A panel of international experts was convened in Madison, Wisconsin, in 2005, as part of the 8th International Conference on Mercury as a Global Pollutant. Our charge was to address the state of science pertinent to source attribution, specifically our key question was: "For a given location, can we ascertain with confidence the relative contributions of local, regional, and global sources, and of natural versus anthropogenic emissions to mercury deposition?" The panel synthesized new research pertinent to this question published over the past decade, with emphasis on four major research topics: long-term anthropogenic change, current emission and deposition trends, chemical transformations and cycling, and modeling and uncertainty. Within each topic, the panel drew a series of conclusions, which are presented in this paper. These conclusions led us to concur that the answer to our question is a "qualified yes," with the qualification being dependent upon the level of uncertainty one is willing to accept. We agreed that the uncertainty is strongly dependent upon scale and that our question as stated is answerable with greater confidence both very near and very far from major point sources, assuming that the "global pool" is a recognizable "source." Many regions of interest from an ecosystem-exposure standpoint lie in between, where source attribution carries the greatest degree of uncertainty.

Abstract. It was discovered in 1995 that, during the spring time, unexpectedly low concentrations of gaseous elemental mercury (GEM) occurred in the Arctic air. This was surprising for a pollutant known to have a long residence time in the atmosphere; however conditions appeared to exist in the Arctic that promoted this depletion of mercury (Hg). This phenomenon is termed atmospheric mercury depletion events (AMDEs) and its discovery has revolutionized our understanding of the cycling of Hg in Polar Regions while stimulating a significant amount of research to understand its impact to this fragile ecosystem. Shortly after the discovery was made in Canada, AMDEs were confirmed to occur throughout the Arctic, sub-Artic and Antarctic coasts. It is now known that, through a series of photochemically initiated reactions involving halogens, GEM is converted to a Correspondence to: A. Steffen (alexandra.steffen@ec.gc.ca) more reactive species and is subsequently associated to particles in the air and/or deposited to the polar environment. AMDEs are a means by which Hg is transferred from the atmosphere to the environment that was previously unknown. In this article we review Hg research taken place in Polar Regions pertaining to AMDEs, the methods used to collect Hg in different environmental media, research results of the current understanding of AMDEs from field, laboratory and modeling work, how Hg cycles around the environment after AMDEs, gaps in our current knowledge and the future impacts that AMDEs may have on polar environments. The research presented has shown that while considerable improvements in methodology to measure Hg have been made but the main limitation remains knowing the speciation of Hg in the various media. The processes that drive AMDEs and how they occur are discussed. As well, the role that the snow pack and the sea ice play in the cycling of Hg is presented. It has been found that deposition of Hg from AMDEs occurs at marine coasts and not far inland and that a fraction of the Published by Copernicus Publications on behalf of the European Geosciences Union. deposited Hg does not remain in the same form in the snow. Kinetic studies undertaken have demonstrated that bromine is the major oxidant depleting Hg in the atmosphere. Modeling results demonstrate that there is a significant deposition of Hg to Polar Regions as a result of AMDEs. Models have also shown that Hg is readily transported to the Arctic from source regions, at times during springtime when this environment is actively transforming Hg from the atmosphere to the snow and ice surfaces. The presence of significant amounts of methyl Hg in snow in the Arctic surrounding AMDEs is important because this species is the link between the environment and impacts to wildlife and humans. Further, much work on methylation and demethylation processes has occurred but these processes are not yet fully understood. Recent changes in the climate and sea ice cover in Polar Regions are likely to have strong effects on the cycling of Hg in this envir...

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Unlike other heavy metals that are inherently associated with atmospheric aerosols, mercury in ambient air exists predominantly in the gaseous elemental form. Because of its prolonged atmospheric residence time, elemental mercury vapor is distributed on a global scale. Recently, Canadian researchers have discovered that total gaseous mercury levels in the lower tropospheric boundary layer in the Canadian Arctic are often significantly depleted during the months after polar sunrise. A possible explanation may involve oxidation of elemental mercury, followed by adsorption and deposition of the oxidized form, leading to an increased input of atmospheric mercury into the Arctic ecosystem. Here we present the first continuous high-time-resolution measurements of total gaseous mercury in the Antarctic covering a 12-month period between January 2000 and January 2001 at the German Antarctic research station Neumayer (70 degrees 39' S, 8 degrees 15' W). We report that mercury depletion events also occur in the Antarctic after polar sunrise and compare our measurements with a data setfrom Alert, Nunavut, Canada. We also present indications that BrO radicals and ozone play a key role in the boundary-layer chemistry during springtime mercury depletion events in the Antarctic troposphere.

Anthropogenic mercury emissions are transported through the atmosphere as gaseous elemental mercury (Hg(0)) prior to deposition to Earth's surface. Strong seasonality in atmospheric Hg(0) concentrations in the Northern Hemisphere has been explained by two factors: anthropogenic Hg(0) emissions are thought to peak in winter due to higher energy consumption, and atmospheric oxidation rates of Hg(0) are faster in summer. Oxidationdriven Hg(0) seasonality should be equally pronounced in the Southern Hemisphere, which is inconsistent with observations of constant year-round Hg(0) levels. Here, we assess the role of Hg(0) uptake by vegetation as an alternative mechanism for driving Hg(0) seasonality. We find that at terrestrial sites in the Northern Hemisphere, Hg(0) co-varies with CO2, which is

Organophosphorus compounds (OPs) being applied as flame retardants and plasticizers were investigated in airborne particles over the Pacific, Indian, Arctic, and Southern Ocean. Samples taken during two polar expeditions in 2010/11, one from East Asia to the high Arctic (CHINARE 4) and another from East Asia toward the Indian Ocean to the Antarctic (CHINARE 27), were analyzed for three halogenated OPs (tris(2-chloroethyl) phosphate (TCEP), tris(2-chloroisopropyl) phosphate (TCPP) and tris(1,3-dichloro-2-isopropyl) phosphate (TDCP)), four alkylated OPs (tri-n-butyl phosphate (TnBP), tri-iso-butyl phosphate (TiBP), tris(2-butoxyethyl)phosphate (TBEP), and tris(2-ethylhexyl) phosphate (TEHP)), and triphenyl phosphate (TPhP). The sum of the eight investigated OPs ranged from 230 to 2900 pg m(-3) and from 120 to 1700 pg m(-3) during CHINARE 4 and CHINARE 27, respectively. TCEP and TCPP were the predominating compounds, both over the Asian seas as well as in the polar regions, with concentrations from 19 to 2000 pg m(-3) and 22 to 620 pg m(-3), respectively. Elevated concentrations were observed in proximity to the Asian continent enhanced by continental air masses. They decreased sharply toward the open oceans where they remained relatively stable. This paper shows the first occurrence of OPs over the global oceans proving that they undergo long-range atmospheric transport over the global oceans toward the Arctic and Antarctica.

Mercury and many of its compounds behave exceptionally in the environment because of their volatility, capability for methylation, and subsequent biomagnification in contrast with most of the other heavy metals. Long-range atmospheric transport of elemental mercury, its transformation to more toxic methylmercury compounds, the ability of some to undergo photochemical reactions, and their bioaccumulation in the aquatic food chain have made it a subject of global research activities, even in polar regions. The first continuous high-time-resolution measurements of total gaseous mercury in the Antarctic covering a 12-month period were carried out at the German Antarctic research station Neumayer (70 degrees 39' S, 8 degrees 15' W) between January 2000 and February 2001. We recently reported that mercury depletion events (MDEs) occur in the Antarctic after polar sunrise, as was previously shown for Arctic sites. These events (MDEs) end suddenly during Antarctic summer. A possible explanation of this phenomenon is presented in this paper, showing that air masses originating from the sea-ice surface were a necessary prerequisite for the observations of depletion of atmospheric mercury at polar spring. Our extensive measurements at Neumayer of atmospheric mercury species during December 2000-February 2001 show that fast oxidation of gaseous elemental mercury leads to variable Hg0 concentrations during Antarctic summer, accompanied by elevated concentrations, up to more than 300 pg/m3, of reactive gaseous mercury. For the first time in the Southern Hemisphere, atmospheric mercury species measurements were also performed onboard of a research vessel, indicating the existence of homogeneous background concentrations over the south Atlantic Ocean. These new findings contain evidence for an enhanced oxidizing potential of the Antarctic atmosphere over the continent that needs to be considered for the interpretation of dynamic transformations of mercury during summertime.

The production and use of long-chain perfluoroalkyl substances (PFASs) must comply with national and international regulations. Driven by increasingly stringent regulations, their production has been outsourced to less regulated countries in Asia. In addition, the fluoropolymer industry started to use fluorinated alternatives, such as 2,3,3,3tetrafluoro-2-(1,1,2,2,3,3,3-heptafluoropropoxy)propanoic acid (HFPO-DA). Between August 2013 and September 2014, we investigated the occurrence and distribution of HFPO-DA and legacy PFASs in surface waters of the following river/estuary systems: the Elbe and Rhine Rivers in Germany, the Rhine-Meuse delta in The Netherlands, and the Xiaoqing River in China. Distinct differences were revealed among the study areas; notably, the Chinese samples were highly polluted by an industrial point source discharging mainly perfluorooctanoic acid (PFOA). This particular point source resulted in concentrations more than 6000 times higher than an industrial point source observed in the Scheur River, where HFPO-DA was the dominant compound with a concentration of 73.1 ng/L. Moreover, HFPO-DA was detected in all samples along the coastline of the North Sea, indicating that the compound may be transported from the Rhine-Meuse delta into the German Bight via the water current. To the best of our knowledge, the fluorinated alternative, HFPO-DA, was detected for the first time in surface waters of Germany and China.