H216O and HDO measurements with IASI/MetOp

International audienceIn this paper we analyze distributions of water vapour isotopologues in the troposphere using infrared spectra recorded by the Infrared Atmospheric Sounding Interferometer (IASI), which operates onboard the Metop satellite in nadir geometry. The simultaneous uncorrelated retrievals of H216O and HDO are performed on radiance measurements using a line-by-line radiative transfer model and an inversion procedure based on the Optimal Estimation Method (OEM). The characterizations of the retrieved products in terms of vertical sensitivity and error budgets show that IASI measurements contain up to 6 independent pieces of information on the vertical distribution of H216O and up to 3.5 for HDO from the surface up to the upper troposphere (0–20 km). Although the purpose of the paper is not validation, a restricted comparison with sonde measurements shows that the retrieved H216O profiles capture the seasonal/latitudinal variations of the water content, with good accuracy in the lowest layer but with larger uncertainties higher in the free and upper troposphere. Our results then demonstrate the ability of the IASI instrument to monitor atmospheric isotopologic water vapour distributions and to provide information on the partitioning of HDO as compared to H216O. The derivation of the δD is challenging and associated with large errors in the uncorrelated retrieval approach chosen here. As a result averaging on the vertical to produce a column-averaged δD is required to produce meaningful results for geophysical interpretation. As a case study, we analyse concentration distributions and spatio-temporal variations of H216O and δD during the October 2007 Krosa super-typhoon over South-East Asia. We show that individual δD have uncertainties of 37‰ for the vertically averaged values. Using the latter, we suggest that the typhoon produces a so-called amount-effect, where the δD is negatively correlated to the water amounts as a result of intense depletion of the deuterated species

Tracking the emission and transport of pollution from wildfires using the IASI CO retrievals: analysis of the summer 2007 Greek fires

International audienceIn this paper, we analyze the performance of the Infrared Atmospheric Sounding Interferometer (IASI), launched in October 2006 on board METOP-A, for the monitoring of carbon monoxide (CO) during extreme fire events, focusing on the record-breaking fires which devastated thousands of square kilometers of forest in Greece during the last week (23–30) of August 2007. After an assessment of the quality of the profiles retrieved using the Fast Optimal Retrievals on Layers for IASI (FORLI) algorithm, the information provided on fire emissions and subsequent pollution outflow is discussed. Large CO plumes were observed above the Mediterranean Basin and North Africa, with total CO columns exceeding 24×1018 molecules/cm2 and absolute volume mixing ratios up to 4 ppmv on the 25 August. Up to 30×1018 molecules/cm2 and 22 ppmv in the lower troposphere are retrieved close to the fires above the Peloponnese, but with larger uncertainty. The average root-mean-square (RMS) difference between simulated and observed spectra is close to the estimated radiometric noise level, slightly increasing (by ~14%) in the fresh fire plumes. CO profiles are retrieved with a vertical resolution of about 8 km, with ~1.7 pieces of independent information on the vertical in the region considered and a maximum sensitivity in the free troposphere (~4–5 km). Using the integrated total amount, the increase in CO burden due to these fires is estimated to 0.321 Tg, ~40% of the total annual anthropogenic emissions in Greece. The patterns of these CO enhancements are in good agreement with the aerosol optical depth (AOD) retrieved from the MODIS measurements, highlighting a rapid transport of trace gases and aerosols across the Mediterranean Basin (less than one day). While the coarse vertical resolution will not allow the location of the exact plume height, the large CO enhancements observed in the lower troposphere are consistent with the maximum aerosol backscatter coefficient at ~2 km detected by the CALIPSO lidar in space (CALIOP)

Constraining industrial ammonia emissions using hyperspectral infrared imaging

Atmospheric emissions of reactive nitrogen in the form of nitrogen dioxide (NO) and ammonia (NH) worsen air quality and upon deposition, dramatically affect the environment. Recent infrared satellite measurements have revealed that NH emitted by industries are an important and underestimated emission source. Yet, to assess these emissions, current satellite sounders are severely limited by their spatial resolution. In this paper, we analyse measurement data recorded in a series of imaging surveys that were conducted over industries in the Greater Berlin area (Germany). On board the aircraft were the Telops Hyper-Cam LW, targeting NH measurements in the longwave infrared at a resolution of 4 m and the SWING+ spectrometer targeting NO measurements in the UV–Vis at a resolution of 180 m. Two flights were carried out over German’s largest production facility of synthetic NH , urea and other fertilizers. In both cases, a large NH plume was observed originating from the factory. Using a Gaussian plume model to take into account plume rise and dispersion, coupled with well-established radiative transfer and inverse methods, we retrieve vertical column densities. From these, we calculate NH emission fluxes using the integrated mass enhancement and cross-sectional flux methods, yielding consistent emissions of the order of 2200 t yr−1 for both flights, assuming constant fluxes across the year. These estimates are about five times larger than those reported in the European Pollutant Release and Transfer Register (E-PRTR) for this plant. In the second campaign, a co-emitted NO plume was measured, likely related to the production of nitric acid at the plant. A third flight was carried out over an area comprising the cities of Staßfurt and Bernburg. Several small NH plumes were seen, one over a production facility of mineral wool insulation, one over a sugar factory and two over the soda ash plants in Staßfurt and Bernburg. A fifth and much larger plume was seen to originate from the sedimentation basins associated with the soda ash plant in Staßfurt, indicating rapid volatilization of ammonium rich effluents. We use the different measurement campaigns to simulate measurements of Nitrosat, a potential future satellite sounder dedicated to the sounding of reactive nitrogen at a resolution of 500 m. We demonstrate that such measurements would allow accurately constraining emissions in a single overpass, overcoming a number of important drawbacks of current satellite sounders

Cross-validation of IASI/MetOp derived tropospheric δD with TES and ground-based FTIR observations

International audienceThe Infrared Atmospheric Sounding Interferometer (IASI) flying on-board MetOpA and MetOpB is able to capture fine isotopic variations of the HDO to H2O ratio (δD) in the troposphere. Such observations at the high spatio temporal resolution of the sounder are of great interest to improve our understanding of the mechanisms controlling humidity in the troposphere. In this study we aim to empirically assess the validity of our error estimation previously evaluated theoretically. To achieve this, we compare IASI δD retrieved profiles with other available profiles of δD, from the TES infrared sounder onboard AURA and from three ground-based FTIR stations produced within the MUSICA project: the NDACC (Network for the Detection of Atmospheric Composition Change) sites Kiruna and Izana, and the TCCON site Karlsruhe, which in addition to near-infrared TCCON spectra also records mid-infrared spectra. We describe the achievable level of agreement between the different retrievals and show that these theoretical errors are in good agreement with empirical differences. The comparisons are made at different locations from tropical to Arctic latitudes, above sea and above land. Generally IASI and TES are similarly sensitive to δD in the free troposphere which allows to compare their measurements directly. At tropical latitudes where IASI's sensitivity is lower than that of TES, we show that the agreement improves when taking into account the sensitivity of IASI in the TES retrieval. For the comparison IASI-FTIR only direct comparisons are performed because of similar sensitivities. We identify a quasi negligible bias in the free troposphere (−3‰) between IASI retrieved δD with the TES one, which are bias corrected, but an important with the ground-based FTIR reaching −47‰. We also suggest that model-satellite observations comparisons could be optimized with IASI thanks to its high spatial and temporal sampling

NH3 spatiotemporal variability over Paris, Mexico City, and Toronto, and its link to PM2.5 during pollution events

Megacities can experience high levels of fine particulate matter (PM2.5) pollution linked to ammonia (NH3) mainly emitted from agricultural activities. Here, we investigate such pollution in the cities of Paris, Mexico, and Toronto, each of which have distinct emission sources, agricultural regulations, and topography. Ten years of measurements from the infrared atmospheric sounding interferometer (IASI) are used to assess the spatiotemporal NH3 variability over and around the three cities. In Europe and North America, we determine that temperature is associated with the increase in NH3 atmospheric concentrations with a coefficient of determination (r2) of 0.8 over agricultural areas. The variety of the NH3 sources (industry and agricultural) and the weaker temperature seasonal cycle in southern North America induce a lower correlation factor (r2=0.5). The three regions are subject to long-range transport of NH3, as shown using HYSPLIT cluster back trajectories. The highest NH3 concentrations measured at the city scale are associated with air masses coming from the surrounding and north/northeast regions of Paris, the south/southwest areas of Toronto, and the southeast/southwest zones of Mexico City. Using NH3 and PM2.5 measurements derived from IASI and surface observations from 2008 to 2017, annually frequent pollution events are identified in the three cities. Wind roses reveal statistical patterns during these pollution events with dominant northeast/southwest directions in Paris and Mexico City, and the transboundary transport of pollutants from the United States in Toronto. To check how well chemistry transport models perform during pollution events, we evaluate simulations made using the GEOS-Chem model for March 2011. In these simulations we find that NH3 concentrations are underestimated overall, though day-to-day variability is well represented. PM2.5 is generally underestimated over Paris and Mexico City, but overestimated over Toronto.</p

An examination of the long-term CO records from MOPITT and IASI: comparison of retrieval methodology

International audienceCarbon monoxide (CO) is a key atmospheric compound that can be remotely sensed by satellite on the global scale. Fifteen years of continuous observations are now available from the MOPITT/Terra mission (2000 to present). Another fifteen and more years of observations will be provided by the IASI/MetOp instrument series (2007–2023>). In order to study long term variability and trends, a homogeneous record is required, which is not straightforward as the retrieved products are instrument and processing dependent. The present study aims at evaluating the consistency between the CO products derived from the MOPITT and IASI missions, both for total columns and vertical profiles, during a six year overlap period (2008–2013). The analysis is performed by first comparing the available 2013 versions of the retrieval algorithms, and second using a dedicated reprocessing of MOPITT CO profiles and columns based on the IASI a priori constraints. MOPITT v5T total columns are generally slightly higher over land (bias ranging from 0 to 13%) than IASI v20100815 data. When IASI and MOPITT data are retrieved with the same a priori constraints, correlation coefficients are slightly improved. Large discrepancies (total column bias over 15%) observed in the Northern Hemisphere during the winter months are reduced by a factor of 2 to 2.5. The detailed analysis of retrieved vertical profiles compared with collocated aircraft data from the MOZAIC-IAGOS network, illustrates the advantages and disadvantages of a constant vs. a variable a priori. On one hand, MOPITT agrees better with the aircraft profiles for observations with persisting high levels of CO throughout the year due to pollution or seasonal fire activity (because the climatology-based a priori is supposed to be closer to the real atmospheric state). On the other hand, IASI performs better when unexpected events leading to high levels of CO occur, due to the less constrained variance-covariance matrix

Towards IASI-New Generation (IASI-NG): impact of improved spectral resolution and radiometric noise on the retrieval of thermodynamic, chemistry and climate variables

Besides their strong contribution to weather forecast improvement through data assimilation, thermal infrared sounders onboard polar-orbiting platforms are now playing a key role for monitoring atmospheric composition changes. The Infrared Atmospheric Sounding Interferometer (IASI) instrument developed by the French space agency (CNES) and launched by Eumetsat onboard the Metop satellite series is providing essential inputs for weather forecasting and pollution/climate monitoring owing to its smart combination of large horizontal swath, good spectral resolution and high radiometric performance. EUMETSAT is currently preparing the next polar-orbiting program (EPS-SG) with the Metop-SG satellite series that should be launched around 2020. In this framework, CNES is studying the concept of a new instrument, the IASI-New Generation (IASI-NG), characterized by an improvement of both spectral and radiometric characteristics as compared to IASI, with three objectives: (i) continuity of the IASI/Metop series; (ii) improvement of vertical resolution; (iii) improvement of the accuracy and detection threshold for atmospheric and surface components. In this paper, we show that an improvement of spectral resolution and radiometric noise fulfill these objectives by leading to (i) a better vertical coverage in the lower part of the troposphere, thanks to the increase in spectral resolution; (ii) an increase in the accuracy of the retrieval of several thermodynamic, climate and chemistry variables, thanks to the improved signal-to-noise ratio as well as less interferences between the signatures of the absorbing species in the measured radiances. The detection limit of several atmospheric species is also improved. We conclude that IASI-NG has the potential for strongly benefiting the numerical weather prediction, chemistry and climate communities now connected through the European GMES/Copernicus initiative

Advanced exploitation of Ground-Based measurements for Atmospheric Chemistry and Climate Applications "AGACC"

We live in an era in which human activities are causing significant changes to the atmospheric environment which result in local to global consequences on the ecosystems. Changes in the atmospheric composition impact our climate via chemical and dynamical feedback mechanisms; in many instances they also affect air quality, and the health of the biosphere. Monitoring and understanding those changes and their consequences is fundamental to establish adequate actions for adaptation to and mitigation of the environmental changes. Furthermore, after implementation of regulatory measures like the Montreal Protocol, it is necessary to verify whether the measures are effective. This can only be achieved if we have adequate detection methods and a reliable long record of a series of key geophysical parameters. Thus the AGACC project contributes to the provision of basic new knowledge regarding the atmospheric composition and its changes, based on advanced groundbased monitoring, in combination with satellite and numerical modelling data. Its results are integrated in ongoing international research programmes. The general objective of AGACC has been to improve and extend the groundbased detection capabilities for a number of climate-related target species and, based hereupon, analyse past and present observations to derive new information about the atmospheric composition, its variability and long-term changes. Despite the advent of a growing and more performant fleet of Earth Observation satellites, ground-based observations are still indispensable to (1) guarantee long-term continuity, homogeneity and high quality of the data, and (2) to underpin the satellite data for calibration and (long-term) validation. A first target gas is atmospheric water vapour. It is the key trace gas controlling weather and climate. It is also the most important greenhouse gas in the Earth’s atmosphere. Its amount and vertical distribution are changing, but how and why? Especially in the upper troposphere - lower stratosphere, the radiative effects of changes in the water vapour are significant and should be quantified. The measurement of water vapour is a hot topic since several years. It is a challenge, because water vapour exhibits a large gradient in its concentration when going from the ground to the stratosphere, and because it is highly variable in time and space. For example, we have found that the time scale of the variations of the total water vapour amount at Jungfraujoch is in the order of minutes. In AGACC, we have therefore investigated various experimental techniques to measure the concentration of water vapour in the atmosphere, focusing on the total column as well as on the vertical distribution in the troposphere up to the lower stratosphere. The retrieval of water vapour vertical profiles and total columns from ground-based FTIR data has been initiated at three very different stations where correlative data for verification are available, namely Ukkel (± sea level, mid-latitude), Ile de La Réunion (± sea level, tropical) and Jungfraujoch (high altitude, mid-latitude), with promising results. In particular, at Jungfraujoch, it has been demonstrated that the precision of the FTIR integrated water vapour (IWV) measurements is of order 2%. The capability to retrieve individual isotopologues of water vapour, and to monitor their daily and diurnal variations, has also been demonstrated. This could open new ways to study in the future the role of water vapour in the radiative balance, the global circulation, precipitation etc. We also started joint exploitation of ground-based FTIR and satellite IASI data for water vapour and its isotopologues, in order to exploit fully the potential of the existing instrumentation. A correction method for the radiosoundings at Ukkel has been successfully implemented, resulting in a homogeneous and reliable time series from 1990 to 2008 from which trends in upper troposphere humidity (UTH) and tropopause characteristics have been derived. One observes a rising UTH until September 2001, followed by a decline, accompanied by a descent and heating of the tropopause up to the turning point and an ascent and cooling afterwards. The changes after September 2001 in the upper troposphere can be explained by surface heating and convective uplift. At Jungfraujoch, one does not observe any significant trend in the total water vapour abundance above the station over the 1988-2010 time period, although significant positive summer and negative winter trends have been detected. We have made a quantitative statistical comparison between ground-based FTIR, CIMEL, GPS and integrated (corrected) radio sounding measurements of the IWV at Ukkel. This work is important to better characterize the different sensors in order to exploit together different observations made by different instruments. A second target species is atmospheric aerosol. There is a very large variety of aerosol both from natural or anthropogenic origin. One of the reasons why they are so important is that they affect the optical properties of the atmosphere. In particular, it has been demonstrated in previous studies that the aerosols have a large impact on the quantity of harmful UV-B radiation received at the Earth’s surface. The latest IPCC Report also stressed that the radiative forcing caused by atmospheric aerosols is one of the largest uncertainties in determining the total radiative forcing in the atmosphere. Better monitoring capabilities of aerosol properties can therefore improve our understanding and forecasting of the atmospheric processes and evolution, and in particular of UV-B and climate changes. Several measurement techniques are now operational in the AGACC consortium for the ground-based monitoring of aerosol properties. These are the Brewer spectrometer and CIMEL observations at Ukkel, the latter contributing also to the AERONET network since July 2006, and the newly developed MAXDOAS observations. Unlike CIMEL and Brewer measurements, that provide the total Aerosol Optical Depth, it has been demonstrated that the MAXDOAS measurements also provide additional information about the vertical distribution of the aerosol extinction in the lowest kilometres of the troposphere. A better understanding of the ultimate capabilities of MAXDOAS aerosol remote sensing has been gained through participation to the international CINDI campaign (Cabauw Intercomparison Campaign of Nitrogen Dioxide measuring Instruments ) in summer 2009. The combination of Brewer, CIMEL and MAXDOAS instruments gives us a remote-sensing dataset that will enable a more comprehensive characterization of the tropospheric aerosol optical properties. The usefulness of these aerosol observations has already been demonstrated in the improvement of the UVindex predictions for the general public. Another application is their use as input data in the retrieval of vertical profiles of tropospheric pollutants from MAXDOAS measurements, like tropospheric NO2 and formaldehyde. Third we have focused on a few climate-related trace gases. Changing greenhouse gas and aerosol concentrations directly affect the radiative budget of the atmosphere, and therefore climate. But many species known as pollutants like carbon monoxide (CO), nitrogen oxides (NOx) and hydrocarbons, - often related to fossil fuel or biomass burning -, also affect climate through their role in chemical reactions that produce tropospheric ozone, which is a well-known greenhouse gas, or that modify the lifetime of gases like methane, or the oxidation capacity of the atmosphere. Therefore in AGACC, we have focused on the measurement of a number of trace gases that are subject to changing concentrations, that directly or indirectly affect climate, and that are either difficult to monitor or that have not yet been measured from the ground. We have included attempts to observe distinctly some isotopologues, because the isotopic ratios observed in an airmass provide information on its history, and because the FTIR solar absorption measurements provide a rather unique capability hereto. The investigated species are the isotopologues of CH4 and CO, and hydrogen cyanide (HCN), as examples of biomass burning tracers, some hydrocarbons like formaldehyde (HCHO), ethylene (C2H4) and acetylene (C2H2), and HCFC-142b, a replacement product for CFCs and a greenhouse gas. In many cases, retrieval strategies had to be adapted when going from one site to another with different atmospheric conditions, especially when the local humidity and abundances are very different as is the case between Jungfraujoch (dry, high altitude, mid-latitude) and Ile de La Réunion (humid, low altitude, low latitude). Still we have been able to show the feasibility of retrieving particular trace gas information even under difficult conditions. Many of our results have been compared to correlative data, to validate the approach and to gain complementary information. It is also important to note that the retrieval strategies developed in AGACC have regularly been presented to the global Network for the Detection of Atmospheric Composition Change (NDACC) UV-Vis and Infrared communities and have often been adopted by others or even proposed for adoption as a standard in the community (e.g., for hydrogen cyanide (HCN)). In particular: We have been able to study the seasonal variations of HCN at the Jungfraujoch and at Ile de La Réunion, and to show the dominant impact of biomass burning. Formaldehyde was studied in much detail at Ukkel, Jungfraujoch and Ile de la Réunion. The challenge for detection at Jungfraujoch is the small abundance (about 10 times smaller than at Ukkel and Ile de La Réunion); a particular observation strategy was developed successfully, resulting in a time series that already shows the day-to-day and seasonal variations. At Ile de La Réunion, comparisons of FTIR, MAXDOAS, satellite and model data have (1) shown the good agreement between the various data sets, but also, (2), the variability of HCHO (diurnal, seasonal, day-to-day), and (3), thanks to the complementarities of the various data sets, they have enabled us to learn more about the long-range transport of Non-methane Volatile Organic Compounds (NMVOCS, precursors of HCHO) and deficiencies in the models. It was shown that fast, direct transport of NMVOCS from Madagascar has a significant impact on the HCHO abundance and its variability at Ile de La Réunion, and that this is underestimated in the model. Significant progress was made as to the detection of 13CH4 and CH3D from ground-based FTIR observations, both at Jungfraujoch and Ile de La Réunion. To our knowledge, it is the first time that a d13C data set is derived from ground-based FTIR observations. More work is needed to improve the CH3D retrieval at Ile de La Réunion, and to interpret the results, in combination with models. Also for the first time, 12CO and 13CO have been retrieved individually at Jungfraujoch. The d13C time series shows significant seasonal and interannual changes. As to the hydrocarbon ethylene, it is shown that it can be detected at Jungfraujoch only in spectra at low solar elevation, given its small atmospheric abundance. Regarding acetylene, the observed time series at Jungfraujoch and Ile de La Réunion show clear seasonal variations and enhancements due to the impact of biomass burning events, correlated with enhancements in CO, C2H6 and HCN. It is not clear yet whether we can reliably retrieve the concentration of HCFC- 142b, a replacement product that is increasing strongly in the troposphere. New line parameters for the interfering species HFC-134a are required to confirm/infirm the preliminary results. This highlights again the importance of the laboratory work for providing such parameters. Improved line parameters have been obtained for water vapour and its isotopologues, ethylene and formic acid. These AGACC results have been integrated in the international spectroscopic databases. We also showed that line intensities available around 2096 cm–1 for the 13C16O isotopologue of carbon monoxide in the HITRAN database seem to be accurate to 2%. We failed to improve line intensities for the 13.6 μm region of acetylene. The new data sets that have been derived in AGACC from FTIR and MAXDOAS observations have been archived in the NDACC data centre, where they are available for users (generally modelers and satellite teams). In addition, they are stored locally and are available to users upon request. AGACC results have been reported to the international scientific community, via the literature, via integration in geophysical or spectroscopic databases, and via participation to international research initiatives like the Atmospheric Water Vapour in the Climate System (WAVACS) Cost Action, the International Space Science Institute (ISSI) Working Group on Atmospheric Water Vapour, the International Union of Pure and Applied Chemistry (IUPAC) project, the International CINDI campaign, etc. The results have already found important scientific applications. A few examples are worth mentioning: the re-evaluation of methane emissions in the tropics from SCIAMACHY based on the new H2O spectroscopy, and the improved retrievals of HCOOH from the satellite experiments ACE-FTS and IASI, and from the ground. In the longer-term, the AGACC results will no doubt benefit the research in atmospheric sciences –in particular in the monitoring of its composition changes–, which is the fundamental basis of environmental assessment reports for supporting policy makers.Advanced exploitation of ground-based measurements for atmospheric chemistry and climate applications "AGACC

Tropospheric methanol observations from space: retrieval evaluation and constraints on the seasonality of biogenic emissions

Methanol retrievals from nadir-viewing space-based sensors offer powerful new information for quantifying methanol emissions on a global scale. Here we apply an ensemble of aircraft observations over North America to evaluate new methanol measurements from the Tropospheric Emission Spectrometer (TES) on the Aura satellite, and combine the TES data with observations from the Infrared Atmospheric Sounding Interferometer (IASI) on the MetOp-A satellite to investigate the seasonality of methanol emissions from northern midlatitude ecosystems. Using the GEOS-Chem chemical transport model as an intercomparison platform, we find that the TES retrieval performs well when the degrees of freedom for signal (DOFS) are above 0.5, in which case the model : TES regressions are generally consistent with the model : aircraft comparisons. Including retrievals with DOFS below 0.5 degrades the comparisons, as these are excessively influenced by the a priori. The comparisons suggest DOFS > 0.5 as a minimum threshold for interpreting retrievals of trace gases with a weak tropospheric signal. We analyze one full year of satellite observations and find that GEOS-Chem, driven with MEGANv2.1 biogenic emissions, underestimates observed methanol concentrations throughout the midlatitudes in springtime, with the timing of the seasonal peak in model emissions 1-2 months too late. We attribute this discrepancy to an underestimate of emissions from new leaves in MEGAN, and apply the satellite data to better quantify the seasonal change in methanol emissions for midlatitude ecosystems. The derived parameters (relative emission factors of 11.0, 1.0, 0.05 and 8.6 for new, growing, mature, and old leaves, respectively, plus a leaf area index activity factor of 0.75 for expanding canopies with leaf area index < 2.0) provide a more realistic simulation of seasonal methanol concentrations in midlatitudes on the basis of IASI, TES, and ground-based measurements