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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.

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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.

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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.

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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.

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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.

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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.

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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.