ALBERT

Description: The Gradient in Longitude of Atmospheric Constituents above the Mediterranean Basin (GLAM) airborne campaign was set up to investigate the summertime variability of gaseous pollutants, greenhouse gases, and aerosols between the western (∼3°E) and eastern (∼35°E) sections of the Mediterranean basin as well as how this connects with the impact of the Asian monsoon anticyclone on the eastern Mediterranean in the mid- to upper troposphere (∼5–10 km). GLAM falls within the framework of the Chemistry–Aerosol Mediterranean Experiment (ChArMEx) program. GLAM used the French Falcon-20 research aircraft to measure aerosols, humidity, and chemical compounds: ozone, carbon monoxide, methane, and carbon dioxide. GLAM took place between 6 and 10 August 2014, following a route from Toulouse (France) to Larnaca (Cyprus) and back again via Minorca (Spain), Lampedusa (Italy), and Heraklion (Crete, Greece). The aircraft flew at an altitude of 5 km on its outbound journey and 10 km on the return leg. GLAM also collected vertical profiles around the landing sites listed above. A combination of model outputs, chemical mapping analyses, and spaceborne and surface station measurements gathered prior to and during the campaign were used to interpret the in situ airborne measurements. The main outcome of this study is the impact of intercontinental transport on the longitudinal variability of pollutants, greenhouse gases, and aerosols at an altitude of 10 km. The eastern Mediterranean is affected by air masses from the Arabian Sea surface, and the western Mediterranean is impacted by air masses from North America (biomass burning) and West Africa (desert dust).

Description: The use of the noble gas radon (222Rn) as a tracer for different research studies, for example observation-based estimation of greenhouse gas (GHG) fluxes, has led to the need of high-quality 222Rn activity concentration observations with high spatial and temporal resolution. So far a robust metrology chain for these measurements is not yet available. A portable direct atmospheric radon monitor (ARMON), based on electrostatic collection of 218Po, is now running at Spanish stations. This monitor has not yet been compared with other 222Rn and 222Rn progeny monitors commonly used at atmospheric stations. A 3-month intercomparison campaign of atmospheric 222Rn and 222Rn progeny monitors based on different measurement techniques was realized during the fall and winter of 2016–2017 to evaluate (i) calibration and correction factors between monitors necessary to harmonize the atmospheric radon observations and (ii) the dependence of each monitor's response in relation to the sampling height and meteorological and atmospheric aerosol conditions. Results of this study have shown the following. (i) All monitors were able to reproduce the atmospheric radon variability on a daily basis. (ii) Linear regression fits between the monitors exhibited slopes, representing the correction factors, between 0.62 and 1.17 and offsets ranging between −0.85 and −0.23 Bq m−3 when sampling 2 m above ground level (a.g.l.). Corresponding results at 100 m a.g.l. exhibited slopes of 0.94 and 1.03 with offsets of −0.13 and 0.01 Bq m−3, respectively. (iii) No influence of atmospheric temperature and relative humidity on monitor responses was observed for unsaturated conditions at 100 m a.g.l., whereas slight influences (order of 10−2) of ambient temperature were observed at 2 m a.g.l. (iv) Changes in the ratio between 222Rn progeny and 222Rn monitor responses were observed under very low atmospheric aerosol concentrations. Results also show that the new ARMON could be useful at atmospheric radon monitoring stations with space restrictions or as a mobile reference instrument to calibrate in situ 222Rn progeny monitors and fixed radon monitors. In the near future a long-term comparison study between ARMON, HRM, and ANSTO monitors would be useful to better evaluate (i) the uncertainties of radon measurements in the range of a few hundred millibecquerels per cubic meter to a few becquerels per cubic meter and (ii) the response time correction of the ANSTO monitor for representing fast changes in the ambient radon concentrations.

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 increasing availability of atmospheric measurements of greenhouse gases (GHGs) from surface stations can improve the retrieval of their fluxes at higher spatial and temporal resolutions by inversions, provided that transport models are able to properly represent the variability of concentrations observed at different stations. South and East Asia (SEA; the study area in this paper including the regions of South Asia and East Asia) is a region with large and very uncertain emissions of carbon dioxide (CO2) and methane (CH4), the most potent anthropogenic GHGs. Monitoring networks have expanded greatly during the past decade in this region, which should contribute to reducing uncertainties in estimates of regional GHG budgets. In this study, we simulate concentrations of CH4 and CO2 using zoomed versions (abbreviated as “ZAs”) of the global chemistry transport model LMDz-INCA, which have fine horizontal resolutions of ∼0.66∘ in longitude and ∼0.51∘ in latitude over SEA and coarser resolutions elsewhere. The concentrations of CH4 and CO2 simulated from ZAs are compared to those from the same model but with standard model grids of 2.50∘ in longitude and 1.27∘ in latitude (abbreviated as “STs”), both prescribed with the same natural and anthropogenic fluxes. Model performance is evaluated for each model version at multi-annual, seasonal, synoptic and diurnal scales, against a unique observation dataset including 39 global and regional stations over SEA and around the world. Results show that ZAs improve the overall representation of CH4 annual gradients between stations in SEA, with reduction of RMSE by 16–20 % compared to STs. The model improvement mainly results from reduction in representation error at finer horizontal resolutions and thus better characterization of the CH4 concentration gradients related to scattered distributed emission sources. However, the performance of ZAs at a specific station as compared to STs is more sensitive to errors in meteorological forcings and surface fluxes, especially when short-term variabilities or stations close to source regions are examined. This highlights the importance of accurate a priori CH4 surface fluxes in high-resolution transport modeling and inverse studies, particularly regarding locations and magnitudes of emission hotspots. Model performance for CO2 suggests that the CO2 surface fluxes have not been prescribed with sufficient accuracy and resolution, especially the spatiotemporally varying carbon exchange between land surface and atmosphere. In addition, the representation of the CH4 and CO2 short-term variabilities is also limited by model's ability to simulate boundary layer mixing and mesoscale transport in complex terrains, emphasizing the need to improve sub-grid physical parameterizations in addition to refinement of model resolutions.

Description: This study deals with the problem of identifying atmospheric data influenced by local emissions that can result in spikes in time series of greenhouse gases and long-lived tracer measurements. We considered three spike detection methods known as coefficient of variation (COV), robust extraction of baseline signal (REBS) and standard deviation of the background (SD) to detect and filter positive spikes in continuous greenhouse gas time series from four monitoring stations representative of the European ICOS (Integrated Carbon Observation System) Research Infrastructure network. The results of the different methods are compared to each other and against a manual detection performed by station managers. Four stations were selected as test cases to apply the spike detection methods: a continental rural tower of 100 m height in eastern France (OPE), a high-mountain observatory in the south-west of France (PDM), a regional marine background site in Crete (FKL) and a marine clean-air background site in the Southern Hemisphere on Amsterdam Island (AMS). This selection allows us to address spike detection problems in time series with different variability. Two years of continuous measurements of CO2, CH4 and CO were analysed. All methods were found to be able to detect short-term spikes (lasting from a few seconds to a few minutes) in the time series. Analysis of the results of each method leads us to exclude the COV method due to the requirement to arbitrarily specify an a priori percentage of rejected data in the time series, which may over- or underestimate the actual number of spikes. The two other methods freely determine the number of spikes for a given set of parameters, and the values of these parameters were calibrated to provide the best match with spikes known to reflect local emissions episodes that are well documented by the station managers. More than 96 % of the spikes manually identified by station managers were successfully detected both in the SD and the REBS methods after the best adjustment of parameter values. At PDM, measurements made by two analyzers located 200 m from each other allow us to confirm that the CH4 spikes identified in one of the time series but not in the other correspond to a local source from a sewage treatment facility in one of the observatory buildings. From this experiment, we also found that the REBS method underestimates the number of positive anomalies in the CH4 data caused by local sewage emissions. As a conclusion, we recommend the use of the SD method, which also appears to be the easiest one to implement in automatic data processing, used for the operational filtering of spikes in greenhouse gases time series at global and regional monitoring stations of networks like that of the ICOS atmosphere network.

Description: 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.

Description: Methane emissions on the national scale in France in 2012 are inferred by assimilating continuous atmospheric mixing ratio measurements from nine stations of the European network ICOS located in France and surrounding countries. To assess the robustness of the fluxes deduced by our inversion system based on an objectified quantification of uncertainties, two complementary inversion set-ups are computed and analysed: (i) a regional run correcting for the spatial distribution of fluxes in France and (ii) a sectorial run correcting fluxes for activity sectors on the national scale. In addition, our results for the two set-ups are compared with fluxes produced in the framework of the inversion inter-comparison exercise of the InGOS project. The seasonal variability in fluxes is consistent between different set-ups, with maximum emissions in summer, likely due to agricultural activity. However, very high monthly posterior uncertainties (up to ≈ 65 to 74 % in the sectorial run in May and June) make it difficult to attribute maximum emissions to a specific sector. On the yearly and national scales, the two inversions range from 3835 to 4050 Gg CH4 and from 3570 to 4190 Gg CH4 for the regional and sectorial runs, respectively, consistently with the InGOS products. These estimates are 25 to 55 % higher than the total national emissions from bottom-up approaches (biogeochemical models from natural emissions, plus inventories for anthropogenic ones), consistently pointing at missing or underestimated sources in the inventories and/or in natural sources. More specifically, in the sectorial set-up, agricultural emissions are inferred as 66% larger than estimates reported to the UNFCCC. Uncertainties in the total annual national budget are 108 and 312 Gg CH4, i.e, 3 to 8 %, for the regional and sectorial runs respectively, smaller than uncertainties in available bottom-up products, proving the added value of top-down atmospheric inversions. Therefore, even though the surface network used in 2012 does not allow us to fully constrain all regions in France accurately, a regional inversion set-up makes it possible to provide estimates of French methane fluxes with an uncertainty in the total budget of less than 10 % on the yearly timescale. Additional sites deployed since 2012 would help to constrain French emissions on finer spatial and temporal scales and attributing missing emissions to specific sectors.

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.