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We present a city-scale inversion over Cape Town, South Africa. Measurement sites for atmospheric CO2 concentrations were installed at Robben Island and Hangklip lighthouses, located downwind and upwind of the metropolis. Prior estimates of the fossil fuel fluxes were obtained from a bespoke inventory analysis where emissions were spatially and temporally disaggregated and uncertainty estimates determined by means of error propagation techniques. Net ecosystem exchange (NEE) fluxes from biogenic processes were obtained from the land atmosphere exchange model CABLE (Community Atmosphere Biosphere Land Exchange). Uncertainty estimates were based on the estimates of net primary productivity. CABLE was dynamically coupled to the regional climate model CCAM (Conformal Cubic Atmospheric Model), which provided the climate inputs required to drive the Lagrangian particle dispersion model. The Bayesian inversion framework included a control vector where fossil fuel and NEE fluxes were solved for separately.Due to the large prior uncertainty prescribed to the NEE fluxes, the current inversion framework was unable to adequately distinguish between the fossil fuel and NEE fluxes, but the inversion was able to obtain improved estimates of the total fluxes within pixels and across the domain. The median of the uncertainty reductions of the total weekly flux estimates for the inversion domain of Cape Town was 28 %, but reach as high as 50 %. At the pixel level, uncertainty reductions of the total weekly flux reached up to 98 %, but these large uncertainty reductions were for NEE-dominated pixels. Improved corrections to the fossil fuel fluxes would be possible if the uncertainty around the prior NEE fluxes could be reduced. In order for this inversion framework to be operationalised for monitoring, reporting, and verification (MRV) of emissions from Cape Town, the NEE component of the CO2 budget needs to be better understood. Additional measurements of Δ14C and δ13C isotope measurements would be a beneficial component of an atmospheric monitoring programme aimed at MRV of CO2 for any city which has significant biogenic influence, allowing improved separation of contributions from NEE and fossil fuel fluxes to the observed CO2 concentration.

Long-term measurements of gaseous elemental mercury (GEM) concentrations at Cape Point, South Africa, reveal a downward trend between September 1995 and December 2005 and an upward one from March 2007 until June 2015, implying a change in trend sign between 2004 and 2007. The trend change is qualitatively consistent with the trend changes in GEM concentrations observed at Mace Head, Ireland, and in mercury wet deposition over North America, suggesting a change in worldwide mercury emissions. Seasonally resolved trends suggest a modulation of the overall trend by regional processes. The trends in absolute terms (downward in 1995–2004 and upward in 2007–2015) are highest in austral spring (SON), coinciding with the peak in emissions from biomass burning in South America and southern Africa. The influence of trends in biomass burning is further supported by a biennial variation in GEM concentration found here and an El Niño–Southern Oscillation (ENSO) signature in GEM concentrations reported recently.

The International Halocarbons in Air Comparison Experiment (IHALACE) was conducted to document relationships between calibration scales among various laboratories that measure atmospheric greenhouse and ozone depleting gases. This study included trace gases such as chlorofluorocarbons (CFCs), hydrochlorofluorocarbons (HCFCs), and hydrofluorocarbons (HFCs), as well as nitrous oxide, methane, sulfur hexafluoride, very short-lived halocompounds, and carbonyl sulfide. Many of these gases are present in the unpolluted atmosphere at pmol mol−1 (parts per trillion) or nmol mol−1 (parts per billion) levels. Six stainless steel cylinders containing natural and modified natural air samples were circulated among 19 laboratories. Results from this experiment reveal relatively good agreement (within a few percent) among commonly used calibration scales. Scale relationships for some gases, such as CFC-12 and CCl4, were found to be consistent with those derived from estimates of global mean mole fractions, while others, such as halon-1211 and CH3Br, revealed discrepancies. The transfer of calibration scales among laboratories was problematic in many cases, meaning that measurements tied to a particular scale may not, in fact, be compatible. Large scale transfer errors were observed for CH3CCl3 (10–100%) and CCl4 (2–30%), while much smaller scale transfer errors (< 1%) were observed for halon-1211, HCFC-22, and HCFC-142b. These results reveal substantial improvements in calibration over previous comparisons. However, there is room for improvement in communication and coordination of calibration activities with respect to the measurement of halogenated and related trace gases.

The authors evaluated continuous high-resolution gaseous elemental mercury (GEM) data from the Cape Point Global Atmosphere Watch (CPT GAW) station with different statistical analysis techniques. GEM data were evaluated by cluster analysis and the results indicated that two clusters, separated at 0.904 ng m−3, existed. The air mass history for the two-cluster solution was investigated by means of back-trajectory analysis. The air mass back-trajectory net result showed lower GEM concentrations originating from the sparsely populated semi-arid interior of South Africa and the marine environment, whereas higher GEM concentrations originated predominately along the coast of South Africa that most likely coincide with trade routes and industrial activities in urban areas along the coast. Considering the net result from the air mass back-trajectories, it is evident that not all low GEM concentrations are from marine origin, and similarly, not all high GEM concentrations have a terrestrial origin. Equations were developed by means of multi-linear regression (MLR) analysis that allowed for the estimation and/or prediction of atmospheric GEM concentrations from other atmospheric parameters measured at the CPT GAW station. These equations also provided some insight into the relation and interaction of GEM with other atmospheric parameters. Both measured and MLR calculated data confirm a decline in GEM concentrations at CPT GAW over the period evaluated.

Gaseous elemental mercury (GEM) and 222Rn, a radioactive gas of primarily terrestrial origin with a half-life of 3.8 days, have been measured simultaneously at Cape Point, South Africa, since March 2007. Between March 2007 and December 2011 altogether 191 events with high 222Rn concentrations were identified. GEM correlated with 222Rn in 94 of the events and was constant during almost all the remaining events without significant correlation. The average GEM/222Rn emission ratio of all events including the non-significant ones was −0.0001 &pm; 0.0030 pg mBq−1, with 0.0030 pg mBq−1 being the standard error of the average. With an emission rate of 1.1 222Rn atoms cm−2 s−1 and a correction for the transport duration, this emission ratio corresponds to a radon calibrated flux of about −0.01 ng GEM m−2 h−1 with a standard error of &pm;0.34 ng GEM m−2 h−1 (n = 191). With wet deposition, which is not included in this estimate, the terrestrial surface of southern Africa seems to be a net mercury sink of about −1.01 ng m−2 h−1.

The recent increase of atmospheric methane is investigated by using two atmospheric inversions to quantify the global distribution of sources and sinks for the 2006–2008 period, and a process-based model of CH4 emissions by natural wetland ecosystems. Global emissions derived from inversions are found to have increased by 19 Tg on average in 2007 (16 to 21 Tg) and by 13 Tg in 2008 (6 to 20 Tg), as compared to the 1999–2006 period. A positive anomaly of tropical emissions is found to be the main contributor to the global emission anomaly of 2007 (~60–75%), with a dominant share attributed to natural wetlands (~66%). Abnormally high wetlands emissions from high latitudes are also detected by both inversions in 2007, contributing 15–30% of the global anomaly. Good agreement is found between the results of the wetland ecosystem model and the inversions for 2007. The inferred distribution of the source anomaly in 2007 is shown to be consistent with the observation of a more pronounced increase in near surface methane atmospheric growth rate at high latitudes, because the dilution of surface fluxes by convection is strong in the tropics and weak at high latitudes. The source anomaly in 2008 is found to be much larger in the wetland ecosystem model than in the inversions, suggesting a too strong sensitivity of bottom-up modeled emissions to precipitation. Changes in OH radicals during 2006–2008 are found to be less than 1% in inversions, with only a small impact on the inferred methane emissions.

International audience; No abstract available.