New metrology for radon at the environmental level

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Simulating CH_4 and CO_2 over South and East Asia using the zoomed chemistry transport model LMDz-INCA

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 (CO_2) and methane (CH_4), 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 CH_4 and CO_2 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 CH_4 and CO_2 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 CH_4 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 CH_4 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 CH_4 surface fluxes in high-resolution transport modeling and inverse studies, particularly regarding locations and magnitudes of emission hotspots. Model performance for CO_2 suggests that the CO_2 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 CH_4 and CO_2 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

Simulating CH_4 and CO_2 over South and East Asia using the zoomed chemistry transport model LMDz-INCA

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 (CO_2) and methane (CH_4), 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 CH_4 and CO_2 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 CH_4 and CO_2 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 CH_4 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 CH_4 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 CH_4 surface fluxes in high-resolution transport modeling and inverse studies, particularly regarding locations and magnitudes of emission hotspots. Model performance for CO_2 suggests that the CO_2 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 CH_4 and CO_2 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

New contributions of measurements in Europe to the global inventory of the stable isotopic composition of methane

Recent climate change mitigation strategies rely on the reduction of methane (CH4) emissions. Carbon and hydrogen isotope ratio (δ13CCH4 and δ2HCH4) measurements can be used to distinguish sources and thus to understand the CH4 budget better. The CH4 emission estimates by models are sensitive to the isotopic signatures assigned to each source category, so it is important to provide representative estimates of the different CH4 source isotopic signatures worldwide. We present new measurements of isotope signatures of various, mainly anthropogenic, CH4 sources in Europe, which represent a substantial contribution to the global dataset of source isotopic measurements from the literature, especially for δ2HCH4. They improve the definition of δ13CCH4 from waste sources, and demonstrate the use of δ2HCH4 for fossil fuel source attribution. We combined our new measurements with the last published database of CH4 isotopic signatures and with additional literature, and present a new global database. We found that microbial sources are generally well characterised. The large variability in fossil fuel isotopic compositions requires particular care in the choice of weighting criteria for the calculation of a representative global value. The global dataset could be further improved by measurements from African, South American, and Asian countries, and more measurements from pyrogenic sources. We improved the source characterisation of CH4 emissions using stable isotopes and associated uncertainty, to be used in top-down studies. We emphasise that an appropriate use of the database requires the analysis of specific parameters in relation to source type and the region of interest. The final version of the European CH4 isotope database coupled with a global inventory of fossil and non-fossil δ13CCH4 and δ2HCH4 source signature measurements is available at 10.24416/UU01-YP43IN

The fingerprint of the summer 2018 drought in Europe on ground-based atmospheric CO2 measurements

During the summer of 2018, a widespread drought developed over Northern and Central Europe. The increase in temperature and the reduction of soil moisture have influenced carbon dioxide (CO2) exchange between the atmosphere and terrestrial ecosystems in various ways, such as a reduction of photosynthesis, changes in ecosystem respiration, or allowing more frequent fires. In this study, we characterize the resulting perturbation of the atmospheric CO2 seasonal cycles. 2018 has a good coverage of European regions affected by drought, allowing the investigation of how ecosystem flux anomalies impacted spatial CO2 gradients between stations. This density of stations is unprecedented compared to previous drought events in 2003 and 2015, particularly thanks to the deployment of the Integrated Carbon Observation System (ICOS) network of atmospheric greenhouse gas monitoring stations in recent years. Seasonal CO2 cycles from 48 European stations were available for 2017 and 2018.The UK sites were funded by the UK Department of Business, Energy and Industrial Strategy (formerly the Department of Energy and Climate Change) through contracts TRN1028/06/2015 and TRN1537/06/2018. The stations at the ClimaDat Network in Spain have received funding from the ‘la Caixa’ Foundation, under agreement 2010-002624

Mapping Urban Methane Sources in Paris, France

International audienceMegacities, with their large and complex infrastructures, are significant sources of methane emissions. To develop a simple, low-cost methodology to quantify these globally important methane sources, this study focuses on mobile measurements of methane (CH 4) and its isotopic composition in Paris. Data collected between September 2018 to March 2019 resulted in 17 days of measurements, which provided spatial distribution of street-level methane mixing ratios, source type identification, and emission quantification. Consequently, 90 potential leaks were detected in Paris sorted into three leak categories: natural gas distribution network emissions (63%), sewage network emissions (33%), and emissions from heating furnaces of buildings (4%). The latter category has not previously been reported in urban methane studies. Accounting for the detectable emissions from the ground, the total estimated CH 4 emission rate of Paris was 5000 L/min (190 t/yr), with the largest contribution from gas leaks (56%). This ranks Paris as a city with medium CH 4 emissions. Two areas of clusters were found, where 22% and 56% of the total potential emissions of Paris were observed. Our findings suggest that the natural gas distribution network, the sewage system, and furnaces of buildings are ideal targets for street-level CH 4 emission reduction efforts for Paris

Comparison of optical-feedback cavity-enhanced absorption spectroscopy and gas chromatography for ground-based and airborne measurements of atmospheric CO concentration

International audienceWe 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 ro-bustness 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 (< 1 ppb) and stability without any periodic calibration

Statistical atmospheric inversion of local gas emissions by coupling the tracer release technique and local-scale transport modelling: a test case with controlled methane emissions

International audienceThis study presents a new concept for estimating the pollutant emission rates of a site and its main facilities using a series of atmospheric measurements across the pollutant plumes. This concept combines the tracer release method, local-scale atmospheric transport modelling and a statistical atmospheric inversion approach. The conversion between the controlled emission and the measured atmospheric concentrations of the released tracer across the plume places valuable constraints on the atmospheric transport. This is used to optimise the configuration of the transport model parameters and the model uncertainty statistics in the inversion system. The emission rates of all sources are then inverted to optimise the match between the concentrations simulated with the transport model and the pollutants' measured atmospheric concentrations, accounting for the transport model uncertainty. In principle, by using atmospheric transport modelling, this concept does not strongly rely on the good colocation between the tracer and pollutant sources and can be used to monitor multiple sources within a single site, unlike the classical tracer release technique. The statistical inversion framework and the use of the tracer data for the configuration of the transport and inversion modelling systems should ensure that the transport modelling errors are correctly handled in the source estimation. The potential of this new concept is evaluated with a relatively simple practical implementation based on a Gaussian plume model and a series of inversions of controlled methane point sources using acetylene as a tracer gas. The experimental conditions are chosen so that they are suitable for the use of a Gaussian plume model to simulate the atmospheric transport. In these experiments, different configurations of methane and acetylene point source locations are tested to assess the efficiency of the method in comparison to the classic tracer release technique in coping with the distances between the different methane and acetylene sources. The results from these controlled experiments demonstrate that, when the targeted and tracer gases are not well collocated, this new approach provides a better estimate of the emission rates than the tracer release technique. As an example, the relative error between the estimated and actual emission rates is reduced from 32 % with the tracer release technique to 16 % with the combined approach in the case of a tracer located 60 m upwind of a single methane source. Further studies and more complex implementations with more advanced transport models and more advanced optimisations of their configuration will be required to generalise the applicability of the approach and strengthen its robustness

A top-down approach of sources and non-photosynthetic sinks of carbonyl sulfide from atmospheric measurements over multiple years in the Paris region (France)

International audienceCarbonyl sulfide (COS) has been proposed as a proxy for carbon dioxide (CO2) taken up by plants at the leaf and ecosystem scales. However, several additional production and removal processes have been identified which could complicate its use at larger scales, among which are soil uptake, dark uptake by plants, and soil and anthropogenic emissions. This study evaluates the significance of these processes at the regional scale through a top-down approach based on atmospheric COS measurements at Gif-sur-Yvette (GIF), a suburban site near Paris (France). Over a period of four and a half years, hourly measurements at 7 m above ground level were performed by gas chromatography and combined with 222Radon measurements to calculate nocturnal COS fluxes using the Radon-Tracer Method. In addition, the vertical distribution of COS was investigated at a second site, 2 km away from GIF, where a fast gas analyzer deployed on a 100 m tower for several months during winter 2015–2016 recorded mixing ratios at 3 heights (15, 60 and 100 m). COS appears to be homogeneously distributed both horizontally and vertically in the sampling area. The main finding is that the area is a persistent COS sink even during wintertime episodes of strong pollution. Nighttime net uptake rates ranged from -1.5 to -32.8 pmol m-2 s-1, with an average of -7.3 ± 4.5 pmol m-2 s-1 (n = 253). However, episodes of biogenic emissions happened each year in June-July (11.9 ± 6.2 pmol m-2 s-1, n = 24). Preliminary analyses of simulated footprints of source areas influencing the recorded COS data suggest that long-range transport of COS from anthropogenic sources located in Benelux, Eastern France and Germany occasionally impacts the Paris area during wintertime. These production and removal processes may limit the use of COS to assess regional-scale CO2 uptake in Europe by plants through inverse modeling

Carbonyl sulfide (COS) emissions in two agroecosystems in central France

International audienceCarbonyl sulfide (COS) fluxes simulated by vegetation and soil component models, both implemented in the ORCHIDEE land surface model, were evaluated against field observations at two agroecosystems in central France. The dynamics of a biogenic process not yet accounted for by this model, i.e., COS emissions from croplands, was examined in the context of three independent and complementary approaches. First, during the growing seasons of 2019 and 2020, monthly variations in the nighttime ratio of vertical mole fraction gradients of COS and carbon dioxide measured between 5 and 180 m height (Grad COS / Grad CO2), a proxy of the ratio of their respective nocturnal net fluxes, were monitored at a rural tall tower site near Orle ´ans (i.e., a "profile vs. model" approach). Second, field observations of COS nocturnal fluxes, obtained by the Radon Tracer Method (RTM) at a suburban site near Paris, were used for that same purpose (i.e., a "RTM vs. model" approach of unaccounted biogenic emissions). This site has observations going back to 2014. Third, during the growing seasons of 2019, 2020 and 2021, horizontal mole fraction gradients of COS were calculated from downwind-upwind surveys of wheat and rapeseed crops as a proxy of their respective exchange rates at the plot scale (i.e., a "crop based" comparative approach). The "profile vs. model" approach suggests that the nocturnal net COS uptake gradually weakens during the peak growing season and recovers from August on. The "RTM vs. model" approach suggests that there exists a biogenic source of COS, the intensity of which culminates in late June early July. Our "crop based" comparative approach demonstrates that rapeseed crops shift from COS uptake to emission in early summer during the late stages of growth (ripening and senescence) while wheat crops uptake capacities lower markedly. Hence, rapeseed appears to be a much larger source of COS than wheat at the plot scale. Nevertheless, compared to current estimates of the largest COS sources (i.e., marine and anthropogenic emissions), agricultural emissions during the late stages of growth are of secondary importance