Anthropogenic activities have led to large-scale mercury (Hg) pollution in the Arctic. It has been suggested that sea-salt-induced chemical cycling of Hg (through 'atmospheric mercury depletion events', or AMDEs) and wet deposition via precipitation are sources of Hg to the Arctic in its oxidized form (Hg(ii)). However, there is little evidence for the occurrence of AMDEs outside of coastal regions, and their importance to net Hg deposition has been questioned. Furthermore, wet-deposition measurements in the Arctic showed some of the lowest levels of Hg deposition via precipitation worldwide, raising questions as to the sources of high Arctic Hg loading. Here we present a comprehensive Hg-deposition mass-balance study, and show that most of the Hg (about 70%) in the interior Arctic tundra is derived from gaseous elemental Hg (Hg(0)) deposition, with only minor contributions from the deposition of Hg(ii) via precipitation or AMDEs. We find that deposition of Hg(0)-the form ubiquitously present in the global atmosphere-occurs throughout the year, and that it is enhanced in summer through the uptake of Hg(0) by vegetation. Tundra uptake of gaseous Hg(0) leads to high soil Hg concentrations, with Hg masses greatly exceeding the levels found in temperate soils. Our concurrent Hg stable isotope measurements in the atmosphere, snowpack, vegetation and soils support our finding that Hg(0) dominates as a source to the tundra. Hg concentration and stable isotope data from an inland-to-coastal transect show high soil Hg concentrations consistently derived from Hg(0), suggesting that the Arctic tundra might be a globally important Hg sink. We suggest that the high tundra soil Hg concentrations might also explain why Arctic rivers annually transport large amounts of Hg to the Arctic Ocean.

( 1 and Fig. 1(a)). These trends are primarily due to stricter air quality emission controls that candidate species for studying hemispheric gradients and long-term changes. 57We analyzed ten years of NMHC data collected at 44 remote global sampling sites from NOAA's 58 Global Greenhouse Gas Reference Network (GGGRN). We also include data from in-situ moni-59 toring at Summit, Greenland 8 , at Hohenpeissenberg (HPB) in Southern Germany 9 , Jungfraujoch resolved in-situ record from HPB has its minimum in 2009 ( Fig. 1 (e)), in agreement with the JFJ 78 FTIR column observations ( Fig. 1(c)). Focusing on the most recent five years (2009.5 -2014.5) 79 we find variable results in the observed rate of change; however, a consistent picture emerges 80 that shows the largest increases at NH sites (Fig. 3). Of 33 NH sites, 7 exhibit ethane growth 81 rates > 50 pmol mol -1 yr -1 , and 10 sites exhibit growth rates between 25-50 pmol -1 yr -1 (Table S1). one from JFJ ( Fig. 1(c)) 12 , and the other one from Lauder, New Zealand ( Fig. 1(d) emission increases outside of NA that currently cannot be well defined due to the sparsity of 170 observations in those regions (for instance in the middle-East, Africa, and Asia).

The radiative properties of soot particles depend on their morphology and mixing state, but their evolution during transport is still elusive. Here we report observations from an electron microscopy analysis of individual particles transported in the free troposphere over long distances to the remote Pico Mountain Observatory in the Azores in the North Atlantic. Approximately 70% of the soot particles were highly compact and of those 26% were thinly coated. Discrete dipole approximation simulations indicate that this compaction results in an increase in soot single scattering albedo by a factor of ≤2.17. The top of the atmosphere direct radiative forcing is typically smaller for highly compact than mass-equivalent lacy soot. The forcing estimated using Mie theory is within 12% of the forcing estimated using the discrete dipole approximation for a high surface albedo, implying that Mie calculations may provide a reasonable approximation for compact soot above remote marine clouds.