Person:

Soerensen, Anne

[1] We analyze 1977–2010 trends in atmospheric mercury (Hg) from 21 ship cruises over the North Atlantic (NA) and 15 over the South Atlantic (SA). We find a steep 1990–2009 decline of −0.046 ± 0.010 ng m−3 a−1 (−2.5% a−1) over the NA (steeper than at Northern Hemispheric land sites) but no significant decline over the SA. Surface water Hg0 measurements in the NA show a decline of −5.7% a−1since 1999, and limited subsurface ocean data show an ∼80% decline from 1980 to present. We use a coupled global atmosphere-ocean model to show that the decline in NA atmospheric concentrations can be explained by decreasing oceanic evasion from the NA driven by declining subsurface water Hg concentrations. We speculate that this large historical decline of Hg in the NA Ocean could have been caused by decreasing Hg inputs from rivers and wastewater and by changes in the oxidant chemistry of the atmospheric marine boundary layer.

We develop an improved treatment of the surface ocean in the GEOS-Chem global 3-D biogeochemical model for mercury (Hg). We replace the globally uniform subsurface ocean Hg concentrations used in the original model with basin-specific values based on measurements. Updated chemical mechanisms for Hg0/HgII redox reactions in the surface ocean include both photochemical and biological processes, and we improved the parametrization of particle-associated Hg scavenging. Modeled aqueous Hg concentrations are consistent with limited surface water observations. Results more accurately reproduce high-observed MBL concentrations over the North Atlantic (NA) and the associated seasonal trends. High seasonal evasion in the NA is driven by inputs from Hg enriched subsurface waters through entrainment and Ekman pumping. Globally, subsurface waters account for 40% of Hg inputs to the ocean mixed layer, and 60% is from atmospheric deposition. Although globally the ocean is a net sink for 3.8 Mmol Hg y−1, the NA is a net source to the atmosphere, potentially due to enrichment of subsurface waters with legacy Hg from historical anthropogenic sources.

Air–sea exchange of elemental mercury (Hg0) is a critical component of the global biogeochemical Hg cycle. To better understand variability in atmospheric and oceanic Hg0, we collected high-resolution measurements across large gradients in seawater temperature, salinity, and productivity in the Pacific Ocean (20°N-15°S). We modeled surface ocean Hg inputs and losses using an ocean general circulation model (MITgcm) and an atmospheric chemical transport model (GEOS-Chem). Observed surface seawater Hg0 was much more variable than atmospheric concentrations. Peak seawater Hg0 concentrations (∼130 fM) observed in the Pacific intertropical convergence zone (ITCZ) were ∼3-fold greater than surrounding areas (∼50 fM). This is similar to observations from the Atlantic Ocean. Peak evasion in the northern Pacific ITCZ was four times higher than surrounding regions and located at the intersection of high wind speeds and elevated seawater Hg0. Modeling results show that high Hg inputs from enhanced precipitation in the ITCZ combined with the shallow ocean mixed layer in this region drive elevated seawater Hg0 concentrations. Modeled seawater Hg0 concentrations reproduce observed peaks in the ITCZ of both the Atlantic and Pacific Oceans but underestimate its magnitude, likely due to insufficient deep convective scavenging of oxidized Hg from the upper troposphere. Our results demonstrate the importance of scavenging of reactive mercury in the upper atmosphere driving variability in seawater Hg0 and net Hg inputs to biologically productive regions of the tropical ocean.