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

Abstract. Our knowledge of the distribution of mercury concentrations in air of the Southern Hemisphere was until recently based mostly on intermittent measurements made during ship cruises. In the last few years continuous mercury monitoring has commenced at several sites in the Southern Hemisphere, providing new and more refined information. In this paper we compare mercury measurements at several remote sites in the Southern Hemisphere made over a period of at least 1 year at each location. Averages of monthly medians show similar although small seasonal variations at both Cape Point and Amsterdam Island. A pronounced seasonal variation at Troll research station in Antarctica is due to frequent mercury depletion events in the austral spring. Due to large scatter and large standard deviations of monthly average median mercury concentrations at Cape Grim, no systematic seasonal variation could be found there. Nevertheless, the annual average mercury concentrations at all sites during the 2007-2013 period varied only between 0.85 and 1.05 ng m −3 . Part of this variability is likely due to systematic measurement uncertainties which we propose can be further reduced by improved calibration procedures. We conclude that mercury is much more uniformly distributed throughout the Southern Hemisphere than the distributions suggested by measurements made onboard ships. This finding implies that smaller trends can be detected in shorter time periods. We also report a change in the trend sign at Cape Point from decreasing mercury concentrations in 1996-2004 to increasing concentrations since 2007.

We perform global-scale inverse modeling to constrain present-day atmospheric mercury emissions and relevant physiochemical parameters in the GEOS-Chem chemical transport model. We use Bayesian inversion methods combining simulations with GEOS-Chem and ground-based Hg-0 observations from regional monitoring networks and individual sites in recent years. Using optimized emissions/parameters, GEOS-Chem better reproduces these ground-based observations and also matches regional over-water Hg-0 and wet deposition measurements. The optimized global mercury emission to the atmosphere is 5.8 Gg yr(-1). The ocean accounts for 3.2 Gg yr(-1) (55 % of the total), and the terrestrial ecosystem is neither a net source nor a net sink of Hg-0. The optimized Asian anthropogenic emission of Hg-0 (gas elemental mercury) is 650-1770 Mg yr(-1), higher than its bottom-up estimates (550-800 Mg yr(-1)). The ocean parameter inversions suggest that dark oxidation of aqueous elemental mercury is faster, and less mercury is removed from the mixed layer through particle sinking, when compared with current simulations. Parameter changes affect the simulated global ocean mercury budget, particularly mass exchange between the mixed layer and subsurface waters. Based on our inversion results, we re-evaluate the long-term global biogeochemical cycle of mercury, and show that legacy mercury becomes more likely to reside in the terrestrial ecosystem than in the ocean. We estimate that primary anthropogenic mercury contributes up to 23 % of present-day atmospheric deposition

Abstract. Long term atmospheric mercury measurements in the Southern Hemisphere are scarce and in Antarctica completely absent. Recent studies have shown that the Antarctic continent plays an important role in the global mercury cycle. Therefore, long term measurements of gaseous elemental mercury (GEM) were initiated at the Norwegian Antarctic Research Station, Troll (TRS) in order to improve our understanding of atmospheric transport, transformation and removal processes of GEM. GEM measurements started in February 2007 and are still ongoing, and this paper presents results from the first four years. The mean annual GEM concentration of 0.93 ± 0.19 ng m −3 is in good agreement with other recent southern-hemispheric measurements. Measurements of GEM were combined with the output of the Lagrangian particle dispersion model FLEXPART, for a statistical analysis of GEM source and sink regions. It was found that the ocean is a source of GEM to TRS year round, especially in summer and fall. On time scales of up to 20 days, there is little direct transport of GEM to TRS from Southern Hemisphere continents, but sources there are important for determining the overall GEM load in the Southern Hemisphere and for the mean GEM concentration at TRS. Further, the sea ice and marginal ice zones are GEM sinks in spring as also seen in the Arctic, but the Antarctic oceanic sink seems weaker. Contrary to the Arctic, a strong summer time GEM sink was found, when air originates from the Antarctic plateau, which shows that the summertime removal mechanism of GEM is completely different and is caused by other chemical processes than the springtime atmospheric mercury depletion events. The results were corroborated by an analysis of ozone source and sink regions.

Global emissions of mercury continue to change at the same time as the Arctic is experiencing ongoing climatic changes. Continuous monitoring of atmospheric mercury provides important information about long-term trends in the balance between transport, chemistry, and deposition of this pollutant in the Arctic atmosphere. Ten-year records of total gaseous mercury (TGM) from 2000 to 2009 were analyzed from two high Arctic sites at Alert (Nunavut, Canada) and Zeppelin Station (Svalbard, Norway); one sub-Arctic site at Kuujjuarapik (Nunavik, Québec, Canada); and three temperate Canadian sites at St. Anicet (Québec), Kejimkujik (Nova Scotia) and Egbert (Ontario). Five of the six sites examined showed a decreasing trend over this time period. Overall trend estimates at high latitude sites were: −0.9% yr⁻¹ (95% confidence limits: −1.4, 0) at Alert and no trend (−0.5, +0.7) at Zeppelin Station. Faster decreases were observed at the remainder of the sites: −2.1% yr⁻¹ (−3.1, −1.1) at Kuujjuarapik, −1.9% yr⁻¹ (−2.1, −1.8) at St. Anicet, −1.6% yr⁻¹ (−2.4, −1.0) at Kejimkujik and −2.2% yr⁻¹ (−2.8, −1.7) at Egbert. Trends at the sub-Arctic and mid-latitude sites agree with reported decreases in background TGM concentration since 1996 at Mace Head, Ireland, and Cape Point, South Africa, but conflict with estimates showing an increase in global anthropogenic emissions over a similar period. Trends in TGM at the two high Arctic sites were not only less negative (or neutral) overall but much more variable by season. Possible reasons for differences in seasonal and overall trends at the Arctic sites compared to those at lower latitudes are discussed, as well as implications for the Arctic mercury cycle. The first calculations of multi-year trends in reactive gaseous mercury (RGM) and total particulate mercury (TPM) at Alert were also performed, indicating increases from 2002 to 2009 in both RGM and TPM in the spring when concentrations are highest