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Atmospheric concentration measurements are used to adjust the daily to monthly budget of fossil fuel CO2 emissions of the Paris urban area from the prior estimates established by the Airparif local air quality agency. Five atmospheric monitoring sites are available, including one at the top of the Eiffel Tower. The atmospheric inversion is based on a Bayesian approach, and relies on an atmospheric transport model with a spatial resolution of 2 km with boundary conditions from a global coarse grid transport model. The inversion adjusts prior knowledge about the anthropogenic and biogenic CO2 fluxes from the Airparif inventory and an ecosystem model, respectively, with corrections at a temporal resolution of 6 h, while keeping the spatial distribution from the emission inventory. These corrections are based on assumptions regarding the temporal autocorrelation of prior emissions uncertainties within the daily cycle, and from day to day. The comparison of the measurements against the atmospheric transport simulation driven by the a priori CO2 surface fluxes shows significant differences upwind of the Paris urban area, which suggests a large and uncertain contribution from distant sources and sinks to the CO2 concentration variability. This contribution advocates that the inversion should aim at minimising model-data misfits in upwind-downwind gradients rather than misfits in mole fractions at individual sites. Another conclusion of the direct model-measurement comparison is that the CO2 variability at the top of the Eiffel Tower is large and poorly represented by the model for most wind speeds and directions. The model's inability to reproduce the CO2 variability at the heart of the city makes such measurements ill-suited for the inversion. This and the need to constrain the budgets for the whole city suggests the assimilation of upwind-downwind mole fraction gradients between sites at the edge of the urban area only. The inversion significantly improves the agreement between measured and modelled concentration gradients. Realistic emissions are retrieved for two 30-day periods and suggest a significant overestimate by the AirParif inventory. Similar inversions over longer periods are necessary for a proper evaluation of the optimised CO2 emissions against independent data.

The 2018 drought was one of the worst European droughts of the twenty-first century in terms of its severity, extent and duration. The effects of the drought could be seen in a reduction in harvest yields in parts of Europe, as well as an unprecedented browning of vegetation in summer. Here, we quantify the effect of the drought on net ecosystem exchange (NEE) using five independent regional atmospheric inversion frameworks. Using a network of atmospheric CO 2 mole fraction observations, we estimate NEE with at least monthly and 0.5° × 0.5° resolution for 2009–2018. We find that the annual NEE in 2018 was likely more positive (less CO 2 uptake) in the temperate region of Europe by 0.09 ± 0.06 Pg C yr −1 (mean ± s.d.) compared to the mean of the last 10 years of −0.08 ± 0.17 Pg C yr −1 , making the region close to carbon neutral in 2018. Similarly, we find a positive annual NEE anomaly for the northern region of Europe of 0.02 ± 0.02 Pg C yr −1 compared the 10-year mean of −0.04 ± 0.05 Pg C yr −1 . In both regions, this was largely owing to a reduction in the summer CO 2 uptake. The positive NEE anomalies coincided spatially and temporally with negative anomalies in soil water. These anomalies were exceptional for the 10-year period of our study. This article is part of the theme issue ‘Impacts of the 2018 severe drought and heatwave in Europe: from site to continental scale’.

Although essential to fully understand the cycling of mercury at the global scale, mercury species records in the Southern Hemisphere are scarce. Under the framework of the Global Mercury Observation System (GMOS) project, a monitoring station has been set up on Amsterdam Island (37°48´ S, 77°34´ E) in the remote southern Indian Ocean. For the first time in the Southern Hemisphere, a 2-year record of gaseous elemental mercury (GEM), reactive gaseous mercury (RGM) and particle-bound mercury (PBM) is presented. GEM concentrations were remarkably steady (1.03 ± 0.08 ng m−3) while RGM and PBM concentrations were very low and exhibited a strong variability (mean: 0.34 pg m−3, range: < detection limit–4.07 pg m−3; and mean: 0.67 pg m−3, range: < detection limit–12.67 pg m−3, respectively). Despite the remoteness of the island, wind sector analysis, air mass back trajectories and the observation of radonic storms highlighted a long-range contribution from the southern African continent to the GEM and PBM budgets from July to September during the biomass burning season. Low concentrations of GEM were associated with southerly polar and marine air masses from the remote southern Indian Ocean. This unique data set provides new baseline GEM concentrations in the Southern Hemisphere midlatitudes while mercury speciation along with upcoming wet deposition data will help to improve our understanding of the mercury cycle in the marine boundary layer.

Atmospheric carbon monoxide (CO) and methane (CH4) mole fractions are measured by ground-based in situ cavity ring-down spectroscopy (CRDS) analyzers and Fourier transform infrared (FTIR) spectrometers at two sites (St Denis and Maïdo) on Reunion Island (21∘ S, 55∘ E) in the Indian Ocean. Currently, the FTIR Bruker IFS 125HR at St Denis records the direct solar spectra in the near-infrared range, contributing to the Total Carbon Column Observing Network (TCCON). The FTIR Bruker IFS 125HR at Maïdo records the direct solar spectra in the mid-infrared (MIR) range, contributing to the Network for the Detection of Atmospheric Composition Change (NDACC). In order to understand the atmospheric CO and CH4 variability on Reunion Island, the time series and seasonal cycles of CO and CH4 from in situ and FTIR (NDACC and TCCON) measurements are analyzed. Meanwhile, the difference between the in situ and FTIR measurements are discussed. The CO seasonal cycles observed from the in situ measurements at Maïdo and FTIR retrievals at both St Denis and Maïdo are in good agreement with a peak in September–November, primarily driven by the emissions from biomass burning in Africa and South America. The dry-air column averaged mole fraction of CO (XCO) derived from the FTIR MIR spectra (NDACC) is about 15.7 ppb larger than the CO mole fraction near the surface at Maïdo, because the air in the lower troposphere mainly comes from the Indian Ocean while the air in the middle and upper troposphere mainly comes from Africa and South America. The trend for CO on Reunion Island is unclear during the 2011–2017 period, and more data need to be collected to get a robust result. A very good agreement is observed in the tropospheric and stratospheric CH4 seasonal cycles between FTIR (NDACC and TCCON) measurements, and in situ and the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) satellite measurements, respectively. In the troposphere, the CH4 mole fraction is high in August–September and low in December–January, which is due to the OH seasonal variation. In the stratosphere, the CH4 mole fraction has its maximum in March–April and its minimum in August–October, which is dominated by vertical transport. In addition, the different CH4 mole fractions between the in situ, NDACC and TCCON CH4 measurements in the troposphere are discussed, and all measurements are in good agreement with the GEOS-Chem model simulation. The trend of XCH4 is 7.6±0.4 ppb yr−1 from the TCCON measurements over the 2011 to 2017 time period, which is consistent with the CH4 trend of 7.4±0.5 ppb yr−1 from the in situ measurements for the same time period at St Denis.

Measurements of the mole fraction of the CO2 and its isotopes were performed in Paris during the MEGAPOLI winter campaign (January-February 2010). Radiocarbon (14 CO2 ) measurements were used to identify the relative contributions of 77% CO2 from fossil fuel consumption (CO2 ff from liquid and gas combustion) and 23% from biospheric CO2 (CO2 from the use of biofuels and from human and plant respiration: CO2 bio). These percentages correspond to average mole fractions of 26.4 ppm and 8.2 ppm for CO2 ff and CO2 bio, respectively. The 13 CO2 analysis indicated that gas and liquid fuel contributed 70% and 30%, respectively, of the CO2 emission from fossil fuel use. Continuous measurements of CO and NOx and the ratios CO/CO2 ff and NOx /CO2 ff derived from radiocarbon measurements during four days make it possible to estimate the fossil fuel CO2 contribution over the entire campaign. The ratios CO/CO2 ff and NOx /CO2 ff are functions of air mass origin and exhibited daily ranges of 7.9 to 14.5 ppb ppm-1 and 1.1 to 4.3 ppb ppm-1 , respectively. These ratios are consistent with different emission inventories given the uncertainties of the different approaches. By using both tracers to derive the fossil fuel CO2 , we observed similar diurnal cycles with two maxima during rush hour traffic.

With the rapid growth in population and economic development, emissions of greenhouse gases (GHGs) from the Indian subcontinent have sharply increased during recent decades. However, evaluation of regional fluxes of GHGs and characterization of their spatial and temporal variations by atmospheric inversions remain uncertain due to a sparse regional atmospheric observation network. As a result of an Indo-French collaboration, three new atmospheric stations were established in India at Hanle (HLE), Pondicherry (PON) and Port Blair (PBL), with the objective of monitoring the atmospheric concentrations of GHGs and other trace gases. Here we present the results of the measurements of CO2, CH4, N2O, SF6, CO, and H2 from regular flask sampling at these three stations over the period 2007–2011. For each species, annual means, seasonal cycles and gradients between stations were calculated and related to variations in natural GHG fluxes, anthropogenic emissions, and monsoon circulations. Covariances between species at the synoptic scale were analyzed to investigate the likely source(s) of emissions. The flask measurements of various trace gases at the three stations have the potential to constrain the inversions of fluxes over southern and northeastern India. However, this network of ground stations needs further extension to other parts of India to better constrain the GHG budgets at regional and continental scales.

Dual carbon isotope analysis of marine aerosol samples has been performed for the first time demonstrating a potential in organic matter apportionment between three principal sources: marine, terrestrial (non-fossil) and fossil fuel due to unique isotopic signatures. The results presented here, utilising combinations of dual carbon isotope analysis, provides conclusive evidence of a dominant biogenic organic fraction to organic aerosol over biologically active oceans. In particular, the NE Atlantic, which is also subjected to notable anthropogenic influences via pollution transport processes, was found to contain 80 % organic aerosol matter of biogenic origin directly linked to plankton emissions. The remaining carbonaceous aerosol was of terrestrial origin. By contrast, for polluted air advected out from Europe into the NE Atlantic, the source apportionment is 30 % marine biogenic, 40 % fossil fuel, and 30 % continental non-fossil fuel. The dominant marine organic aerosol source in the atmosphere has significant implications for climate change feedback processes.

The Total Carbon Column Observing Network (TCCON) is a ground-based network of Fourier Transform Spectrometer (FTS) sites around the globe, where the column abundances of CO2 , CH4 , N2 O, CO and O2 are measured. CO2 is constrained with a precision better than 0.25% (1-σ). To achieve a similarly high accuracy, calibration to World Meteorological Organization (WMO) standards is required. This paper introduces the first aircraft calibration campaign of five European TCCON sites and a mobile FTS instrument. A series of WMO standards in-situ profiles were obtained over European TCCON sites via aircraft and compared with retrievals of CO2 column amounts from the TCCON instruments. The results of the campaign show that the FTS measurements are consistently biased 1.1% ± 0.2% low with respect to WMO standards, in agreement with previous TCCON calibration campaigns. The standard a priori profile for the TCCON FTS retrievals is shown to not add a bias. The same calibration factor is generated using aircraft profiles as a priori and with the TCCON standard a priori. With a calibration to WMO standards, the highly precise TCCON CO2 measurements of total column concentrations provide a suitable database for the calibration and validation of nadir-viewing satellites.

To develop an accurate measurement network of greenhouse gases, instruments in the field need to be stable and precise and thus require infrequent calibrations and a low consumption of consumables. For about 10 years, cavity ring-down spectroscopy (CRDS) analyzers have been available that meet these stringent requirements for precision and stability. Here, we present the results of tests of CRDS instruments in the laboratory (47 instruments) and in the field (15 instruments). The precision and stability of the measurements are studied. We demonstrate that, thanks to rigorous testing, newer models generally perform better than older models, especially in terms of reproducibility between instruments. In the field, we see the importance of individual diagnostics during the installation phase, and we show the value of calibration and target gases that assess the quality of the data. Finally, we formulate recommendations for use of these analyzers in the field.

European CH 4 and N 2 O emissions are estimated for 2006 and 2007 using four inverse modelling systems, based on different global and regional Eulerian and La-grangian transport models. This ensemble approach is designed to provide more realistic estimates of the overall uncertainties in the derived emissions, which is particularly important for verifying bottom-up emission inventories. We use continuous observations from 10 European stations (including 5 tall towers) for CH 4 and 9 continuous stations for N 2 O, complemented by additional European and global discrete air sampling sites. The available observations mainly constrain CH 4 and N 2 O emissions from northwestern and eastern Europe. The inversions are strongly driven by the observations and the derived total emissions of larger countries show little dependence on the emission inventories used a priori. Three inverse models yield 26-56 % higher total CH 4 emissions from northwestern and eastern Europe compared Published by Copernicus Publications on behalf of the European Geosciences Union. 716 P. Bergamaschi et al.: Top-down estimates of European CH 4 and N 2 O emissions to bottom-up emissions reported to the UNFCCC, while one model is close to the UNFCCC values. In contrast, the inverse modelling estimates of European N 2 O emissions are in general close to the UNFCCC values, with the overall range from all models being much smaller than the UNFCCC uncertainty range for most countries. Our analysis suggests that the reported uncertainties for CH 4 emissions might be underestimated , while those for N 2 O emissions are likely overestimated .