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Atmospheric gaseous elemental mercury (GEM) concentrations in the Arctic exhibit a clear summertime maximum, while the origin of this peak is still a matter of debate in the community. Based on summertime observations during the Multidisciplinary drifting Observatory for the Study of Arctic Climate (MOSAiC) expedition and a modeling approach, we further investigate the sources of atmospheric Hg in the central Arctic. Simulations with a generalized additive model (GAM) show that long-range transport of anthropogenic and terrestrial Hg from lower latitudes is a minor contribution (~2%), and more than 50% of the explained GEM variability is caused by oceanic evasion. A potential source contribution function (PSCF) analysis further shows that oceanic evasion is not significant throughout the ice-covered central Arctic Ocean but mainly occurs in the Marginal Ice Zone (MIZ) due to the specific environmental conditions in that region. Our results suggest that this regional process could be the leading contributor to the observed summertime GEM maximum. In the context of rapid Arctic warming and the observed increase in width of the MIZ, oceanic Hg evasion may become more significant and strengthen the role of the central Arctic Ocean as a summertime source of atmospheric Hg. Oceanic evasion, which mainly occurs in the Marginal Ice Zone, is the main cause of the summertime maximum of gaseous elemental mercury in the central Arctic Ocean [ABSTRACT FROM AUTHOR]

Despite the key role of the Arctic in the global Earth system, year-round in-situ atmospheric composition observations within the Arctic are sparse and mostly rely on measurements at ground-based coastal stations. Measurements of a suite of in-situ trace gases were performed in the central Arctic during the Multidisciplinary drifting Observatory for the Study of Arctic Climate (MOSAiC) expedition. These observations give a comprehensive picture of year-round near-surface atmospheric abundances of key greenhouse and trace gases, i.e., carbon dioxide, methane, nitrous oxide, ozone, carbon monoxide, dimethylsulfide, sulfur dioxide, elemental mercury, and selected volatile organic compounds (VOCs). Redundancy in certain measurements supported continuity and permitted cross-evaluation and validation of the data. This paper gives an overview of the trace gas measurements conducted during MOSAiC and highlights the high quality of the monitoring activities. In addition, in the case of redundant measurements, merged datasets are provided and recommended for further use by the scientific community. Measurement(s) atmospheric ozone • atmospheric carbon dioxide • atmospheric methane • atmospheric carbon monoxide • atmospheric nitrous oxide • atmospheric dimethylsulfide • atmospheric sulfur dioxide • atmospheric gaseous elemental mercury • volatile organic compounds Technology Type(s) ozone analyzer • carbon dioxide analyzer • methane analyzer • carbon monoxide analyzer • nitrous oxide analyzer • dimethylsulfide analyzer • sulfur dioxide analyzer • gaseous elemental mercury analyzer • gas chromatography-mass spectrometry Sample Characteristic - Environment Atmosphere Sample Characteristic - Location central Arctic [ABSTRACT FROM AUTHOR]

Mercury (Hg) is an environmental toxicant dangerous to human health and the environment. Its anthropogenic emissions are regulated by global, regional, and local policies. Here, we investigate Hg sources in the coastal city of Boston, the third largest metropolitan area in the Northeastern United States. With a median of 1.37 ng m³, atmospheric Hg concentrations measured from August 2017 to April 2019 were at the low end of the range reported in the Northern Hemisphere and in the range reported at North American rural sites. Despite relatively low ambient Hg concentrations, we estimate anthropogenic emissions to be 3-7 times higher than in current emission inventories using a measurement-model framework, suggesting an underestimation of small point and/or nonpoint emissions. We also test the hypothesis that a legacy Hg source from the ocean contributes to atmospheric Hg concentrations in the study area; legacy emissions (recycling of previously deposited Hg) account for ~60% of Hg emitted annually worldwide (and much of this recycling takes place through the oceans). We find that elevated concentrations observed during easterly oceanic winds can be fully explained by low wind speeds and recirculating air allowing for accumulation of land-based emissions. This study suggests that the influence of nonpoint land-based emissions may be comparable in size to point sources in some regions and highlights the benefits of further top-down studies in other areas. [ABSTRACT FROM AUTHOR]

Understanding the processes that influence and control carbon cycling in Arctic tundra ecosystems is essential for making accurate predictions about what role these ecosystems will play in potential future climate change scenarios. Particularly, air–surface fluxes of methane and carbon dioxide are of interest as recent observations suggest that the vast stores of soil carbon found in the Arctic tundra are becoming more available to release to the atmosphere in the form of these greenhouse gases. Further, harsh wintertime conditions and complex logistics have limited the number of year-round and cold-season studies and hence too our understanding of carbon cycle processes during these periods. We present here a two-year micrometeorological data set of methane and carbon dioxide fluxes, along with supporting soil pore gas profiles, that provide near-continuous data throughout the active summer and cold winter seasons. Net emission of methane and carbon dioxide in one of the study years totalled 3.7 and 89 g C m -2 a -1 respectively, with cold-season methane emission representing 54 % of the annual total. In the other year, net emission totals of methane and carbon dioxide were 4.9 and 485 g C m -2 a -1 respectively, with cold-season methane emission here representing 82 % of the annual total – a larger proportion than has been previously reported in the Arctic tundra. Regression tree analysis suggests that, due to relatively warmer air temperatures and deeper snow depths, deeper soil horizons – where most microbial methanogenic activity takes place – remained warm enough to maintain efficient methane production whilst surface soil temperatures were simultaneously cold enough to limit microbial methanotrophic activity. These results provide valuable insight into how a changing Arctic climate may impact methane emission, and highlight a need to focus on soil temperatures throughout the entire active soil profile, rather than rely on air temperature as a proxy for modelling temperature–methane flux dynamics. [ABSTRACT FROM AUTHOR]

Understanding the processes that influence and control carbon cycling in Arctic tundra ecosystems is essential for making accurate predictions about what role these ecosystems will play in potential future climate change scenarios. Particularly, air--surface fluxes of methane and carbon dioxide are of interest as recent observations suggest that the vast stores of soil carbon found in the Arctic tundra are becoming more available to release to the atmosphere in the form of these greenhouse gases. Further, harsh wintertime conditions and complex logistics have limited the number of year-round and cold season studies and hence too our understanding of carbon cycle processes during these periods. We present here a two-year micrometeorological data set of methane and carbon dioxide fluxes that provides near-continuous data throughout the active summer and cold winter seasons. Net emission of methane and carbon dioxide in one of the study years totalled 3.7 and 89 g C m-2 a-1 respectively, with cold season methane emission representing 54% of the annual total. In the other year, net emission totals of methane and carbon dioxide were 4.9 and 485 g C m-2 a-1 respectively, with cold season methane emission here representing 82 % of the annual total - a larger proportion than has been previously reported in the Arctic tundra. Regression tree analysis suggests that, due to relatively warmer air temperatures and deeper snow depths, deeper soil horizons - where most microbial methanogenic activity takes place - remained warm enough to maintain efficient methane production whilst surface soil temperatures were simultaneously cold enough to limit microbial methanotrophic activity. These results provide valuable insight into how a changing Arctic climate may impact methane emission, and highlight a need to focus on soil temperatures throughout the entire active soil profile, rather than rely on air temperature as a proxy for modelling temperature--methane flux dynamics. [ABSTRACT FROM AUTHOR]

A total of 1360 weeks of mercury (Hg) wet deposition data were collected by the state of Alaska Department of Environmental Conservation and the U.S. National Park Service across five stations spanning up to 8 years. Here, we analyze concentration patterns, source regions, and seasonal and annual Hg deposition loadings across these five sites in Alaska, along with auxiliary trace metals including Cr, Ni, As, and Pb. We found that Hg concentrations in precipitation at the two northernmost stations, Nome (64.5 ∘ N) along the coast of the Bering Sea and the inland site of Gates of the Arctic (66.9 ∘ N), were statistically higher (average of 5.3 and 5.5 ng L -1 , respectively) than those at the two lowest-latitude sites, Kodiak Island (57.7 ∘ N, 2.7 ng L -1) and Glacier Bay (58.5 ∘ N, 2.6 ng L -1). These differences were largely explained by different precipitation regimes, with higher precipitation at the lower-latitude stations leading to dilution effects. The highest annual Hg deposition loads were consistently observed at Kodiak Island (4.80±1.04 µ g m -2) , while the lowest annual deposition was at Gates of the Arctic (2.11±0.67 µ g m -2). Across all stations and collection years, annual precipitation strongly controlled annual Hg deposition, explaining 73 % of the variability in observed annual Hg deposition. The data further showed that annual Hg deposition loads across all five Alaska sites were consistently among the lowest in the United States, ranking in the lowest 1 % to 5 % of over 99 monitoring stations. Detailed back-trajectory analyses showed diffuse source regions for most Hg deposition sites suggesting largely global or regional Hg sources. One notable exception was Nome, where we found increased Hg contributions from the western Pacific Ocean downwind of East Asia. Analysis of other trace elements (As, Cr, Cu, Ni, Pb, Se, Zn) from Dutch Harbor, Nome, and Kodiak Island showed generally higher trace metal concentrations at the northern station Nome compared to Kodiak Island further to the south, with concentrations at Dutch Harbor falling in between. Across all sites, we find two distinct groups of correlating elements: Cr and Ni and As and Pb. We attribute these associations to possibly different source origins, whereby sources of Ni and Cr may be derived from crustal (e.g., dust) sources while As and Pb may include long-range transport of anthropogenic pollution. Hg was not strongly associated with either of these two groups. [ABSTRACT FROM AUTHOR]

A total of 1,360 weeks of mercury (Hg) wet deposition data were collected by the State of Alaska Department of Environmental Conservation and the U.S. National Park Service, across five stations covering up to eight years. Here, we analyze concentration patterns, source regions, and seasonal and annual deposition loadings across these five sites in Alaska, along with auxiliary trace metals including Cr, Ni, As, and Pb. We found that Hg concentrations in precipitation at the two northern-most stations, Nome (64.5°N) along the coast of the Bering Sea and the inland site of Gates of the Arctic (66.9°N), were significantly higher (average of 5.3 ng L-1 and 5.5 ng L-1, respectively) than those at the two lowest-latitude sites, Kodiak Island (57.7°N, 2.7 ng L-1) and Glacier Bay (58.5°N, 2.6 ng L-1). These differences were largely explained by different precipitation regimes, with higher amounts of precipitation at the lower latitude stations leading to dilution effects. Highest annual Hg deposition loads were consistently observed at Kodiak Island (4.80 +/- 1.04μg m-2), while lowest annual deposition was at Gates of the Arctic (2.11 +/- 0.67μg m-2). Across all stations and collection years, annual precipitation overwhelmingly controlled annual Hg deposition, explaining 73% of the variability in observed annual Hg deposition. Our analyses further showed that annual Hg deposition loads across all five Alaska sites were consistently among the lowest in the United States, ranking in the lowest 1 to 5 percent of over 99 monitoring stations. Detailed back trajectory analyses showed diffuse source regions for most Hg deposition sites, which were almost identical with precipitation origins, suggesting global or regional Hg sources. One notable exception was Nome where we found pronounced differences between precipitation and Hg source origins with increased Hg contributions from the western Pacific Ocean downwind of East Asia. Analysis of multiple trace elements from Dutch Harbor, Nome, and Kodiak Island showed generally higher trace metal concentrations at the northern station Nome compared to Kodiak Island further to the south, with concentrations at Dutch Harbor falling in-between. Across all sites, we find two distinct groups of correlating elements: Cr and Ni and As and Pb. We attribute these associations to possibly different source origins, whereby sources of Ni and Cr may be derived from crustal (e.g., dust) sources while As and Pb may include long-range transport of anthropogenic pollution. Neither Hg nor any of the other trace elements analyzed, consistently associated with these two groups of elements, suggesting largely diffuse source origins. Calculations of enrichment factors (i.e., elemental enrichment compared to the upper continental crust) show low enrichment for Cr and Ni which is in support of a predominantly crustal source. High enrichment factors for Pb and Se are indicative of anthropogenic or additional natural sources for these elements. For most other elements including Hg, enrichment factors fell in-between these groups showing no clear source attribution to either crustal or anthropogenic source origins. [ABSTRACT FROM AUTHOR]

Passive air samplers (PASs) for gaseous mercury (Hg) were deployed for time periods between 1 month and 1 year at 20 sites across the globe with continuous atmospheric Hg monitoring using active Tekran instruments. The purpose was to evaluate the accuracy of the PAS vis-à-vis the industry standard active instruments and to determine a sampling rate (SR; the volume of air stripped of gaseous Hg per unit of time) that is applicable across a wide range of conditions. The sites spanned a wide range of latitudes, altitudes, meteorological conditions, and gaseous Hg concentrations. Precision, based on 378 replicated deployments performed by numerous personnel at multiple sites, is 3.6 ±3.0 %1 confirming the PAS's excellent reproducibility and ease of use. Using a SR previously determined at a single site, gaseous Hg concentrations derived from the globally distributed PASs deviate from Tekran-based concentrations by 14.2 ±10 %. A recalibration using the entire new data set yields a slightly higher SR of 0.1354 ±0.016m3 day-1. When concentrations are derived from the PAS using this revised SR the difference between concentrations from active and passive sampling is reduced to 8.8 ±7.5 %. At the mean gaseous Hg concentration across the study sites of 1.54 ngm-3, this represents an ability to resolve concentrations to within 0.13 ngm-3. Adjusting the sampling rate to deployment specific temperatures and wind speeds does not decrease the difference in active- passive concentration further (8.7 ±5.7 %), but reduces its variability by leading to better agreement in Hg concentrations measured at sites with very high and very low temperatures and very high wind speeds. This value (8.7 ±5.7 %) represents a conservative assessment of the overall uncertainty of the PAS due to inherent uncertainties of the Tekran instruments. Going forward, the recalibrated SR adjusted for temperature and wind speed should be used, especially if conditions are highly variable or deviate considerably from the average of the deployments in this study (9.89 °C, 3.41 ms-1/. Overall, the study demonstrates that the sampler is capable of recording background gaseous Hg concentrations across a wide range of environmental conditions with accuracy similar to that of industry standard active sampling instruments. Results at sites with active speciation units were inconclusive on whether the PASs take up total gaseous Hg oxidized Hg concentrations were in a similar range as the uncertainty of the PAS. or solely gaseous elemental Hg primarily because gaseous [ABSTRACT FROM AUTHOR]

Passive air samplers (PASs) for gaseous mercury (Hg) were deployed for time periods between 1 month and 1 year at 20 sites across the globe with continuous atmospheric Hg monitoring using active Tekran instruments. The purpose was to evaluate the accuracy of the PAS vis-à-vis the industry standard active instruments and to determine a sampling rate (SR; the volume of air stripped of gaseous Hg per unit of time) that is applicable across a broad variety of conditions. The sites spanned a wide range of latitudes, altitudes, meteorological conditions, and gaseous Hg concentrations. Precision, based on 378 replicated deployments performed by numerous personnel at multiple sites, is 3.6 ± 3.0 %*, confirming the PAS's excellent reproducibility and ease-of-use. Using a SR previously determined at a single site, gaseous Hg concentrations derived from the globally distributed PASs deviate from Tekran-based concentrations by 14.2 ± 10 %. A recalibration using the entire new data set yields a slightly higher SR of 0.1354 ± 0.016 m3 day−1. When concentrations are derived from the PAS using this revised SR the difference is reduced to 8.8 ± 7.5 %. At the mean gaseous Hg concentration across the study sites of 1.54 ng m−3, this represents an ability to resolve concentrations to within 0.13 ng m−3. Adjusting the sampling rate to deployment specific temperatures and wind speeds does not decrease the difference in active–passive concentration further (8.7 ± 5.7 %), but reduces its variability by leading to better agreement in Hg concentrations measured at sites with very high and very low temperatures and very high wind speeds. This value (8.7 ± 5.7 %) represents a conservative assessment of the overall uncertainty of the PAS due to inherent uncertainties of the Tekran instruments. Going forward, the recalibrated SR adjusted for temperature and wind speed should be used, especially if conditions are highly variable or deviate considerably from the average of the deployments in this study (9.89 °C, 3.41 m s−1). Overall, the study demonstrates that the sampler is capable of recording background gaseous Hg concentrations across a wide range of environmental conditions with accuracy similar to that of industry standard active sampling instruments. Results at sites with active speciation units were inconclusive on whether the PASs take up total gaseous Hg or solely gaseous elemental Hg primarily because gaseous oxidized Hg concentrations were in a similar range as the uncertainty of the PAS. [ABSTRACT FROM AUTHOR]

Aerodynamic gradient measurements of the air- surface exchange of gaseous elemental mercury (GEM) were undertaken over a 40 ha alpine grassland in Australia's Snowy Mountains region across a 3-week period during the late austral summer. Bi-directional GEM fluxes were observed throughout the study, with overall mean value of 0.2±14.5 ngm-2 h-1 and mean nocturnal fluxes of -1.5±7.8 ngm-2 h-1 compared to diurnal fluxes of 1.8±18.6 ngm-2 h-1 . Deposition velocities ranged from -2.2 to 2.9 cm s-1, whilst ambient GEM concentrations throughout the study were 0.59±0.10 ngm-3. Cumulative GEM fluxes correlated well with 24 h running mean soil temperatures, and one precipitation event was shown to have a positive impact on diurnal emission fluxes. The underlying vegetation had largely senesced and showed little stomatal control on fluxes. Nocturnal atmospheric mercury depletion events (NAMDEs) were observed concomitant with O3 depletion and dew formation under shallow, stable nocturnal boundary layers. A mass balance box model was able to reproduce ambient GEM concentration patterns during NAMDE and non-NAMDE nights without invoking chemical oxidation of GEM throughout the column, indicating a significant role of surface processes controlling deposition in these events. Surface deposition was enhanced under NAMDE nights, though uptake to dew likely represents less than one-fifth of this enhanced deposition. Instead, enhancement of the surface GEM gradient as a result of oxidation at the surface in the presence of dew is hypothesised to be responsible for a large portion of GEM depletion during these particular events. GEM emission pulses following nights with significant deposition provide evidence for the prompt recycling of 17% of deposited mercury, with the remaining portion retained in surface sinks. The long-term impacts of any sinks are however likely to be minimal, as cumulative GEM flux across the study period was close to zero. [ABSTRACT FROM AUTHOR]

Aerodynamic gradient measurements of the air-surface exchange of gaseous elemental mercury (GEM) were undertaken over a 40 hectare alpine grassland in Australia's Snowy Mountains region during the austral summer. Bi-directional GEM fluxes were observed throughout the study, with overall mean value of 0.2 ± 14.8 ng m-2 h-1 and mean nocturnal fluxes of -1.5 ± 7.8 ng m-2 h-1 compared to diurnal fluxes of 1.8 ± 18.6 ng m-2 h-1. Deposition velocities ranged from -2.2 cm s-1 to 2.9 cm s-1, whilst ambient GEM concentrations throughout the study were 0.59 ± 0.10 ng m-3. Cumulative GEM fluxes correlated well with 24-hour running mean soil temperatures, and one precipitation event was shown to have a positive impact on diurnal emission fluxes. The underlying vegetation had largely senesced and showed little stomatal control on fluxes. Nocturnal atmospheric mercury depletion events (NAMDEs) were observed concomitant with O3 depletion and dew formation under shallow, stable nocturnal boundary layers. A mass balance box model was able to reproduce ambient GEM concentration patterns during NAMDE and non-NAMDE nights without invoking chemical oxidation of GEM throughout the column, indicating the role of surface processes controlling deposition in these events. Surface deposition was enhanced under NAMDE nights, though uptake to dew likely represents less than one fifth of this enhanced deposition. Instead, enhancement of the surface GEM gradient as a result of oxidation at the surface in the presence of dew is hypothesised to be responsible for a large portion of GEM depletion during these particular events. GEM emission pulses following nights with significant deposition provide evidence for the prompt recycling of 17 % of deposited mercury, with the remaining portion retained in surface sinks. The long-term impacts of any sinks are however likely to be minimal, as cumulative GEM flux across the 3-week study period was close to zero. [ABSTRACT FROM AUTHOR]

Mercury is a toxic element of serious concern for human and environmental health. Understanding its natural cycling in the environment is an important goal towards assessing its impacts and the effectiveness of mitigation strategies. Due to the unique chemical and physical properties of mercury, the atmosphere is the dominant transport pathway for this heavy metal, with the consequence that regions far removed from sources can be impacted. However, there exists a dearth of long-term monitoring of atmospheric mercury, particularly in the tropics and southern hemisphere. This paper presents the first two years of gaseous elemental mercury (GEM) measurements taken at the Australian Tropical Atmospheric Research Station (ATARS) in northern Australia, as part of the Global Mercury Observation System (GMOS). Annual mean GEM concentrations determined at ATARS (0.95 ± 0.12 ng m-3) are consistent with recent observations at other sites in the southern hemisphere. Comparison with GEM data from other Australian monitoring sites suggests a concentration gradient that decreases with increasing latitude. Seasonal analysis shows that GEM concentrations at ATARS are significantly lower in the distinct wet monsoon season than in the dry season. This result provides insight into alterations of natural mercury cycling processes as a result of changes in atmospheric humidity, oceanic/terrestrial fetch and convective mixing, and invites future investigation using wet mercury deposition measurements. Due to its location relative to the atmospheric equator, ATARS intermittently samples air originating from the northern hemisphere, allowing an opportunity to gain greater understanding of inter-hemispheric transport of mercury and other atmospheric species. Diurnal cycles of GEM at ATARS show distinct nocturnal depletion events that are attributed to dry deposition under stable boundary layer conditions. These cycles provide strong further evidence for the multi-hop model of global GEM cycling, whereby long-range transport is characterised by multiple surface depositions and re-emissions, rather than continuous transport over long distances. [ABSTRACT FROM AUTHOR]

The genetic basis of chronic lymphocytic leukemia (CLL) has not been fully elucidated to date. Although it is the most common haematological malignancy in Caucasians, it is uncommon among Asians. A recent genome-wide scan of CLL in Caucasians, which was carried out in the UK, identified six variants showing strong association. We attempted to replicate these findings in 71 patients with CLL and 1273 controls in Hong Kong Chinese. Three of the six variants were significantly associated with CLL. The rs872071 variant (Odds Ratio (95% Confidence Interval) = 1.78 (1.25-2.53), P = 0.0013) in the IRF4 gene region showed the strongest association, similar to that reported in the UK study. Polymorphisms in SP140 and ACOXL were also associated with risk of CLL. Further, the mean allele frequencies of the six variants were moderately (59%) to extremely (0.5%) lower in the Chinese population compared with Caucasians. These results suggest that variants in three loci may contribute to risk of CLL among Chinese. [ABSTRACT FROM AUTHOR]

Lung cancer rates in Xuanwei County have been among the highest in China for both males and females and have been causally associated with exposure to indoor smoky (bituminous) coal emissions that contain very high levels of polycyclic aromatic hydrocarbons. There are numerous coal mines across the County. Although lung cancer risk is strongly associated with the use of smoky coal as a whole, variation in risk by smoky coal subtype has not been characterized as yet. We conducted a population-based case-control study of 498 lung cancer cases and 498 controls, individually matched to case subjects on age (±2 years) and sex to examine risk by coal subtype. Odds ratios (ORs) and 95% confidence intervals (CIs) for coal subtype were calculated by conditional logistic regression, adjusting for potential confounders. Overall, smoky coal use was positively and statistically significantly associated with lung cancer risk, when compared with the use of smokeless coal or wood (OR = 7.7, 95% CI = 4.5-13.3). Furthermore, there was a marked heterogeneity in risk estimates for specific subtypes of smoky coal (test for heterogeneity: p = 5.17 × 10 [ABSTRACT FROM AUTHOR]