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In 2015, the Greenhouse gas Laser Imaging Tomography Experiment (GreenLITE™) measurement system was deployed for a long-duration experiment in the center of Paris, France. The system measures near-surface atmospheric CO2 concentrations integrated along 30 horizontal chords ranging in length from 2.3 to 5.2 km and covering an area of 25 km2 over the complex urban environment. In this study, we use this observing system together with six conventional in situ point measurements and the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem) and two urban canopy schemes (Urban Canopy Model – UCM; Building Effect Parameterization – BEP) at a horizontal resolution of 1 km to analyze the temporal and spatial variations in CO2 concentrations within the city of Paris and its vicinity for the 1-year period spanning December 2015 to November 2016. Such an analysis aims at supporting the development of CO2 atmospheric inversion systems at the city scale. Results show that both urban canopy schemes in the WRF-Chem model are capable of reproducing the seasonal cycle and most of the synoptic variations in the atmospheric CO2 point measurements over the suburban areas as well as the general corresponding spatial differences in CO2 concentration that span the urban area. However, within the city, there are larger discrepancies between the observations and the model results with very distinct features during winter and summer. During winter, the GreenLITE™ measurements clearly demonstrate that one urban canopy scheme (BEP) provides a much better description of temporal variations and horizontal differences in CO2 concentrations than the other (UCM) does. During summer, much larger CO2 horizontal differences are indicated by the GreenLITE™ system than both the in situ measurements and the model results, with systematic east–west variations.

Providing timely information on urban greenhouse gas (GHG) emissions and their trends to stakeholders relies on reliable measurements of atmospheric concentrations and the understanding of how local emissions and atmospheric transport influence these observations. Portable Fourier transform infrared (FTIR) spectrometers were deployed at five stations in the Paris metropolitan area to provide column-averaged concentrations of CO2 (XCO2) during a field campaign in spring of 2015, as part of the Collaborative Carbon Column Observing Network (COCCON). Here, we describe and analyze the variations of XCO2 observed at different sites and how they changed over time. We find that observations upwind and downwind of the city centre differ significantly in their XCO2 concentrations, while the overall variability of the daily cycle is similar, i.e. increasing during night-time with a strong decrease (typically 2–3 ppm) during the afternoon. An atmospheric transport model framework (CHIMERE-CAMS) was used to simulate XCO2 and predict the same behaviour seen in the observations, which supports key findings, e.g. that even in a densely populated region like Paris (over 12 million people), biospheric uptake of CO2 can be of major influence on daily XCO2 variations. Despite a general offset between modelled and observed XCO2, the model correctly predicts the impact of the meteorological parameters (e.g. wind direction and speed) on the concentration gradients between different stations. When analyzing local gradients of XCO2 for upwind and downwind station pairs, those local gradients are found to be less sensitive to changes in XCO2 boundary conditions and biogenic fluxes within the domain and we find the model–data agreement further improves. Our modelling framework indicates that the local XCO2 gradient between the stations is dominated by the fossil fuel CO2 signal of the Paris metropolitan area. This further highlights the potential usefulness of XCO2 observations to help optimize future urban GHG emission estimates.

The ability of a Bayesian atmospheric inversion to quantify the Paris region's fossil fuel CO2 emissions on a monthly basis, based on a network of three surface stations operated for 1 year as part of the CO2-MEGAPARIS experiment (August 2010–July 2011), is analysed. Differences in hourly CO2 atmospheric mole fractions between the near-ground monitoring sites (CO2 gradients), located at the north-eastern and south-western edges of the urban area, are used to estimate the 6 h mean fossil fuel CO2 emission. The inversion relies on the CHIMERE transport model run at 2 km × 2 km horizontal resolution, on the spatial distribution of fossil fuel CO2 emissions in 2008 from a local inventory established at 1 km × 1 km horizontal resolution by the AIRPARIF air quality agency, and on the spatial distribution of the biogenic CO2 fluxes from the C-TESSEL land surface model. It corrects a prior estimate of the 6 h mean budgets of the fossil fuel CO2 emissions given by the AIRPARIF 2008 inventory. We found that a stringent selection of CO2 gradients is necessary for reliable inversion results, due to large modelling uncertainties. In particular, the most robust data selection analysed in this study uses only mid-afternoon gradients if wind speeds are larger than 3 m s−1 and if the modelled wind at the upwind site is within ±15° of the transect between downwind and upwind sites. This stringent data selection removes 92 % of the hourly observations. Even though this leaves few remaining data to constrain the emissions, the inversion system diagnoses that their assimilation significantly reduces the uncertainty in monthly emissions: by 9 % in November 2010 to 50 % in October 2010. The inverted monthly mean emissions correlate well with independent monthly mean air temperature. Furthermore, the inverted annual mean emission is consistent with the independent revision of the AIRPARIF inventory for the year 2010, which better corresponds to the measurement period than the 2008 inventory. Several tests of the inversion's sensitivity to prior emission estimates, to the assumed spatial distribution of the emissions, and to the atmospheric transport modelling demonstrate the robustness of the measurement constraint on inverted fossil fuel CO2 emissions. The results, however, show significant sensitivity to the description of the emissions' spatial distribution in the inversion system, demonstrating the need to rely on high-resolution local inventories such as that from AIRPARIF. Although the inversion constrains emissions through the assimilation of CO2 gradients, the results are hampered by the improperly modelled influence of remote CO2 fluxes when air masses originate from urbanised and industrialised areas north-east of Paris. The drastic data selection used in this study limits the ability to continuously monitor Paris fossil fuel CO2 emissions: the inversion results for specific months such as September or November 2010 are poorly constrained by too few CO2 measurements. The high sensitivity of the inverted emissions to the prior emissions' diurnal variations highlights the limitations induced by assimilating data only during the afternoon. Furthermore, even though the inversion improves the seasonal variation and the annual budget of the city's emissions, the assimilation of data during a limited number of suitable days does not necessarily yield robust estimates for individual months. These limitations could be overcome through a refinement of the data processing for a wider data selection, and through the expansion of the observation network.

Both balloon-borne electrochemical ozonesondes and MOZAIC (measurements of ozone, water vapour, carbon monoxide and nitrogen oxides by in-service Airbus aircraft) provide very valuable data sets for ozone studies in the upper troposphere/lower stratosphere (UTLS). Although MOZAIC's highly accurate UV-photometers are regularly inspected and recalibrated annually, recent analyses cast some doubt on the long-term stability of their ozone analysers. To investigate this further, we perform a 16 yr comparison (1994–2009) of UTLS ozone measurements from balloon-borne ozonesondes and MOZAIC. The analysis uses fully three-dimensional trajectories computed from ERA-Interim (European Centre for Medium-Range Weather Forecasts Re-analysis) wind fields to find matches between the two measurement platforms. Although different sensor types (Brewer-Mast and Electrochemical Concentration Cell ozonesondes) were used, most of the 28 launch sites considered show considerable differences of up to 25% compared to MOZAIC in the mid-1990s, followed by a systematic tendency to smaller differences of around 5–10% in subsequent years. The reason for the difference before 1998 remains unclear, but observations from both sondes and MOZAIC require further examination to be reliable enough for use in robust long-term trend analyses starting before 1998. According to our analysis, ozonesonde measurements at tropopause altitudes appear to be rather insensitive to changing the type of the Electrochemical Concentration Cell ozonesonde, provided the cathode sensing solution strength remains unchanged. Scoresbysund (Greenland) showed systematically 5% higher readings after changing from Science Pump Corporation sondes to ENSCI Corporation sondes, while a 1.0% KI cathode electrolyte was retained.