Lead Isotopic Constraints on the Provenance of Antarctic Dust and Atmospheric Circulation Patterns Prior to the Mid-Brunhes Event (~430 kyr ago).

A lead (Pb) isotopic record, covering the two oldest glacial-interglacial cycles (~572 to 801 kyr ago) characterized by lukewarm interglacials in the European Project for Ice Coring in Antarctica Dome C ice core, provides evidence for dust provenance in central East Antarctic ice prior to the Mid-Brunhes Event (MBE), ~430 kyr ago. Combined with published post-MBE data, distinct isotopic compositions, coupled with isotope mixing model results, suggest Patagonia/Tierra del Fuego (TdF) as the most important sources of dust during both pre-MBE and post-MBE cold and intermediate glacial periods. During interglacials, central-western Argentina emerges as a major contributor, resulting from reduced dust supply from Patagonia/TdF after the MBE, contrasting to the persistent dominance of dust from Patagonia/TdF before the MBE. The data also show a small fraction of volcanic Pb transferred from extra-Antarctic volcanoes during post-MBE interglacials, as opposed to abundant transfer prior to the MBE. These differences are most likely attributed to the enhanced wet removal efficiency with the hydrological cycle intensified over the Southern Ocean, associated with a poleward shift of the southern westerly winds (SWW) during warmer post-MBE interglacials, and vice versa during cooler pre-MBE ones. Our results highlight sensitive responses of the SWW and the associated atmospheric conditions to stepwise Antarctic warming.

Reliable Ultra Trace Analysis of Cd, U and Zn Concentrations in Greenland Snow and Ice by Using Ultraclean Methods for Contamination Control.

This study presents ultraclean procedures used in the challenging task of determining trace elements at or below the pg/g concentration level encountered in Greenland snow and ice. In order to validate these ultraclean procedures, recent snowfall and Holocene ice from northwest Greenland were analyzed for Cd, U, and Zn concentrations. The total procedural blanks brought through the entire measurement procedure proved to be negligible, compared to trace element concentrations, measured in snow and ice samples. This validates the overall practicality of the proposed ultraclean procedures, thereby ensuring the reliable measurements of ultra-trace analysis. A comparison between our study and published data shows that improper procedures employed throughout all stages, from field sampling to analysis to elevate the concentrations by several orders of magnitude, relative to the reliable concentration ranges. The risk of contamination exposure for selected trace elements appears to increase in the order of U < As ≤ Pb < Cd < Zn. Reliable measurements of Cd, U, and Zn concentrations in snow and ice allowed us to interpret the data in terms of seasonal variations in the inputs of crustal and anthropogenic sources to Greenland ice sheet.

A 300-Year High-Resolution Greenland Ice Record of Large-Scale Atmospheric Pollution by Arsenic in the Northern Hemisphere.

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.

Persistent Pb Pollution in Central East Antarctic Snow: A Retrospective Assessment of Sources and Control Policy Implications.

Well-defined variations in the enrichments and isotopic compositions of Pb have been observed in snow from Dome Fuji and Dome A in the central East Antarctic Plateau (EAP) over the past few decades. The Pb isotopic fingerprints indicate that the rapid increase in Pb enrichments from the mid-1970s, reaching a peak in ∼1980, is due to the massive use of leaded gasoline in northern South America, especially Brazil. Since then, they show a continuous decline, mostly due to the significant removal of the Pb additives from gasoline in Brazil in the 1980s and, subsequently, in Argentina and Chile in the 1990s. After the phase-out of Pb in gasoline, Cu smelting in Chile has become the major source of Pb, contributing ∼90% to the total Pb emissions in northern South America in 2005. Nevertheless, Pb pollution in the central EAP declined substantially until recently as a result of the regulatory efforts to curb toxic trace metal emissions from the Cu industry in Chile. However, more than 90% of the Pb in the most remote places on Earth are still of anthropogenic origin, highlighting the need for the continuation of environmental regulations for the further reduction of Pb emissions.

Recent decline in atmospheric Pb deposition and isotopic constraints on changes in source contributions in snow from northwestern Greenland.

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.

Evidence of global-scale As, Mo, Sb, and Tl atmospheric pollution in the antarctic snow.

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.

Glaciers as microbial habitats: current knowledge and implication.

Glaciers, formed from the gradual accumulation of snow, can be continuous records representing past environments and recognized as a time capsule of our planetary evolution. Due to extremely harsh conditions, glacial ice has long been considered an uninhabitable ecosystem for microorganisms to sustain their life. However, recent developments in microbiological analysis techniques revealed the presence of unexpectedly diverse microbial strains. Glacial microorganisms could also provide valuable information, including not only biological diversity and structure but also molecular systematics, metabolic profiles, and evolutionary changes from the past climate and ecosystem. However, there are several obstacles in investigating the glacier environment, such as low regional accessibility, technical difficulties of ice coring, potential contamination during the sampling process, and low microbial biomass. This review aims to summarize recent knowledge on decontamination methods, biomass, diversity based on culture-dependent and -independent methods, application of biological proxies, greenhouse gas production and adaptive strategies in glaciers from various regions and to imply further directions for a comprehensive understanding of habitatility in an icy world including outer of our planet.

A 50-year record of platinum, iridium, and rhodium in Antarctic snow: volcanic and anthropogenic sources.

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.

Record of North American boreal forest fires in northwest Greenland snow.

We present boreal forest fire proxies in a northwest Greenland snowpit spanning a period of six years, from spring 2003 to summer 2009. Levoglucosan (C6H10O5) is a specific organic molecular marker of biomass burning caused by boreal forest fires. In this study, levoglucosan was determined via liquid chromatography/negative ion electrospray ionization-tandem mass spectrometry, wherein isotope-dilution and multiple reaction monitoring methods are employed. Ammonium (NH4+) and oxalate (C2O42-), traditional biomass burning proxies, were determined using two-channel ion chromatography. In the northwest Greenland snowpit, peaks in levoglucosan, ammonium, and oxalate were observed in snow layers corresponding to the summer-fall seasons of 2004 and 2005. Considered together, these spikes are a marker for large boreal forest fires. The levoglucosan deposited in the Greenland snow was strongly dependent on long-range atmospheric transportation. A 10-day backward air mass trajectory analysis supports that the major contributors were air masses from North America. In addition, satellite-derived carbon monoxide (CO) and ammonia (NH3) concentrations suggest that chemicals from North American boreal forest fires during the summer-fall of 2004 and 2005 were transported to Greenland. However, large boreal fires in Siberia in 2003 and 2008 were not recorded in the snowpit. The sub-annual resolution measurements of levoglucosan and ammonium can distinguish between the contributions of past boreal forest fires and soil emissions from anthropogenic activity to Greenland snow and ice.

Plutonium fallout reconstructed from an Antarctic Plateau snowpack using inductively coupled plasma sector field mass spectrometry.

Anthropogenic plutonium (Pu) in the environment is a result of atmospheric nuclear testing during the second half of the 20th century. In this work, we analyzed a 4-meter deep Antarctic Plateau snowpack characterized by a low snow accumulation rate and negligible snow impurities. These sample conditions enabled us to measure the snowpack Pu fallout by applying inductively coupled plasma sector field mass spectrometry to a few mL of snow melt without purification or preconcentration. Pu concentrations in the reconstructed Pu fallout record for the period after 1956 CE increased and decreased in agreement with past atmospheric nuclear testing. Two peaks and two dips associable with historical events were observed, and the highest peak in 1964(±1) CE approximately coincided with the maximum concentration of non-sea-salt sulfate caused by the Mt. Agung eruption in 1963 CE. Enhanced Pu fallout in the 1970s was attributed the geographical proximity of the Southern Hemispheric nuclear test sites. Our results suggest that by improving the instrumental sensitivity and precision, the potential of the Antarctic ice sheet as an archive of Pu fallout can be further explored and utilized for understanding atmospheric dispersion and for dating ice cores.

Characteristic concentrations and isotopic composition of airborne lead at urban, rural and remote sites in western Korea.

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.

Atmospheric pollution for trace elements in the remote high-altitude atmosphere in central Asia as recorded in snow from Mt. Qomolangma (Everest) of the Himalayas.

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.

Pb concentrations and isotopic record preserved in northwest Greenland snow.

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 206Pb/207Pb 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 206Pb/207Pb isotope ratio increased gradually between 2003 and 2009. The similarity of the three-isotope plot (206Pb/207Pb versus 208Pb/207Pb) between some of our samples and Chinese urban aerosols suggests a steadily increasing contribution of Chinese Pb to northwest Greenland snow.

Net deposition of mercury to the Antarctic Plateau enhanced by sea salt.

Photochemically driven mercury (Hg) exchange between the atmosphere and the Antarctic Plateau snowpack has been observed. An imbalance in bidirectional flux causes a fraction of Hg to remain in the snowpack perennially, but the factors that control the amount of Hg sequestered on the Antarctic Plateau are not fully understood. We analyzed sub-annual variations in total Hg (HgT) deposition to Dome Fuji over the period of 1986-2010 using cold vapor inductively coupled plasma mass spectrometry and compared concentrations with those of sea salt components (Na+ and Cl-). HgT ranged from 0.12 to 5.19pgg-1 (n=78) and was relatively high when the Na+ concentrations were high in the same or underlying snow layers. A significant correlation (r=0.7) was found between the annual deposition fluxes of HgT and Na+. Despite different origins and behavior of Hg and sea salt, the near-synchronous increases in the concentrations and correlation between the fluxes suggest that sea salt can intervene in the air-snow Hg exchange and promote the net deposition of Hg in the Antarctic Plateau.

Characteristics of elemental and Pb isotopic compositions in aerosols (PM10-2.5) at the Ieodo Ocean Research Station in the East China Sea.

A total of 82 aerosol samples (PM10-2.5) 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.

Seasonal variation in the input of atmospheric selenium to northwestern Greenland snow.

Oxygen isotope ratio (δ(18)O) and concentrations of Al, Na(+), methanesulfonic acid (MSA), SO4(2-), and selenium (Se) in a continuous series of 70 snow samples from a 3.2-m snow pit at a site in northwestern Greenland were determined using ultraclean procedures. Well-defined depth profiles of δ(18)O, Al, and sea-salt-Na(+) allowed the determination of chronology of the snow pit that spanned approximately 6 years from spring 2003 to summer 2009. Se concentrations were at a low pg/g level, ranging from 7.2 to 45 pg/g, and exhibited high variability with generally higher values during winter and spring and lower values during summer and fall. Very high crustal enrichment factors (EFc) of Se averaging approximately 26,600 for the entire time period indicate a small contribution from crust dust. High Se/MSA ratios are generally observed in the winter and spring snow layers, in which the Se concentrations were relatively high (>20 pg/g). This suggests that a significant component of the Se present in the snow layers is of anthropogenic origin. During the summer season, however, high EFc values are accompanied with low Se/MSA, indicating an increased contribution of marine biogenic sources. Significant correlations between Se, Al, and non-sea-salt SO4(2-) highlight that significant inputs of Se to the snow are likely controlled by the seasonality in the transport efficiency of anthropogenic Se from the source regions to the site. Based on the seasonal changes in Se concentrations, Se/MSA, and Se/S ratios observed in the samples, the input of anthropogenic Se to the site appears to be governed by the long-range transportation of Se emitted from coal combustion in East Asian countries, especially in China.

Determination of lead isotopes in a new Greenland deep ice core at the sub-picogram per gram level by thermal ionization mass spectrometry using an improved decontamination method.

An improved decontamination method and ultraclean analytical procedures have been developed to minimize Pb contamination of processed glacial ice cores and to achieve reliable determination of Pb isotopes in North Greenland Eemian Ice Drilling (NEEM) deep ice core sections with concentrations at the sub-picogram per gram level. A PL-7 (Fuso Chemical) silica-gel activator has replaced the previously used colloidal silica activator produced by Merck and has been shown to provide sufficiently enhanced ion beam intensity for Pb isotope analysis for a few tens of picograms of Pb. Considering the quantities of Pb contained in the NEEM Greenland ice core and a sample weight of 10 g used for the analysis, the blank contribution from the sample treatment was observed to be negligible. The decontamination and analysis of the artificial ice cores and selected NEEM Greenland ice core sections confirmed the cleanliness and effectiveness of the overall analytical process.

Mineralogical and chemical changes in pyrite after traditional processing for use in medicines.

Pyrite has been the most commonly used medicinal mineral, and its toxicity was reduced by traditional processing operations including heating and quenching in vinegar. To verify the scientific effects of this process, pyrite was processed at temperatures up to 850 degrees C and through as many as five processing cycles. A metal extraction test was carried out from the processed pyrites on the assumption that pyrite medicines with the lowest toxic metal content would be most desirable. Increasing temperature and the number of processing cycles promoted phase change of pyrite to hematite, reduction of toxic metals in pyrite and their concentrations in the extraction solutions. However, the relationships between variations in extracted elements and the number of processing cycles at the same processing temperature were not clearly defined. Heating temperature is more important than the number of processing cycles for effective processing, and pyrite should be processed at the highest possible temperature in order to diminish highly toxic metals such as As and Pb.

Deposition of organochlorine pesticides into the surface snow of East Antarctica.

Organochlorine pesticides (OCPs) were measured in surface snow collected on a ~1400-km inland traverse beginning from the coastal regions of East Antarctica during the Japanese Antarctic Research Expedition (JARE) of 2007/2008. Of the 22 OCPs, α-hexachlorocyclohexane (HCH), γ-HCH, and hexachlorobenzene (HCB) were frequently detected in the snow with concentration ranges of 17.5-83.2, 33-137, and ND-182 pg L(-1), respectively. The most abundant pesticide was γ-HCH, with a mean concentration of 69.9 pg L(-1), followed by α-HCH, with an average concentration of 44.5 pg L(-1). The spatial variability of α-HCH and γ-HCH was narrow, and the concentrations of α-HCH and γ-HCH increased slightly with increasing altitude along the traverse route. Dome Fuji, the highest altitude sampling point, had the highest γ-HCH concentrations in the snow. Backward air trajectory analysis showed that the air masses at the sampling sites came mainly from the Indian and Atlantic Oceans and over the Antarctic continent, indicating that the OCPs were subjected to long-range atmospheric transport and were deposited in the surface snow. Our data suggest that the snow of Antarctica contains low levels of OCPs.

Isotopic signatures for natural versus anthropogenic Pb in high-altitude Mt. Everest ice cores during the past 800 years.

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.