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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.

Abstract. Two aerosol samples collected at King Sejong Korean scientific research station, Antarctica, on 9 December 2011 in the austral summer (sample S1) and 23 July 2012 in the austral winter (sample S2), when the oceanic chlorophyll a levels on the collection days of the samples were quite different, by  ∼  19 times (2.46 vs. 0.13 µg L−1, respectively), were investigated on a single-particle basis using quantitative energy-dispersive electron probe X-ray microanalysis (ED-EPMA), called low-Z particle EPMA, Raman microspectrometry (RMS), and attenuated total reflection Fourier transform infrared (ATR-FTIR) imaging techniques to obtain their characteristics based on the elemental chemical compositions, molecular species, and mixing state. X-ray analysis showed that the supermicron summertime and wintertime Antarctic aerosol samples have different elemental chemical compositions, even though all the individual particles analyzed were sea spray aerosols (SSAs); i.e., the contents of C, O, Ca, S, and Si were more elevated, whereas Cl was more depleted, for sample S1 than for sample S2. Based on qualitative analysis of the chemical species present in individual SSAs by the combined application of RMS and ATR-FTIR imaging, different organic species were observed in samples S1 and S2; i.e., Mg hydrate salts of alanine were predominant in samples S1 and S2, whereas Mg salts of fatty acids internally mixed with Mg hydrate salts of alanine were significant in sample S2. Although CaSO4 was observed significantly in both samples S1 and S2, other inorganic species, such as Na2SO4, NaNO3, Mg(NO3)2, SiO2, and CH3SO3Mg, were observed more significantly in sample S1, suggesting that those compounds may be related to the higher phytoplankton activity in summer.

As, Mo, Sn, and Sb have been determined by inductively coupled plasma sector field mass spectrometry (ICP-SFMS) in 143 depth intervals of high-altitude ice cores from Mt. Everest, covering an 800-year time period from 1205 to 2002 AD. The results clearly demonstrate the long-term historical record of atmospheric transport and deposition of As, Mo, Sn, and Sb that has prevailed at high altitudes in the central Himalayas. Natural contributions, mainly from mineral dust, have dominated the atmospheric cycles of As, Mo, Sn, and to some extent Sb during the 700 years prior to the 20th century. Compared to those of the pre-1900 period, pronounced increases of both concentrations and crustal enrichment factors are observed since the 1970s, with the highest increase factor for Sn and the lowest for As. Such increases are attributed to anthropogenic emissions of these elements, largely from stationary fossil fuel combustion and nonferrous metals production, particularly in India. Our central Himalayan ice core record provides an explicit recognition of rising atmospheric As, Mo, Sn, and Sb pollution in response to rapid economic growth in central Asia.

Antarctic snow preserves an atmospheric archive that enables the study of global atmospheric changes and anthropogenic disturbances from the past. We report atmospheric deposition rates of platinum group elements (PGEs) in Antarctica during the last ∼ 50 years based on determinations of Pt, Ir, and Rh in snow samples collected from Queen Maud Land, East Antarctica to evaluate changes in the global atmospheric budget of these noble metals. The 50-year average PGE concentrations in Antarctic snow were 17 fg g(-1) (4.7-76 fg g(-1)) for Pt, 0.12 fg g(-1) (<0.05-0.34 fg g(-1)) for Ir, and 0.71 fg g(-1) (0.12-8.8 fg g(-1)) for Rh. The concentration peaks for Pt, Ir, and Rh were observed at depths corresponding to volcanic eruption periods, indicating that PGEs can be used as a good tracer of volcanic activity in the past. A significant increase in concentrations and crustal enrichment factors for Pt and a slight enhancement in enrichment factors for Rh were observed after the 1980s. This suggests that there has been large-scale atmospheric pollution for Pt and probably for Rh since the 1980s, which may be attributed to the increasing emissions of these metals from anthropogenic sources such as automobile catalysts and metal production processes.

Dust concentrations in Greenland ice show pronounced glacial/interglacial variations with almost two orders of magnitude increase during the Last Glacial Maximum. Greenland glacial dust was previously sourced to two East Asian deserts: the Taklimakan and Gobi deserts. Here we report the first high-resolution Pb and Sr isotopic evidence for a significant Saharan dust influence in Greenland during the last glacial period, back to ~31 kyr ago, from the Greenland NEEM ice core. We find that during Greenland Stadials 3–5.1 (~31 to 23 kyr ago), the primary dust provenance was East Asia, as previously proposed. Subsequently, the Saharan isotopic signals emerge during Greenland Stadials 2.1a–2.1c (~22.6 to 14.7 kyr ago) and from the late Bølling-Allerød to the Younger Dryas periods (~13.6 to 12 kyr ago), coincident with increased aridity in the Sahara and efficient northward transport of dust during these cold periods. A mixing isotopic model proposes the Sahara as an important source, accounting for contribution to Greenland glacial dust of up to 50%, particularly during Greenland Stadial 2.1b and the late Bølling-Allerød to the Younger Dryas periods. Our findings provide new insights into climate-related dust provenance changes and essential paleoclimatic constraints on dust-climate feedbacks in northern high latitudes.