteries in the 1930s and 40s are, respectively, 3.9, 2.4, and 6.6 times more concentrated than those during industry-dominated time periods. Shifts in elemental ratios suggest these changes in metal concentrations coincide with increased contributions from road and parking lot traffic, and to a lesser extent, from airborne sources. The metal mixture analysis demonstrates that in near-road environments, contributions from modern surface water pathways can obscure historical atmospheric industrial inputs.

Metal ratio mixing models clarify metal contamination sources to lake sediments in Yunnan, China.

Contaminated legacy sediments contribute to modern pollution loadings, particularly trace metals. These contributions are challenging to quantify as metal histories reconstructed from sediment records cannot be easily divided into legacy and concurrent contamination. In particular, the contribution from re-mobilization and delivery of legacy metals stored in catchment soil, colluvial, and fluvial environments are rarely considered or quantified when interpreting sediment records. Here, extended records of metals accumulation for a set of three lakes in Yunnan, China are compared with endmember chemistries using Monte Carlo-Markov Chain mixing models to help identify source contributions to the sediments. This approach allows attribution of metals transported by atmospheric and fluvial mechanisms in a region with a history of mining and metallurgy spanning millennia. These analyses reveal distinct source mixtures and demonstrate the sensitivity of lake records to basin sediment dynamics. In particular, substantial proportions of elevated metal concentrations in these lake systems seem to arise from soil contributions more than from atmospheric deposition of smelting emissions. The largest soil contributions seem to be in Erhai, a lake with erosion prone soils closely "connected" to the lake. Moreover, these invesigations illustrate the potential for mixing approaches to accommodate and clarify uncertainties in metal source and extraction as differences in extraction efficiency can be incorporated into source uncertainty estimates. Ultimately, these approaches emphasize the need to account for fluvial metal transport in interpretation of sediment histories.

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.

Severe Little Ice Age drought in the midcontinental United States during the Mississippian abandonment of Cahokia.

Drought has long been suspected as playing an important role in the abandonment of pre-Columbian Native American settlements across the midcontinental United States between 1350 and 1450 CE. However, high-resolution paleoclimatic reconstructions reflecting local effective moisture (the ratio of precipitation to evaporation) that are located in proximity to Mississippi period (1050-1450 CE) population centers are lacking. Here, we present a 1600-year-long decadally resolved oxygen isotope (δ18O) record from Horseshoe Lake (Collinsville, IL), an evaporatively influenced oxbow lake that is centrally located within the largest and mostly densely populated series of Mississippian settlements known as Greater Cahokia. A shift to higher δ18O in the Horseshoe Lake sediment record from 1200 to 1400 CE indicates that strongly evaporative conditions (i.e., low effective moisture) were persistent during the leadup to Cahokia's abandonment. These results support the hypothesis that climate, and drought specifically, strongly impacted agriculturally based pre-Columbian Native American cultures in the midcontinental US and highlights the susceptibility of this region, presently a global food production center, to hydroclimate extremes.

Contrasting ecosystem responses to climatic events and human activity revealed by a sedimentary record from Lake Yilong, southwestern China.

Global climate change and human activities have significantly impacted lake ecosystems at an accelerating rate in recent decades, but the differences between the responses of lake ecosystems to these two stressors remain unclear. Thus an improved understanding of the long-term influences of climatic and anthropogenic disturbances is necessary for the management of lake ecosystems. In order to address these issues, a sedimentary record was obtained from Lake Yilong in Yunnan Province in southwestern China, where the climate and natural environment are dominated by the Indian Summer Monsoon and there is a long history of human occupation and intensive human activity. The chronology is based on AMS 14C dates from 13 samples of plant macrofossils and charcoal, which show that the record spans the last ~12,000 yr. Geochemical indices were used to reconstruct hydro-climatic variations and lake ecosystem responses. The results indicate that a cold and humid climate prevailed from the late Pleistocene to the beginning of the Holocene, which was interrupted by an abrupt decrease in precipitation during 9.7-8.7 ka (1 ka = 1000 cal yr BP, corresponding to the 9.3 ka event). A persistent drying trend occurred during the middle and late Holocene, and there was an increase in the intensity of human activity during the past 1500 years. A comparison of the effects of a natural climatic event and human disturbance reveals contrasting lake ecosystem responses. The lake ecosystem was resilient to the 9.3 ka event and subsequently recovered; however, long-term human activity in the watershed, including deforestation and cultivation, reduced the stability of the lake ecosystem and positive feedback effects were strengthened, leading to the deviation of the system far from its previous stable state. It is concluded that, compared to climate change, human activities have had a much more serious impact on lake ecosystem.

Andean drought and glacial retreat tied to Greenland warming during the last glacial period.

Abrupt warming events recorded in Greenland ice cores known as Dansgaard-Oeschger (DO) interstadials are linked to changes in tropical circulation during the last glacial cycle. Corresponding variations in South American summer monsoon (SASM) strength are documented, most commonly, in isotopic records from speleothems, but less is known about how these changes affected precipitation and Andean glacier mass balance. Here we present a sediment record spanning the last ~50 ka from Lake Junín (Peru) in the tropical Andes that has sufficient chronologic precision to document abrupt climatic events on a centennial-millennial time scale. DO events involved the near-complete disappearance of glaciers below 4700 masl in the eastern Andean cordillera and major reductions in the level of Peru's second largest lake. Our results reveal the magnitude of the hydroclimatic disruptions in the highest reaches of the Amazon Basin that were caused by a weakening of the SASM during abrupt arctic warming. Accentuated warming in the Arctic could lead to significant reductions in the precipitation-evaporation balance of the southern tropical Andes with deleterious effects on this densely populated region of South America.

A paleolimnological perspective on industrial-era metal pollution in the central Andes, Peru.

To date, few studies have investigated the environmental legacy associated with industrialization in the South American Andes. Here, we present an environmental archive of industrial pollution from (210)Pb-dated lake cores recovered from Laguna Chipian, located near the Cerro de Pasco metallurgical region and Laguna Pirhuacocha, located near the Morococha mining region and the La Oroya smelting complex. At Laguna Chipian, trace metal concentrations increase beginning ~1900 AD, coincident with the construction of the central Peruvian railway, and the rapid industrial development of the Cerro de Pasco region. Trace metal concentrations and fluxes peak during the 1950s before subsequently declining up-core (though remaining well above background levels). While Colonial mining and smelting operations are known to have occurred at Cerro de Pasco since at least 1630 AD, our sediment record preserves no associated metal deposition. Based on our (14)C and (210)Pb data, we suggest that this is due to a depositional hiatus, rather than a lack of regional Colonial pollution. At Laguna Pirhuacocha, industrial trace metal deposition first begins ~1925 AD, rapidly increasing after ~1950 AD and peaking during either the 1970s or 1990s. Trace metal concentrations from these lakes are comparable to some of the most polluted lakes in North America and Europe. There appears to be little diagenetic alteration of the trace metal record at either lake, the exception being arsenic (As) accumulation at Laguna Pirhuacocha. There, a correlation between As and the redox-sensitive element manganese (Mn) suggests that the sedimentary As burden is undergoing diagenetic migration towards the sediment-water interface. This mobility has contributed to surface sediment As concentrations in excess of 1100 microg g(-1). The results presented here chronicle a rapidly changing Andean environment, and highlight a need for future research in the rate and magnitude of atmospheric metal pollution.

A millennium of metallurgy recorded by lake sediments from Morococha, Peruvian Andes.

To date, information concerning pre-Colonial metallurgy in South America has largely been limited to the archaeological record of artifacts. Here, we reconstruct a millennium of smelting activity in the Peruvian Andes using the lake-sediment stratigraphy of atmospherically derived metals (Pb, Zn, Cu, Ag, Sb, Bi, and Ti) and lead isotopic ratios (206Pb/ 207Pb) associated with smelting from the Morococha mining region in the central Peruvian Andes. The earliest evidence for metallurgy occurs ca. 1000 A.D., coinciding with the fall of the Wari Empire and decentralization of local populations. Smelting during this interval appears to have been aimed at copper and copper alloys, because of large increases in Zn and Cu relative to Pb. A subsequent switch to silver metallurgy under Inca control (ca. 1450 to conquest, 1533 A.D.) is indicated by increases in Pb, Sb, and Bi, a conclusion supported by further increases of these metals during Colonial mining, which targeted silver extraction. Rapid development of the central Andes during the 20th century raised metal burdens by an order of magnitude above previous levels. Our results represent the first evidence for pre-Colonial smelting in the central Peruvian Andes, and corroborate the sensitivity of lake sediments to pre-Colonial metallurgical activity suggested by earlier findings from Bolivia.

Intensive pre-Incan metallurgy recorded by lake sediments from the Bolivian Andes.

The history of pre-Columbian metallurgy in South America is incomplete because looting of metal artifacts has been pervasive. Here, we reconstruct a millennium of metallurgical activity in southern Bolivia using the stratigraphy of metals associated with smelting (Pb, Sb, Bi, Ag, Sn) from lake sediments deposited near the major silver deposit of Cerro Rico de Potosí. Pronounced metal enrichment events coincide with the terminal stages of Tiwanaku culture (1000 to 1200 A.D.) and Inca through early Colonial times (1400 to 1650 A.D.). The earliest of these events suggests that Cerro Rico ores were actively smelted at a large scale in the Late Intermediate Period, providing evidence for a major pre-Incan silver industry.