Abstract. We have developed a new nested-grid mercury (Hg) simulation over North America with a 1/2 • latitude by 2/3 • longitude horizontal resolution employing the GEOSChem global chemical transport model. Emissions, chemistry, deposition, and meteorology are self-consistent between the global and nested domains. Compared to the global model (4 • latitude by 5 • longitude), the nested model shows improved skill at capturing the high spatial and temporal variability of Hg wet deposition over North America observed by the Mercury Deposition Network (MDN) in [2008][2009]. The nested simulation resolves features such as higher deposition due to orographic precipitation, land/ocean contrast and and predicts more efficient convective rain scavenging of Hg over the southeast United States. However, the nested model overestimates Hg wet deposition over the Ohio River Valley region (ORV) by 27 %. We modify anthropogenic emission speciation profiles in the US EPA National Emission Inventory (NEI) to account for the rapid inplume reduction of reactive to elemental Hg (IPR simulation). This leads to a decrease in the model bias to −2.3 % over the ORV region. Over the contiguous US, the correlation coefficient (r) between MDN observations and our IPR simulation increases from 0.60 to 0.78. The IPR nested simulation generally reproduces the seasonal cycle in surface concentrations of speciated Hg from the Atmospheric Mercury Network (AMNet) and Canadian Atmospheric Mercury Network (CAMNet). In the IPR simulation, annual mean gaseous and particulate-bound Hg(II) are within 140 % and 11 % of observations, respectively. In contrast, the simulation with unmodified anthropogenic Hg speciation profiles overestimates these observations by factors of 4 and 2 for gaseous and particulate-bound Hg(II), respectively. The nested model shows improved skill at capturing the horizontal variability of Hg observed over California during the ARCTAS aircraft campaign. The nested model suggests that North American anthropogenic emissions account for 10-22 % of Hg wet deposition flux over the US, depending on the anthropogenic emissions speciation profile assumed. The modeled percent contribution can be as high as 60 % near large point sources in ORV. Our results indicate that the North American anthropogenic contribution to dry deposition is 13-20 %.

Abstract. The National Atmospheric Deposition Program (NADP) developed and operates a collaborative network of atmospheric-mercury-monitoring sites based in North America – the Atmospheric Mercury Network (AMNet). The justification for the network was growing interest and demand from many scientists and policy makers for a robust database of measurements to improve model development, assess policies and programs, and improve estimates of mercury dry deposition. Many different agencies and groups support the network, including federal, state, tribal, and international governments, academic institutions, and private companies. AMNet has added two high-elevation sites outside of continental North America in Hawaii and Taiwan because of new partnerships forged within NADP. Network sites measure concentrations of atmospheric mercury fractions using automated, continuous mercury speciation systems. The procedures that NADP developed for field operations, data management, and quality assurance ensure that the network makes scientifically valid and consistent measurements. AMNet reports concentrations of hourly gaseous elemental mercury (GEM), two-hour gaseous oxidized mercury (GOM), and two-hour particulate-bound mercury less than 2.5 microns in size (PBM2.5). As of January 2012, over 450 000 valid observations are available from 30 stations. AMNet also collects ancillary meteorological data and information on land use and vegetation, when available. We present atmospheric mercury data comparisons by time (3 yr) at 21 individual sites and instruments. Highlighted are contrasting values for site locations across the network: urban versus rural, coastal versus high elevation and the range of maximum observations. The data presented should catalyze the formation of many scientific questions that may be answered through further in-depth analysis and modeling studies of the AMNet database. All data and methods are publically available through an online database on the NADP website (http://nadp.sws.uiuc.edu/amn/). Future network directions are to foster new network partnerships and continue to collect, quality assure, and post data, including dry deposition estimates, for each fraction.

A partnership of federal and state agencies, tribes, industry, and scientists from academic research and environmental organizations is establishing a national, policy-relevant mercury monitoring network, called MercNet, to address key questions concerning changes in anthropogenic mercury emissions and deposition, associated linkages to ecosystem effects, and recovery from mercury contamination. This network would quantify mercury in the atmosphere, land, water, and biota in terrestrial, freshwater, and coastal ecosystems to provide a national scientific capability for evaluating the benefits and effectiveness of emission controls. Program development began with two workshops, convened to establish network goals, to select key indicators for monitoring, to propose a geographic network of monitoring sites, and to design a monitoring plan. MercNet relies strongly on multi-institutional partnerships to secure the capabilities and comprehensive data that are needed to develop, calibrate, and refine predictive mercury models and to guide effective management. Ongoing collaborative efforts include the: (1) development of regional multi-media databases on mercury in the Laurentian Great Lakes, northeastern United States, and eastern Canada; (2) syntheses and reporting of these data for the scientific and policy communities; and (3) evaluation of potential monitoring sites. The MercNet approach could be applied to the development of other monitoring programs, such as emerging efforts to monitor and assess global mercury emission controls.

We have developed a new high-resolution (1/2° latitude by 2/3° longitude) nested-grid mercury (Hg) simulation over North America employing the GEOS-Chem global chemical transport model. Emissions, chemistry, deposition, and meteorology are self-consistent between the global and nested domains. Compared to the global model (4° latitude by 5° longitude), the nested model shows improved skill at capturing the high spatial and temporal variability of Hg wet deposition over North America observed by the Mercury Deposition Network (MDN) in 2008–2009. The nested simulation resolves features such as land/ocean contrast and higher deposition due to orographic precipitation, and predicts more efficient convective rain scavenging of Hg over the southeast United States. However, the nested model overestimates Hg wet deposition over the Ohio River Valley region (ORV) by 27%. We modify anthropogenic emission speciation profiles in the US EPA National Emission Inventory (NEI) to account for the rapid in-plume reduction of reactive to elemental Hg (IPR simulation). This leads to a decrease in the model bias to +3% over the ORV region. Over the contiguous US, the correlation coefficient (<i>r</i>) between MDN observations and our IPR simulation increases from 0.63 to 0.78. The IPR nested simulation generally reproduces the seasonal cycle in surface concentrations of speciated Hg from the Atmospheric Mercury Network (AMNet) and Canadian Atmospheric Mercury Network (CAMNet). In the IPR simulation, annual mean reactive gaseous and particulate-bound Hg are within 80% and 10% of observations, respectively. In contrast, the simulation with unmodified anthropogenic Hg speciation profiles overestimates these observations by factors of 2 to 4. The nested model shows improved skill at capturing the horizontal variability of Hg observed over California during the ARCTAS aircraft campaign. We find that North American anthropogenic emissions account for 10–22% of Hg wet deposition flux over the US, depending on the anthropogenic emissions speciation profile assumed. The percent contribution can be as high as 60% near large point emission sources in ORV. The contribution for the dry deposition is 13–20%

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