European Emissions of Halogenated Greenhouse Gases Inferred from Atmospheric Measurements

2011 ◽  
Vol 46 (1) ◽  
pp. 217-225 ◽  
Author(s):  
Christoph A. Keller ◽  
Matthias Hill ◽  
Martin K. Vollmer ◽  
Stephan Henne ◽  
Dominik Brunner ◽  
...  
2020 ◽  
Author(s):  
Morten Hundt ◽  
Oleg Aseev ◽  
Herbert Looser

<p>Observation of air pollutants and greenhouse gases with high selectivity and sensitivity is of great importance for our understanding of their sources and sinks. For air pollution modelling and validation of emission inventories measurements at various spatial and temporal scales are required. Infrared laser absorption spectroscopy is often the method of choice, offering outstanding performance and reliability. Most frequently, however, this technology is used in a “one-species-one-instrument” solution because of the narrow spectral coverage of DFB-lasers. This can be overcome by combining several Quantum Cascade Lasers (QCLs), providing unique solutions in compact laser absorption spectrometers for environmental monitoring of multiple species in a single instrument.</p><p>We combined multiple DFB-QCLs into a single, compact laser absorption spectrometer to measure up to ten different compounds. We present simultaneous atmospheric measurements of the greenhouse gases CO<sub>2</sub>, N<sub>2</sub>O, H<sub>2</sub>O and CH<sub>4</sub>, and the pollutants CO, NO, NO<sub>2</sub>, O<sub>3</sub>, SO<sub>2</sub> and NH<sub>3</sub> with a single instrument. Furthermore, the instrument performance, first field results and comparison to standard air-quality and greenhouse gas monitoring instrumentation are discussed. The results demonstrate that spectrometers using QCLs can serve as an all-in-one solution for environmental monitoring stations replacing up to seven instruments at once. Furthermore, due to their reduced size and robustness, they can be used on mobile platforms, opening up new applications of air quality and greenhouse gas monitoring in cities.</p>


2010 ◽  
Vol 10 (6) ◽  
pp. 2655-2662 ◽  
Author(s):  
I. Levin ◽  
T. Naegler ◽  
R. Heinz ◽  
D. Osusko ◽  
E. Cuevas ◽  
...  

Abstract. Emissions of sulphur hexafluoride (SF6), one of the strongest greenhouse gases on a per molecule basis, are targeted to be collectively reduced under the Kyoto Protocol. Because of its long atmospheric lifetime (estimated as 800 to 3200 years), the accumulation of SF6 in the atmosphere is a direct measure of its global emissions. Examination of our extended data set of globally distributed high-precision SF6 observations shows an increase in SF6 abundance from near zero in the 1970s to a global mean of 6.7 ppt by the end of 2008. In-depth evaluation of our long-term data records shows that the global source of SF6 decreased after 1995, most likely due to SF6 emission reductions in industrialised countries, but increased again after 1998. By subtracting those emissions reported by Annex I countries to the United Nations Framework Convention of Climatic Change (UNFCCC) from our observation-inferred SF6 source leaves a surprisingly large gap of more than 70–80% of non-reported SF6 emissions in the last decade. This suggests a strong under-estimation of emissions in Annex I countries and underlines the urgent need for independent atmospheric verification of greenhouse gases emissions accounting.


Metrologiya ◽  
2020 ◽  
pp. 19-30 ◽  
Author(s):  
Natig H. Djavadov ◽  
Hikmat H. Asadov ◽  
Reyhana V. Kazimli

To increase effectiveness of measurements of concentration of greenhouse gases questions on optimum accounting of non-certainty of results of measurements of low gases concentrations at the ground distributed nets of atmospheric measurements are considered. It is noted that temporal and structural non-stability of atmospheric aerosol leads to occurrence of non-certainty of carried out measurements. It is suggested to use the method of non-conditional variation optimization to determine the optimum interrelation between cost functions of researched atmospheric gas and aerosol which provides best metrological support for carried out measurements. In order to form the functional of optimization the newly suggested method of double averaging is used. The matter of suggested method of double averaging is that two following different averaging operations should be carried out sequentially: geometrical weighted averaging and algebraic averaging. To form the target functional of optimization the limitation condition should be adopted which is imposed to searched for optimum function. Solution of the formulated optimization task of non-conditional variation optimization does show that upon presence of linear interrelation between scalar cost functions of gas and aerosol the target functional could reach its maximum that is the uttermost value of non-certainty of measurements results are reached. On the base of aforesaid the heuristically recommendations on necessity to form the inverse interrelation between scalar values of cost functions of researched gas and atmospheric aerosol are formulated.


2021 ◽  
Author(s):  
Dominique Rust ◽  
Martin K. Vollmer ◽  
Ioannis Katharopoulos ◽  
Stephan Henne ◽  
Matthias Hill ◽  
...  

<p>Synthetic halocarbons reach the atmosphere due to a wide range of anthropogenic activities. They are, for example, used as propellants in foam blowing or as cooling agents in refrigeration and air conditioning. Long-lived halocarbons act as strong greenhouse gases. They are responsible for about 11% of the radiative forcing by long-lived greenhouse gases (LLGHGs). In addition, chlorinated or brominated halocarbons contribute to stratospheric ozone depletion. There are only two in situ long-term measurement programs, operated by the Advanced Global Atmospheric Gases Experiment (AGAGE) and the National Oceanic and Atmospheric Administration (NOAA) that monitor the worldwide abundance of halocarbons in the atmosphere. Based on these observations, halocarbon emissions are estimated by top-down box- or inverse modelling approaches on a global to transnational scale. However, to capture regional pollution sources and to validate country-specific bottom-up emission estimates by top-down methods, additional regional-scale measurements are required.</p><p>We present the first continuous halocarbon measurements at the Beromünster tall tower, representing the most industrialized and densely populated area of Switzerland, the Swiss Plateau. During one year, high precision, high accuracy atmospheric measurements were performed with the analytical setup of the global AGAGE network. This involves sample pre-concentration at low temperatures (down to -180 <sup>o</sup>C), and analyte separation and detection by gas chromatography and quadrupole mass spectrometry. All halocarbon compound classes of the Montreal and Kyoto Protocols are covered by our measurements. This includes the banned chlorofluorocarbons (CFCs) and halons, the regulated hydrochlorofluorocarbons (HCFCs), hydrofluorocarbons (HFCs) and perfluorocarbons (PFCs), as well as the recently introduced unregulated hydrochfluoroolefins (HFOs). The results improve our understanding of important source areas in Switzerland, and, for the first time offer the possibility to robustly quantify Swiss national halocarbon emissions with observation-based top-down methods, i.e. the tracer ratio method and Bayesian inverse modeling.</p>


2019 ◽  
Author(s):  
Lilian Joly ◽  
Olivier Coopmann ◽  
Vincent Guidard ◽  
Thomas Decarpenterie ◽  
Nicolas Dumelié ◽  
...  

Abstract. We report in this paper the development of an embedded ultralight spectrometer (< 3 kg) based on tuneable diode laser absorption spectroscopy (with a sampling rate of 24 Hz) in the mid-infrared spectral region. This instrument is dedicated to in-situ measurements of the vertical profile concentrations of three main greenhouse gases: carbon dioxide (CO2), methane (CH4) and water vapour (H2O) under weather and tethered balloons. The plug and play instrument is compact, robust and cost-effective, autonomous, having a low power consumption, a non-intrusive probe. It was first calibrated during an in situ campaign on an ICOS (Integrated Carbon Observation System) site for several days, then used in a tethered balloon campaign and for a balloon campaign several balloon flights up to 30 km altitude in the Reims-France in 2017–2018 in collaboration with Météo-France/CNRM. This paper shows the valuable interest of the data measured by AMULSE instrument during the APOGEE measurement campaign, specifically for the vertical profiles of CO2 and CH4, which remain very sparse. We have carried out several experiments showing that the measured profiles have several applications: for the validation of simulations of infrared satellite observations, for evaluating the quality of chemical profiles from Chemistry Transport Models (CTM) and for evaluating the quality of retrieved chemical profiles from the assimilation of infrared satellite observations. The results show that the simulations of infrared satellite observations from IASI and CrIS instruments performed in operational mode for NWP by the Radiative Transfer Model (RTM) RTTOV are of good quality. We also show that the MOCAGE and CAMS CTMs modeled ozone profiles fairly accurately and that the CAMS CTM represents the methane in the troposphere well compared to MOCAGE. Finally, the measured in situ ozone profiles allowed us to show the good quality of the retrieved ozone profiles by assimilating ozone-sensitive infrared spectral radiances from IASI and CrIS.


2020 ◽  
Author(s):  
El Kattar Marie-Thérèse ◽  
Auriol Frédérique ◽  
Herbin Hervé

&lt;p&gt;Ground-based high spectral resolution infrared measurements are considered to be the most efficient way to obtain accurate tropospheric abundances of different gaseous species and in particular greenhouse gases, such as CO&lt;sub&gt;2&lt;/sub&gt; and CH&lt;sub&gt;4&lt;/sub&gt;. Furthermore, this type of measurement is also commonly used to validate the satellite retrievals. Despite the outstanding capabilities of the spectrometers used by the TCCON and NDACC networks, they are inadequate for field campaigns; therefore, more compact and stable spectrometers have been developed. &lt;strong&gt;CHRIS&lt;/strong&gt; (&lt;strong&gt;C&lt;/strong&gt;ompact &lt;strong&gt;H&lt;/strong&gt;igh &lt;strong&gt;S&lt;/strong&gt;pectral &lt;strong&gt;R&lt;/strong&gt;esolution &lt;strong&gt;I&lt;/strong&gt;nfrared &lt;strong&gt;S&lt;/strong&gt;pectrometer) is a new prototype based on the EM27-SUN from Bruker, with unique characteristics such as its high spectral resolution (0.135 cm&lt;sup&gt;-1&lt;/sup&gt; non-apodized) with a spectral sampling every 0.065 cm&lt;sup&gt;-1&lt;/sup&gt; to satisfy the Nyquist criterion. This optically stable instrument allows recording solar transmission light spectra in a wide spectral range (680 to 5200 cm&lt;sup&gt;-1&lt;/sup&gt;) with a relatively high SNR (~780 in average).&lt;/p&gt;&lt;p&gt;&amp;#160;&lt;/p&gt;&lt;p&gt;&amp;#160;&amp;#160;&amp;#160;&amp;#160;&amp;#160;&amp;#160;&amp;#160;&amp;#160;&amp;#160;&amp;#160;&amp;#160; This instrumental prototype is designed to perform measurements of greenhouse gases (CO&lt;sub&gt;2&lt;/sub&gt;, CH&lt;sub&gt;4&lt;/sub&gt; and H&lt;sub&gt;2&lt;/sub&gt;O), trace gases (SO&lt;sub&gt;2&lt;/sub&gt;, CO, HCl, NO&lt;sub&gt;x&lt;/sub&gt;&amp;#8230;) but also aerosols and clouds that have very typical spectral features in particular in the thermal infrared region. The main objective of this study is the accurate retrieval of tropospheric abundances of the greenhouse gases, CO&lt;sub&gt;2&lt;/sub&gt; and CH&lt;sub&gt;4&lt;/sub&gt;, in the TIR/SWIR regions, and study the synergy between them especially for the MAGIC campaign. CHRIS is a part of this ongoing campaign in an attempt to monitor the GHG and validate the actual space missions like IASI, OCO-2, GOSAT-2 and future space missions like Merlin, MicroCarb and IASI-NG.&lt;/p&gt;&lt;p&gt;&amp;#160;&lt;/p&gt;&lt;p&gt;&amp;#160;&amp;#160;&amp;#160;&amp;#160;&amp;#160;&amp;#160;&amp;#160;&amp;#160;&amp;#160;&amp;#160;&amp;#160; Here, the spectral and radiometric characterization of this instrument is briefly explained. Furthermore, we present CHRIS&amp;#8217;s capabilities to measure CO&lt;sub&gt;2&lt;/sub&gt; and CH&lt;sub&gt;4&lt;/sub&gt; vertical profiles through a complete information content analysis, a channel selection and an error budget estimation. The preliminary results of the retrieval of these gases using the radiative transfer model ARAHMIS developed at the LOA is also presented. CHRIS is also part of other campaigns such as ImagEtna and Shadow-2 to study the trace gases and aerosols respectively.&lt;/p&gt;


2020 ◽  
Vol 13 (6) ◽  
pp. 3099-3118
Author(s):  
Lilian Joly ◽  
Olivier Coopmann ◽  
Vincent Guidard ◽  
Thomas Decarpenterie ◽  
Nicolas Dumelié ◽  
...  

Abstract. We report in this paper the development of an embedded ultralight spectrometer (<3 kg) based on tuneable diode laser absorption spectroscopy (with a sampling rate of 24 Hz) in the mid-infrared spectral region. This instrument is dedicated to in situ measurements of the vertical profile concentrations of three main greenhouse gases – carbon dioxide (CO2), methane (CH4) and water vapour (H2O) – via standard weather and tethered balloons. The plug and play instrument is compact, robust, cost-effective, and autonomous. The instrument also has low power consumption and is non-intrusive. It was first calibrated during an in situ experiment on an ICOS (Integrated Carbon Observation System) site for several days, then used in two experiments with several balloon flights of up to 30 km altitude in the Reims region of France in 2017–2018 in collaboration with Météo-France CNRM (Centre National de Recherches Météorologiques). This paper shows the valuable interest of the data measured by the AMULSE (Atmospheric Measurements by Ultra-Light Spectrometer) instrument during the APOGEE (Atmospheric Profiles of Greenhouse Gases) measurement experiment, specifically for the vertical profiles of CO2 and CH4, measurements of which remain very sparse. We have carried out several experiments showing that the measured profiles have several applications: the validation of simulations of infrared satellite observations, evaluating the quality of chemical profiles from chemistry transport models (CTMs) and evaluating the quality of retrieved chemical profiles from the assimilation of infrared satellite observations. The results show that the simulations of infrared satellite observations from IASI (Infrared Atmospheric Sounding Interferometer) and CrIS (Cross-track Infrared Sounder) instruments performed in operational mode for numerical weather prediction (NWP) by the radiative transfer model (RTM) RTTOV (Radiative Transfer for the TIROS Operational Vertical Sounder) are of good quality. We also show that the MOCAGE (Modèle de Chimie Atmosphérique de Grande Echelle) and CAMS (Copernicus Atmospheric Monitoring Service) CTMs modelled ozone profiles fairly accurately and that the CAMS CTM represents the methane in the troposphere well compared to MOCAGE. Finally, the measured in situ ozone profiles allowed us to show the good quality of the retrieved ozone profiles by assimilating ozone-sensitive infrared spectral radiances from the IASI and CrIS.


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