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Retrieving global observations of gravity waves (GW) from recent satellite missions is challenging. Nadir viewing satellites such as AIRS provide directional momentum fluxes, but lack fine vertical resolution and hence observe only those GW with exceptionally high intrinsic phase speed. Limb scanning instruments such as HIRDLS and SABER have only a single measurement track and hence provide only an estimate of absolute GW momentum flux. In addition, the sparse along-track sampling of these limb sounders introduce uncertainties in horizontal wavelength. GPS-RO can provide GW profile triplets, allowing in principle the horizontal direction of GW propagation to be inferred, but these triplets are rare. Finally, direct wind measurements from Aeolus are restricted in altitude to less than ~25km and only provide the wind component in the direction of the lidar beam from one observational track. In consequence, also Aeolus cannot reveal horizontal propagation direction and GW momentum flux.This situation could be dramatically improved by bringing a limb imager into space. A limb imager combines the very dense spatial sampling of a nadir viewing instrument with the high vertical resolution of a limb sounder. This will provide an almost complete description of the vertical spectrum of GWs, necessary for inferring drag estimates. Such global GW momentum flux data would for the first time allow to retrieve a global momentum budget from the mid-troposphere to the upper mesosphere.The changing-atmosphere infra-Red Tomography (CAIRT) mission candidate for ESA's earth explorer 11 proposes a limb imager for spatial sampling of 25 km across-track, 50 km along-track and 1 km in the vertical. From this we expect to infer directional GW momentum fluxes from the tropopause to 70 km or higher. This will allow longstanding scientific questions to be addressed such as the quantification of tropospheric GW sources and their related phase speed spectra and the identification of secondary wave generation in the stratosphere and lower mesosphere. Considering the momentum flux at higher altitudes, secondary wave generation competes with oblique GW propagation which allows GWs from low latitude sources to reach the high latitudes mesosphere and thus avoid critical levels. In general, two-way interaction with the background flow will be considered via the modulation of the GW spectrum by the winds and the mean wind accelerations by the GWs. In this contribution we will outline the CAIRT instrument concept, give an overview of the mission’s objectives and demonstrate its potential using simulated observations.

Spectral emissivity is a key property of the Earth surface of which only very few measurements exist so far in the far-infrared (FIR) spectral region, even though recent work has shown its FIR contribution is important for accurate modelling of global climate. The European Space Agency's 9th Earth Explorer, FORUM (Far-infrared Outgoing Radiation Understanding and Monitoring) will provide the first global spectrally resolved measurements of the Earth's top-of-the-atmosphere (TOA) spectrum in the FIR. In clear-sky conditions with low water vapour content, these measurements will provide a unique opportunity to retrieve spectrally resolved FIR surface emissivity. In preparation for the FORUM mission with an expected launch in 2026, this study takes the first steps towards the development of an operational emissivity retrieval for FORUM by investigating the sensitivity of the emissivity product of a full spectrum optimal estimation retrieval method to different physical and operational parameters. The tool used for the sensitivity tests is the FORUM mission's end-to-end simulator. These tests show that spectral emissivity of most surface types can be retrieved for dry scenes in the 350–600 cm−1 region with an uncertainty ranging from 0.005 to 0.01. In addition, the quality of retrieval is quantified with respect to the precipitable water vapour content of the scene, and the uncertainty caused by the correlation of emissivity with surface temperature is investigated. Two main recommendations are made based on these investigations: (1) As the extent of TOA sensitivity to the surface in the FIR depends on the atmospheric state, the spectral region of the emissivity product should be decided using a so-called information quantifier, calculated from the ratio of the retrieval uncertainty to the a-priori uncertainty. (2) Depending on retrieval input parameters, the correlation of emissivity with surface temperature allows for retrieved emissivities within a small range around the true emissivity. Thus the impact of this correlation on the uncertainty estimates of the product should be quantified in detail during further development of the operational retrieval.

Satellite data records of stratospheric water vapour have been compared to balloon-borne frost point hygrometer (FP) profiles that are coincident in space and time. The satellite data records of 15 different instruments cover water vapour data available from January 2000 through December 2016. The hygrometer data are from 27 stations all over the world in the same period. For the comparison, real or constructed averaging kernels have been applied to the hygrometer profiles to adjust them to the measurement characteristics of the satellite instruments. For bias evaluation, we have compared satellite profiles averaged over the available temporal coverage to the means of coincident FP profiles for individual stations. For drift determinations, we analyzed timeseries of relative differences between spatiotemporally coincident satellite and hygrometer profiles at individual stations. In a synopsis we have also calculated the mean biases and drifts (and their respective uncertainties) for each satellite record over all applicable hygrometer stations in three altitude ranges (10–30 hPa, 30–100 hPa, and 100 hPa to tropopause). Most of the satellite data have biases < 10 % and average drifts < 1 % yr−1 in at least one of the respective altitude ranges. Virtually all biases are significant in the sense that their uncertainty range in terms of twice the standard error of the mean does not include zero. Statistically significant drifts (95 % confidence) are detected for 35 % of the ~1200 timeseries of relative differences between satellites and hygrometers.

The long-term comparison between simulated and observed spectrally resolved outgoing longwave radiation (OLR) can represent a stringent test for the direct verification and improvement of general circulation models (GCMs), which are regularly tuned by adjusting parameters related to subgrid processes not explicitly represented in the model to constrain the integrated OLR energy fluxes to observed values. However, a good agreement between simulated and observed integrated OLR fluxes may be obtained from the cancellation of opposite-in-sign systematic errors localized in specific spectral ranges. Since the mid-2000s, stable hyperspectral observations of the mid-infrared region (667 to 2750 cm−1) of the Earth emission spectrum have been provided by different sensors (e.g. AIRS, IASI and CrIS). Furthermore, the FORUM (Far-infrared Outgoing Radiation Understanding and Monitoring) mission, selected to be the ninth ESA Earth Explorer, will measure, starting from 2027, the terrestrial radiation emitted to space at the top of the atmosphere (TOA) from 100 to 1600 cm−1, filling the observational gap in the far-infrared (FIR) region, from 100 to 667 cm−1. In this work, in anticipation of FORUM measurements, we compare Infrared Atmospheric Sounding Interferometer (IASI) Metop-A observations to radiances simulated on the basis of the atmospheric fields predicted by the EC-Earth Global Climate Model (version 3.3.3) in clear-sky conditions. To simulate spectra based on the atmospheric and surface state provided by the climate model, the radiative transfer model σ-IASI has been integrated in the Cloud Feedback Model Intercomparison Project (COSP) package. Therefore, online simulations, provided by the EC-Earth model equipped with the new COSP–σ-IASI module, have been performed in clear-sky conditions with prescribed sea surface temperature and sea ice concentration, every 6 h, over a time frame consistent with the availability of IASI data. Systematic comparisons between observed and simulated brightness temperature (BT) have been performed in 10 cm−1 spectral intervals, on a global scale over the ocean, with a specific focus on the latitudinal belt between 30∘ S and 30∘ N. The analysis has shown a warm BT bias of about 3.5 K in the core of the CO2 absorption band and a cold BT bias of approximately 1 K in the wing of the CO2 band, due to a positive temperature bias in the stratosphere and a negative temperature bias in the middle troposphere of the climate model, respectively. Finally, considering a warm BT bias in the rotational–vibrational water vapour band, we have highlighted a dry bias of the water vapour concentration in the upper troposphere of the model.

The long-term comparison between simulated and observed spectrally resolved outgoing longwave radiation (OLR) can represent a stringent test for the direct verification and improvement of general circulation models (GCMs), which are regularly tuned by adjusting parameters related to subgrid processes not explicitly represented in the model to constrain the integrated OLR energy fluxes to observed values. However, a good agreement between simulated and observed integrated OLR fluxes may be obtained from the cancellation of opposite-in-sign systematic errors localized in specific spectral ranges. Since the mid-2000s, stable hyperspectral observations of the mid-infrared region (667 to 2750 cm−1) of the Earth emission spectrum have been provided by different sensors (e.g. AIRS, IASI and CrIS). Furthermore, the FORUM (Far-infrared Outgoing Radiation Understanding and Monitoring) mission, selected to be the ninth ESA Earth Explorer, will measure, starting from 2027, the terrestrial radiation emitted to space at the top of the atmosphere (TOA) from 100 to 1600 cm−1, filling the observational gap in the far-infrared (FIR) region, from 100 to 667 cm−1. In this work, in anticipation of FORUM measurements, we compare Infrared Atmospheric Sounding Interferometer (IASI) Metop-A observations to radiances simulated on the basis of the atmospheric fields predicted by the EC-Earth Global Climate Model (version 3.3.3) in clear-sky conditions. To simulate spectra based on the atmospheric and surface state provided by the climate model, the radiative transfer model σ-IASI has been integrated in the Cloud Feedback Model Intercomparison Project (COSP) package. Therefore, online simulations, provided by the EC-Earth model equipped with the new COSP–σ-IASI module, have been performed in clear-sky conditions with prescribed sea surface temperature and sea ice concentration, every 6 h, over a time frame consistent with the availability of IASI data. Systematic comparisons between observed and simulated brightness temperature (BT) have been performed in 10 cm−1 spectral intervals, on a global scale over the ocean, with a specific focus on the latitudinal belt between 30∘ S and 30∘ N. The analysis has shown a warm BT bias of about 3.5 K in the core of the CO2 absorption band and a cold BT bias of approximately 1 K in the wing of the CO2 band, due to a positive temperature bias in the stratosphere and a negative temperature bias in the middle troposphere of the climate model, respectively. Finally, considering a warm BT bias in the rotational–vibrational water vapour band, we have highlighted a dry bias of the water vapour concentration in the upper troposphere of the model.

The Changing-Atmosphere Infra-Red Tomography Explorer (CAIRT) is one of the four candidates for ESA’s Earth Explorer 11. This mission has been proposed in order to achieve a step change in our understanding of the coupling of atmospheric circulation, composition and climate. The CAIRT concept proposes to perform limb tomography of the atmosphere from the troposphere to the lower thermosphere (about 5 to 115 km altitude) with a swath between 300 and 500 km and high spatial and spectral resolution to provide a three-dimensional picture of atmospheric structure at unprecedented scales. This contribution will investigate the capability of CAIRT to analyse stratosphere to troposphere exchange using an Observing System Simulation Experiment (OSSE). In this effort, a reference atmosphere – the nature run in the OSSE terminology – is built based on the Copernicus Atmosphere Monitoring Services (CAMS) control run (i.e. with a horizontal resolution ~40 km and a vertical resolution ~500 m in the tropopause region). The nature run is used to generate CAIRT ozone profiles, along with a CAIRT orbit simulator and a simulator to generate CAIRT ozone retrieval responses and error covariance matrix. Simulated CAIRT ozone profiles are then assimilated by the Belgian Assimilation System for Chemical ObsErvations (BASCOE) to provide ozone analyses – the assimilation run. In order to measure the added value of CAIRT data in the assimilation run, a BASCOE control run without CAIRT assimilation, is also done. Ozone fluxes across the tropopause are calculated from three numerical experiments which will be discussed in this presentation., The 28th IUGG General Assembly (IUGG2023) (Berlin 2023)

The Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) was a limb-viewing infrared Fourier transform spectrometer that operated from 2002 to 2012 aboard the Environmental Satellite (ENVISAT). The final re-processing of the full MIPAS mission Level 2 data was performed with the ESA operational version 8 (v8) processor. This MIPAS dataset includes not only the retrieval results of pressure–temperature and the standard species H2O, O3, HNO3, CH4, N2O, and NO2 but also vertical profiles of volume mixing ratios of the more difficult-to-retrieve molecules N2O5, ClONO2, CFC-11, CFC-12 (included since v6 processing), HCFC-22, CCl4, CF4, COF2, and HCN (included since v7 processing). Finally, vertical profiles of the species C2H2, C2H6, COCl2, OCS, CH3Cl, and HDO were additionally retrieved by the v8 processor. The balloon-borne limb-emission sounder MIPAS-B was a precursor of the MIPAS satellite instrument. Several flights with MIPAS-B were carried out during the 10-year operational phase of ENVISAT at different latitudes and seasons, including both operational periods when MIPAS measured with full spectral resolution (FR mode) and with optimised spectral resolution (OR mode). All MIPAS operational products (except HDO) were compared to results inferred from dedicated validation limb sequences of MIPAS-B. To enhance the statistics of vertical profile comparisons, a trajectory match method has been applied to search for MIPAS coincidences along the 2 d forward and backward trajectories running from the MIPAS-B measurement geolocations. This study gives an overview of the validation results based on the ESA operational v8 data comprising the MIPAS FR and OR observation periods. This includes an assessment of the data agreement of both sensors, taking into account the combined errors of the instruments. The differences between the retrieved temperature profiles of both MIPAS instruments generally stays within ±2 K in the stratosphere. For most gases – namely H2O, O3, HNO3, CH4, N2O, NO2, N2O5, ClONO2, CFC-11, CFC-12, HCFC-22, CCl4, CF4, COF2, and HCN – we find a 5 %–20 % level of agreement for the retrieved vertical profiles of both MIPAS instruments in the lower stratosphere. For the species C2H2, C2H6, COCl2, OCS, and CH3Cl, however, larger differences (within 20 %–50 %) appear in this altitude range.

Nineteen limb-viewing data sets (occultation, passive thermal, and UV scattering) and two nadir upper tropospheric humidity (UTH) data sets are intercompared and also compared to frost-point hygrometer balloon sondes. The upper troposphere considered here covers the pressure range from 300–100 hPa. UTH is a challenging measurement, because concentrations vary between 2–1000 ppmv (parts per million by volume), with sharp changes in vertical gradients near the tropopause. Cloudiness in this region also makes the measurement challenging. The atmospheric temperature is also highly variable ranging from 180–250 K. The assessment of satellite-measured UTH is based on coincident comparisons with balloon frost-point hygrometer sondes, multi-month mapped comparisons, zonal mean time series comparisons, and coincident satellite-to-satellite comparisons. While the satellite fields show similar features in maps and time series, quantitatively they can differ by a factor of 2 in concentration, with strong dependencies on the amount of UTH. Additionally, time-lag response-corrected Vaisala RS92 radiosondes are compared to satellites and the frost-point hygrometer measurements. In summary, most satellite data sets reviewed here show on average ∼30 % agreement amongst themselves and frost-point data but with an additional ∼30 % variability about the mean bias. The Vaisala RS92 sonde, even with a time-lag correction, shows poor behavior for pressures less than 200 hPa.

Retrieving global observations of gravity waves (GWs) from recent satellite missions is challenging. Nadir viewing satellites such as AIRS provide directional momentum fluxes, but lack fine vertical resolution and hence observe only those GWs with exceptionally high intrinsic phase speed. Limb scanning instruments such as HIRDLS and SABER have only a single measurement track and hence provide only an estimate of absolute GW momentum flux. In addition, the sparse along-track sampling of these limb sounders introduce uncertainties in horizontal wavelength. GPS-RO can provide GW profile triplets, allowing in principle the horizontal direction of GW propagation to be inferred, but these triplets are rare. Finally, direct wind measurements from Aeolus are restricted in altitude to less than ~25km and only provide the wind component in the direction of the lidar beam from one observational track. In consequence, also Aeolus cannot reveal horizontal propagation direction and GW momentum flux.This situation could be dramatically improved by bringing a limb imager into space. A limb imager combines the very dense spatial sampling of a nadir viewing instrument with the high vertical resolution of a limb sounder. This will provide an almost complete description of the vertical spectrum of GWs, necessary for inferring drag estimates. Such global GW momentum flux data would for the first time allow to retrieve a global momentum budget from the mid-troposphere to the upper mesosphere.The Changing-Atmosphere Infra-Red Tomography (CAIRT) mission candidate for ESA's Earth Explorer 11 proposes a limb imager for spatial sampling of 25 km across-track, 50 km along-track and 1 km in the vertical. From this we expect to infer directional GW momentum fluxes from the tropopause to 70 km or higher. This will allow longstanding scientific questions to be addressed such as the quantification of tropospheric GW sources and their related phase speed spectra and the identification of secondary wave generation in the stratosphere and lower mesosphere. Considering the momentum flux at higher altitudes, secondary wave generation competes with oblique GW propagation which allows GWs from low latitude sources to reach the high latitudes mesosphere and thus avoid critical levels. In general, two-way interaction with the background flow will be considered via the modulation of the GW spectrum by the winds and the mean wind accelerations by the GWs. In this contribution we will outline the CAIRT instrument concept, giving an overview of the mission’s objectives and demonstrate its potential using simulated observations.

Nineteen limb viewing (occultation and passive thermal) and two nadir humidity data sets are intercompared and also compared to frostpoint hygrometer balloon sondes. The upper troposphere considered here covers the pressure range from 300–100 hPa. Water vapor in this region is a challenging measurement because concentrations vary between 2–1000 parts per million volume with sharp changes in vertical gradients near the tropopause. The atmospheric temperature is also highly variable ranging from 180–250 K. The assessment of satellite measured humidity is based on coincident comparisons with frostpoint hygrometer sondes, multi month mapped comparisons, zonal mean time series comparisons and coincident satellite to satellite comparisons. While the satellite fields show similar features in maps and time series, quantitatively, they can differ by a factor of two in concentration, with strong dependencies on the amount of H2O. Additionally, time-lag response corrected Vaisala-RS92 radiosondes are compared to satellites and the frostpoint hygrometer measurements. In summary, most satellite data sets reviewed here show on average ~30 % agreement amongst themselves and frostpoint data but with an additional ~30 % variability about the mean. The Vaisala-RS92 sonde even with a time-lag correction shows poor behavior for pressure less than 200 hPa.

FORUM (Far-infrared Outgoing Radiation Understanding and Monitoring) will flight as the 9th ESA’s Earth Explorer mission, and an End-to-End Simulator (E2ES) has been developed as a support tool for the mission selection process and the subsequent development phases. The current status of the FORUM E2ES project is presented, together with the characterization of the capabilities of a full physics retrieval code applied to FORUM data. We show how the instrument characteristics and5the observed scene conditions impact on the spectrum measured by the instrument, accounting for the main sources of error related to the entire acquisition process, and the consequences on the retrieval algorithm. Both homogeneous and heterogeneous case studies are simulated in clear and cloudy conditions, validating the E2ES against two independent codes: KLIMA (clear sky) and SACR (cloudy sky). The performed tests show that the performance of the retrieval algorithm is compliant with the project requirements both in clear and cloudy conditions. The far infrared (FIR) part of the FORUM spectrum is shown to be10sensitive to surface emissivity, in dry atmospheric conditions, and to cirrus clouds, resulting in improved performance of the retrieval algorithm in these conditions. The retrieval errors increase with increasing the scene heterogeneity, both in terms of surface characteristics and in terms of fractional cloud cover of the scene.

To improve our knowledge of the coupling of atmospheric circulation, composition and regional climate change, and to provide the urgently needed observations of the on-going changes and processes involved, we have recently proposed the Changing-Atmosphere Infra-Red Tomography Explorer (CAIRT) to ESA as Earth Explorer 11 candidate. CAIRT will be the first limb-sounder with imaging Fourier-transform infrared technology in space. By observing simultaneously the atmosphere from the troposphere to the lower thermosphere (about 5 to 115 km altitude), CAIRT will provide global observations of temperature, ozone, water vapour, as well as key halogen and nitrogen compounds. The latter will help to better constrain coupling with the upper atmosphere, solar variability and space weather. Observation of long-lived tracers (such as N2O, CH4, SF6, CF4) will provide information on transport, mixing and circulation changes. CAIRT will deliver essentially a complete budget of stratospheric sulfur (by observations of OCS, SO2, and H2SO4-aerosols), as well as observations of ammonia and ammonium nitrate aerosols. Biomass burning and other pollution plumes, and their impact on ozone chemistry in the UTLS region, will be detected from observations of HCN, CO and a further wealth of volatile organic compounds. The potential to measure water vapour isotopologues will help to constrain water vapour and cloud processes and interactions at the Earth’s surface. The high-resolution measurements of temperature will provide the momentum flux, phase speed and direction of atmospheric gravity waves. CAIRT thus will provide comprehensive information on the driving of the large-scale circulation by different types of waves. Tomographic retrievals will provide temperature and trace gas profiles at a much higher horizontal resolution and coverage than achieved from space so far. Flying in formation with the Second Generation Meteorological Operational Satellite (MetOp-SG) will enable combined retrievals with observations by the New Generation Infrared Atmospheric Sounding Interferometer (IASI-NG) and Sentinel-5, resulting in consistent atmospheric profile information from the surface up to the lower thermosphere. Our presentation will give an overview of the proposed CAIRT mission, its objectives and synergies with other sensors.

The Far-infrared Outgoing Radiation Understanding and Monitoring (FORUM) mission, selected for the ESA's 9th Earth Explorer (EE9) mission, will be launched in 2026. For the first time, spectrally resolved radiance observations covering the Far InfraRed (FIR) band from 100 to 667 cm ?¹ with global coverage and with high spectral resolution and radiometric accuracy will be available. This spectral region is highly sensitive to upper-tropospheric-lower-stratospheric (UTLS) water vapor concentration. One of the tools used to support the FORUM proposal during the EE9 competition, and previously, for the data analysis of the REFIR-PAD (Radiation Explorer in the Far InfraRed - Prototype for Applications and Development) balloon observations, is KLIMA (Kyoto protocoL Informed Management of the Adaptation) retrieval code. KLIMA analysed the synthetic FORUM observations in clear sky providing simultaneously the vertical profile of the minor atmospheric gases (such as the water vapour), atmospheric temperature profile, surface temperature, and surface emissivity. During the EE9 phase A selection, KLIMA was employed in various ESA studies such as: FORUM-req for the assessment of the FORUM mission requirements definition; FORUM-E2E for the validation of the End-to-End Simulator (E2ES); FIRMOS for the analysis of the ground-based observations of the FORUM prototype FIRMOS (Far-Infrared Radiation Mobile Observation System). Recently, the KLIMA code was used in the context of the ASI FORUM-science project for the generation of gases optical thicknesses used by the fast code ?-FORUM. In this framework, KLIMA has been upgraded to retrieve also the concentration of the isotopologues of the atmospheric gases. In this work, we will show the assessment of the performance of the retrieval of water vapour isotopologues using the spectral coverage and radiometric accuracy of the FORUM observations, and the comparison with the results obtained when only the middle-infrared information is used. Results both on single measurement and averaged measurements will be shown to evaluate the effect of the radiometric accuracy of the FORUM observations.

In 2019, the Italian Space Agency (ASI) started a new project entitled FORUM - scienza (FORUM science). One of the project objectives is to improve and share, within the interested National scientific community, the models needed for interpretation and analysis of the measurements of the forthcoming FORUM (Far-infrared Outgoing Radiation Understanding and Monitoring) experiment. FORUM will be the ninth Earth Explorer mission of the European Space Agency (ESA), scheduled for launch on a polar satellite in 2026. The core instrument will be a Fourier Transform Spectrometer covering the spectral region from 100 to 1600 cm-1 (from 100 to 6.25 microns in wavelength), with a full-width-half-maximum spectral resolution of 0.5 cm-1. The spectrometer will measure the Earth's upwelling spectrum in the nadir-looking geometry. FORUM will fly in loose formation with the MetOp-SG-A satellite, hosting the Infrared Atmospheric Sounding Interferometer - New Generation (IASI-NG). The MIR (645 to 2760 cm-1) upwelling atmospheric spectrum measured by IASI-NG will complement the FORUM FIR spectrum, providing an unprecedented spectral coverage, from 100 to 2760 cm-1. While the FIR part of the spectrum (100-667 cm-1) measured by FORUM is the most sensitive to the water vapour content in the UTLS, the atmospheric windows in the MIR are measured by IASI-NG with a very high signal-to-noise ratio, thus supplying very precise information on the surface temperature and on the temperature profile, which are essential to constrain the retrieval parameters. Among the models improved in the frame of the FORUM - scienza project, ?-FORUM is a fast parametric radiative transfer code with the capability of simulating the upwelling spectrum, from 50 to 2810 cm-1, with sufficiently high spectral resolution (0.01 cm-1), in all sky conditions. Along with the spectral radiance, the model computes its Jacobians with respect to relevant atmospheric, cloud and surface parameters. The characteristics and the accuracy figures of the ?-FORUM model are presented by Masiello et al., within this conference. Based on ?-FORUM, we have built a fast and flexible Bayesian inversion model. This model includes the possibility of performing the synergistic inversion of both FORUM and IASI-NG measurements and to apply various types of constraints in the inversion, such as Optimal Estimation and / or Tikhonov regularization. Profile retrieval grids, together with the set of parameters to be retrieved are selected via input files. Currently, the following sets of parameters can be retrieved: temperature, water vapour and ozone profiles, surface temperature and surface spectral emissivity (at a selectable set of wavenumbers). The program also offers the possibility to minimize the effect of possible frequency scale errors of the spectrum by retrieving a frequency scale factor. The possibility to retrieve profiles of ice- and liquid- water contents and of droplet- and ice- effective dimensions will be implemented in the near future. In this work we illustrate the structure of the developed retrieval model, its performance, and the results of the first tests we made to optimize the retrieval setup in clear-sky conditions.

The Far-Infrared Outgoing Radiation Understanding and Monitoring (FORUM) mission will provide a significant opportunity to verify and potentially improve the ability of global circulation models (GCMs) in simulating the Outgoing Longwave Radiation (OLR). Accurate simulation of the OLR is in fact crucial to better constrain the different radiative feedbacks. Planned for launch in 2026, FORUM will measure nadir-looking, spectrally resolved radiances of the Earth's emission spectrum at the top of the atmosphere (TOA) from 100 to 1600 cm-1 filling the existing observational gap of the far-infrared (FIR) region, from 100 to 667 cm-1. In addition, FORUM will fly in loose formation with IASI-NG, which will continue to cover the middle infrared range of IASI from 675 to 2760 cm-1. In anticipation of FORUM measurements, we aim at comparing IASI existing observations to synthetic radiances extracted from the EC-Earth GCM (version 3.3.2), a recent European model based on ECMWF's Integrated Forecasting System (IFS) for the atmosphere-land component and the ocean model NEMO, including sea ice (LIM2) and land surface components (1). Climate model outputs only provide simulated energy fluxes integrated over the whole Earth emission spectrum making difficult the detection of biases and the identification of possible compensation errors in the estimation of the OLR. Conversely, comparing simulated to observed spectra, allows to point out the potential model criticalities in specific spectral bands which contain the signatures of particular climate variables. In order to extract simulated spectra from the climate model, EC-Earth has been equipped with COSP, a simulator package able to map the model state into synthetic observations from different satellite-borne active (CloudSat (radar) and CALIPSO (lidar)) and passive (ISCCP, MISR and MODIS) (2) sensors. We have further developed the package by implementing inside COSP the radiative transfer model ?-FORUM, a monochromatic code able to reproduce synthetic radiances in the Far-Infrared and Mid-Infrared regions compatible with future FORUM and existing IASI observations (3). Due to the high computation cost of the operation, the efficiency of the EC-Earth model equipped with the new COSP module has been improved by modifying the ?-FORUM original code structure and by reducing the original resolution of the model. Therefore, simulations provided by EC-Earth model equipped with the new COSP + ?-FORUM module have been performed with prescribed sea surface temperature and sea-ice cover every 6 hours, over a timeframe consistent with the availability of IASI METOP-A L1C data, from 2007 to 2016. The comparison between nadir radiances simulated by the EC-Earth climate model and the climatology built from ten years of IASI observations represents a very high confidence test for the direct verification and improvement of the GCM avoiding potential uncertainties related to application of retrieval methods. The same approach could be extended to other climate models and, in the near future, it will involve FORUM measurements for a comprehensive analysis of the climate model ability in reproducing the whole Earth emission spectrum. References 1. Hazeleger, Wilco, et al. "EC-Earth: a seamless earth-system prediction approach in action." Bulletin of the American Meteorological Society 91.10 (2010): 1357-1364. 2. Bodas-Salcedo, Alejandro, et al. "COSP: Satellite simulation software for model assessment." Bulletin of the American Meteorological Society 92.8 (2011): 1023-1043. 3. Amato, Umberto, et al. "Corrigendum to: "The sigma-IASI code for the calculation of infrared atmospheric radiance and its derivatives" [Environmental Modelling & Software (2002) 17 (7) 651-667]." Environmental Modelling and Software 18.1 (2003): 97

As part of the second SPARC (Stratosphere–troposphere Processes And their Role in Climate) water vapor assessment (WAVAS-II), we present measurements taken from or coincident with seven sites from which ground-based microwave instruments measure water vapor in the middle atmosphere. Six of the ground-based instruments are part of the Network for the Detection of Atmospheric Composition Change (NDACC) and provide datasets that can be used for drift and trend assessment. We compare measurements from these ground-based instruments with satellite datasets that have provided retrievals of water vapor in the lower mesosphere over extended periods since 1996. We first compare biases between the satellite and ground-based instruments from the upper stratosphere to the upper mesosphere. We then show a number of time series comparisons at 0.46 hPa, a level that is sensitive to changes in H2O and CH4 entering the stratosphere but, because almost all CH4 has been oxidized, is relatively insensitive to dynamical variations. Interannual variations and drifts are investigated with respect to both the Aura Microwave Limb Sounder (MLS; from 2004 onwards) and each instrument's climatological mean. We find that the variation in the interannual difference in the mean H2O measured by any two instruments is typically ∼ 1%. Most of the datasets start in or after 2004 and show annual increases in H2O of 0–1 % yr−1. In particular, MLS shows a trend of between 0.5 % yr−1 and 0.7 % yr−1 at the comparison sites. However, the two longest measurement datasets used here, with measurements back to 1996, show much smaller trends of +0.1 % yr−1 (at Mauna Loa, Hawaii) and −0.1 % yr−1 (at Lauder, New Zealand).

Atmospheric emissions of carbon tetrachloride (CCl4) are regulated by the Montreal Protocol due to its role as a strong ozone-depleting substance. The molecule has been the subject of recent increased interest as a consequence of the so-called mystery of CCl4, the discrepancy between atmospheric observations and reported production and consumption. Surface measurements of CCl4 atmospheric concentrations have declined at a rate almost 3 times lower than its lifetime-limited rate, suggesting persistent atmospheric emissions despite the ban. In this paper, we study CCl4 vertical and zonal distributions in the upper troposphere and lower stratosphere (including the photolytic loss region, 70–20 hPa), its trend, and its stratospheric lifetime using measurements from the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS), which operated onboard the ENVISAT satellite from 2002 to 2012. Specifically, we use the MIPAS data product generated with Version 7 of the Level 2 algorithm operated by the European Space Agency.The CCl4 zonal means show features typical of long-lived species of anthropogenic origin that are destroyed primarily in the stratosphere, with larger quantities in the troposphere and a monotonic decrease with increasing altitude in the stratosphere. MIPAS CCl4 measurements have been compared with independent measurements from other satellite and balloon-borne remote sounders, showing a good agreement between the different datasets.CCl4 trends are calculated as a function of both latitude and altitude. Negative trends of about −10 to −15 pptv decade−1 (−10 to −30 % decade−1) are found at all latitudes in the upper troposphere–lower stratosphere region, apart from a region in the southern midlatitudes between 50 and 10 hPa where the trend is positive with values around 5–10 pptv decade−1 (15–20 % decade−1). At the lowest altitudes sounded by MIPAS, we find trends consistent with those determined on the basis of long-term ground-based measurements (−10 to −13 pptv decade−1). For higher altitudes, the trend shows a pronounced asymmetry between the Northern and Southern hemispheres, and the magnitude of the decline rate increases with altitude. We use a simplified model assuming tracer–tracer linear correlations to determine CCl4 lifetime in the lower stratosphere. The calculation provides a global average lifetime of 47 (39–61) years, considering CFC-11 as the reference tracer. This value is consistent with the most recent literature result of 44 (36–58) years.

The Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) was an infrared (IR) limb emission spectrometer on the Envisat platform. Currently, there are four MIPAS ozone data products, including the operational Level-2 ozone product processed at ESA, with the scientific prototype processor being operated at IFAC Florence, and three independent research products developed by the Istituto di Fisica Applicata Nello Carrara (ISAC-CNR)/University of Bologna, Oxford University, and the Karlsruhe Institute of Technology–Institute of Meteorology and Climate Research/Instituto de Astrofísica de Andalucía (KIT–IMK/IAA). Here we present a dataset of ozone vertical profiles obtained by merging ozone retrievals from four independent Level-2 MIPAS processors. We also discuss the advantages and the shortcomings of this merged product. As the four processors retrieve ozone in different parts of the spectra (microwindows), the source measurements can be considered as nearly independent with respect to measurement noise. Hence, the information content of the merged product is greater and the precision is better than those of any parent (source) dataset. The merging is performed on a profile per profile basis. Parent ozone profiles are weighted based on the corresponding error covariance matrices; the error correlations between different profile levels are taken into account. The intercorrelations between the processors' errors are evaluated statistically and are used in the merging. The height range of the merged product is 20–55km, and error covariance matrices are provided as diagnostics. Validation of the merged dataset is performed by comparison with ozone profiles from ACE-FTS (Atmospheric Chemistry Experiment–Fourier Transform Spectrometer) and MLS (Microwave Limb Sounder). Even though the merging is not supposed to remove the biases of the parent datasets, around the ozone volume mixing ratio peak the merged product is found to have a smaller (up to 0.1ppmv) bias with respect to ACE-FTS than any of the parent datasets. The bias with respect to MLS is of the order of 0.15ppmv at 20–30km height and up to 0.45ppmv at larger altitudes. The agreement between the merged data MIPAS dataset with ACE-FTS is better than that with MLS. This is, however, the case for all parent processors as well.

Earth's emitted energy in the wavelength range 4 ?m-100 ?m is commonly termed Outgoing Longwave radiation (OLR) and its accurate measurement is a first-priority requirement to assess the energy balance of the planet. Integrated broadband OLR fluxes provided by CERES energy balanced and filled (EBAF) dataset constitutes the standard reference to study the Earth's energy budget and consequently represents the target values of energy fluxes at top of atmosphere (TOA) for climate models tuning. Even if tuning operations guarantee a good agreement on a global basis between observed and simulated OLR at TOA, large regional biases are present all over the globe and a significant spread exists between different climate model simulations. The Far-Infrared Outgoing Radiation and Monitoring (FORUM) mission, planned for launch in 2026, will provide nadir-looking spectrally resolved radiance measurements of the Earth's emission spectrum at TOA from 100 to 1600 cm-1 (6.25 ?m-100 ?m) with a resolution better than 0.50 cm-1. For the first time FORUM measurements will fill the existing observational gap in the far-infrared (FIR) radiation range from 100 to 667 cm-1 (15 ?m-100 ?m) also providing spectrally resolved OLR fluxes (level 2 data product). In anticipation of FORUM measurements, we want to quantify the potential improvement of climate models in simulating OLR fluxes at TOA due to the future availability of spectrally resolved fluxes data from FORUM, extending to the Far InfraRed. At this stage, we focus on the analyses of simulations provided by EC-Earth (version 3.3.2), a new climate model developed by the joint effort of 27 research institutes of 10 European countries which has directly contributed to Coupled Model Intercomparison (CMIP) in its phases 5 and 6. The EC-Earth model is based on ECMWF's Integrated Forecasting System (IFS) for the atmosphere-land component and the ocean model NEMO, including sea ice (LIM2) and land surface components. Atmospheric profiles and information on the surface and on the clouds produced by EC-Earth simulations in realistic but simplified conditions are provided in input to SIGMA-IASI, a radiative transfer model able to calculate spectral radiances compatible with those that will be measured by FORUM. From these synthetic measurements, we estimate OLR fluxes by applying angular distribution models (ADM) of increasing complexity. The comparison between the OLR fluxes provided by the EC-Earth simulation and those calculated from synthetic FORUM measurements may allow to identify potential improvements for the parametric radiative module included in EC-Earth to estimate the OLR radiative fluxes.

FIRMOS (Far-Infrared Radiation Mobile Observation System) is a Fourier transform spectrometer covering the range from 100 to 1000 cm-1, developed to support the preparation of the satellite mission FORUM (Far-infrared Outgoing Radiation Understanding and Monitoring) planned in 2025/2026 (Earth Explorer 9 - ESA). FIRMOS was deployed at the Alpine observatory of Mt. Zugspitze, in the South of Germany, at about 3000 m a.s.l. for 2 months (December 2018 and January-February 2019). In January-February 2019, FIRMOS acquired about 600 measurements of the downwelling spectral radiance in clear sky condition. In this presentation, we present results of the retrieval of the water vapour and temperature profiles obtained from Level 2 analysis of the FIRMOS measurements in clear sky condition. Dedicated and coincident measurements allowed us to perform a comparison with integrated water vapour obtained from E-AERI (Extended-range Atmospheric Emitted Radiance Interferometer) at Zugspitze summit station and with radio-sounding launched at Garmisch-Partenkirchen. Comparisons with further independent information are also shown. Acknowledgments. The authors gratefully acknowledge the funding support by the European Space Agency with the FIRMOS project (ESA-ESTEC Contract No. 4000123691/18/NL/LF) and the Italian Space Agency with the research projects SCIEF (Italian acronym of Development of the National Competences for the FORUM experiment - ASI contract No. 2016-010-U.0)

MIPAS (Michelson Interferometer for Passive Atmospheric Sounding), a limb-viewing infrared interferometer, operated on-board the ENVISAT satellite from 2002 to 2012. In the past years a huge effort was performed in correcting the time dependent non-linear response of its detectors, in order to produce calibrated measurements stable in time. The new calibration strategy has been implemented into the latest version (V8) of the Level 1 processor. Also the Level 2 (L2) processor has been upgraded, the main improvements being the handling of horizontal gradients and the use of an upgraded spectroscopic database. Both new processors have been used to generate three Diagnostic Datasets. The new L2 datasets contain the vertical distributions of Temperature and the VMR of H2O, O3, HNO3, CH4, N2O, NO2, CFC-11, CFC-12, N2O5, ClONO2, HCFC-22, COF2, CF4, HCN, CCl4, OCS, CH3Cl, HDO, C2H2, C2H6, and COCl2. For each month of MIPAS lifetime, the data have been averaged in latitudinal bins at fixed pressure levels, and for each level, trends have been estimated using the same method described in Valeri et al. (2017). In this paper we will show some examples of the estimated trends, concentrating on reactive molecules like phosgene.

MIPAS on ENVISAT performed almost continuous measurements of atmospheric composition for approximately 10 years, from June 2002 to April 2012. ESA processor, based on the algorithm ORM (Optimized Retrieval Model), originally designed for the Near Real Time analysis, is currently used for the reanalysis of the full MIPAS mission. Version 7 of the full mission data was released in 2016, but further improvements have been recently performed in ORM V8 to be used in next full mission reanalysis. For these latest releases (V7 and V8) L1 data corrected for reducing the instrumental drift are used.TheinstrumentaldriftisduetoMIPASphotometricdetectorsnonlinearitiesthatchangewithtimeduetothe ageing of the instrument. Numerous species are retrieved from MIPAS measurements. Among them, CCl4 has been recently studied. This species has received increasing interest due to the so called "mystery of CCl4", since it was found that its atmospheric concentration at the surface declines with a rate significantly smaller than its lifetime-limited rate. Indeed there is a discrepancy between the atmospheric observations and the estimated distribution based on the reported production and consumption. MIPAS products generated with Version 7 of the L2 ESA algorithm were used to estimate CCl4 distributions, its trend, and atmospheric lifetime in the upper troposphere / lower stratosphere (UTLS) region. The trends derived by these observations between 2002 and 2012 as a function of both latitude and altitude confirm the decline of atmospheric mixing ratios, in agreement with ground based observations. Stratospheric trend derived from the MIPAS data are non-uniform, with some positive trends even being found in the middle stratosphere, mainly at high altitudes in the Southern Hemisphere. The variability in stratospheric trends reflects the impact of variability in stratospheric transport on trace gases and their temporal evolution. In addition to CCl4, some preliminary results obtained with the latest version of the processor (V8), that performs the analysis of a larger number of species and takes into account horizontal inhomogeneities, will be shown.

This paper discusses assimilation experiments of methane (CH4) and nitrous oxide (N2O) profiles retrieved from the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS). Here we focus on data versions 6 and 7 provided by the ESA processor. These data sets have been assimilated by the Belgian Assimilation System for Chemical ObsErvations (BASCOE). The CH4 and N2O retrieved profiles can oscillate, especially in the tropical lower stratosphere. Using the averaging kernels of the observations and a background error covariance matrix, which has previously been calibrated, allows the system to partly remedy this issue and provide assimilated fields that are more regular vertically. In general, there is a good agreement between the BASCOE analyses and independent observations from ACE–FTS (CH4 and N2O) and MLS (N2O), demonstrating the general good quality of CH4 and N2O retrievals provided by MIPAS ESA. Nevertheless, this study also identifies two issues in these data sets. First, time series of the observations show unexpected discontinuities due to an abrupt change in the gain of MIPAS band B, generally occurring after the instrument decontamination. Since the calibration is performed weekly, the abrupt change in the gain affects the measurements until the subsequent calibration is performed. Second, the correlations between BASCOE analyses and independent observations are poor in the lower stratosphere, especially in the tropics, probably due to the presence of outliers in the assimilated data. In this region, we recommend using MIPAS CH4 and N2O retrievals with caution.

The ACE-FTS (Atmospheric Chemistry Experiment – Fourier Transform Spectrometer) instrument on the Canadian SCISAT satellite, which has been in operation for over 12 years, has the capability of deriving stratospheric profiles of many of the NOy (N + NO + NO2+ NO3+ 2 × N2O5+ HNO3+ HNO4+ ClONO2+ BrONO2) species. Version 2.2 of ACE-FTS NO, NO2, HNO3, N2O5, and ClONO2 has previously been validated, and this study compares the most recent version (v3.5) of these five ACE-FTS products to spatially and temporally coincident measurements from other satellite instruments – GOMOS, HALOE, MAESTRO, MIPAS, MLS, OSIRIS, POAM III, SAGE III, SCIAMACHY, SMILES, and SMR. For each ACE-FTS measurement, a photochemical box model was used to simulate the diurnal variations of the NOy species and the ACE-FTS measurements were scaled to the local times of the coincident measurements. The comparisons for all five species show good agreement with correlative satellite measurements. For NO in the altitude range of 25–50 km, ACE-FTS typically agrees with correlative data to within −10 %. Instrument-averaged mean relative differences are approximately −10 % at 30–40 km for NO2, within ±7 % at 8–30 km for HNO3, better than −7 % at 21–34 km for local morning N2O5, and better than −8 % at 21–34 km for ClONO2. Where possible, the variations in the mean differences due to changes in the comparison local time and latitude are also discussed.

The Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) is a Fourier transform spectrometer that measured mid-infrared atmospheric limb emission spectra from July 2002 to April 2012 on board the polar-orbiting satellite ENVISAT. We have used MIPAS data to study the latitudinal variations of phosgene (COCl2 or carbonyl chloride) and, for the first time, its seasonal variation in the upper troposphere/lower stratosphere region (UTLS). Retrievals of phosgene were made using the 830–860 cm−1 region, corresponding to the ν5 bands of COCl2. Unfortunately, in that region, the ν4 band of CFC-11, which is much stronger than COCl2 ν5, hides the phosgene emission. In order to evaluate seasonality and latitudinal distribution of phosgene we have analysed all the measurements made by MIPAS on days 18 and 20 of each month of 2008 with the optimized retrieval model (ORM) recently upgraded with the multi-target retrieval technique and with the optimal estimation functionality to apply external constraints to the state vector. Average seasonal profiles of phosgene show an evident latitudinal variability with the largest values observed in the tropical regions (maximum ≈ 35 parts per trillion by volume (pptv) at about 300 hPa). In the midlatitude and polar regions, the volume mixing ratio (VMR) values do not exceed 30 pptv and the vertical distributions are less peaked. Our analysis highlights that COCl2 seasonal variability is fairly low, apart from the polar regions.

The primary goal of the FORUM mission is to measure the Earth's top-of-atmosphere emission spectrum in the 100 to 1600 cm-¹ spectral region covering the observational gap of the Far IR (100-667 cm-¹), which has never been observed from space in its entirety. This measurement will provide an improved understanding of the climate system by supplying, for the first time, most of the spectral features of the Far IR contribution to the Earth radiation budget, particularly focusing on the water vapour contribution related to the continuum absorption in the rotational band, cirrus cloud and ice/snow surface emissivity. This goal is achieved by measuring the spectrum with a nominal resolution of 0.3 cm-¹, and with an absolute calibration accuracy of 0.1 K, benchmarked against international standards. A precision of 0.4 mW/m² sr cm-¹ on the radiance will also allow the retrieval of the atmospheric state and cloud parameters with improved accuracy. A demonstration of the FORUM capabilities in improving the characterisation of the atmospheric radiative properties using the Far IR is shown by means of ground-based observations performed at high-altitude sites where the air is sufficiently transparent to sound the Far IR spectral features of the atmospheric emission. To this aim, two instruments are used: the REFIR-PAD (Radiation Explorer in the Far InfraRed - Prototype for Applications and Development) instrument, which has been deployed on the Antarctic Plateau, where it has been acquiring downwelling longwave radiation spectra continuously since 2012, and the FORUM prototype, which will be deployed at the Zugspitze summit at the end of 2018 - early 2019. Both instruments are Fourier transform spectrometers with an optical configuration of the interferometer similar to FORUM. They cover the Far IR spectral region down to 100cm-¹ and can be operated under all sky non-precipitating conditions. In this presentation, a review of the measurement requirements of the FORUM mission will be provided with a description of the measurement results obtained during the high-altitude Antarctic and Zugspitze campaigns.

MIPAS (Michelson Interferometer for Passive Atmospheric Sounding) is a Fourier transform spectrometer designed for measuring the earth atmospheric emission at limb in the 685-2410 cm-1 range. It flew onboard the polar orbit ENVISAT satellite for approximately 10 years, from June 2002 to April 2012, performing measurements during both day and night with an unprecedented spectral resolution from space (0.025 cm-1 in the first part of the mission and 0.0625 cm-1 in the second part). MIPAS measurements on ENVISAT represent a unique database for the study of the vertical distribution and time variation of the atmospheric composition on a global scale. While the focus of the instrument is the study of the chemistry and the physics of the stratosphere, also information on constituents in the upper troposphere has been derived. The ESA products include more than 20 minor atmospheric constituents [1]. The retrieval of the vertical profiles of atmospheric constituents is performed by fitting the observations to a full-physics model taking into account emission and absorption of all molecules. As a consequence the possibility of performing the retrievals is directly linked to the availability of the spectroscopic parameters and the quality of the retrieval depends on their quality. Indeed, in the estimation of the total error budget of the retrieved profiles the error due to the spectroscopic database is often one of the largest ones. The need of exploiting the information contained in the measurements of MIPAS, as well as of other instruments operating in the same spectral region like ACE-FTS, has driven studies for improving spectroscopic parameters in the middle infrared spectral region. MIPAS measurements provided not only the motivation, but also the guideline and the validation of the spectroscopic studies. Thanks to the their high spectral resolution and broadband coverage, the differences between observations and simulations of MIPAS measurements have been used to detect inconsistencies and validate subsequent improvements in the spectroscopic database (obtained with laboratory measurements and new calculations). In some cases MIPAS measurements have been used to convert the relative line intensities of a given spectral band to absolute intensities by comparing the retrieved profiles from MIPAS radiances from two different regions covering the two different spectral bands [2]. In this talk we will show how MIPAS measurements were used to validate the most recent improvements in the spectroscopic database of HNO3 and COCl2.

Open access. © Author(s) 2018. This work is distributed under the Creative Commons Attribution 4.0 License., Time series of stratospheric and lower mesospheric water vapour using 33 data sets from 15 different satellite instruments were compared in the framework of the second SPARC (Stratosphere-troposphere Processes And their Role in Climate) water vapour assessment (WAVAS-II). This comparison aimed to provide a comprehensive overview of the typical uncertainties in the observational database that can be considered in the future in observational and modelling studies, e.g addressing stratospheric water vapour trends. The time series comparisons are presented for the three latitude bands, the Antarctic (80°-70°S), the tropics (15°S-15°N) and the Northern Hemisphere mid-latitudes (50°-60°N) at four different altitudes (0.1, 3, 10 and 80hPa) covering the stratosphere and lower mesosphere. The combined temporal coverage of observations from the 15 satellite instruments allowed the consideration of the time period 1986-2014. In addition to the qualitative comparison of the time series, the agreement of the data sets is assessed quantitatively in the form of the spread (i.e. the difference between the maximum and minimum volume mixing ratios among the data sets), the (Pearson) correlation coefficient and the drift (i.e. linear changes of the difference between time series over time). Generally, good agreement between the time series was found in the middle stratosphere while larger differences were found in the lower mesosphere and near the tropopause. Concerning the latitude bands, the largest differences were found in the Antarctic while the best agreement was found for the tropics. From our assessment we find that most data sets can be considered in future observational and modelling studies, e.g. addressing stratospheric and lower mesospheric water vapour variability and trends, if data set specific characteristics (e.g. drift) and restrictions (e.g. temporal and spatial coverage) are taken into account. © Author(s) 2018., The Atmospheric Chemistry Experiment (ACE), also known as SCISAT, is a Canadian-led mission mainly supported by the Canadian Space Agency and the Natural Sciences and Engineering Research Council of Canada. We would like to thank the European Space Agency (ESA) for making the MIPAS level-1b data set available. MLS data were obtained from the NASA Goddard Earth Sciences and Information Center. Work at the Jet Propulsion Laboratory, California Institute of Technology, was done under contract with the National Aeronautics and Space Administration. SCIAMACHY spectral data have been provided by ESA. The work on the SCIAMACHY water vapour data products has been funded by DLR (German Aerospace Center) and the University of Bremen. The SCIAMACHY limb water vapour data set v3.01 is a result of the DFG (German Research Council) Research Unit "Stratospheric Change and its Role for Climate Prediction" (SHARP) and the ESA SPIN (ESA SPARC Initiative) project and were partly calculated using resources of the German HLRN (High-Performance Computer Center North). We would like to thank Mark Hervig for providing the SOFIE data and Takafumi Sugita for providing the ILAS-II data. We acknowledge the HALOE science team and the many members of the HALOE project for producing and characterising the high-quality HALOE data set. Further, we would like to thank Ellis Remsberg for valuable comments on the manuscript. Stefan Lossow was funded by the SHARP project under contract STI 210/9-2. We want to express our gratitude to SPARC and WCRP (World Climate Research Programme) for their guidance, sponsorship and support of the WAVAS-II programme. We acknowledge support by Deutsche Forschungsgemeinschaft and Open Access Publishing Fund of Karlsruhe Institute of Technology.

The primary instrument on the Greenhouse gases Observing SATellite (GOSAT) is the Thermal And Near infrared Sensor for carbon Observations (TANSO) Fourier Transform Spectrometer (FTS). TANSO-FTS uses three short-wave infrared (SWIR) bands to retrieve total columns of CO2 and CH4 along its optical line-of-sight, and one thermal infrared (TIR) channel to retrieve vertical profiles of CO2 and CH4 volume mixing ratios (VMRs) in the troposphere. We examine version 1 of the TANSO-FTS TIR CH4 product by comparing co-located CH4 VMR vertical profiles from two other remote sensing FTS systems: the Canadian Space Agency's Atmospheric Chemistry Experiment-FTS (ACE-FTS) on SCISAT (version 3.5), and the European Space Agency's Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) on Envisat (ESA ML2PP version 6 and IMK-IAA reduced-resolution version V5R_CH4_224/225), as well as 16 ground stations with the Network for the Detection of Atmospheric Composition Change (NDACC). This work follows an initial inter-comparison study over the Arctic, which incorporated a ground-based FTS at the Polar Environment Atmospheric Research Laboratory (PEARL) at Eureka, Canada, and focuses on tropospheric and lower-stratospheric measurements made at middle and tropical latitudes between 2009 to 2013 (mid 2012 for MIPAS). For comparison, vertical profiles from all instruments are interpolated onto a common pressure grid, and the ACE-FTS, MIPAS, and NDACC vertical profiles are smoothed using the TANSO-FTS averaging kernels. We present zonally-averaged mean CH4 differences between each instrument and TANSO-FTS with and without smoothing, examine their information content, sensitive altitude range, correlation, a priori dependence, and the variability within each data set. Partial columns are calculated from the VMR vertical profiles, and their correlations are examined. We find that the TANSO-FTS vertical profiles agree with the ACE-FTS and both MIPAS retrievals' vertical profiles within 4 % below 15 km when smoothing is applied to the profiles from instruments with finer vertical resolution, but that the relative differences can increase to on the order of 25 % when no smoothing is applied. Computed partial columns are tightly correlated for each pair of data sets. We investigated whether the difference between TANSO-FTS and other CH4 VMR data products varies with latitude. Our study reveals a small dependence of around 0.1 % per ten degrees latitude, with smaller differences over the equator, and greater differences towards the poles.

Atmospheric emissions of Carbon tetrachloride CCl4 are regulated by the Montreal Protocol due to its role as a strong ozone-depleting substance. The molecule has been the subject of recent increased interest as a consequence of the so called ``mystery of CCl4,'' the discrepancy between atmospheric observations and reported production and consumption. Surface measurements of CCl4 atmospheric concentrations have declined at a rate almost three times smaller than its lifetime-limited rate, suggesting persistent atmospheric emissions despite the ban. In this paper, we study CCl4 vertical and zonal distributions in the upper troposphere and lower stratosphere (including the photolytic loss region, 70–20 hPa), its trend, and its stratospheric lifetime using measurements from the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS), which operated onboard the ENVISAT satellite from 2002 to 2012. Specifically, we use the MIPAS data product generated with Version 7 of the Level 2 algorithm operated by the European Space Agency. The CCl4 zonal means show features typical of long-lived species of anthropogenic origin that are destroyed primarily in the stratosphere, with larger quantities in the troposphere and a monotonic decrease with increasing altitude in the stratosphere. In the troposphere, the largest concentrations are observed at the latitudes of major industrial countries (20/50°N). The good agreement we find between MIPAS CCl4 and independent measurements from other satellite and balloon-borne remote sounders proves the reliability of the MIPAS dataset. CCl4 trends are calculated as a function of both latitude and altitude. Negative trends are found at all latitudes in the upper-troposphere / lower-stratosphere region, apart from a region in the Southern mid-latitudes between 50 and 10 hPa where the trend is positive. At the lowest altitudes sounded by MIPAS, we find trends consistent with those determined on the basis of long-term ground-based measurements. For higher altitudes, the trend shows a pronounced asymmetry between Northern and Southern Hemispheres, and the magnitude of the decline rate increases with altitude. At 50 hPa the decline is about 30–35 %/decade, close to the lifetime-limited trend. We use a simplified model assuming tracer-tracer linear correlations to determine CCl4 lifetime in the lower stratosphere. The calculation provides a global average lifetime of 46(38–60) years considering CFC-11 as the reference tracer. This value is consistent with the most recent literature result of 44(36–58) years.

The MIPAS (Michelson Interferometer for Passive Atmospheric Sounding) instrument on the Envisat (Environmental satellite) satellite has provided vertical profiles of the atmospheric composition on a global scale for almost ten years. The MIPAS mission is divided in two phases: the full resolution phase, from 2002 to 2004, and the optimized resolution phase, from 2005 to 2012, which is characterized by a finer vertical and horizontal sampling attained through a reduction of the spectral resolution. While the description and characterization of the products of the ESA processor for the full resolution phase has been already described in previous papers, in this paper we focus on the performances of the latest version of the ESA (European Space Agency) processor, named ML2PP V6 (MIPAS Level 2 Prototype Processor), which has been used for reprocessing the entire mission. The ESA processor had to perform the operational near real time analysis of the observations and its products needed to be available for data assimilation. Therefore, it has been designed for fast, continuous and automated analysis of observations made in quite different atmospheric conditions and for a minimum use of external constraints in order to avoid biases in the products. The dense vertical sampling of the measurements adopted in the second phase of the MIPAS mission resulted in sampling intervals finer than the instantaneous field of view of the instrument. Together with the choice of a retrieval grid aligned with the vertical sampling of the measurements, this made ill-conditioned the retrieval problem of the MIPAS operational processor. This problem has been handled with minimal changes to the original retrieval approach but with significant improvements nonetheless. The Levenberg-Marquardt method, already present in the retrieval scheme for its capability to provide fast convergence for nonlinear problems, is now also exploited for the reduction of the ill-conditioning of the inversion. An expression specifically designed for the regularizing Levenberg-Marquardt method has been implemented for the computation of the covariance matrices and averaging kernels of the retrieved products. The regularization of the Levenberg-Marquardt method is controlled by the convergence criteria and is deliberately kept weak. The resulting oscillations of the retrieved profile are a posteriori damped by an innovative self-adapting Tikhonov regularization. The convergence criteria and the weakness of the self-adapting regularization ensure that minimum constraints are used and the best vertical resolution obtainable from the measurements is achieved in all atmospheric conditions. Random and systematic errors, as well as vertical and horizontal resolution are compared in the two phases of the mission for all products, namely: temperature, H2O, O3, HNO3, CH4, N2O, NO2, CFC-11, CFC-12, N2O5 and ClONO2. The use in the two phases of the mission of different optimized sets of spectral intervals ensures that, despite the different spectral resolutions, comparable performances are obtained in the whole MIPAS mission in terms of random and systematic errors, while the vertical resolution and the horizontal resolution are significantly better in the case of the optimized resolution measurements. © Author(s) 2013., This work has been performed under the ESA study >Support to MIPAS Level 2 product validation>, contract ESA-ESRIN no. 21719/08/I-OL. The authors are grateful to the Astrium team that developed the industrial prototype ML2PP using the ORM code as reference, to Thorsten Fehr and Rolf von Kulhmann for the coordination of the MIPAS Quality Working Group activities and to Michael Kiefer for the work done within the MIPAS Quality Working Group.

Water vapour (H2O) is one of the operationally retrieved key species of the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) instrument aboard the Environmental Satellite (ENVISAT) which was launched into its sun-synchronous orbit on 1 March 2002 and operated until April 2012. Within the MIPAS validation activities, independent observations from balloons, aircraft, satellites, and ground-based stations have been compared to European Space Agency (ESA) version 4.61 operational H2O data comprising the time period from July 2002 until March 2004 where MIPAS measured with full spectral resolution. No significant bias in the MIPAS H2O data is seen in the lower stratosphere (above the hygropause) between about 15 and 30 km. Differences of H2O quantities observed by MIPAS and the validation instruments are mostly well within the combined total errors in this altitude region. In the upper stratosphere (above about 30 km), a tendency towards a small positive bias (up to about 10%) is present in the MIPAS data when compared to its balloon-borne counterpart MIPAS-B, to the satellite instruments HALOE (Halogen Occultation Experiment) and ACE-FTS (Atmospheric Chemistry Experiment, Fourier Transform Spectrometer), and to the millimeter-wave airborne sensor AMSOS (Airborne Microwave Stratospheric Observing System). In the mesosphere the situation is unclear due to the occurrence of different biases when comparing HALOE and ACE-FTS data. Pronounced deviations between MIPAS and the correlative instruments occur in the lowermost stratosphere and upper troposphere, a region where retrievals of H2O are most challenging. Altogether it can be concluded that MIPAS H2O profiles yield valuable information on the vertical distribution of H2O in the stratosphere with an overall accuracy of about 10 to 30% and a precision of typically 5 to 15% – well within the predicted error budget, showing that these global and continuous data are very valuable for scientific studies. However, in the region around the tropopause retrieved MIPAS H2O profiles are less reliable, suffering from a number of obstacles such as retrieval boundary and cloud effects, sharp vertical discontinuities, and frequent horizontal gradients in both temperature and H2O volume mixing ratio (VMR). Some profiles are characterized by retrieval instabilities.

Peak stratospheric chlorofluorocarbon (CFC) and other ozone depleting substance (ODS) concentrations were reached in the mid- to late 1990s. Detection and attribution of the expected recovery of the stratospheric ozone layer in an atmosphere with reduced ODSs as well as efforts to understand the evolution of stratospheric ozone in the presence of increasing greenhouse gases are key current research topics. These require a critical examination of the ozone changes with an accurate knowledge of the spatial (geographical and vertical) and temporal ozone response. For such an examination, it is vital that the quality of the measurements used be as high as possible and measurement uncertainties well quantified. In preparation for the 2014 United Nations Environment Programme (UNEP)/World Meteorological Organization (WMO) Scientific Assessment of Ozone Depletion, the SPARC/IO3C/IGACO-O3/NDACC (SI2N) Initiative was designed to study and document changes in the global ozone profile distribution. This requires assessing long-term ozone profile data sets in regards to measurement stability and uncertainty characteristics. The ultimate goal is to establish suitability for estimating long-term ozone trends to contribute to ozone recovery studies. Some of the data sets have been improved as part of this initiative with updated versions now available. This summary presents an overview of stratospheric ozone profile measurement data sets (ground and satellite based) available for ozone recovery studies. Here we document measurement techniques, spatial and temporal coverage, vertical resolution, native units and measurement uncertainties. In addition, the latest data versions are briefly described (including data version updates as well as detailing multiple retrievals when available for a given satellite instrument). Archive location information for each data set is also given.

The Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) is a mid-infrared emission spectrometer which is part of the core payload of the Envisat satellite, launched by ESA in March 2002. It provides unique observations of the atmospheric spectral radiances in the 4.15 - 14.6 μm spectral interval with innovative limb scanning capabilities for the three dimensional observation of the atmospheric composition and processes. The species, the processes and events that have been studied with this instrument in its 10 years of operation are briefly reviewed. © 2012 IEEE.

This paper discusses assimilation experiments of methane (CH4) and nitrous oxide (N2O) profiles observed by the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS). Here we focus on data versions 6 and 7 retrieved by the ESA processor. These datasets have been assimilated by the Belgian Assimilation System for Chemical ObsErvations (BASCOE). The CH4 and N2O profiles can be noisy especially in the tropical lower stratosphere. Using the averaging kernels of the observations and a background error covariance matrix – the B matrix, which has been previously calibrated, allows the system to partly remedy this issue and provide assimilated fields that are more regular vertically. In general, there is a good agreement between the BASCOE analyses and independent observations demonstrating the general good quality of these two retrievals provided by MIPAS ESA. Nevertheless, this study also identifies two issues in these datasets. First, time-series of the observations show unexpected discontinuities, due to the calibration method used for the level-1 data. Second, the correlations between BASCOE analyses and independent observations are poor in the lower stratosphere, especially in the tropics, probably due to the presence of outliers in the assimilated data. In this region, we recommend using MIPAS CH4 and N2O observations with caution.

The ACE-FTS (Atmospheric Chemistry Experiment – Fourier Transform Spectrometer) instrument on the Canadian SCISAT satellite, which has been in operation for over 12 years, has the capability of deriving stratospheric profiles of many of the NOy (NO + NO2 + NO3 + 2 × N2O5 + HNO3 + HNO4 + ClONO2 + BrONO2) species. Version 2.2 of ACE-FTS NO, NO2, HNO3, N2O5, and ClONO2 have previously been validated, and this study compares the most recent version (v3.5) of these five ACE-FTS products to spatially and temporally coincident measurements from other satellite instruments–GOMOS, HALOE, MAESTRO, MIPAS, MLS, OSIRIS, POAM III, SAGE III, SCIAMACHY, SMILES, and SMR. For each ACE-FTS measurement, a photochemical box model was used to simulate the diurnal variations of the NOy species and the ACE-FTS measurements were scaled to the local times of the coincident measurements. The comparisons for all five species show good agreement with correlative satellite measurements. For NO in the altitude range of 25–50 km, the instrument-averaged mean relative differences are on the order of 0 to −10 %. They are approximately −10 % at 30–40 km for NO2, they are within ±7 % at 8–30 km for HNO3, they are better than −7% at 21–34 km for local morning N2O5, and better than −8 % at 21–34 km for ClONO2. Where possible, the variations in the mean differences due to changes in the comparison local time and latitude are also discussed.

Vertical profiles of NO2 and NO have been obtained from solar occultation measurements by the Atmospheric Chemistry Experiment (ACE), using an infrared Fourier Transform Spectrometer (ACE-FTS) and (for NO2) an ultraviolet-visible-near-infrared spectrometer, MAESTRO (Measurement of Aerosol Extinction in the Stratosphere and Troposphere Retrieved by Occultation). In this paper, the quality of the ACE-FTS version 2.2 NO2 and NO and the MAESTRO version 1.2 NO2 data are assessed using other solar occultation measurements (HALOE, SAGE II, SAGE III, POAM III, SCIAMACHY), stellar occultation measurements (GOMOS), limb measurements (MIPAS, OSIRIS), nadir measurements (SCIAMACHY), balloon-borne measurements (SPIRALE, SAOZ) and ground-based measurements (UV-VIS, FTIR). Time differences between the comparison measurements were reduced using either a tight coincidence criterion, or where possible, chemical box models. ACE-FTS NO2 and NO and the MAESTRO NO2 are generally consistent with the correlative data. The ACE-FTS and MAESTRO NO2 volume mixing ratio (VMR) profiles agree with the profiles from other satellite data sets to within about 20% between 25 and 40 km, with the exception of MIPAS ESA (for ACE-FTS) and SAGE II (for ACE-FTS (sunrise) and MAESTRO) and suggest a negative bias between 23 and 40 km of about 10%. MAESTRO reports larger VMR values than the ACE-FTS. In comparisons with HALOE, ACE-FTS NO VMRs typically (on average) agree to ±8% from 22 to 64 km and to +10% from 93 to 105 km, with maxima of 21% and 36%, respectively. Partial column comparisons for NO2 show that there is quite good agreement between the ACE instruments and the FTIRs, with a mean difference of +7.3% for ACE-FTS and +12.8% for MAESTRO.

The Atmospheric Chemistry Experiment (ACE), also known as SCISAT, was launched on 12 August 2003, carrying two instruments that measure vertical profiles of atmospheric constituents using the solar occultation technique. One of these instruments, the ACE Fourier Transform Spectrometer (ACE-FTS), is measuring volume mixing ratio (VMR) profiles of nitrous oxide (N 2 O) from the upper troposphere to the lower mesosphere at a vertical resolution of about 3–4 km. In this study, the quality of the ACE-FTS version 2.2 N 2 O data is assessed through comparisons with coincident measurements made by other satellite, balloon-borne, aircraft, and ground-based instruments. These consist of vertical profile comparisons with the SMR, MLS, and MIPAS satellite instruments, multiple aircraft flights of ASUR, and single balloon flights of SPIRALE and FIRS-2, and partial column comparisons with a network of ground-based Fourier Transform InfraRed spectrometers (FTIRs). Overall, the quality of the ACE-FTS version 2.2 N 2 O VMR profiles is good over the entire altitude range from 5 to 60 km. Between 6 and 30 km, the mean absolute differences for the satellite comparisons lie between -42 ppbv and +17 ppbv, with most within ±20 ppbv. This corresponds to relative deviations from the mean that are within ±15%, except for comparisons with MIPAS near 30 km, for which they are as large as 22.5%. Between 18 and 30 km, the mean absolute differences are generally within ±10 ppbv, again excluding the aircraft and balloon comparisons. From 30 to 60 km, the mean absolute differences are within ±4 ppbv, and are mostly between -2 and +1 ppbv. Given the small N 2 O VMR in this region, the relative deviations from the mean are therefore large at these altitudes, with most suggesting a negative bias in the ACE-FTS data between 30 and 50 km. In the comparisons with the FTIRs, the mean relative differences between the ACE-FTS and FTIR partial columns are within ±6.6% for eleven of the twelve contributing stations. This mean relative difference is negative at ten stations, suggesting a small negative bias in the ACE-FTS partial columns over the altitude regions compared. Excellent correlation ( R =0.964) is observed between the ACE-FTS and FTIR partial columns, with a slope of 1.01 and an intercept of -0.20 on the line fitted to the data.

The Atmospheric Chemistry Experiment (ACE) satellite was launched on 12 August 2003. Its two instruments measure vertical profiles of over 30 atmospheric trace gases by analyzing solar occultation spectra in the ultraviolet/visible and infrared wavelength regions. The reservoir gases HNO3, ClONO2, and N2O5 are three of the key species provided by the primary instrument, the ACE Fourier Transform Spectrometer (ACE-FTS). This paper describes the ACE-FTS version 2.2 data products, including the N2O5 update, for the three species and presents validation comparisons with available observations. We have compared volume mixing ratio (VMR) profiles of HNO3, ClONO2, and N2O5 with measurements by other satellite instruments (SMR, MLS, MIPAS), aircraft measurements (ASUR), and single balloon-flights (SPIRALE, FIRS-2). Partial columns of HNO3 and ClONO2 were also compared with measurements by ground-based Fourier Transform Infrared (FTIR) spectrometers. Overall the quality of the ACE-FTS v2.2 HNO3 VMR profiles is good from 18 to 35 km. For the statistical satellite comparisons, the mean absolute differences are generally within ±1 ppbv ±20%) from 18 to 35 km. For MIPAS and MLS comparisons only, mean relative differences lie within±10% between 10 and 36 km. ACE-FTS HNO3 partial columns (~15–30 km) show a slight negative bias of −1.3% relative to the ground-based FTIRs at latitudes ranging from 77.8° S–76.5° N. Good agreement between ACE-FTS ClONO2 and MIPAS, using the Institut für Meteorologie und Klimaforschung and Instituto de Astrofísica de Andalucía (IMK-IAA) data processor is seen. Mean absolute differences are typically within ±0.01 ppbv between 16 and 27 km and less than +0.09 ppbv between 27 and 34 km. The ClONO2 partial column comparisons show varying degrees of agreement, depending on the location and the quality of the FTIR measurements. Good agreement was found for the comparisons with the midlatitude Jungfraujoch partial columns for which the mean relative difference is 4.7%. ACE-FTS N2O5 has a low bias relative to MIPAS IMK-IAA, reaching −0.25 ppbv at the altitude of the N2O5 maximum (around 30 km). Mean absolute differences at lower altitudes (16–27 km) are typically −0.05 ppbv for MIPAS nighttime and ±0.02 ppbv for MIPAS daytime measurements.