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We present lead (Pb) concentrations and isotope ratios in a continuous series of 38 snow samples from a 1.9-m snow pit, covering the period from winter 2012 to summer 2017, at the East Greenland Ice-core Project (EGRIP) ice core drill site in northwestern Greenland. Pb concentrations were highly variable, ranging from 1.53 to 94.9 pg g -1 (mean value of 10.6 pg g -1 ), with higher concentrations during winter and spring and lower concentrations during summer and fall. Our results show a substantial reduction in the Pb concentration of ∼50% between the 2000s and 2010s, reaching a level close to that observed in the mid-18th century, that is, the time of the Industrial Revolution. Remarkably low radiogenic Pb isotope compositions were observed in our samples compared to previously reported values during the 2000s. The Pb isotope mixing model results indicated a decreasing Chinese contribution from the 2000s onwards, while Europe/Russia emerged as a relatively more important contributor to the anthropogenic Pb input to central Greenland during the corresponding period. Thus, we hypothesized that the reduction in Pb pollution in central Greenland is largely due to a decreasing contribution from Chinese sources in response to the effectiveness of stringent emission control measures in China., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2023 Elsevier Ltd. All rights reserved.)

We report the first high-resolution record of arsenic (As) observed in Greenland snow and ice for the periods 1711-1970 and 2003-2009 AD. The results show well-defined large-scale atmospheric pollution by this toxic element in the northern hemisphere, beginning as early as the 18th century. The most striking feature is an abrupt, unprecedented enrichment factor (EF) peak in the late 1890s, with an ∼30-fold increase in the mean value above the Holocene natural level. Highly enriched As was evident until the late 1910s; a sharp decline was observed after the First World War, reaching a minimum in the early 1930s during the Great Depression. A subsequent increase lasted until the mid-1950s, before decreasing again. Comparisons between the observed variations and Cu smelting data indicate that Cu smelting in Europe and North America was the likely source of early anthropogenic As in Greenland. Despite a significant reduction of ∼80% in concentration and ∼60% in EF from the 1950s to the 2000s, more than 80% of present-day As in Greenland is of anthropogenic origin, probably due to increasing As emissions from coal combustion in China. This highlights the demand for the implementation of national and international environmental regulations to further reduce As emissions.

Anthropogenic Pb emitted from East Asia, particularly China, is often long-range transported to the east by the prevailing westerlies. To characterize the geographical properties of varying atmospheric Pb concentrations by transboundary and domestic source(s)-related Pb in Korea, closely adjacent to China, the Al and Pb concentrations and the stable Pb isotopic composition were determined in the total suspended particles (TSP) collected at urban (IC), rural (TA), and remote background (JJ) sites in western Korea from August 2015 to October 2016. The annual average Pb concentrations were significantly higher in urban and rural areas (IC, 16.2 ng m -3 and TA, 11.1 ng m -3 ) than in remote area (JJ, 6.41 ng m -3 ), showing pronounced seasonal variations with relatively higher concentrations in winter and spring and lower concentrations in summer and autumn. Significantly high enrichment factors (EF) for Pb indicate that anthropogenic contributions are important for this toxic element in TSP. Coupling the Pb isotopic signatures with the air mass back trajectories identified the major potential source regions for individual samples. The results show that during winter, China was the dominant contributor, accounting for 92%, 82%, and 100% of the sampling periods at IC, TA, and JJ, respectively. The Chinese contribution decreased in summer and autumn, whereas the Korean contribution increased, according to the East Asian monsoon system. The Pb concentrations increased by 2.2 (IC), 1.2 (TA) and 1.4 (JJ) times when the Chinese contribution was dominant, compared to the Korea-dominant periods. The Pb isotopic systematics for the samples characterized by the dominant Korean contribution differed substantially between the three sites, implying that the relative importance of various domestic sources varied with geographical areas in western Korea., (Copyright © 2019 Elsevier Ltd. All rights reserved.)

A total of 82 aerosol samples (PM 10-2.5 ) were collected from June 18, 2015 to October 1, 2016 at the remote sea site, the Ieodo Ocean Research Station (IORS), in the East China Sea. Samples were analyzed for 10 elements (Al, Fe, Cu, Zn, As, Mo, Cd, Sb, Tl, and Pb) as well as Pb isotopic composition to characterize temporal variations in elemental concentration levels, and to identify the potential source regions of atmospheric pollutants transported over the remote East China Sea. The results showed that the annual average element concentrations were lowest compared to those at different sites in East Asia, suggesting a very clean background area of IORS, with values ranging from 114 ng m -3 for Al to 0.045 ng m -3 for Tl. Concentrations averaged seasonally for all the elements revealed the highest levels occurring between winter and spring, and the lowest levels in summer. High enrichment factors (EF) of more than 100 for trace elements suggest that these elements originated mostly from anthropogenic sources. Coupling the Pb isotopic composition with a back trajectory analysis identified the potential source regions for each sample. Our approach identified China as a dominant contributor affecting atmospheric composition changes at IORS, the remote area of the East China Sea. As the largest anthropogenic emission source in East Asia, China contributed to almost 100% of the elemental concentration levels in winter and spring, ∼53% in summer and ∼63% in autumn. Because IORS's ambient air is sensitive to even slight changes in pollutant loading due to the significantly low pollution levels, long-term monitoring of air quality at IORS will provide invaluable information on the progress and efforts of atmospheric pollution management linked to emission controls in East Asian countries, especially China., (Copyright © 2017 Elsevier Ltd. All rights reserved.)

We present high-resolution lead (Pb) concentrations and isotopic ratios from a northwest Greenland snow pit covering a six-year period between 2003 and 2009. Pb concentrations ranged widely from 2.7 pg g -1 to 97.3 pg g -1 , with a mean concentration of 21.6 pg g -1 . These values are higher than those recorded for the pre-industrial period. Pb concentrations exhibit seasonal spikes in winter-spring layers. Crustal Pb enrichment factors (EF) suggest that the northwest Greenland snow pit is highly enriched with Pb of predominantly anthropogenic origin. The 206 Pb/ 207 Pb ratios ranged from 1.144 to 1.169 with a mean value of 1.156, which fall between less radiogenic Eurasian-type and more radiogenic Canadian-type signatures. This result suggests that several potential source areas of Pb impact on northwest Greenland. Abrupt changes in Pb concentrations and Pb isotope ratios were observed and related to seasonal shifts in source regions of aerosol transport. The 206 Pb/ 207 Pb isotope ratio increased gradually between 2003 and 2009. The similarity of the three-isotope plot ( 206 Pb/ 207 Pb versus 208 Pb/ 207 Pb) between some of our samples and Chinese urban aerosols suggests a steadily increasing contribution of Chinese Pb to northwest Greenland snow., (Copyright © 2017. Published by Elsevier Ltd.)

Lead (Pb) isotopic compositions and concentrations, and barium (Ba) and indium (In) concentrations have been analysed at sub-annual resolution in three sections from a <110 m ice core dated to the 18th and 20th centuries, as well as snow pit samples dated to 2004/2005, recovered from the East Rongbuk Glacier in the high-altitude Himalayas. Ice core sections indicate that atmospheric chemistry prior to ~1,953 was controlled by mineral dust inputs, with no discernible volcanic or anthropogenic contributions. Eighteenth century monsoon ice core chemistry is indicative of dominant contributions from local Himalayan sources; non-monsoon ice core chemistry is linked to contributions from local (Himalayan), regional (Indian/Thar Desert) and long-range (North Africa, Central Asia) sources. Twentieth century monsoon and non-monsoon ice core data demonstrate similar seasonal sources of mineral dust, however with a transition to less-radiogenic isotopic signatures that suggests local and regional climate/environmental change. The snow pit record demonstrates natural and anthropogenic contributions during both seasons, with increased anthropogenic influence during non-monsoon times. Monsoon anthropogenic inputs are most likely sourced to South/South-East Asia and/or India, whereas non-monsoon anthropogenic inputs are most likely sourced to India and Central Asia., (Copyright © 2014 Elsevier B.V. All rights reserved.)

We report the first comprehensive and reliable time series for As, Mo, Sb, and Tl in the snowpack from Dome Fuji in the central East Antarctic Plateau. Our results show significant enrichment of these elements due to either anthropogenic activities or large volcanic eruptions during the past 50 years. With respect to the values reported from 1960 to 1964, we observed the maximum increases in crustal enrichment factors (EFs) for As (a factor of ~15), Mo (~4), Sb (~4), and Tl (~2) during the period between the 1970s and 1990s, reflecting the global dispersion of anthropogenic pollutants of these elements, even to the most remote areas on Earth. Such enrichments are likely related to emissions of trace elements from nonferrous metal smelting and fossil fuel combustion processes in South America, especially in Chile. A drastic decrease in the As concentration and its EF values was observed after the year 2000 in response to the introduction of environmental regulations in the 1990s to reduce As emissions from the copper industry, primarily in Chile. The observed decrease suggests that governmental regulations for pollution control are effective in reducing air pollution at both the regional and global level.

A long-term record, extending back 800 years (1205 to 2002 AD), of the Pb isotopic composition ((206)Pb/(207)Pb and (208)Pb/(207)Pb) as well as Pb concentrations from high altitude Mt. Everest ice cores has the potential to identify sources and source regions affecting natural and anthropogenic Pb deposition in central Asia. The results show that the regional natural background Pb isotope signature (~1.20 for (206)Pb/(207)Pb and ~2.50 for (208)Pb/(207)Pb) in the central Himalayas was dominated by mineral dust over the last ~750 years from 1205 to 1960s, mostly originating from local sources with occasional contributions of long-range transported dust probably from Sahara desert and northwestern India. Since the 1970s, the Pb isotope ratios are characterized by a continuous decline toward less radiogenic ratios with the least mean ratios of 1.178 for (206)Pb/(207)Pb and 2.471 for (208)Pb/(207)Pb in the period 1990-1996. The depression of the (206)Pb/(207)Pb and (208)Pb/(207)Pb values during the corresponding periods is most likely due to an increasing influence of less radiogenic Pb of anthropogenic origin mainly from leaded gasoline used in South Asia (India as well as possibly Bangladesh and Nepal). From 1997 to 2002, isotopic composition tends to show a shift to slightly more radiogenic signature. This is likely attributed to reducing Pb emissions from leaded gasoline in source regions, coinciding with the nationwide reduction of Pb in gasoline and subsequent phase-out of leaded gasoline in South Asia since 1997. An interesting feature is the relatively high levels of Pb concentrations and enrichment factors (EF) between 1997 and 2002. Although the reason for this feature remains uncertain, it would be probably linked with an increasing influence of anthropogenic Pb emitted from other sources such as fossil fuel combustion and non-ferrous metal production., (Copyright © 2011 Elsevier B.V. All rights reserved.)

A series of 42 snow samples covering over a one-year period from the fall of 2004 to the summer of 2005 were collected from a 2.1-m snow pit at a high-altitude site on the northeastern slope of Mt. Everest. These samples were analyzed for Al, V, Cr, Mn, Co, Ni, Cu, Zn, As, Rb, Sr, Cd, Sb, Pb, and Bi in order to characterize the relative contributions from anthropogenic and natural sources to the fallout of these elements in central Himalayas. Our data were also considered in the context of monsoon versus non-monsoon seasons. The mean concentrations of the majority of the elements were determined to be at the pg g(-1) level with a strong variation in concentration with snow depth. While the mean concentrations of most of the elements were significantly higher during the non-monsoon season than during the monsoon season, considerable variability in the trace element inputs to the snow was observed during both periods. Cu, Zn, As, Cd, Sb, and Bi displayed high crustal enrichment factors (EFc) in most samples, while Cr, Ni, Rb, and Pb show high EFc values in some of the samples. Our data indicate that anthropogenic inputs are potentially important for these elements in the remote high-altitude atmosphere in the central Himalayas. The relationship between the EFc of each element and the Al concentration indicates that a dominant input of anthropogenic trace elements occurs during both the monsoon and non-monsoon seasons, when crustal contribution is relatively minor. Finally, a comparison of the trace element fallout fluxes calculated in our samples with those recently obtained at Mont Blanc, Greenland, and Antarctica provides direct evidence for a geographical gradient of the atmospheric pollution with trace elements on a global scale.

V, Co, Cu, Zn, As, Rb, Sr, Ag, Cd, Ba, Pb, Bi and U have been analysed by inductively coupled plasma sector field mass spectrometry in various sections of a dated snow/ice core drilled at an altitude of 6542 m on the Sajama ice cap in Bolivia. The analysed sections were dated from the Last Glacial Stage ( approximately 22,000 years ago), the Mid-Holocene and the last centuries. The observed variations of crustal enrichment factors (EFc) for the various metals show contrasting situations. For V, Co, Rb, Sr and U, EFc values close to unity are observed for all sections, then showing that these elements are mainly derived from rock and soil dust. For the other metals, clear time trends are observed, with a pronounced increase of EFc values during the 19th and 20th centuries. This increase shows evidence of metal pollution associated with human activity in South America. For Pb an important contribution was from gasoline additives. For metals such as Cu, Zn, Ag and Cd an important contribution was from metal production activities, with a continuous increase of production during the 20th century in countries such as Peru, Chile and Bolivia.