Long-term monitoring of data of ambient mercury (Hg) on a global scale to assess its emission, transport, atmospheric chemistry, and deposition processes is vital to understanding the impact of Hg pollution on the environment. The Global Mercury Observation System (GMOS) project was funded by the European Commission (http://www.gmos.eu) and started in November 2010 with the overall goal to develop a coordinated global observing system to monitor Hg on a global scale, including a large network of ground-based monitoring stations, ad hoc periodic oceanographic cruises and measurement flights in the lower and upper troposphere as well as in the lower stratosphere. To date, more than 40 ground-based monitoring sites constitute the global network covering many regions where little to no observational data were available before GMOS. This work presents atmospheric Hg concentrations recorded worldwide in the framework of the GMOS project (2010-2015), analyzing Hg measurement results in terms of temporal trends, seasonality and comparability within the network. Major findings highlighted in this paper include a clear gradient of Hg concentrations between the Northern and Southern hemispheres, confirming that the gradient observed is mostly driven by local and regional sources, which can be anthropogenic, natural or a combination of both.

Abstract. Current understanding of mercury (Hg) behavior in the atmosphere contains significant gaps. Some key characteristics of Hg processes, including anthropogenic and geogenic emissions, atmospheric chemistry, and air–surface exchange, are still poorly known. This study provides a complex analysis of processes governing Hg fate in the atmosphere involving both measured data from ground-based sites and simulation results from chemical transport models. A variety of long-term measurements of gaseous elemental Hg (GEM) and reactive Hg (RM) concentration as well as Hg wet deposition flux have been compiled from different global and regional monitoring networks. Four contemporary global-scale transport models for Hg were used, both in their state-of-the-art configurations and for a number of numerical experiments to evaluate particular processes. Results of the model simulations were evaluated against measurements. As follows from the analysis, the interhemispheric GEM gradient is largely formed by the prevailing spatial distribution of anthropogenic emissions in the Northern Hemisphere. The contributions of natural and secondary emissions enhance the south-to-north gradient, but their effect is less significant. Atmospheric chemistry has a limited effect on the spatial distribution and temporal variation of GEM concentration in surface air. In contrast, RM air concentration and wet deposition are largely defined by oxidation chemistry. The Br oxidation mechanism can reproduce successfully the observed seasonal variation of the RM ∕ GEM ratio in the near-surface layer, but it predicts a wet deposition maximum in spring instead of in summer as observed at monitoring sites in North America and Europe. Model runs with OH chemistry correctly simulate both the periods of maximum and minimum values and the amplitude of observed seasonal variation but shift the maximum RM ∕ GEM ratios from spring to summer. O3 chemistry does not predict significant seasonal variation of Hg oxidation. Hence, the performance of the Hg oxidation mechanisms under study differs in the extent to which they can reproduce the various observed parameters. This variation implies possibility of more complex chemistry and multiple Hg oxidation pathways occurring concurrently in various parts of the atmosphere.

The atmospheric deposition of mercury (Hg) occurs via several mechanisms, including dry and wet scavenging by precipitation events. In an effort to understand the atmospheric cycling and seasonal depositional characteristics of Hg, wet deposition samples were collected for approximately 5 years at 17 selected GMOS monitoring sites located in the Northern and Southern hemispheres in the framework of the Global Mercury Observation System (GMOS) project. Total mercury (THg) exhibited annual and seasonal patterns in Hg wet deposition samples. Interannual differences in total wet deposition are mostly linked with precipitation volume, with the greatest deposition flux occurring in the wettest years. This data set provides a new insight into baseline concentrations of THg concentrations in precipitation worldwide, particularly in regions such as the Southern Hemisphere and tropical areas where wet deposition as well as atmospheric Hg species were not investigated before, opening the way for future and additional simultaneous measurements across the GMOS network as well as new findings in future modeling studies

<p><strong>Abstract.</strong> Current understanding of mercury (Hg) behaviour in the atmosphere contains significant gaps. Some key characteristics of Hg processes including anthropogenic and geogenic emissions, atmospheric chemistry, and air-surface exchange are still poorly known. This study provides a complex analysis of processes governing Hg fate in the atmosphere involving both measurement data from ground-based sites and simulation results of chemical transport models. A variety of long-term measurements of gaseous elemental Hg (GEM) and reactive Hg (RM) concentration as well as Hg wet deposition flux has been compiled from different global and regional monitoring networks. Four contemporary global-scale transport models for Hg were applied both in their state-of-the-art configurations and for a number of numerical experiments aimed at evaluation of particular processes. Results of the model simulation were evaluated against measurements. As it follows from the analysis the inter-hemispheric gradient of GEM is largely formed by the spatial distribution of anthropogenic emissions which prevail in the Northern Hemisphere. Contribution of natural and secondary emissions enhances the south-to-north gradient but their effect is less significant. The atmospheric chemistry does not affect considerably both spatial distribution and temporal variation of GEM concentration in the surface air. On the other hand, RM air concentration and wet deposition are largely defined by oxidation chemistry. The Br oxidation mechanism allows successfully reproducing observed seasonal variation of the RM / GEM ratio in the near-surface layer, whereas it predicts maximum in wet deposition in spring instead of summer as observed at monitoring sites located in North America and Europe. Model runs with the OH chemistry correctly simulate both the periods of maximum and minimum values and the amplitude of observed seasonal variation but lead to shifting the maximum RM / GEM ratios from spring to summer. The O<sub>3</sub> chemistry does not provide significant seasonal variation of Hg oxidation. Thus, performance of the considered Hg oxidation mechanisms differs in reproduction of different observed parameters that can imply possibility of more complex chemistry and multiple pathways of Hg oxidation occurring concurrently in various parts of the atmosphere.</p>

The overall goal of the on-going Global Mercury Observation System (GMOS) project is to develop a coordinated global monitoring network for mercury, including ground-based, high altitude and sea level stations. In order to ensure data reliability and comparability, a significant effort has been made to implement a centralized system, which is designed to quality assure and quality control atmospheric mercury datasets. This system, GMOS-Data Quality Management (G-DQM), uses a web-based approach with real-time adaptive monitoring procedures aimed at preventing the production of poor-quality data. G-DQM is plugged on a cyberinfrastructure and deployed as a service. Atmospheric mercury datasets, produced during the first-three years of the GMOS project, are used as the input to demonstrate the application of the G-DQM and how it identifies a number of key issues concerning data quality. The major issues influencing data quality are presented and discussed for the GMOS stations under study. Atmospheric mercury data collected at the Longobucco (Italy) station is used as a detailed case study.