Concern about the adverse effects of mercury on human health and ecosystems has led to tightening emission controls since the mid 1980s. But the resulting mercury emissions reductions in many parts of the world are believed to be offset or even surpassed by the increasing emissions in rapidly industrializing countries. Consequently, concentrations of atmospheric mercury are expected to remain roughly constant. Here we show that the worldwide atmospheric mercury concentrations have decreased by about 20 to 38 % since 1996 as indicated by long-term monitoring at stations in the Southern and Northern Hemispheres combined with intermittent measurements of latitudinal distribution over the Atlantic Ocean. The total reduction of the atmospheric mercury burden of this magnitude within 14 years is unusually large among most atmospheric trace gases and is at odds with the current mercury emission inventories with nearly constant anthropogenic emissions over this period. This suggests a major shift in the biogeochemical cycle of mercury including oceans and soil reservoirs. Decreasing reemissions from the legacy of historical mercury emissions are the most likely explanation for this decline since the hypothesis of an accelerated oxidation rate of elemental mercury in the atmosphere is not supported by the observed trends of other trace gases. Acidification of oceans, climate change, excess nutrient input and pollution may also contribute by their impact on the biogeochemistry of ocean and soils. Consequently, models of the atmospheric mercury cycle have to include soil and ocean mercury pools and their dynamics to be able to make projections of future trends.

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.

Goal of the project CARIBIC (Civil Aircraft for the Regular Investigation of the atmosphere Based on an Instrumented Container) is to carry out regular and detailed observations of atmospheric composition (particles and gases) at cruising altitudes of passenger aircraft, i.e. at 9–12 km. Continuous, fast measurement of CO is indispensable for the chemical characterization of encountered air masses, for the detection of plumes of polluted air and for studying troposphere-stratosphere transport. CO is measured by a commercial resonance fluorescence UV instrument modified for the use onboard passenger aircraft. Modifications were necessary to optimize the instrument reliability allowing unattended operation for several days. The instrument has a precision of 1–2 ppbv at an integration time of 1 s. The response time to reach 63.2% signal strength is 2 s. We describe the modifications of the instrument, the experiences made during its operation since December 2004, the quality control of CO measurements onboard CARIBIC, and suggest a regular service routine that guarantees long-term high-quality data.

The Minamata Convention on Mercury (Hg) entered into force in 2017, committing its 116 parties (as of January 2019) to curb anthropogenic emissions. Monitoring of atmospheric concentrations and trends is an important part of the effectiveness evaluation of the convention. A few years ago (in 2017) we reported an increasing trend in atmospheric Hg concentrations at the Cape Point Global Atmosphere Watch (GAW) station in South Africa (34.3535^∘ S, 18.4897^∘ E) for the 2007–2015 period. With 2 more years of measurements at Cape Point and the 2012–2017 data from Amsterdam Island (37.7983^∘ S, 77.5378^∘ E) in the remote southern Indian Ocean, a more complex picture emerges: at Cape Point the upward trend for the 2007–2017 period is still significant, but no trend or a slightly downward trend was detected for the period 2012–2017 at both Cape Point and Amsterdam Island. The upward trend at Cape Point is driven mainly by the Hg concentration minimum in 2009 and maxima in 2014 and 2012. Using ancillary data on ²²²Rn, CO, O₃, CO₂, and CH₄ from Cape Point and Amsterdam Island, the possible reasons for the trend and its change are investigated. In a companion paper this analysis is extended for the Cape Point station by calculations of source and sink regions using backward-trajectory analysis.

Goal of the project CARIBIC (Civil Aircraft for the Regular Investigation of the atmosphere Based on an Instrumented Container) is to carry out regular and detailed observations of atmospheric composition (particles and gases) at cruising altitudes of passenger aircraft, i.e. at 9–12 km. Mercury has been measured since May 2005 by a modified Tekran instrument (Tekran Model 2537 A analyser, Tekran Inc., Toronto, Canada) during monthly intercontinental flights between Europe and South and North America, Africa, and Asia. Here we describe the instrument modifications, the post-flight processing of the raw instrument signal, and the fractionation experiments.