Extending methane profiles from aircraft into the stratosphere for satellite total column validation using the ECMWF C-IFS and TOMCAT/SLIMCAT 3-D model
Abstract:Abstract. Airborne observations of greenhouse gases are a very useful reference for validation of satellite-based column-averaged dry air mole fraction data. However, since the aircraft data are available only up to about 9–13 km altitude, these profiles do not fully represent the depth of the atmosphere observed by satellites and therefore need to be extended synthetically into the stratosphere. In the near future, observations of CO2 and CH4 made from passenger aircraft are expected to be available through t… Show more
“…The first was filled on 7 June, at 9.2 km altitude, over Czechia, and second on 12 June, at 7.6 km, during the downward profile over the Po Valley. The potential source of these two observations might be worth investigating, especially in light of the constant atmospheric increase of the SF 6 , despite substantial efforts to curb emissions of this potent greenhouse gas (Weiss and Prinn, 2011). Some attention was also given to molecular hydrogen (H 2 ) due to its potential feedbacks to the atmosphere oxidative capacity and stratospheric ozone levels (see Batenburg et al, 2012, and references therein).…”
Abstract. The intensive measurement campaign CoMet 1.0 (Carbon Dioxide and Methane Mission) took place during May and June 2018, with a focus on greenhouse gases over Europe. CoMet 1.0 aimed at characterising the distribution of CH4 and CO2 over significant regional sources with the use of a fleet of research aircraft as well as validating remote sensing measurements from state-of-the-art instrumentation installed on board against a set of independent in situ observations. Here we present the results of over 55 h of accurate and precise in situ measurements of CO2, CH4 and CO mole fractions made during CoMet 1.0 flights with a cavity ring-down spectrometer aboard the German research aircraft HALO (High Altitude and LOng Range Research Aircraft), together with results from analyses of 96 discrete air samples collected aboard the same platform. A careful in-flight calibration strategy together with post-flight quality assessment made it possible to determine both the single-measurement precision as well as biases against respective World Meteorological Organization (WMO) scales. We compare the result of greenhouse gas observations against two of the available global modelling systems, namely Jena CarboScope and CAMS (Copernicus Atmosphere Monitoring Service). We find overall good agreement between the global models and the observed mole fractions in the free tropospheric range, characterised by very low bias values for the CAMS CH4 and the CarboScope CO2 products, with a mean free tropospheric offset of 0 (14) nmol mol−1 and 0.8 (1.3) µmol mol−1 respectively, with the numbers in parentheses giving the standard uncertainty in the final digits for the numerical value. Higher bias is observed for CAMS CO2 (equal to 3.7 (1.5) µmol mol−1), and for CO the model–observation mismatch is variable with height (with offset equal to −1.0 (8.8) nmol mol−1). We also present laboratory analyses of air samples collected throughout the flights, which include information on the isotopic composition of CH4, and we demonstrate the potential of simultaneously measuring δ13C−CH4 and δ2H−CH4 from air to determine the sources of enhanced methane signals using even a limited number of discrete samples. Using flasks collected during two flights over the Upper Silesian Coal Basin (USCB, southern Poland), one of the strongest methane-emitting regions in the European Union, we were able to use the Miller–Tans approach to derive the isotopic signature of the measured source, with values of δ2H equal to −224.7 (6.6) ‰ and δ13C to −50.9 (1.1) ‰, giving significantly lower δ2H values compared to previous studies in the area.
“…The first was filled on 7 June, at 9.2 km altitude, over Czechia, and second on 12 June, at 7.6 km, during the downward profile over the Po Valley. The potential source of these two observations might be worth investigating, especially in light of the constant atmospheric increase of the SF 6 , despite substantial efforts to curb emissions of this potent greenhouse gas (Weiss and Prinn, 2011). Some attention was also given to molecular hydrogen (H 2 ) due to its potential feedbacks to the atmosphere oxidative capacity and stratospheric ozone levels (see Batenburg et al, 2012, and references therein).…”
Abstract. The intensive measurement campaign CoMet 1.0 (Carbon Dioxide and Methane Mission) took place during May and June 2018, with a focus on greenhouse gases over Europe. CoMet 1.0 aimed at characterising the distribution of CH4 and CO2 over significant regional sources with the use of a fleet of research aircraft as well as validating remote sensing measurements from state-of-the-art instrumentation installed on board against a set of independent in situ observations. Here we present the results of over 55 h of accurate and precise in situ measurements of CO2, CH4 and CO mole fractions made during CoMet 1.0 flights with a cavity ring-down spectrometer aboard the German research aircraft HALO (High Altitude and LOng Range Research Aircraft), together with results from analyses of 96 discrete air samples collected aboard the same platform. A careful in-flight calibration strategy together with post-flight quality assessment made it possible to determine both the single-measurement precision as well as biases against respective World Meteorological Organization (WMO) scales. We compare the result of greenhouse gas observations against two of the available global modelling systems, namely Jena CarboScope and CAMS (Copernicus Atmosphere Monitoring Service). We find overall good agreement between the global models and the observed mole fractions in the free tropospheric range, characterised by very low bias values for the CAMS CH4 and the CarboScope CO2 products, with a mean free tropospheric offset of 0 (14) nmol mol−1 and 0.8 (1.3) µmol mol−1 respectively, with the numbers in parentheses giving the standard uncertainty in the final digits for the numerical value. Higher bias is observed for CAMS CO2 (equal to 3.7 (1.5) µmol mol−1), and for CO the model–observation mismatch is variable with height (with offset equal to −1.0 (8.8) nmol mol−1). We also present laboratory analyses of air samples collected throughout the flights, which include information on the isotopic composition of CH4, and we demonstrate the potential of simultaneously measuring δ13C−CH4 and δ2H−CH4 from air to determine the sources of enhanced methane signals using even a limited number of discrete samples. Using flasks collected during two flights over the Upper Silesian Coal Basin (USCB, southern Poland), one of the strongest methane-emitting regions in the European Union, we were able to use the Miller–Tans approach to derive the isotopic signature of the measured source, with values of δ2H equal to −224.7 (6.6) ‰ and δ13C to −50.9 (1.1) ‰, giving significantly lower δ2H values compared to previous studies in the area.
“…Long-range transport in the free troposphere and upper troposphere/lower stratosphere also plays an important role, as depicted by the green/orange bars with higher r 2 values than the near-surface layers in purple/red. The dataset can also be used to assess the important contribution of the stratosphere in the variability of XCH 4 45 . Fig.…”
The CO2 Human Emissions project has generated realistic high-resolution 9 km global simulations for atmospheric carbon tracers referred to as nature runs to foster carbon-cycle research applications with current and planned satellite missions, as well as the surge of in situ observations. Realistic atmospheric CO2, CH4 and CO fields can provide a reference for assessing the impact of proposed designs of new satellites and in situ networks and to study atmospheric variability of the tracers modulated by the weather. The simulations spanning 2015 are based on the Copernicus Atmosphere Monitoring Service forecasts at the European Centre for Medium Range Weather Forecasts, with improvements in various model components and input data such as anthropogenic emissions, in preparation of a CO2 Monitoring and Verification Support system. The relative contribution of different emissions and natural fluxes towards observed atmospheric variability is diagnosed by additional tagged tracers in the simulations. The evaluation of such high-resolution model simulations can be used to identify model deficiencies and guide further model improvements.
“…While the number of observations at these higher altitudes is relatively low compared to those below 10 km, we believe that these differences are also caused by errors in both transport and chemistry schemes in the IFS system. These have been investigated in some detail in the case of CH 4 , for which the errors in the stratosphere have been found to be larger than those observed in the troposphere (Verma et al, 2017).…”
Abstract. The intensive measurement campaign CoMet 1.0 (Carbon dioxide and Methane mission) took place during May and June 2018, with a focus on greenhouse gases over Europe. CoMet 1.0 aimed at characterising the distribution of CH4 and CO2 over significant regional sources with the use of a fleet of research aircraft, as well as validating remote sensing measurements from state-of-the-art instrumentation installed on-board against a set of independent in-situ observations. Here we present the results of over 55 hours of accurate and precise in situ measurements of CO2, CH4 and CO mixing ratios made during CoMet 1.0 flights with a cavity ring-down spectrometer aboard the German research aircraft HALO, together with results from analyses of 96 discrete air samples collected aboard the same platform. A careful in-flight calibration strategy together with post-flight quality assessment made it possible to determine both the single measurement precision as well as biases against respective WMO scales. We compare the result of greenhouse gas observations against two of the available global modelling systems, namely Jena CarboScope and CAMS (Copernicus Atmosphere Monitoring Service). We find overall good agreement between the global models and the observed mixing ratios in the free-tropospheric range, characterised by very low bias values for the CAMS CH4 and the CarboScope CO2 products, with a mean free tropospheric offset of 0 (14) ppb and 0.8 (1.3) ppm respectively, with the quoted number giving the standard uncertainty in the final digits for the numerical value. Higher bias is observed for CAMS CO2 (equal to 3.7 (1.5) ppm), and for CO the model-observation mismatch is variable with height (with offset equal to −1.0 (8.8)). We also present laboratory analyses of air samples collected throughout the flights, which include information on the isotopic composition of CH_4, and we demonstrate the potential of simultaneously measuring δ13C-CH4 and δ2H-CH4 from air to determine the sources of enhanced methane signals using even a limited amount of discrete samples. Using flasks collected during two flights over the Upper Silesian Coal Basin (USCB, southern Poland), one of the strongest methane-emitting regions in the European Union, we were able to use the Miller-Tans approach to derive the isotopic signature of the measured source, with values of δ2H equal to −224.7 (6.6) permil and δ13C to −50.9 (1.1) permil, giving significantly lower d2H values compared to previous studies in the area.
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