ALBERT

Description: For the last 25 years, CO-PDD (Cézeaux-Aulnat-Opme-puy de Dôme) has evolved to become a full instrumented platform for atmospheric research. It has received credentials as a national observing platform in France and is internationally recognized as a global station in the GAW (Global Atmosphere Watch) network. It is a reference site of European and national research infrastructures ACTRIS (Aerosol Cloud and Trace gases Research Infrastructure) and ICOS (Integrated Carbon Observing System). The site located on top of the puy de Dôme mountain (1465 m a.s.l.) is completed by additional sites located at lower altitudes and adding the vertical dimension to the atmospheric observations: Opme (660 m a.s.l.), Cézeaux (410 m), and Aulnat (330 m). The integration of different sites offers a unique combination of in situ and remote sensing measurements capturing and documenting the variability of particulate and gaseous atmospheric composition, but also the optical, biochemical, and physical properties of aerosol particles, clouds, and precipitations. Given its location far away from any major emission sources, its altitude, and the mountain orography, the puy de Dôme station is ideally located to sample different air masses in the boundary layer or in the free troposphere depending on time of day and seasons. It is also an ideal place to study cloud properties with frequent presence of clouds at the top in fall and winter. As a result of the natural conditions prevailing at the site and of the very exhaustive instrumental deployment, scientific studies at the puy de Dôme strongly contribute to improving knowledge in atmospheric sciences, including the characterization of trends and variability, the understanding of complex and interconnected processes (microphysical, chemical, biological, chemical and dynamical), and the provision of reference information for climate/chemistry models. In this context, CO-PDD is a pilot site to conduct instrumental development inside its wind tunnel for testing liquid and ice cloud probes in natural conditions, or in situ systems to collect aerosol and cloud. This paper reviews 25 years (1995–2020) of atmospheric observation at the station and related scientific research contributing to atmospheric and climate science.

Description: The carbon isotopic signature (δ13CH4) of several methane sources in Germany (around Heidelberg and in North Rhine-Westphalia) were characterised. Mobile measurements of the plume of CH4 sources are carried out using an analyser based on cavity ring-down spectroscopy (CRDS). To achieve precise results a CRDS analyser, which measures methane (CH4), carbon dioxide (CO2) and their 13C-to-12C ratios, was characterised especially with regard to cross sensitivities of composition differences of the gas matrix in air samples or calibration tanks. The two most important gases which affect δ13CH4 are water vapour (H2O) and ethane (C2H6). To avoid the cross sensitivity with H2O, the air is dried with a Nafion dryer during mobile measurements. C2H6 is typically abundant in natural gases and thus in methane plumes or samples originating from natural gas. A C2H6 correction and calibration are essential to obtain accurate δ13CH4 results, which can deviate by up to 3 ‰ depending on whether a C2H6 correction is applied. The isotopic signature is determined with the Miller–Tans approach and the York fitting method. During 21 field campaigns the mean δ13CH4 signatures of three dairy farms (-63.9±0.9‰), a biogas plant (-62.4±1.2‰), a landfill (-58.7±3.3‰), a wastewater treatment plant (-52.5±1.4‰), an active deep coal mine (-56.0±2.3‰) and two natural gas storage and gas compressor stations (-46.1±0.8‰) were recorded. In addition, between December 2016 and November 2018 gas samples from the Heidelberg natural gas distribution network were measured with a mean δ13CH4 value of -43.3±0.8‰. Contrary to previous measurements between 1991 and 1996 by Levin et al. (1999), no strong seasonal cycle is shown.

Description: We present the first comparison of carbon monoxide (CO) measurements performed with a portable laser spectrometer that exploits the optical-feedback cavity-enhanced absorption spectroscopy (OF-CEAS) technique, against a high-performance automated gas chromatograph (GC) with a mercuric oxide reduction gas detector (RGD). First, measurements of atmospheric CO mole fraction were continuously collected in a Paris (France) suburb over 1 week. Both instruments showed an excellent agreement within typically 2 ppb (part per billion in volume), fulfilling the World Meteorological Organization (WMO) recommendation for CO inter-laboratory comparison. The compact size and robustness of the OF-CEAS instrument allowed its operation aboard a small aircraft employed for routine tropospheric air analysis over the French Orléans forest area. Direct OF-CEAS real-time CO measurements in tropospheric air were then compared with later analysis of flask samples by the gas chromatograph. Again, a very good agreement was observed. This work establishes that the OF-CEAS laser spectrometer can run unattended at a very high level of sensitivity ( 

Description: We present inverse modelling (top down) estimates of European methane (CH4) emissions for 2006–2012 based on a new quality-controlled and harmonised in situ data set from 18 European atmospheric monitoring stations. We applied an ensemble of seven inverse models and performed four inversion experiments, investigating the impact of different sets of stations and the use of a priori information on emissions. The inverse models infer total CH4 emissions of 26.8 (20.2–29.7) Tg CH4 yr−1 (mean, 10th and 90th percentiles from all inversions) for the EU-28 for 2006–2012 from the four inversion experiments. For comparison, total anthropogenic CH4 emissions reported to UNFCCC (bottom up, based on statistical data and emissions factors) amount to only 21.3 Tg CH4 yr−1 (2006) to 18.8 Tg CH4 yr−1 (2012). A potential explanation for the higher range of top-down estimates compared to bottom-up inventories could be the contribution from natural sources, such as peatlands, wetlands, and wet soils. Based on seven different wetland inventories from the Wetland and Wetland CH4 Inter-comparison of Models Project (WETCHIMP), total wetland emissions of 4.3 (2.3–8.2) Tg CH4 yr−1 from the EU-28 are estimated. The hypothesis of significant natural emissions is supported by the finding that several inverse models yield significant seasonal cycles of derived CH4 emissions with maxima in summer, while anthropogenic CH4 emissions are assumed to have much lower seasonal variability. Taking into account the wetland emissions from the WETCHIMP ensemble, the top-down estimates are broadly consistent with the sum of anthropogenic and natural bottom-up inventories. However, the contribution of natural sources and their regional distribution remain rather uncertain. Furthermore, we investigate potential biases in the inverse models by comparison with regular aircraft profiles at four European sites and with vertical profiles obtained during the Infrastructure for Measurement of the European Carbon Cycle (IMECC) aircraft campaign. We present a novel approach to estimate the biases in the derived emissions, based on the comparison of simulated and measured enhancements of CH4 compared to the background, integrated over the entire boundary layer and over the lower troposphere. The estimated average regional biases range between −40 and 20 % at the aircraft profile sites in France, Hungary and Poland.

Description: Most of the global fossil fuel CO2 emissions arise from urbanized and industrialized areas. Bottom-up inventories quantify them but with large uncertainties. In 2010–2011, the first atmospheric in situ CO2 measurement network for Paris, the capital of France, began operating with the aim of monitoring the regional atmospheric impact of the emissions coming from this megacity. Five stations sampled air along a northeast–southwest axis that corresponds to the direction of the dominant winds. Two stations are classified as rural (Traînou – TRN; Montgé-en-Goële – MON), two are peri-urban (Gonesse – GON; Gif-sur-Yvette – GIF) and one is urban (EIF, located on top of the Eiffel Tower). In this study, we analyze the diurnal, synoptic and seasonal variability of the in situ CO2 measurements over nearly 1 year (8 August 2010–13 July 2011). We compare these datasets with remote CO2 measurements made at Mace Head (MHD) on the Atlantic coast of Ireland and support our analysis with atmospheric boundary layer height (ABLH) observations made in the center of Paris and with both modeled and observed meteorological fields. The average hourly CO2 diurnal cycles observed at the regional stations are mostly driven by the CO2 biospheric cycle, the ABLH cycle and the proximity to urban CO2 emissions. Differences of several µmol mol−1 (ppm) can be observed from one regional site to the other. The more the site is surrounded by urban sources (mostly residential and commercial heating, and traffic), the more the CO2 concentration is elevated, as is the associated variability which reflects the variability of the urban sources. Furthermore, two sites with inlets high above ground level (EIF and TRN) show a phase shift of the CO2 diurnal cycle of a few hours compared to lower sites due to a strong coupling with the boundary layer diurnal cycle. As a consequence, the existence of a CO2 vertical gradient above Paris can be inferred, whose amplitude depends on the time of the day and on the season, ranging from a few tenths of ppm during daytime to several ppm during nighttime. The CO2 seasonal cycle inferred from monthly means at our regional sites is driven by the biospheric and anthropogenic CO2 flux seasonal cycles, the ABLH seasonal cycle and also synoptic variations. Enhancements of several ppm are observed at peri-urban stations compared to rural ones, mostly from the influence of urban emissions that are in the footprint of the peri-urban station. The seasonal cycle observed at the urban station (EIF) is specific and very sensitive to the ABLH cycle. At both the diurnal and the seasonal scales, noticeable differences of several ppm are observed between the measurements made at regional rural stations and the remote measurements made at MHD, that are shown not to define background concentrations appropriately for quantifying the regional (∼ 100 km) atmospheric impact of urban CO2 emissions. For wind speeds less than 3 m s−1, the accumulation of local CO2 emissions in the urban atmosphere forms a dome of several tens of ppm at the peri-urban stations, mostly under the influence of relatively local emissions including those from the Charles de Gaulle (CDG) Airport facility and from aircraft in flight. When wind speed increases, ventilation transforms the CO2 dome into a plume. Higher CO2 background concentrations of several ppm are advected from the remote Benelux–Ruhr and London regions, impacting concentrations at the five stations of the network even at wind speeds higher than 9 m s−1. For wind speeds ranging between 3 and 8 m s−1, the impact of Paris emissions can be detected in the peri-urban stations when they are downwind of the city, while the rural stations often seem disconnected from the city emission plume. As a conclusion, our study highlights a high sensitivity of the stations to wind speed and direction, to their distance from the city, but also to the ABLH cycle depending on their elevation. We learn some lessons regarding the design of an urban CO2 network: (1) careful attention should be paid to properly setting regional (∼ 100 km) background sites that will be representative of the different wind sectors; (2) the downwind stations should be positioned as symmetrically as possible in relation to the city center, at the peri-urban/rural border; (3) the stations should be installed at ventilated sites (away from strong local sources) and the air inlet set up above the building or biospheric canopy layer, whichever is the highest; and (4) high-resolution wind information should be available with the CO2 measurements.

Description: We present inverse modelling (top-down) estimates of European methane (CH4) emissions for 2006–2012 based on a new quality-controlled and harmonized in-situ data set from 18 European atmospheric monitoring stations. We applied an ensemble of seven inverse models and performed four inversion experiments, investigating the impact of different sets of stations and the use of a priori information on emissions. The inverse models infer total CH4 emissions of 26.7 (20.2–29.7) Tg CH4 yr−1 (mean, 10th and 90th percentiles from all inversions) for the EU-28 for 2006–2012 from the four inversion experiments. For comparison, total anthropogenic CH4 emissions reported to UNFCCC (bottom-up, based on statistical data and emissions factors) amount to only 21.3 Tg CH4 yr−1 (2006) to 18.8 Tg CH4 yr−1 (2012). A potential explanation for the higher range of top-down estimates compared to bottom-up inventories could be the contribution from natural sources, such as peatlands, wetlands, and wet soils. Based on seven different wetland inventories from the Wetland and Wetland CH4 Inter-comparison of Models Project (WETCHIMP) total wetland emissions of 4.3 (2.3–8.2) CH4 yr−1 from EU-28 are estimated. The hypothesis of significant natural emissions is supported by the finding that several inverse models yield significant seasonal cycles of derived CH4 emissions with maxima in summer, while anthropogenic CH4 emissions are assumed to have much lower seasonal variability. Furthermore, we investigate potential biases in the inverse models by comparison with regular aircraft profiles at four European sites and with vertical profiles obtained during the Infrastructure for Measurement of the European Carbon Cycle (IMECC) aircraft campaign. We present a novel approach to estimate the biases in the derived emissions, based on the comparison of simulated and measured enhancements of CH4 compared to the background, integrated over the entire boundary layer and over the lower troposphere. This analysis identifies regional biases for several models at the aircraft profile sites in France, Hungary and Poland.

Description: Most of the global fossil fuel CO2 emissions arise out of urbanized and industrialized areas. Bottom-up inventories quantify them but with large uncertainties. In 2010–2011, the first atmospheric in-situ CO2 measurement network for Paris, the capital of France, has been operated with the aim of monitoring the regional atmospheric impact of the emissions out coming from this megacity. Five stations sampled air along a northeast-southwest axis that corresponds to the direction of the dominant winds. Two stations are classified as rural (TRN and MON), two are peri-urban (GON and GIF) and one is urban (EIF, located on top of the Eiffel tower). In this study, we analyze the diurnal, synoptic and seasonal variability of the in-situ CO2 measurements over nearly one year (8 August 2010–13 July 2011). We compare these datasets with remote CO2 measurements made at Mace Head (MHD) on the Atlantic coast of Ireland, and support our analysis with atmospheric boundary layer height (ABLH) observations made in the centre of Paris and with both modeled and observed meteorological fields. The average hourly CO2 diurnal cycles observed at the regional stations are mostly driven by the CO2 biospheric cycle, the ABLH cycle, and the proximity to urban CO2 emissions. Differences of several μmol mol−1 (ppm) can be observed from one regional site to the other. The more the site is surrounded by urban sources (mostly traffic, residential and commercial heating), the more the CO2 concentration is elevated, as is the associated variability which reflects the variability of the urban sources. Furthermore, two elevated sites (EIF and TRN) show a phase shift of the CO2 diurnal cycle of a few hours compared to lower sites due to a strong coupling with the boundary layer diurnal cycle. As a consequence, the existence of a CO2 vertical gradient above Paris can be inferred, whose amplitude depends on the time of the day and on the season, ranging from a few tenths of ppm during daytime to several ppm during nighttime. The CO2 seasonal cycle inferred from monthly means at our regional sites are driven by the biospheric and anthropogenic CO2 flux seasonal cycles, by the ABLH seasonal cycle and also by synoptic variations. Gradients of several ppm are observed between the rural and peri-urban stations, mostly from the influence of urban emissions that are in the footprint of the peri-urban station. The seasonal cycle observed at the urban station (EIF) is specific and very sensitive to the ABLH cycle. At both the diurnal and the seasonal scales, noticeable differences of several ppm can be observed between the measurements made at regional rural stations and the remote measurements made at MHD, that are shown not to define background concentrations appropriately for quantifying the regional atmospheric impact of urban CO2 emissions. For wind speeds less than 3 m s−1, the accumulation of the local CO2 emissions in the urban atmosphere forms a dome of several tens of ppm at the peri-urban stations, mostly under the influence of relatively local emissions including those from the Charles-De-Gaulle (CDG) airport facility and from aircrafts in flight. When wind speed increases, ventilation transforms the CO2 dome into a plume. Higher CO2 background concentrations of several ppm are advected from the remote Benelux-Ruhr and London regions, impacting concentrations at the five stations of the network even at wind speeds higher than 9 m s−1. For wind speeds ranging between 3 and 8 m s−1, the impact of Paris emissions can be detected in the peri-urban stations when they are downwind of the city, while the rural stations often seem disconnected from the city emission plume. As a conclusion, our study highlights a high sensitivity of the stations to wind speed and direction, to their distance from the city, but also to the ABLH cycle depending on their elevation. We learn some lessons regarding the design of an urban CO2 network: 1/ careful attention should be paid to properly setting background sites that will be representative of the different wind sectors; 2/ the downwind stations should as much as possible be positioned symmetrically in relation to the city centre, at the peri-urban/rural border; 3/ the stations should be installed at ventilated sites (away from strong local sources) and the air inlet set-up above the building or biospheric canopy layer, whichever is the greatest; and 4/ high resolution wind information should be available with the CO2 measurements.

Description: 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 during one year as part of the CO2-MEGAPARIS experiment (August 2010–July 2011), is analysed. Differences in hourly CO2 atmospheric mole fraction 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 degrees of the transect between downwind and upwind site. 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 like September 2010 or November 2010 are poorly constrained by too few CO2 measurements. The high sensitivity of the inverted emissions to the prior emissions' day-to-day variations highlights the limitations induced by assimilating data during a limited number of suitable days. Therefore, even though the inversion improves the seasonal variation and the annual budget of the city's emissions, it 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.

Description: The carbon isotopic signature (δ13CH4) of several methane sources in Germany (around Heidelberg and in North Rhine-Westphalia) were characterised. Therefore, mobile measurements of the plume of CH4 sources are carried out using a cavity ring-down spectrometer (CRDS). To achieve precise results a CRDS analyser, which measures methane (CH4), carbon dioxide (CO2) and their 13C to 12C ratios, was characterised especially with regard to cross sensitivities of the gas matrix. The two most important gases which affect the measurements are water vapour (H2O) and ethane (C2H6). To avoid the cross sensitivity with H2O, the air is dried with a nafion dryer during mobile measurements. C2H6 is abundant in natural gas and thus in methane plumes or samples originating from natural gas. A C2H6 correction and calibration are essential to obtain accurate δ13CH4 results, which can deviate up to 3‰ depending on whether an ethane correction is applied. The isotopic signature is determined with the Miller-Tans approach and the York fitting method. During 21 field campaigns the mean δ13CH4 values of three dairy farms (−63.9±0.9‰), a biogas plant (−62.4±1.2‰), a landfill (−58.7±3.3‰), a wastewater treatment plant (−52.5±1.4‰), an active deep coal mine (−56.0±2.3‰) and two natural gas storage and gas compressor stations (−46.1±0.8‰) were recorded. In addition, between December 2016 and June 2018 gas samples from the Heidelberg natural gas distribution network were measured. Contrary to former measurements between 1991 and 1996 (Levin et al., 1999) no strong seasonal cycle is shown. The mean δ13CH4 value of this study is −43.1±0.8‰ which is 2.8‰ more depleted than in former years.